Self-assembled molecule, perovskite solar cell, photovoltaic module, power generation device and power utilization device

Abstract

The invention relates to a self-assembly molecule, a perovskite solar cell, a photovoltaic module, a power generation device and a power utilization device. The perovskite solar cell comprises a first electrode, a functional layer, a perovskite light absorption layer and a second electrode which are stacked in the thickness direction of the perovskite solar cell, and the functional layer comprises self-assembly molecules. The self-assembly molecule comprises one or more of a structural formula as shown in a formula I1, a structural formula as shown in a formula I2, a structural formula as shown in a formula I3 and a structural formula as shown in a formula I4,

Description

Technical Field

[0001] This application relates to the field of solar cells, and more particularly to a self-assembled molecule, a perovskite solar cell, a photovoltaic module, a power generation device, and an electrical device. Background Technology

[0002] Perovskite solar cells are solar cells that use organometal halide perovskite materials as light-absorbing layers. They have excellent photoelectric properties and simple fabrication methods, bringing new possibilities and hope to photovoltaic power generation.

[0003] Currently, how to further improve the photoelectric conversion efficiency and device stability of perovskite solar cells is an urgent problem to be solved. Summary of the Invention

[0004] This application provides a self-assembled molecule, a perovskite solar cell, a photovoltaic module, a power generation device, and a power consumption device. The photoelectric conversion efficiency and device stability of the perovskite solar cell described in this application can be improved.

[0005] In a first aspect, embodiments of this application propose a perovskite solar cell. The perovskite solar cell includes a first electrode, a functional layer, a perovskite light-absorbing layer, and a second electrode stacked along the thickness direction of the perovskite solar cell. The functional layer includes self-assembled molecules, and the self-assembled molecules include one or more of the following structural formulas: Formula I1, Formula I2, Formula I3, and Formula I4.

[0006] The self-assembled molecule includes the structure shown in Formula I1.

[0007]

[0008] In formula I1, Ar1 represents a hole-extraction group with a cyclic atom number of C10 to C30;

[0009] D1 includes substituted or unsubstituted deoxyrheterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0010] E1 indicates an oxygen-containing group;

[0011] n1 represents the number of connection sites between D1 and Ar1, where n1 is any positive integer from 1 to 8;

[0012] The self-assembled molecule includes the structural formula shown in Formula I2.

[0013]

[0014] In formula I2, Ar2 represents a hole-extraction group with a cyclic atom number of C10 to C30;

[0015] D 21 and D 22 One of them includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; D 21 and D 22 The other includes a substituted or unsubstituted dehydroaromatic heterocyclic group, or a substituted or unsubstituted alkenyl group;

[0016] E2 indicates an oxygen-containing group;

[0017] n2 represents D 21 The number of connection sites with Ar2, where n2 is any positive integer from 1 to 8;

[0018] The self-assembled molecule includes the structure shown in Formula I3.

[0019]

[0020] In formula I3, Ar3 represents a hole-extraction group with a cyclic atom number of C31 to C60;

[0021] D3 includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0022] E3 indicates an oxygen-containing group;

[0023] n3 represents the number of connection sites between D3 and Ar3, where n3 is any positive integer from 2 to 8;

[0024] The self-assembled molecule includes the structure shown in Formula I4.

[0025]

[0026] In formula I4, Ar4 represents a hole-extraction group with a cyclic atom number of C31 to C60;

[0027] D 41 and D 42 Each independently includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0028] n4 represents D 41 The number of connection sites with Ar4, where n4 is any positive integer from 2 to 8;

[0029] E4 represents an oxygen-containing group.

[0030] Therefore, the self-assembled molecule according to the embodiments of this application includes a hole extraction group, a conjugated group, and an oxygen-containing group. The hole extraction group is connected to the oxygen-containing group through the conjugated group, which can improve the overall conjugability of the molecule, reduce the migration energy barrier of charge carriers in the molecule, and improve the conductivity of the self-assembled molecule. Furthermore, since the electron cloud is distributed throughout the molecule, it can reduce the risk of molecular instability caused by excessively high local energy and improve the intrinsic stability of the self-assembled molecule.

[0031] In some embodiments, the hole-extraction group having a cyclic number of C10 to C30 includes substituted or unsubstituted aniline groups having a cyclic number of C10 to C30, substituted or unsubstituted acridine groups having a cyclic number of C10 to C30, and when the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl-thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0032] When self-assembled molecules are applied to perovskite solar cells, the aforementioned hole-extraction groups are beneficial for hole extraction and transport. Based on the aforementioned hole-extraction groups, conjugated groups are beneficial for improving the overall conjugability of the molecule, reducing the migration energy barrier of charge carriers within the molecule, and improving the conductivity of the self-assembled molecules.

[0033] In some embodiments, the substituted or unsubstituted aniline group having a cyclic number of C10 to C30 includes the structure shown in Formula A1.

[0034]

[0035] In formula A1,

[0036] M 11 and M 12 Each group independently comprises an aromatic group, either substituted or unsubstituted, having a cyclic atom number of C5 to C15;

[0037] M 13 Including substituted or unsubstituted aromatic groups with a cyclic atom number of C5 to C15;

[0038] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0039] When self-assembled molecules are applied to perovskite solar cells, aniline groups, especially triphenylamine groups, act as hole extraction groups. The conjugated groups bring the dipole moment closer to the perovskite material, which is beneficial for hole extraction and transport.

[0040] In some embodiments, the substituted or unsubstituted aniline group having a cyclic number of C10 to C30 includes substituted or unsubstituted formula A. 1-1 The structure shown is used for substituted or unsubstituted formula A. 1-5 One or more of the structures shown,

[0041]

[0042] In the formula, * represents the connection site between the hole extraction group and D1, or * represents the connection site between the hole extraction group and D1. 21 Connection sites;

[0043] s1, s2, s3 and s4 are any integers from 0 to 3, and in the same structure, s1, s2, s3 and s4 are not all 0 at the same time.

[0044] In some embodiments, the substituted or unsubstituted acridine group having a cyclic number of C10 to C30 includes the structure shown in Formula A2.

[0045]

[0046] In formula A2,

[0047] M 21 Including single bonds, substituted or unsubstituted cyclic aromatic groups with a number of C6 to C15 atoms, or substituted or unsubstituted cyclic heterocyclic groups with a number of C5 to C15 atoms;

[0048] M 22 and M 23 Each group independently includes substituted or unsubstituted aromatic groups having a cyclic number of C6 to C15 or substituted or unsubstituted aromatic heterocyclic groups having a cyclic number of C6 to C15; when the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl-thio groups, oxygen-containing substituted groups or C1 to C5 alkyl groups.

[0049] In some embodiments, the substituted or unsubstituted acridine group having a cyclic atom number of C10 to C30 includes substituted or unsubstituted formula A. 2-1 The structure shown is used for substituted or unsubstituted formula A. 2-3 One or more of the structures shown,

[0050]

[0051] In the formula, * represents the connection site between the hole extraction group and D1, or * represents the connection site between the hole extraction group and D1. 21 Connection sites;

[0052] s1 and s2 are any integers from 0 to 3, and in the same structure, s1 and s2 are not both 0.

[0053] In some embodiments, the hole-extracting group having a cyclic number of C31 to C60 includes a substituted or unsubstituted carbazole group having a cyclic number of C31 to C60. When the above group is substituted, the substituted group includes one or more of amine groups, halogen groups, alkyl-sulfur groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups.

[0054] When self-assembled molecules are applied to perovskite solar cells, the aforementioned hole-extraction groups are beneficial for hole extraction and transport. Based on the aforementioned hole-extraction groups, conjugated groups are beneficial for improving the overall conjugability of the molecule, reducing the migration energy barrier of charge carriers within the molecule, and improving the conductivity of the self-assembled molecules.

[0055] In some embodiments, the substituted or unsubstituted carbazole group with a cyclic number of C31 to C60 includes the structure shown in Formula B1.

[0056]

[0057] In equation B1,

[0058] S 20 Including single bonds, substituted or unsubstituted cyclic aromatic groups with a number of C6 to C30 atoms, or substituted or unsubstituted cyclic heterocyclic groups with a number of C5 to C30 atoms;

[0059] S 21 and S 22 Each independently includes substituted or unsubstituted aromatic groups with a cyclic number of C6 to C30 or substituted or unsubstituted nitrogen-containing aromatic heterocyclic groups with a cyclic number of C6 to C30;

[0060] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0061] In some embodiments, the substituted or unsubstituted carbazole group having a cyclic number of C31 to C60 includes substituted or unsubstituted formula B. 1-1 The structure shown is for substituted or unsubstituted formula B. 1-6 One or more of the structures shown,

[0062]

[0063]

[0064] In the formula, * represents the connection site between the hole extraction group and D3, or * represents the connection site between the hole extraction group and D3. 41 Connection sites;

[0065] s1, s2, s3, s4, s5 and s6 are any integers from 0 to 3, and in the same structure, s1, s2, s3, s4, s5 and s6 are not all 0 at the same time.

[0066] In some embodiments, D1 includes substituted or unsubstituted aromatic heterocyclic groups, which are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0067] In some implementations, D 21 and D 22 One of them includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; D 21 and D 22 Another component includes substituted or unsubstituted deoxyrheterocyclic groups. These groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0068] In some embodiments, D3 includes substituted or unsubstituted aromatic hydrocarbon groups or substituted or unsubstituted aromatic heterocyclic groups. These groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0069] In some implementations, D 41 and D 42 Each group independently comprises either a substituted or unsubstituted aromatic hydrocarbon group or a substituted or unsubstituted aromatic heterocyclic group. These groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0070] In some implementations, D 21 D 22 D3, D 41 and D 42 Each component independently comprises a substituted or unsubstituted aromatic hydrocarbon group, wherein the substituted or unsubstituted aromatic hydrocarbon group includes a substituted or unsubstituted aromatic hydrocarbon group having a cyclic atom number of C6 to C15. These groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0071] In some embodiments, the substituted or unsubstituted aromatic hydrocarbon group having a cyclic number of C6 to C15 includes substituted or unsubstituted groups of formula G. 1-1 The structure shown is used for substituted or unsubstituted formula G. 1-3 One or more of the structures shown,

[0072]

[0073] In the formula, * represents D 21 D3, D 41 One of them is the connection site with the hole extraction group;

[0074] # indicates D 22 D3, D 42 One of them is the connection site with the oxygen-containing group.

[0075] In some implementations, D1, D 21 D 22 D3, D 41 and D 42 Each of the components independently comprises a substituted or unsubstituted aromatic heterocyclic group, wherein the substituted or unsubstituted aromatic heterocyclic group comprises an aromatic heterocyclic group having a cyclic atom number of C5 to C15, and the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 further include one or more atoms selected from nitrogen, oxygen, and sulfur.

[0076] In some embodiments, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 include nitrogen atoms, and the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 includes substituted or unsubstituted compounds of formula G. 2-1 The structure shown is used for substituted or unsubstituted formula G. 2-9 One or more of the structures shown,

[0077]

[0078] In the formula, * represents D1, D 21 D3, D 41 One of them is the connection site with the hole extraction group;

[0079] # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group.

[0080] In some embodiments, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 include oxygen atoms, and the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 includes substituted or unsubstituted compounds of formula G. 3-1 The structure shown is used for substituted or unsubstituted formula G. 3-3 One or more of the structures shown,

[0081]

[0082] In the formula, * represents D1, D21 D3, D 41 One of them is the connection site with the hole extraction group;

[0083] # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group.

[0084] In some embodiments, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 include sulfur atoms, and the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 includes substituted or unsubstituted compounds of formula G. 4-1 The structure shown is used for substituted or unsubstituted formula G. 4-3 One or more of the structures shown,

[0085]

[0086] In the formula, * represents D1, D 21 D3, D 41 One of them is the connection site with the hole extraction group;

[0087] # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group.

[0088] In some embodiments, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 include multiple atoms selected from nitrogen, oxygen, and sulfur, and the substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 includes substituted or unsubstituted compounds of formula G. 5-1 The structure shown is used for substituted or unsubstituted formula G. 5-7 One or more of the structures shown,

[0089]

[0090] In the formula,

[0091] * indicates D1, D 21 D3, D 41 One of them is the connection site with the hole extraction group;

[0092] # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group.

[0093] In some implementations, D1, D 21 D 22 D3, D41 and D 42 Each group independently comprises substituted or unsubstituted alkenyl groups, including substituted or unsubstituted C2 to C6 chain alkenyl groups, or substituted or unsubstituted cyclic alkenyl groups having a cyclic number of C5 to C15 atoms. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups.

[0094] In some embodiments, the substituted or unsubstituted C2 to C6 chain alkenyl groups include vinylidene, propenylidene, or buteneide.

[0095] In some embodiments, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group. One of the hole transport layer and the first electrode has an anchoring effect with the oxygen-containing group, which can enhance the binding force between the self-assembled molecules and the hole transport layer, thereby improving the stability of the device.

[0096] In some embodiments, the oxygen-containing group includes one or more of a carboxylic acid group, a phosphate group, a borate group, a carboxylate group, a phosphate group, or a borate group.

[0097] In some embodiments, the self-assembled molecule includes one or more compounds from Formula I1-1 to Formula I4-2.

[0098]

[0099]

[0100]

[0101] In some embodiments, the functional layer is disposed on the first electrode and in contact with at least a portion of the surface of the first electrode. The functional layer can effectively extract and transport holes, thereby improving the photoelectric conversion efficiency of the perovskite solar cell.

[0102] In some embodiments, the thickness of the functional layer is between 1 nm and 30 nm. When the thickness of the functional layer is within this range, holes can be effectively transported, improving the photoelectric conversion efficiency of the device.

[0103] In some embodiments, the perovskite solar cell further includes a hole transport layer, with the functional layer located between the hole transport layer and the perovskite light-absorbing layer. The functional layer effectively passivates defects in the perovskite light-absorbing layer, further improving the device's photoelectric conversion efficiency.

[0104] In some embodiments, the thickness of the functional layer is from 0.1 nm to 20 nm. When the thickness of the functional layer is within this range, defects in the perovskite light-absorbing layer can be effectively passivated, further improving the photoelectric conversion efficiency of the device.

[0105] In some embodiments, the hole transport layer includes a hole transport material, which includes a hole transport organic compound, such as poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], poly(3,4-ethylenedioxythiophene)-polystyrene sulfonic acid, 2,2',7,7'-tetratetra[N,N-di(4-methoxyphenyl)amino]-9,9'-spirodifluorene, poly-3-hexylthiophene, or methoxytriphenylamine. The hole transport layer comprises one or more of the following: fluoroformamidinium, triphenylamine with a triphenylene core, 3,4-ethylenedioxythiophene-methoxytriphenylamine, N-4-anilinecarbazole-spirobisfluorene, polythiophene, phosphonic acid monomers, carboxylic acid monomers, carbazole monomers, sulfonic acid monomers, triphenylamine monomers, and aromatic monomers; and / or the hole transport layer comprises hole transport inorganic materials, wherein the hole transport inorganic materials include one or more of metal oxides, cuprous iodide, and cuprous thiocyanate. Therefore, in the embodiments of this application, the above-mentioned hole transport materials possess excellent hole extraction and transport capabilities, which is beneficial for improving the photoelectric conversion efficiency of perovskite solar cells.

[0106] In some embodiments, the perovskite light-absorbing layer comprises a perovskite material, which includes one or more compounds with the molecular formula ABX3 or M2CDN6, wherein A and M each independently comprise Li. + Na + K + 、Rb + Cs + B includes one or more of the following cations: methylamine cation, ethylamine cation, propylamine cation, butylamine cation, pentamine cation, hexamine cation, formamidin cation, or imidazole cation; B includes Ca. 2+ 、Sr 2+ Cd 2+ Cu 2+ Ni 2+ Mn 2+ Fe 2+ Co 2+ Pd 2+ 、Ge 2+ Sn 2+ Pb 2+ Sn 2+ Yb 2+ and Eu 2+ One or more cations from the group consisting of X and N; X and N each independently include F-, Cl-, Br-, etc.- Or one or more of I-; C includes Cs + Ag + K + Or Ru + One or more of the following; D includes Bi 3+ Ni 3+ Fe 3+ Sb 3+ In 3+ or Cu 3+ One or more of them.

[0107] In some embodiments, the perovskite solar cell further includes an electron transport layer located between the perovskite light-absorbing layer and the second electrode. The electron transport layer enhances electron transport capability, thereby improving the photoelectric conversion efficiency of the perovskite solar cell.

[0108] Secondly, this application also proposes a photovoltaic module, which includes one or more perovskite solar cells as described in any embodiment of the first aspect of this application.

[0109] Thirdly, this application also proposes a power generation device, which includes a photovoltaic module as described in any embodiment of the second aspect of this application.

[0110] Fourthly, this application also proposes an electrical device comprising a photovoltaic module as described in any embodiment of the second aspect of this application.

[0111] Fifthly, this application also proposes a self-assembly molecule, said self-assembly molecule comprising the structural formula shown in Formula I1,

[0112]

[0113] In formula I1, Ar1 represents a hole-extraction group with a cyclic atom number of C10 to C30;

[0114] D1 includes substituted or unsubstituted deoxyrheterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0115] E1 indicates an oxygen-containing group;

[0116] n1 represents the number of connection sites between D1 and Ar1, where n1 is any positive integer from 1 to 8.

[0117] Sixthly, this application also proposes a self-assembly molecule, said self-assembly molecule comprising the structural formula shown in Formula I2.

[0118]

[0119] In formula I2, Ar2 represents a hole-extraction group with a cyclic atom number of C10 to C30;

[0120] D 21 and D 22 One of them includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; D 21 and D 22 The other includes substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0121] E2 indicates an oxygen-containing group;

[0122] n2 represents D 21 The number of connection sites with Ar2, n2 is any positive integer from 1 to 8.

[0123] Seventhly, this application also proposes a self-assembly molecule, said self-assembly molecule comprising the structural formula shown in Formula I3.

[0124]

[0125] In formula I3, Ar3 represents a hole-extraction group with a cyclic atom number of C31 to C60;

[0126] D3 includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0127] E3 indicates an oxygen-containing group;

[0128] n3 represents the number of connection sites between D3 and Ar3, where n3 is any positive integer from 2 to 8.

[0129] Eighthly, this application also proposes a self-assembly molecule, said self-assembly molecule comprising the structural formula shown in Formula I4.

[0130]

[0131] In formula I4, Ar4 represents a hole-extraction group with a cyclic atom number of C31 to C60;

[0132] D 41 and D 42 Each independently includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0133] n4 represents D 41 The number of connection sites with Ar4, where n4 is any positive integer from 2 to 8;

[0134] E4 represents an oxygen-containing group. Attached Figure Description

[0135] To more clearly illustrate the technical solutions of the embodiments of this application, the drawings used in the embodiments of this application will be briefly introduced below. Obviously, the drawings described below are only some embodiments of this application. For those skilled in the art, other drawings can be obtained based on the drawings without creative effort.

[0136] Figure 1 This is a schematic diagram of the structure of a perovskite solar cell provided in some embodiments of this application;

[0137] Figure 2 These are schematic diagrams of the structure of perovskite solar cells provided in other embodiments of this application;

[0138] Figure 3 This is a schematic diagram of the structure of a perovskite solar cell provided in some embodiments of this application;

[0139] Figure 4 This is a schematic diagram of the structure of a perovskite solar cell provided in some embodiments of this application;

[0140] Figure 5 This is a schematic diagram of the structure of a perovskite solar cell provided in some embodiments of this application;

[0141] Figure 6 This is a schematic diagram of the structure of a perovskite solar cell provided in some embodiments of this application;

[0142] Figure 7 These are schematic diagrams of the structure of photovoltaic modules provided in some embodiments of this application;

[0143] Figure 8 These are schematic diagrams of the electrical devices provided in some embodiments of this application;

[0144] Figure 9 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound shown in Formula I1-2 of this application;

[0145] Figure 10 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I1-2 of this application;

[0146] Figure 11 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound shown in Formula I1-3 of this application;

[0147] Figure 12 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I1-3 of this application;

[0148] Figure 13This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound represented by formula I2-1 in this application;

[0149] Figure 14 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound represented by formula I2-1 in this application;

[0150] Figure 15 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound shown in Formula I2-3 of this application;

[0151] Figure 16 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I2-3 of this application;

[0152] Figure 17 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound shown in Formula I3-2 of this application;

[0153] Figure 18 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I3-2 of this application;

[0154] Figure 19 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound represented by formula I3-1 in this application;

[0155] Figure 20 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I3-1 of this application;

[0156] Figure 21 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound represented by formula I4-1 in this application;

[0157] Figure 22 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I4-1 of this application;

[0158] Figure 23 This is a schematic diagram of the nuclear magnetic resonance spectrum of the compound shown in Formula I4-2 of this application;

[0159] Figure 24 This is a grayscale image of the nuclear magnetic resonance spectrum of the compound shown in Formula I4-2 of this application;

[0160] The accompanying drawings are not necessarily drawn to scale.

[0161] The following are the labeling elements in the figure:

[0162] M, thickness direction;

[0163] 10. Perovskite solar cells;

[0164] 11. First electrode;

[0165] 12. Functional layer;

[0166] 13. Hole transport layer;

[0167] 14. Perovskite light-absorbing layer;

[0168] 15. Electron transport layer;

[0169] 16. Second electrode;

[0170] 1. Photovoltaic modules;

[0171] 2. Electrical appliances. Detailed Implementation

[0172] The following detailed description, with appropriate reference to the accompanying drawings, specifically discloses embodiments of the self-assembled molecules, perovskite solar cells, photovoltaic modules, power generation devices, and power consumption devices of this application. However, unnecessary detailed descriptions may be omitted. For example, detailed descriptions of well-known matters and repetitive descriptions of practically identical structures may be omitted. This is to avoid unnecessarily lengthy descriptions and to facilitate understanding by those skilled in the art. Furthermore, the accompanying drawings and the following description are provided to enable those skilled in the art to fully understand this application and are not intended to limit the subject matter of the claims.

[0173] The "range" disclosed in this application is defined by a lower limit and an upper limit. A given range is defined by selecting a lower limit and an upper limit, which define the boundaries of the particular range. Ranges defined in this way can include or exclude endpoints and can be arbitrarily combined; that is, any lower limit can be combined with any upper limit to form a range. For example, if ranges of 60 to 120 and 80 to 110 are listed for a specific parameter, it is also expected that ranges of 60 to 110 and 80 to 120 are also included. Furthermore, if minimum range values ​​of 1 and 2 are listed, and if maximum range values ​​of 3, 4, and 5 are listed, then the following ranges are all expected: 1 to 3, 1 to 4, 1 to 5, 2 to 3, 2 to 4, and 2 to 5. In this application, unless otherwise stated, the numerical range "a to b" represents a shortened representation of any combination of real numbers between a and b, where a and b are real numbers. For example, the numerical range "0 to 5" means that all real numbers between "0 and 5" have been listed in this article; "0 to 5" is just a shortened representation of these numerical combinations. In addition, when a parameter is stated as an integer ≥ 2, it is equivalent to disclosing that the parameter is, for example, an integer 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, etc.

[0174] Unless otherwise specified, all embodiments and optional embodiments of this application can be combined to form new technical solutions.

[0175] Unless otherwise specified, all technical features and optional technical features of this application may be combined to form new technical solutions.

[0176] Unless otherwise specified, all steps of this application may be performed sequentially or randomly, preferably sequentially. For example, if the method includes steps (a) and (b), it means that the method may include steps (a) and (b) performed sequentially, or it may include steps (b) and (a) performed sequentially. For example, if the method may also include step (c), it means that step (c) may be added to the method in any order. For example, the method may include steps (a), (b), and (c), or it may include steps (a), (c), and (b), or it may include steps (c), (a), and (b), etc.

[0177] In this application, "multiple" means two or more (including two).

[0178] Perovskite solar cells convert solar energy into electrical energy. Their operation mainly includes: exciton generation and separation, free carrier transport, carrier collection, and current generation. Specifically, in a perovskite solar cell, sunlight is absorbed by the perovskite light-absorbing layer, which absorbs photons and generates excitons. Due to the low Coulomb force binding of the perovskite layer, the excitons subsequently separate into free electrons and holes. These separated free carriers transport within the perovskite layer, and the electrons and holes are collected by electrodes. When connected to an external load, they form a current.

[0179] To improve the efficiency of carrier extraction and transport, a hole transport layer can be set between the electrode and the perovskite light-absorbing layer. However, side reactions may occur between the perovskite light-absorbing layer and the hole transport layer, such as nickel oxide, for example, trivalent nickel can cause the decomposition of the perovskite material. In related technologies, passivation materials are usually used for passivation. However, the intrinsic stability of the above-mentioned passivation materials is poor, which weakens the passivation effect and may deteriorate the stability and photoelectric conversion efficiency of the device.

[0180] Therefore, this application also provides self-assembled monolayers (SAMs). These SAMs can spontaneously arrange and combine in an orderly manner through non-covalent intermolecular interactions (such as hydrogen bonds and van der Waals forces) to form molecular aggregates with specific structures and functions. The SAMs of this application include hole-extraction groups, which can effectively extract and transport holes. Furthermore, the SAMs also include conjugated groups, which distribute the electron cloud throughout the molecule, improving its conductivity and intrinsic stability. When applied to perovskite solar cells, this improves device stability and photoelectric conversion efficiency.

[0181] Self-assembled molecules

[0182] In a first aspect, embodiments of this application propose a self-assembling molecule.

[0183] The self-assembled molecule includes the structure shown in Formula I1.

[0184]

[0185] In formula I1, Ar1 represents a hole-extraction group with a cyclic atom number of C10 to C30;

[0186] D1 includes substituted or unsubstituted deoxyrheterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0187] E1 indicates an oxygen-containing group;

[0188] n1 represents the number of connection sites between D1 and Ar1, where n1 is any positive integer from 1 to 8.

[0189] The groups included in D1 are conjugated groups, which makes the self-assembled molecule include hole-extracting groups, conjugated groups, and oxygen-containing groups. The hole-extracting groups are connected to the oxygen-containing groups through the conjugated groups, which can improve the overall conjugability of the molecule, reduce the migration energy barrier of charge carriers in the molecule, and improve the conductivity of the self-assembled molecule. Furthermore, since the electron cloud is distributed throughout the molecule, it can reduce the risk of molecular instability caused by excessively high local energy, and improve the intrinsic stability of the self-assembled molecule.

[0190] In the embodiments of this application, a subgroup can be understood as a group that has lost two hydrogen atoms.

[0191] For example, alkylene is an alkane group that has lost two hydrogen atoms in an alkane compound, while alkyl is an alkane group that has lost one hydrogen atom.

[0192] For example, a heteroalkylene group is a heteroalkane group that has lost two hydrogen atoms, while a heteroalkyl group is a heteroalkane group that has lost one hydrogen atom. Heteroalkane can include alkane compounds containing at least one heteroatom of O, S, N, or P, such as ethers and thioethers.

[0193] For example, a dehydroaromatic group is an aromatic group formed by the loss of two hydrogen atoms in an aromatic compound, while an aromatic group is an aromatic group that has lost one hydrogen atom. Aromatic compounds refer to compounds with aromatic properties, such as aromatic hydrocarbons and aromatic heterocyclic compounds. Aromatic hydrocarbons include compounds such as benzene, biphenyl, and fluorene; aromatic heterocyclic compounds include compounds such as carbazole, thiophene, furan, or benzothiophene.

[0194] For example, a subheterocyclic group is a heterocyclic group in a heterocyclic compound that has lost two hydrogen atoms, while a heterocyclic group is a heterocyclic group that has lost one hydrogen atom. Heterocyclic compounds can include heterocyclic compounds containing at least one heteroatom from O, S, N, and P, such as ethylene oxide, pentane oxide, and phosphonopentane.

[0195] For example, an alkenyl group is an olefinic group that has lost two hydrogen atoms, while an alkenyl group is an olefinic group that has lost one hydrogen atom.

[0196] n1 is any positive integer from 1 to 8. n1 can be 1 or greater than or equal to 2, such as 2, 3, 4, 5, 6, 7 or 8.

[0197] When n1 is 1, one hydrogen atom in the hole extraction group is replaced by a conjugated group, and the structural formula of the self-assembled molecule is as follows:

[0198]

[0199] When n1 is greater than or equal to 2, at least two hydrogen atoms in the hole extraction group are replaced by conjugated groups. Taking n1 as 3 as an example, the structural formula of the self-assembled molecule is as follows:

[0200]

[0201] [Hole Extraction Group]

[0202] In some embodiments, the hole-extraction group having a cyclic number of C10 to C30 includes substituted or unsubstituted aniline groups having a cyclic number of C10 to C30, and substituted or unsubstituted acridine groups having a cyclic number of C10 to C30. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl-thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups, and the number of carbon atoms in the substituted groups can be 1 to 5.

[0203] Optionally, the oxygen-containing substituents include one or more of the following: alkoxy group, amide group, carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0204] In some embodiments, the hole-extracting group having a cyclic atom number of C10 to C30 includes substituted or unsubstituted aniline groups having a cyclic atom number of C10 to C30.

[0205] When self-assembled molecules are applied to perovskite solar cells, aniline groups, especially triphenylamine groups, act as hole-extraction groups, which are beneficial for hole extraction and transport. Building upon these hole-extraction groups, conjugated groups enhance the overall conjugability of the molecule, lower the migration barrier for intramolecular charge carriers, and improve the conductivity of the self-assembled molecule.

[0206] Optionally, the substituted or unsubstituted aniline group with a cyclic number of C10 to C30 includes the structure shown in Formula A1.

[0207]

[0208] In formula A1,

[0209] M 11 and M 12 Each group independently comprises an aromatic group, either substituted or unsubstituted, having a cyclic atom number of C5 to C15;

[0210] M 13 Including substituted or unsubstituted aromatic groups with a cyclic atom number of C5 to C15;

[0211] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0212] For example, the substituted or unsubstituted aniline group having a cyclic number of C10 to C30 includes substituted or unsubstituted formula A. 1-1 The structure shown is used for substituted or unsubstituted formula A. 1-5 One or more of the structures shown,

[0213]

[0214] In the formula,

[0215] * indicates the connection site between the hole extraction group and the conjugated group.

[0216] s1, s2, s3, and s4 are any integers from 0 to 3. In the same structure, s1, s2, s3, and s4 are not all 0 at the same time. This can be understood as at least one of s1, s2, s3, and s4 being non-zero. For example, if s1 to s3 are 0, then s4 is a positive integer. Of course, at least two of s1, s2, s3, and s4 can be non-zero, or all of s1, s2, s3, and s4 can be non-zero and all of them can be positive integers.

[0217] The connection site between the hole-extracting group and the conjugated group can be at any position; in other words, any carbon atom of the benzene ring in the aniline-based hole-extracting group can be connected to the conjugated group.

[0218] For example, the substituted or unsubstituted aniline groups with a cyclic number of C10 to C30 include substituted or unsubstituted formula A. 1-11 The structure shown is used for substituted or unsubstituted formula A. 1-17 One or more of the structures shown,

[0219]

[0220] The above structure may or may not be replaced. In the case of replacement, for example, formula A is replaced. 1-5 The structure shown includes one or more of the following structural formulas:

[0221]

[0222] Ar1, Ar2, Ar3, and Ar4 each independently represent a hydrogen atom or a substituent group, and at least one of Ar1, Ar2, Ar3, and Ar4 is a substituent group. In other words, when Ar1, Ar2, Ar3, and Ar4 are each independently non-hydrogen atoms, Ar1, Ar2, Ar3, and Ar4 each independently substitute for any hydrogen atom on an aromatic or dearomatic ring. For example, the substituent group includes one or more of amine groups, halogen groups, alkyl-thionyl groups, oxygen-containing substituent groups, or alkyl groups.

[0223] For example, Ar1, Ar3, and Ar4 are fluorine atoms, Ar2 is a hydrogen atom, and the substitution formula A 1-5 The structure shown includes one or more of the following structural formulas:

[0224]

[0225] In some embodiments, the hole-extracting group includes acridine-like groups with substituted or unsubstituted cyclic atoms having a number of C10 to C30. When the self-assembled molecule is applied to perovskite solar cells, the aforementioned hole-extracting group facilitates hole extraction and transport. Based on the aforementioned hole-extracting group, the conjugated group helps to enhance the overall conjugability of the molecule, lower the migration energy barrier of intramolecular charge carriers, and improve the conductivity of the self-assembled molecule.

[0226] Optionally, the substituted or unsubstituted acridine group with a cyclic number of C10 to C30 includes the structure shown in Formula A2.

[0227]

[0228] In formula A2,

[0229] M 21Including single bonds, substituted or unsubstituted cyclic aromatic groups with a number of C6 to C15 atoms, or substituted or unsubstituted cyclic heterocyclic groups with a number of C5 to C15 atoms;

[0230] M 22 and M 23 Each independently includes substituted or unsubstituted aromatic groups with a cyclic number of C6 to C15 or substituted or unsubstituted aromatic heterocyclic groups with a cyclic number of C6 to C15;

[0231] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0232] In M 21 In the case of a single bond, it can be understood that the carbon atom at that location is directly connected to the conjugated group.

[0233] For example, the substituted or unsubstituted acridine group having a cyclic atom number of C10 to C30 includes substituted or unsubstituted formula A. 2-1 The structure shown is used for substituted or unsubstituted formula A. 2-3 One or more of the structures shown,

[0234]

[0235] In the formula,

[0236] * indicates the connection site between the hole extraction group and the conjugated group;

[0237] s1 and s2 are any integers from 0 to 3, and in the same structure, s1 and s2 are not both 0.

[0238] Optionally, the substituted or unsubstituted acridine group comprises a substituted or unsubstituted formula A. 2-11 The structure shown is used for substituted or unsubstituted formula A. 2-13 One or more of the structures shown,

[0239]

[0240] In the formula, * represents the connection site between the hole extraction group and the conjugated group.

[0241] The above structure may or may not be replaced. In the case of replacement, for example, formula A is replaced. 2-1 The structure shown includes one or more of the following structural formulas:

[0242]

[0243] Ar1, Ar2, and Ar3 each independently represent a hydrogen atom or a substituent group, and at least one of Ar1, Ar2, and Ar3 is a substituent group. In other words, when Ar1, Ar2, and Ar3 are each independently non-hydrogen atoms, Ar1, Ar2, and Ar3 each independently substitute for any hydrogen atom on the aromatic or dearomatic ring. For example, the substituent group includes one or more of amine groups, halogen groups, alkyl-thionyl groups, oxygen-containing substituent groups, or alkyl groups.

[0244] For example, Ar1 and Ar3 are carboxylic acid ester groups, Ar2 is a hydrogen atom, and the substituted A 2-1 The structure shown includes one or more of the following structural formulas:

[0245]

[0246] In the above embodiments, the aromatic group is a group with aromatic function.

[0247] The substituted or unsubstituted aromatic groups having a cyclic number of C5 to C15 may include substituted or unsubstituted aromatic groups having a cyclic number of C6 to C15, or substituted or unsubstituted aromatic heterocyclic groups having a cyclic number of C6 to C15.

[0248] For example, substituted or unsubstituted aromatic groups with cyclic atoms numbering C5 to C15 include aromatic groups with cyclic atoms numbering C5, C6, C7, C8, C9, C10, C11, C12, C13, C14, C15, or any combination thereof.

[0249] Alkyl groups encompass both straight-chain and branched alkyl groups. For example, alkyl groups can be C1 to C5 alkyl groups, including methyl, ethyl, propyl, isopropyl, butyl, isobutyl, sec-butyl, tert-butyl, pentyl, etc.

[0250] [Conjugated groups]

[0251] D1 represents a conjugated group, which includes substituted or unsubstituted aromatic heterocyclic groups or substituted or unsubstituted alkenyl groups.

[0252] When the above-mentioned groups are substituted, the substituent groups include one or more of amine groups, halogen groups, alkylthion groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups. Optionally, the oxygen-containing substituent groups include one or more of alkoxy groups, amide groups, carboxylic acid groups, phosphite groups, phosphate groups, sulfonic acid groups, silicate groups, siloxane groups, borate groups, carboxylic acid ester groups, phosphate ester groups, sulfonate groups, silicate groups, borate groups, carboxyl groups, phosphite groups, phosphate groups, borate groups, or silicate groups.

[0253] In some embodiments, D1 includes substituted or unsubstituted deoxyrhedromic heterocyclic groups. These groups exhibit relatively high stability, further enhancing the intrinsic stability of the self-assembled molecule.

[0254] Optionally, the substituted or unsubstituted aromatic heterocyclic group includes an aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15, and the cyclic atoms in the aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15 further include one or more atoms selected from nitrogen, oxygen, and sulfur.

[0255] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include nitrogen atoms.

[0256] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 2-1 The structure shown is used for substituted or unsubstituted formula G. 2-9 One or more of the structures shown,

[0257]

[0258]

[0259] In the formula,

[0260] * indicates the connection site between the conjugated group and the hole extraction group;

[0261] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0262] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0263] For example, the substituted or unsubstituted formula G 2-1 The structure shown includes one or more of the following structures:

[0264]

[0265] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include oxygen atoms.

[0266] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 3-1 The structure shown is used for substituted or unsubstituted formula G. 3-3 One or more of the structures shown,

[0267]

[0268] In the formula,

[0269] * indicates the connection site between the conjugated group and the hole extraction group;

[0270] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0271] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0272] For example, formula G 3-1 The structure shown includes one or more of the following structures:

[0273]

[0274] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include sulfur atoms.

[0275] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 4-1 The structure shown is used for substituted or unsubstituted formula G. 4-3 One or more of the structures shown,

[0276]

[0277] In the formula,

[0278] * indicates the connection site between the conjugated group and the hole extraction group;

[0279] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0280] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0281] For example, formula G 4-1The structure shown includes one or more of the following structures:

[0282]

[0283] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include multiple atoms of nitrogen, oxygen, and sulfur.

[0284] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 5-1 The structure shown is used for substituted or unsubstituted formula G. 5-7 One or more of the structures shown,

[0285]

[0286] In the formula,

[0287] * indicates the connection site between the conjugated group and the hole extraction group;

[0288] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0289] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0290] For example, formula G 5-1 The structure shown includes one or more of the following structures:

[0291]

[0292] In some embodiments, the conjugated group includes a substituted or unsubstituted alkenyl group. Optionally, the substituted or unsubstituted alkenyl group includes a substituted or unsubstituted C2 to C6 chain alkenyl group, or a substituted or unsubstituted cyclic alkenyl group having a cyclic number of C5 to C15 atoms. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups.

[0293] Optionally, the substituted or unsubstituted C2 to C6 chain alkenyl groups include vinylidene, propenylidene, or butenylidene.

[0294] [Oxygen-containing groups]

[0295] One of the hole transport layer and the first electrode has an anchoring effect with oxygen-containing groups, which can enhance the binding force between the self-assembled molecules and the hole transport layer and improve the stability of the device.

[0296] In some embodiments, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0297] Optionally, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphate group, borate group, carboxylate group, phosphate group, and borate group.

[0298] For example, self-assembled molecules include one or more compounds from Formula I1-1 to Formula I1-4.

[0299]

[0300]

[0301] Self-assembled molecules

[0302] Secondly, this application proposes a self-assembling molecule.

[0303] The self-assembled molecule includes the structural formula shown in Formula I2.

[0304]

[0305] In Equation I2,

[0306] Ar2 represents a hole-extraction group with a cyclic atom number of C10 to C30;

[0307] D 21 and D 22 Both represent conjugated groups, D 21 and D 22 One of them includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; D 21 and D 22 The other includes a substituted or unsubstituted dehydroaromatic heterocyclic group, or a substituted or unsubstituted alkenyl group;

[0308] E2 indicates an oxygen-containing group;

[0309] n2 represents D 21 The number of connection sites with Ar2, where n2 is any positive integer from 1 to 8;

[0310] Self-assembled molecules include hole-extracting groups, conjugated groups, and oxygen-containing groups. Hole-extracting groups are connected to oxygen-containing groups through conjugated groups, which can enhance the overall conjugability of the molecule, reduce the migration energy barrier of charge carriers within the molecule, and improve the conductivity of self-assembled molecules. Furthermore, since the electron cloud is distributed throughout the molecule, it can reduce the problem of decreased molecular stability caused by excessively high local energy, thereby improving the intrinsic stability of self-assembled molecules.

[0311] n2 is any positive integer from 1 to 8. n2 can be 1 or greater than or equal to 2, for example, 2, 3, 4, 5, 6, 7 or 8.

[0312] When n2 is 1, one hydrogen atom in the hole extraction group is replaced by a conjugated group, and the structural formula of the self-assembled molecule is as follows:

[0313]

[0314] When n2 is greater than or equal to 2, at least two hydrogen atoms in the hole-extracting group are replaced by conjugated groups. Taking n2 as an example, the structural formula of the self-assembled molecule is as follows:

[0315]

[0316] [Hole Extraction Group]

[0317] In some embodiments, the hole-extraction group having a cyclic number of C10 to C30 includes substituted or unsubstituted aniline groups having a cyclic number of C10 to C30, and substituted or unsubstituted acridine groups having a cyclic number of C10 to C30. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl-thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups, and the number of carbon atoms in the substituted groups can be 1 to 5.

[0318] Optionally, the oxygen-containing substituents include one or more of the following: alkoxy group, amide group, carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0319] In some embodiments, the hole-extracting group having a cyclic atom number of C10 to C30 includes substituted or unsubstituted aniline groups having a cyclic atom number of C10 to C30.

[0320] When self-assembled molecules are applied to perovskite solar cells, the aforementioned hole-extraction groups facilitate hole extraction and transport. Building upon these hole-extraction groups, conjugated groups enhance the overall conjugability of the molecule, lower the intramolecular carrier migration barrier, and improve the conductivity of the self-assembled molecule.

[0321] Optionally, the substituted or unsubstituted aniline group with a cyclic number of C10 to C30 includes the structure shown in Formula A1.

[0322]

[0323] In formula A1,

[0324] M 11 and M 12 Each group independently comprises an aromatic group, either substituted or unsubstituted, having a cyclic atom number of C5 to C15;

[0325] M 13 Including substituted or unsubstituted aromatic groups with a cyclic atom number of C5 to C15;

[0326] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0327] For example, the substituted or unsubstituted aniline group having a cyclic number of C10 to C30 includes substituted or unsubstituted formula A. 1-1 The structure shown is used for substituted or unsubstituted formula A. 1-5 One or more of the structures shown,

[0328]

[0329] In the formula,

[0330] * indicates the connection site between the hole extraction group and the conjugated group.

[0331] s1, s2, s3, and s4 are any integers from 0 to 3. In the same structure, s1, s2, s3, and s4 are not all 0 at the same time. This can be understood as at least one of s1, s2, s3, and s4 being non-zero. For example, if s1 to s3 are 0, then s4 is a positive integer. Of course, at least two of s1, s2, s3, and s4 can be non-zero, or all of s1, s2, s3, and s4 can be non-zero and all of them can be positive integers.

[0332] The connection site between the hole-extracting group and the conjugated group can be at any position; in other words, any carbon atom of the benzene ring in the aniline-based hole-extracting group can be connected to the conjugated group.

[0333] For example, the substituted or unsubstituted aniline groups with a cyclic number of C10 to C30 include substituted or unsubstituted formula A. 1-11 The structure shown is used for substituted or unsubstituted formula A. 1-17 One or more of the structures shown,

[0334]

[0335]

[0336] The above structure may or may not be replaced. In the case of replacement, for example, formula A is replaced. 1-5 The structure shown includes one or more of the following structural formulas:

[0337]

[0338] Ar1, Ar2, Ar3, and Ar4 each independently represent a hydrogen atom or a substituent group, and at least one of Ar1, Ar2, Ar3, and Ar4 is a substituent group. In other words, when Ar1, Ar2, Ar3, and Ar4 are each independently non-hydrogen atoms, Ar1, Ar2, Ar3, and Ar4 each independently substitute for any hydrogen atom on an aromatic or dearomatic ring. For example, the substituent group includes one or more of amine groups, halogen groups, alkyl-thionyl groups, oxygen-containing substituent groups, or alkyl groups.

[0339] For example, Ar1, Ar3, and Ar4 are fluorine atoms, Ar2 is a hydrogen atom, and the substitution formula A 1-5 The structure shown includes one or more of the following structural formulas:

[0340]

[0341] In some embodiments, the hole-extracting group includes acridine-like groups with substituted or unsubstituted cyclic atoms having a number of C10 to C30. When the self-assembled molecule is applied to perovskite solar cells, the aforementioned hole-extracting group facilitates hole extraction and transport. Based on the aforementioned hole-extracting group, the conjugated group helps to enhance the overall conjugability of the molecule, lower the migration energy barrier of intramolecular charge carriers, and improve the conductivity of the self-assembled molecule.

[0342] Optionally, the substituted or unsubstituted acridine group with a cyclic number of C10 to C30 includes the structure shown in Formula A2.

[0343]

[0344] In formula A2,

[0345] M 21Including single bonds, substituted or unsubstituted cyclic aromatic groups with a number of C6 to C15 atoms, or substituted or unsubstituted cyclic heterocyclic groups with a number of C5 to C15 atoms;

[0346] M 22 and M 23 Each independently includes substituted or unsubstituted aromatic groups with a cyclic number of C6 to C15 or substituted or unsubstituted aromatic heterocyclic groups with a cyclic number of C6 to C15;

[0347] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups.

[0348] In M 21 In the case of a single bond, it can be understood that the carbon atom at that location is directly connected to the conjugated group.

[0349] For example, the substituted or unsubstituted acridine group having a cyclic atom number of C10 to C30 includes substituted or unsubstituted formula A. 2-1 The structure shown is used for substituted or unsubstituted formula A. 2-3 One or more of the structures shown,

[0350]

[0351] In the formula,

[0352] * indicates the connection site between the hole extraction group and the conjugated group;

[0353] s1 and s2 are any integers from 0 to 3, and in the same structure, s1 and s2 are not both 0.

[0354] Optionally, the substituted or unsubstituted acridine group comprises a substituted or unsubstituted formula A. 2-11 The structure shown is used for substituted or unsubstituted formula A. 2-13 One or more of the structures shown,

[0355]

[0356] In the formula, * represents the connection site between the hole extraction group and the conjugated group.

[0357] The above structure may or may not be replaced. In the case of replacement, for example, formula A is replaced. 2-1 The structure shown includes one or more of the following structural formulas:

[0358]

[0359] Ar1, Ar2, and Ar3 each independently represent a hydrogen atom or a substituent group, and at least one of Ar1, Ar2, and Ar3 is a substituent group. In other words, when Ar1, Ar2, and Ar3 are each independently non-hydrogen atoms, Ar1, Ar2, and Ar3 each independently substitute for any hydrogen atom on the aromatic or dearomatic ring. For example, the substituent group includes one or more of amine groups, halogen groups, alkyl-thionyl groups, oxygen-containing substituent groups, or alkyl groups.

[0360] For example, Ar1 and Ar3 are carboxylic acid ester groups, Ar2 is a hydrogen atom, and the substituted A 2-1 The structure shown includes one or more of the following structural formulas:

[0361]

[0362] In the above embodiments, the aromatic group is a group with aromatic function.

[0363] The substituted or unsubstituted aromatic groups having a cyclic number of C5 to C15 may include substituted or unsubstituted aromatic groups having a cyclic number of C6 to C15, or substituted or unsubstituted aromatic heterocyclic groups having a cyclic number of C6 to C15.

[0364] For example, substituted or unsubstituted aromatic groups with cyclic atoms numbering C5 to C15 include aromatic groups with cyclic atoms numbering C5, C6, C7, C8, C9, C10, C11, C12, C13, C14, C15, or any combination thereof.

[0365] Alkyl groups encompass both straight-chain and branched alkyl groups. For example, alkyl groups can be C1 to C5 alkyl groups, including methyl, ethyl, propyl, isopropyl, butyl, isobutyl, sec-butyl, tert-butyl, pentyl, etc.

[0366] [Conjugated groups]

[0367] D 21 and D 22 Both represent conjugated groups, D 21 and D 22 One of them includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; D 21 and D 22 Another component includes substituted or unsubstituted deoxyrheterocyclic groups, or substituted or unsubstituted alkenyl groups.

[0368] When the above-mentioned groups are substituted, the substituent groups include one or more of amine groups, halogen groups, alkylthion groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups. Optionally, the oxygen-containing substituent groups include one or more of alkoxy groups, amide groups, carboxylic acid groups, phosphite groups, phosphate groups, sulfonic acid groups, silicate groups, siloxane groups, borate groups, carboxylic acid ester groups, phosphate ester groups, sulfonate groups, silicate groups, borate groups, carboxyl groups, phosphite groups, phosphate groups, borate groups, or silicate groups.

[0369] Optionally, D 21 and D 22 One of them includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; D 21 and D 22 Another component includes substituted or unsubstituted deoxyrheterocyclic groups. These groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0370] Self-assembled molecules include two conjugated groups, which can further enhance the overall conjugation of the molecule, reduce the migration energy barrier of charge carriers within the molecule, and improve the conductivity of the self-assembled molecule; and because the electron cloud is distributed throughout the molecule, it can reduce the problem of decreased molecular stability caused by excessively high local energy, and improve the intrinsic stability of the self-assembled molecule.

[0371] In some implementations, D 21 Including substituted or unsubstituted aromatic hydrocarbon groups, or substituted or unsubstituted aromatic heterocyclic groups; D 22 This includes substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups.

[0372] Optionally, D 21 Including substituted or unsubstituted aromatic hydrocarbon groups, or substituted or unsubstituted aromatic heterocyclic groups; D 22 This includes substituted or unsubstituted aromatic heterocyclic groups.

[0373] In other implementations, D 22 Including substituted or unsubstituted aromatic hydrocarbon groups, or substituted or unsubstituted aromatic heterocyclic groups; D 21 This includes substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups.

[0374] Optionally, D 22 Including substituted or unsubstituted aromatic hydrocarbon groups, or substituted or unsubstituted aromatic heterocyclic groups; D 21 This includes substituted or unsubstituted aromatic heterocyclic groups.

[0375] Optionally, the substituted or unsubstituted aromatic hydrocarbon group includes a substituted or unsubstituted aromatic hydrocarbon group having a cyclic number of C6 to C15 atoms. Further optionally, the substituted or unsubstituted aromatic hydrocarbon group having a cyclic number of C6 to C15 atoms includes a substituted or unsubstituted aromatic hydrocarbon group of formula G. 1-1 The structure shown is used for substituted or unsubstituted formula G. 1-3 One or more of the structures shown,

[0376]

[0377] In the formula,

[0378] * indicates the connection site between the conjugated group and the hole extraction group;

[0379] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0380] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0381] For example, the substituted or unsubstituted formula G 1-1 The structure shown includes one or more of the following structures:

[0382]

[0383] Optionally, the substituted or unsubstituted aromatic heterocyclic group includes an aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15, and the cyclic atoms in the aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15 further include one or more atoms selected from nitrogen, oxygen, and sulfur.

[0384] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include nitrogen atoms.

[0385] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 2-1 The structure shown is used for substituted or unsubstituted formula G. 2-9 One or more of the structures shown,

[0386]

[0387] In the formula,

[0388] * indicates the connection site between the conjugated group and the hole extraction group;

[0389] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0390] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0391] For example, the substituted or unsubstituted formula G 2-1 The structure shown includes one or more of the following structures:

[0392]

[0393] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include oxygen atoms.

[0394] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 3-1 The structure shown is used for substituted or unsubstituted formula G. 3-3 One or more of the structures shown,

[0395]

[0396] In the formula,

[0397] * indicates the connection site between the conjugated group and the hole extraction group;

[0398] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0399] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0400] For example, formula G 3-1 The structure shown includes one or more of the following structures:

[0401]

[0402] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include sulfur atoms.

[0403] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 4-1 The structure shown is used for substituted or unsubstituted formula G. 4-3 One or more of the structures shown,

[0404]

[0405] In the formula,

[0406] * indicates the connection site between the conjugated group and the hole extraction group;

[0407] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0408] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0409] For example, formula G 4-1 The structure shown includes one or more of the following structures:

[0410]

[0411] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include multiple atoms of nitrogen, oxygen, and sulfur.

[0412] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 5-1 The structure shown is used for substituted or unsubstituted formula G. 5-7 One or more of the structures shown,

[0413]

[0414] In the formula,

[0415] * indicates the connection site between the conjugated group and the hole extraction group;

[0416] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0417] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0418] For example, formula G 5-1 The structure shown includes one or more of the following structures:

[0419]

[0420] In some embodiments, the conjugated group includes a substituted or unsubstituted alkenyl group. Optionally, the substituted or unsubstituted alkenyl group includes a substituted or unsubstituted C2 to C6 chain alkenyl group, or a substituted or unsubstituted cyclic alkenyl group having a cyclic number of C5 to C15 atoms. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups.

[0421] Optionally, the substituted or unsubstituted C2 to C6 chain alkenyl groups include vinylidene, propenylidene, or butenylidene.

[0422] [Oxygen-containing groups]

[0423] One of the hole transport layer and the first electrode has an anchoring effect with oxygen-containing groups, which can enhance the binding force between the self-assembled molecules and the hole transport layer and improve the stability of the device.

[0424] In some embodiments, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0425] Optionally, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphate group, borate group, carboxylate group, phosphate group, and borate group.

[0426] For example, the self-assembled molecules include one or more compounds of formula I2-1 to formula I2-3.

[0427]

[0428] Self-assembled molecules

[0429] Thirdly, this application proposes a self-assembling molecule.

[0430] The self-assembled molecule includes the structure shown in Formula I3.

[0431]

[0432] In Equation I3,

[0433] Ar3 represents a hole-extraction group with cyclic atoms ranging from C31 to C60;

[0434] D3 represents a conjugated group, which includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0435] E3 indicates an oxygen-containing group;

[0436] n3 represents the number of connection sites between D3 and Ar3, where n3 is any positive integer from 2 to 8.

[0437] Self-assembled molecules include hole-extracting groups, conjugated groups, and oxygen-containing groups. Hole-extracting groups are connected to oxygen-containing groups through conjugated groups, which can enhance the overall conjugability of the molecule, reduce the migration energy barrier of charge carriers within the molecule, and improve the conductivity of self-assembled molecules. Furthermore, since the electron cloud is distributed throughout the molecule, it can reduce the problem of decreased molecular stability caused by excessively high local energy, thereby improving the intrinsic stability of self-assembled molecules.

[0438] Furthermore, when n3 is greater than or equal to 2, the number of binding sites between the oxygen-containing groups and adjacent layers increases, which is beneficial to improving the binding energy between the functional layer and adjacent layers and improving device stability. Moreover, compared with the electron transport capability, the hole transport capability is weaker, which can easily lead to an imbalance between electron and hole transport and a decrease in device performance. However, in the embodiments of this application, the multiple conjugated oxygen-containing groups can increase the hole transport capability, so that the electron and hole transport capabilities are matched and the device performance is improved.

[0439] When n3 is greater than or equal to 2, at least two hydrogen atoms in the hole-extracting group are replaced by conjugated groups. Taking n3 as 2 or 3 as examples, the structural formula of the self-assembled molecule is as follows, wherein D3 in each branch independently includes a substituted or unsubstituted aromatic hydrocarbon group, a substituted or unsubstituted aromatic heterocyclic group, or a substituted or unsubstituted alkenyl group:

[0440]

[0441] [Hole Extraction Group]

[0442] In some embodiments, the hole-extraction group having a cyclic atom number of C31 to C60 includes substituted or unsubstituted carbazole groups having a cyclic atom number of C31 to C60, or substituted or unsubstituted aniline groups having a cyclic atom number of C31 to C60, etc.

[0443] Optionally, the hole-extracting group with cyclic atoms of C31 to C60 includes substituted or unsubstituted carbazole groups with cyclic atoms of C31 to C60. When the self-assembled molecule is applied to perovskite solar cells, the aforementioned hole-extracting group facilitates hole extraction and transport. Based on the aforementioned hole-extracting group, the conjugated group helps to enhance the overall conjugability of the molecule, reduce the migration barrier of intramolecular charge carriers, and improve the conductivity of the self-assembled molecule.

[0444] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups, and the number of carbon atoms in the substituted groups can be 1 to 5.

[0445] Optionally, the oxygen-containing substituents include one or more of the following: alkoxy group, amide group, carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0446] Optionally, the substituted or unsubstituted carbazole group with a cyclic number of C31 to C60 includes the structure shown in Formula B1.

[0447]

[0448] In equation B1,

[0449] S 20 Including single bonds, substituted or unsubstituted cyclic aromatic groups with a number of C6 to C30 atoms, or substituted or unsubstituted cyclic heterocyclic groups with a number of C5 to C30 atoms;

[0450] S 21 and S 22 Each independently includes substituted or unsubstituted aromatic groups with a cyclic number of C6 to C30 or substituted or unsubstituted nitrogen-containing aromatic heterocyclic groups with a cyclic number of C6 to C30;

[0451] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups, and the number of carbon atoms in the substituted groups can be 1 to 5.

[0452] In S 20 In the case of a single bond, the nitrogen atom is directly connected to the conjugated group; in the case of S... 20 In the case of a non-single bond, the nitrogen atom passes through S 20 It is directly connected to a conjugated group.

[0453] Optionally,

[0454] The substituted or unsubstituted carbazole group having a cyclic number of C31 to C60 includes substituted or unsubstituted formula B. 1-1 The structure shown is for substituted or unsubstituted formula B. 1-6 One or more of the structures shown,

[0455]

[0456]

[0457] In the formula,

[0458] * indicates the connection site between the hole extraction group and the conjugated group;

[0459] s1, s2, s3, s4, s5 and s6 are any integers from 0 to 3, and in the same structure, s1, s2, s3, s4, s5 and s6 are not all 0 at the same time.

[0460] For example, the substituted or unsubstituted carbazole group having a cyclic atom number of C31 to C60 includes substituted or unsubstituted formula B. 1-11 The structure shown is for substituted or unsubstituted formula B. 1-16 One or more of the structures shown,

[0461]

[0462]

[0463] In the formula, * represents the connection site between the hole extraction group and the conjugated group.

[0464] The above structure may or may not be replaced. In the case of replacement, for example, formula B is replaced. 1-1 The structure shown includes one or more of the following structural formulas:

[0465]

[0466] 5Ar1, Ar2, Ar3, and Ar4 each independently represent a hydrogen atom or the aforementioned substituent group, and Ar1, Ar2, Ar3, and Ar4

[0467] At least one of them is the substituent group; in other words, when Ar1, Ar2, Ar3, and Ar4 are each independently non-hydrogen atoms, Ar1, Ar2, Ar3, and Ar4 each independently substitute for any hydrogen atom on the aromatic or dearomatic ring. For example, the substituent group includes one or more of amine groups, halogen groups, alkyl-thio groups, oxygen-containing substituent groups, or alkyl groups.

[0468] For example, Ar3 and Ar4 are fluorine atoms, and the substitution formula B 1-1 The structure shown includes one or more of the following structural formulas:

[0469]

[0470] Optionally, the substituted or unsubstituted aniline groups with a cyclic number of C31 to C60 include one or more of the following structures:

[0471]

[0472] In the formula, * represents the connection site between the hole extraction group and the conjugated group;

[0473] s1, s2, s3 and s4 are any integers from 0 to 3, and in the same structure, s1, s2, s3 and s4 are not all 0 at the same time.

[0474] For example, aniline groups with substituted or unsubstituted cyclic atoms having a number of C31 to C60 include one or more of the following structures.

[0475]

[0476] [Conjugated groups]

[0477] D3 represents a conjugated group, which includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups.

[0478] When the above-mentioned groups are substituted, the substituent groups include one or more of amine groups, halogen groups, alkylthion groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups. Optionally, the oxygen-containing substituent groups include one or more of alkoxy groups, amide groups, carboxylic acid groups, phosphite groups, phosphate groups, sulfonic acid groups, silicate groups, siloxane groups, borate groups, carboxylic acid ester groups, phosphate ester groups, sulfonate groups, silicate groups, borate groups, carboxyl groups, phosphite groups, phosphate groups, borate groups, or silicate groups.

[0479] Optionally, the conjugated group includes substituted or unsubstituted aromatic hydrocarbon groups or substituted or unsubstituted aromatic heterocyclic groups; these groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0480] Optionally, the substituted or unsubstituted aromatic hydrocarbon groups include substituted or unsubstituted aromatic hydrocarbon groups having a cyclic atom number of C6 to C15.

[0481] Further optionally, the substituted or unsubstituted aromatic hydrocarbon groups having a cyclic number of C6 to C15 include substituted or unsubstituted groups of formula G. 1-1 The structure shown is used for substituted or unsubstituted formula G. 1-3 One or more of the structures shown,

[0482]

[0483] In the formula, * represents the connection site between the conjugated group and the hole extraction group;

[0484] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0485] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0486] For example, the substituted or unsubstituted formula G1-1 The structure shown includes one or more of the following structures:

[0487]

[0488] Optionally, the substituted or unsubstituted aromatic heterocyclic group includes an aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15, and the cyclic atoms in the aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15 further include one or more atoms selected from nitrogen, oxygen, and sulfur.

[0489] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include nitrogen atoms.

[0490] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 2-1 The structure shown is used for substituted or unsubstituted formula G. 2-9 One or more of the structures shown,

[0491]

[0492]

[0493] In the formula,

[0494] * indicates the connection site between the conjugated group and the hole extraction group;

[0495] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0496] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0497] For example, the substituted or unsubstituted formula G 2-1 The structure shown includes one or more of the following structures:

[0498]

[0499] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include oxygen atoms.

[0500] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 3-1 The structure shown is used for substituted or unsubstituted formula G. 3-3 One or more of the structures shown,

[0501]

[0502] In the formula,

[0503] * indicates the connection site between the conjugated group and the hole extraction group;

[0504] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0505] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0506] For example, formula G 3-1 The structure shown includes one or more of the following structures:

[0507]

[0508] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include sulfur atoms.

[0509] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 4-1 The structure shown is used for substituted or unsubstituted formula G. 4-3 One or more of the structures shown,

[0510]

[0511] In the formula,

[0512] * indicates the connection site between the conjugated group and the hole extraction group;

[0513] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0514] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0515] For example, formula G 4-1 The structure shown includes one or more of the following structures:

[0516]

[0517] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include multiple atoms of nitrogen, oxygen, and sulfur.

[0518] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 5-1 The structure shown is used for substituted or unsubstituted formula G. 5-7 One or more of the structures shown,

[0519]

[0520] In the formula,

[0521] * indicates the connection site between the conjugated group and the hole extraction group;

[0522] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0523] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0524] For example, formula G 5-1 The structure shown includes one or more of the following structures:

[0525]

[0526] In some embodiments, the conjugated group includes a substituted or unsubstituted alkenyl group. Optionally, the substituted or unsubstituted alkenyl group includes a substituted or unsubstituted C2 to C6 chain alkenyl group, or a substituted or unsubstituted cyclic alkenyl group having a cyclic number of C5 to C15 atoms. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups.

[0527] Optionally, the substituted or unsubstituted C2 to C6 chain alkenyl groups include vinylidene, propenylidene, or butenylidene.

[0528] [Oxygen-containing groups]

[0529] One of the hole transport layer and the first electrode has an anchoring effect with oxygen-containing groups, which can enhance the binding force between the self-assembled molecules and the hole transport layer and improve the stability of the device.

[0530] In some embodiments, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0531] Optionally, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphate group, borate group, carboxylate group, phosphate group, and borate group.

[0532] For example, the self-assembled molecules include one or more compounds from Formula I3-1 to Formula I3-2.

[0533]

[0534] Self-assembled molecules

[0535] Fourthly, this application proposes a self-assembling molecule.

[0536] The self-assembled molecule includes the structure shown in Formula I4.

[0537]

[0538] In Equation I4,

[0539] Ar4 represents a hole-extraction group with cyclic atoms ranging from C31 to C60;

[0540] D 41 and D 42 Both represent conjugated groups, D 41 and D 42 Each independently includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0541] n4 represents D 41 The number of connection sites with Ar4, where n4 is any positive integer from 2 to 8;

[0542] E4 represents an oxygen-containing group.

[0543] Self-assembled molecules include hole-extracting groups, conjugated groups, and oxygen-containing groups. Hole-extracting groups are connected to oxygen-containing groups through conjugated groups, which can enhance the overall conjugability of the molecule, reduce the migration energy barrier of charge carriers within the molecule, and improve the conductivity of self-assembled molecules. Furthermore, since the electron cloud is distributed throughout the molecule, it can reduce the problem of decreased molecular stability caused by excessively high local energy, thereby improving the intrinsic stability of self-assembled molecules.

[0544] Furthermore, when n4 is greater than or equal to 2, the number of binding sites between the oxygen-containing groups and adjacent layers increases, which is beneficial to improving the binding energy between the functional layer and adjacent layers and improving device stability. Moreover, compared with the electron transport capability, the hole transport capability is weaker, which can easily lead to an imbalance between electron and hole transport and a decrease in device performance. However, in the embodiments of this application, the multiple conjugated oxygen-containing groups can increase the hole transport capability, so that the electron and hole transport capabilities are matched and the device performance is improved.

[0545] When n4 is greater than or equal to 2, at least two hydrogen atoms in the hole-extracting group are replaced by conjugated groups. Taking n4 as 2 or 3 as examples, the structural formula of the self-assembled molecule is as follows, where D in each branch chain 41 and D 42 Each of these groups independently comprises substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups:

[0546]

[0547] [Hole Extraction Group]

[0548] In some embodiments, the hole-extraction group having a cyclic atom number of C31 to C60 includes substituted or unsubstituted carbazole groups having a cyclic atom number of C31 to C60, or substituted or unsubstituted aniline groups having a cyclic atom number of C31 to C60, etc.

[0549] Optionally, the hole-extracting group with cyclic atoms of C31 to C60 includes substituted or unsubstituted carbazole groups with cyclic atoms of C31 to C60. When the self-assembled molecule is applied to perovskite solar cells, the aforementioned hole-extracting group facilitates hole extraction and transport. Based on the aforementioned hole-extracting group, the conjugated group helps to enhance the overall conjugability of the molecule, reduce the migration barrier of intramolecular charge carriers, and improve the conductivity of the self-assembled molecule.

[0550] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups, and the number of carbon atoms in the substituted groups can be 1 to 5.

[0551] Optionally, the oxygen-containing substituents include one or more of the following: alkoxy group, amide group, carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0552] Optionally, the substituted or unsubstituted carbazole group with a cyclic number of C31 to C60 includes the structure shown in Formula B1.

[0553]

[0554] In equation B1,

[0555] S 20 Including single bonds, substituted or unsubstituted cyclic aromatic groups with a number of C6 to C30 atoms, or substituted or unsubstituted cyclic heterocyclic groups with a number of C5 to C30 atoms;

[0556] S 21 and S 22 Each independently includes substituted or unsubstituted aromatic groups with a cyclic number of C6 to C30 or substituted or unsubstituted nitrogen-containing aromatic heterocyclic groups with a cyclic number of C6 to C30;

[0557] When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituted groups, or C1 to C5 alkyl groups, and the number of carbon atoms in the substituted groups can be 1 to 5.

[0558] In S 20 In the case of a single bond, the nitrogen atom is directly connected to the conjugated group; in the case of S... 20 In the case of a non-single bond, the nitrogen atom passes through S 20 It is directly connected to a conjugated group.

[0559] Optionally,

[0560] The substituted or unsubstituted carbazole group having a cyclic number of C31 to C60 includes substituted or unsubstituted formula B. 1-1 The structure shown is for substituted or unsubstituted formula B. 1-6 One or more of the structures shown,

[0561]

[0562]

[0563] In the formula,

[0564] * indicates the connection site between the hole extraction group and the conjugated group;

[0565] s1, s2, s3, s4, s5 and s6 are any integers from 0 to 3, and in the same structure, s1, s2, s3, s4, s5 and s6 are not all 0 at the same time.

[0566] For example, the substituted or unsubstituted carbazole group having a cyclic atom number of C31 to C60 includes substituted or unsubstituted formula B. 1-11 The structure shown is for substituted or unsubstituted formula B. 1-16 One or more of the structures shown,

[0567]

[0568]

[0569] In the formula, * represents the connection site between the hole extraction group and the conjugated group.

[0570] The above structure may or may not be replaced. In the case of replacement, for example, formula B is replaced. 1-1 The structure shown includes one or more of the following structural formulas:

[0571]

[0572] Ar1, Ar2, Ar3, and Ar4 each independently represent a hydrogen atom or a substituent group, and at least one of Ar1, Ar2, Ar3, and Ar4 is a substituent group; in other words, when Ar1, Ar2, Ar3, and Ar4 are each independently non-hydrogen atoms, Ar1, Ar2, Ar3, and Ar4 each independently substitute for any hydrogen atom on the aromatic or dearomatic ring. For example, the substituent group includes one or more of amine groups, halogen groups, alkyl-thionyl groups, oxygen-containing substituent groups, or alkyl groups.

[0573] For example, Ar3 and Ar4 are fluorine atoms, and the substitution formula B 1-1 The structure shown includes one or more of the following structural formulas:

[0574]

[0575] Optionally, the substituted or unsubstituted aniline groups with a cyclic number of C31 to C60 include one or more of the following structures:

[0576]

[0577] In the formula, * represents the connection site between the hole extraction group and the conjugated group;

[0578] s1, s2, s3 and s4 are any integers from 0 to 3, and in the same structure, s1, s2, s3 and s4 are not all 0 at the same time.

[0579] For example, aniline groups with substituted or unsubstituted cyclic atoms having a number of C31 to C60 include one or more of the following structures.

[0580]

[0581] [Conjugated groups]

[0582] D 41 and D 42 Both represent conjugated groups, D 41 and D 42 Each independently includes substituted or unsubstituted aromatic hydrocarbon groups, substituted or unsubstituted aromatic heterocyclic groups, or substituted or unsubstituted alkenyl groups;

[0583] Optionally, D 41 and D 42Each group independently comprises either a substituted or unsubstituted aromatic hydrocarbon group or a substituted or unsubstituted aromatic heterocyclic group. These groups are more stable and can further enhance the intrinsic stability of the self-assembled molecule.

[0584] Optionally, the substituted or unsubstituted aromatic hydrocarbon groups include substituted or unsubstituted aromatic hydrocarbon groups having a cyclic atom number of C6 to C15.

[0585] Further optionally, the substituted or unsubstituted aromatic hydrocarbon groups having a cyclic number of C6 to C15 include substituted or unsubstituted groups of formula G. 1-1 The structure shown is used for substituted or unsubstituted formula G. 1-3 One or more of the structures shown,

[0586]

[0587] In the formula,

[0588] * indicates the connection site between the conjugated group and the hole extraction group;

[0589] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0590] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0591] For example, the substituted or unsubstituted formula G 1-1 The structure shown includes one or more of the following structures:

[0592]

[0593] Optionally, the substituted or unsubstituted aromatic heterocyclic group includes an aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15, and the cyclic atoms in the aromatic heterocyclic group with substituted or unsubstituted cyclic atoms having a number of C5 to C15 further include one or more atoms selected from nitrogen, oxygen, and sulfur.

[0594] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include nitrogen atoms.

[0595] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 2-1 The structure shown is used for substituted or unsubstituted formula G. 2-9 One or more of the structures shown,

[0596]

[0597]

[0598] In the formula,

[0599] * indicates the connection site between the conjugated group and the hole extraction group;

[0600] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0601] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0602] For example, the substituted or unsubstituted formula G 2-1 The structure shown includes one or more of the following structures:

[0603]

[0604] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include oxygen atoms.

[0605] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 3-1 The structure shown is used for substituted or unsubstituted formula G. 3-3 One or more of the structures shown,

[0606]

[0607] In the formula,

[0608] * indicates the connection site between the conjugated group and the hole extraction group;

[0609] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0610] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0611] For example, formula G 3-1 The structure shown includes one or more of the following structures:

[0612]

[0613] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include sulfur atoms.

[0614] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 4-1 The structure shown is used for substituted or unsubstituted formula G. 4-3 One or more of the structures shown,

[0615]

[0616] In the formula,

[0617] * indicates the connection site between the conjugated group and the hole extraction group;

[0618] # indicates the connection site between the conjugated group and the oxygen-containing group;

[0619] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0620] For example, formula G 4-1 The structure shown includes one or more of the following structures:

[0621]

[0622] Further optionally, the cyclic atoms in the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 include multiple atoms of nitrogen, oxygen, and sulfur.

[0623] For example, the substituted or unsubstituted aromatic heterocyclic group having a cyclic atom number of C5 to C15 includes substituted or unsubstituted formula G 5-1 The structure shown is used for substituted or unsubstituted formula G. 5-7 One or more of the structures shown,

[0624]

[0625] In the formula,

[0626] * indicates the connection site between the conjugated group and the hole extraction group;

[0627] # indicates the connection site between the conjugated group and the oxygen-containing group.

[0628] The connection site between the conjugated group and the hole-extracting group can be at any position, and the connection site between the conjugated group and the oxygen-containing group can be at any position.

[0629] For example, formula G 5-1 The structure shown includes one or more of the following structures:

[0630]

[0631] In some embodiments, the conjugated group includes a substituted or unsubstituted alkenyl group. Optionally, the substituted or unsubstituted alkenyl group includes a substituted or unsubstituted C2 to C6 chain alkenyl group, or a substituted or unsubstituted cyclic alkenyl group having a cyclic number of C5 to C15 atoms. When the above groups are substituted, the substituted groups include one or more of amine groups, halogen groups, alkyl thio groups, oxygen-containing substituent groups, or C1 to C5 alkyl groups.

[0632] Optionally, the substituted or unsubstituted C2 to C6 chain alkenyl groups include vinylidene, propenylidene, or butenylidene.

[0633] [Oxygen-containing groups]

[0634] One of the hole transport layer and the first electrode has an anchoring effect with oxygen-containing groups, which can enhance the binding force between the self-assembled molecules and the hole transport layer and improve the stability of the device.

[0635] In some embodiments, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphite group, phosphate group, sulfonic acid group, silicate group, siloxane group, borate group, carboxylic acid ester group, phosphate ester group, sulfonate group, silicate group, borate group, carboxyl group, phosphite group, phosphate group, borate group, or silicate group.

[0636] Optionally, the oxygen-containing group includes one or more of the following: carboxylic acid group, phosphate group, borate group, carboxylate group, phosphate group, and borate group.

[0637] For example, the self-assembled molecules include one or more compounds from Formula I4-1 to Formula I4-2.

[0638]

[0639] In the embodiments described above in this application, the structure of the compound can be tested using nuclear magnetic resonance (NMR) technology.

[0640] Perovskite solar cells

[0641] Fifthly, this application proposes a perovskite solar cell.

[0642] like Figure 1As shown, the perovskite solar cell 10 includes a first electrode 11, a functional layer 12, a perovskite light-absorbing layer 14, and a second electrode 16 stacked along the thickness direction M of the perovskite solar cell 10. The functional layer 12 includes self-assembled molecules, which include one or more of the self-assembled molecules of any embodiment of the first aspect of this application, any embodiment of the second aspect of this application, any embodiment of the third aspect of this application, and any embodiment of the fourth aspect of this application.

[0643] Functional layer 12 includes self-assembled molecules, which include hole extraction groups, conjugated groups, and oxygen-containing groups. The hole extraction groups are connected to the oxygen-containing groups through the conjugated groups, which can improve the overall conjugability of the molecule, reduce the migration energy barrier of charge carriers within the molecule, and improve the conductivity of the self-assembled molecules. Furthermore, since the electron cloud is distributed throughout the molecule, it can reduce the problem of molecular instability caused by excessively high local energy, improve the intrinsic stability of the self-assembled molecules, and enable the self-assembled molecules to effectively perform passivation and hole extraction and transport functions, thereby improving device stability and photoelectric conversion efficiency.

[0644] The functional layer 12 can serve as a hole transport layer or as a passivation layer between the hole transport layer and the perovskite light-absorbing layer 14.

[0645] In some embodiments, the functional layer 12 is a hole transport layer disposed on the surface of the first electrode 11, and the functional layer 12 is in contact with at least a portion of the surface of the first electrode 11.

[0646] In some embodiments, the thickness of the functional layer 12 is from 1 nm to 30 nm, for example, 1 nm, 2 nm, 3 nm, 4 nm, 5 nm, 6 nm, 7 nm, 8 nm, 9 nm, 10 nm, 11 nm, 12 nm, 13 nm, 14 nm, 15 nm, 16 nm, 17 nm, 18 nm, 19 nm, 20 nm, 21 nm, 22 nm, 23 nm, 24 nm, 25 nm, 26 nm, 27 nm, 28 nm, 29 nm, 30 nm, or any combination of two of the above values. When the thickness of the functional layer 12 is within the above range, holes can be effectively transported, improving the photoelectric conversion efficiency of the device.

[0647] like Figure 2As shown, in some other embodiments, the perovskite solar cell 10 may further include a hole transport layer 13, with a functional layer 12 located between the hole transport layer 13 and the perovskite light-absorbing layer 14. The hole transport layer 13, as a carrier transport layer, can effectively transport holes, reduce carrier recombination at the interface between the perovskite light-absorbing layer 14 and the hole transport layer 13, and improve the photoelectric conversion efficiency of the perovskite solar cell 10. The functional layer 12 can effectively passivate defects in the perovskite light-absorbing layer 14, further improving the photoelectric conversion efficiency of the device.

[0648] Optionally, the thickness of the functional layer 12 is from 0.1 nm to 20 nm, for example, 0.1 nm, 0.5 nm, 0.8 nm, 1 nm, 2 nm, 3 nm, 4 nm, 5 nm, 6 nm, 7 nm, 8 nm, 9 nm, 10 nm, 11 nm, 12 nm, 13 nm, 14 nm, 15 nm, 16 nm, 17 nm, 18 nm, 19 nm, 20 nm, or any combination of two of the above values. When the thickness of the functional layer 12 is within the above range, it can effectively passivate the defects of the perovskite light-absorbing layer 14, further improving the photoelectric conversion efficiency of the device.

[0649] Hole transport layer 13 includes hole transport material, which includes one or more of the following materials and their derivatives and materials obtained by doping or passivation: self-assembled molecules and inorganic compounds.

[0650] Self-assembled molecules include one or more of the following: poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], poly(3,4-ethylenedioxythiophene)-polystyrene sulfonic acid, 2,2',7,7'-tetratetra[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene, poly-3-hexylthiophene, methoxytriphenylamine-fluoroformamidinium, triphenylamine with a triphenylene core, 3,4-ethylenedioxythiophene-methoxytriphenylamine, N-4-anilinecarbazole-spirobifluorene, polythiophene, and self-assembled monomolecules.

[0651] Inorganic compounds include one or more of metal oxides, cuprous iodide (CuI), and cuprous thiocyanate; wherein the metal oxides contain one or more of the metal elements Ni, Mo, and Cu, such as nickel oxide (NiO). x One or more of molybdenum oxide (MoO3) and cuprous oxide (CuO).

[0652] Hole transport materials include nickel oxide (NiO). xIn the case of nickel oxide layer rich in trivalent nickel, which has strong oxidizing properties, it will accelerate the degradation of perovskite materials. In the embodiments of this application, a functional layer 12 containing self-assembled molecules is also included. The self-assembled molecules can isolate the perovskite materials from trivalent nickel, which can slow down the degradation rate of the perovskite materials. Moreover, the self-assembled molecules include conjugated groups, which can improve the overall conjugability of the molecules, reduce the migration energy barrier of charge carriers within the molecules, and improve conductivity. Electrons are conjugated throughout the molecules, avoiding the decrease in molecular stability caused by excessive local energy, thereby further improving the stability of the device and improving the photoelectric conversion efficiency of the device.

[0653] The perovskite light-absorbing layer 14 includes a perovskite material. After the perovskite material absorbs photons, it generates electron-hole pairs, which are then thermally heated to form excitons. Charge separation then occurs, with photogenerated electrons transitioning to the LUMO level of the perovskite light-absorbing layer 14 and photogenerated holes transitioning to the HOMO level of the perovskite light-absorbing layer 14.

[0654] Perovskite materials refer to compounds with a perovskite structure. Perovskite materials include one or more compounds with the molecular formula ABX3 or M2CDN6, where A, B, M, C, and D are cations, and X and N are anions.

[0655] Taking ABX3 as an example, in an ideal cubic crystal structure, the B cation has 6-fold coordination and is surrounded by an anionic octahedron, while the A cation has 12-fold cubic octahedral coordination. The cubic unit cell of this compound consists of the A cation located at the cubic corner, the B cation located at the body center, and the X anion located at the face center.

[0656] In some implementations, A and M each independently include Li. + Na + K + 、Rb + Cs + One or more of the following: methylamine cation, ethylamine cation, propylamine cation, butylamine cation, pentamine cation, hexamine cation, formamidin cation, or imidazole cation.

[0657] In some implementations, B includes Ca 2+ 、Sr 2+ Cd 2+ Cu 2+ Ni 2+ Mn 2+ Fe 2+ Co 2+ Pd 2+ 、Ge 2+ Sn 2 + Pb 2+ Sn 2+Yb 2+ and Eu 2+ One or more cations, etc.

[0658] In some implementations, X and N each independently include F. - Cl - ,Br - Or I - One or more of them.

[0659] In some implementations, C includes Cs + Ag + K + Or Ru + One or more of them.

[0660] In some implementations, D includes Bi. 3+ Ni 3+ Fe 3+ Sb 3+ In 3+ or Cu 3+ One or more of them.

[0661] For example, perovskite materials include CH8I3N2Pb (FAPbI3) and Cs. 0.05 (FA 0.83 MA 0.17 ) 0.95 Pb(I 0.83 Br 0.17 3. One or more of methylammonium lead iodide (CH3NH3PbI3, MAPbI3), CsPbBr3, CsPbI3, CsFAPbI3, and MAFAPbI3, wherein MA + The methylamine cation CH3NH3 + FA represents formamidinium cation ((NH2)2CH + ).

[0662] In some embodiments, the thickness of the perovskite light-absorbing layer 14 is between 200 nm and 1000 nm, for example, 200 nm, 250 nm, 300 nm, 400 nm, 500 nm, 600 nm, 700 nm, 800 nm, 900 nm, 1000 nm, or any combination of two of the above values. When the thickness of the perovskite light-absorbing layer 14 is within the above range, the photoelectric conversion function of the perovskite light-absorbing layer 14 can be effectively utilized, thereby improving the photoelectric conversion efficiency of the perovskite solar cell 10.

[0663] like Figure 3 As shown, in some embodiments, the perovskite solar cell 10 further includes an electron transport layer 15 disposed between the perovskite light-absorbing layer 14 and the second electrode 16.

[0664] As a carrier transport layer, the electron transport layer 15 can effectively transport electrons, reduce carrier recombination at the interface between the photoelectric conversion layer and the electron transport layer 15, and improve the photoelectric conversion efficiency of the perovskite solar cell 10.

[0665] The electron transport layer 15 may include an electron transport material, which may include one or more of doped or undoped tin oxide, doped or undoped titanium oxide, doped or undoped zinc oxide, and doped or undoped organic molecular materials. The doping element may include one or more of Mg, Zn, Ag, Li, Rb, Ta, and Nb, for example, by doping with chlorides of the above elements. Specifically, the electron transport material may include [6,6]-phenylC 61 Methyl butyrate (PC) 61 BM), [6,6]-phenyl C 71 Methyl butyrate PC 71 BM, Fullerene C 60 Fullerene C 70 One or more of the following: tin dioxide (SnO2), zinc oxide (ZnO), etc.

[0666] In some embodiments, one or both of the first electrode 11 and the second electrode 16 are transparent electrodes to allow light to enter.

[0667] In some embodiments, the electrode material in the first electrode 11 includes one or more of transparent conductive oxides, metals, and carbon materials. The transparent conductive oxides include one or more of indium tin oxide (ITO), fluorine-doped tin oxide (FTO), indium-doped zinc oxide (IZO), aluminum-doped zinc oxide (AZO), boron-doped zinc oxide (BZO), antimony-doped tin oxide, and indium-doped tungsten oxide (IWO). The metals include, but are not limited to, one or more of silver, copper, gold, aluminum, and platinum. The carbon materials include one or more of graphite, graphene, and carbon nanotubes.

[0668] In some embodiments, the electrode material of the second electrode 16 includes one or more of transparent conductive oxides, metals, and carbon materials. The transparent conductive oxides include one or more of indium tin oxide (ITO), fluorine-doped tin oxide (FTO), indium-doped zinc oxide (IZO), aluminum-doped zinc oxide (AZO), boron-doped zinc oxide (BZO), antimony-doped tin oxide, and indium-doped tungsten oxide (IWO). The metals include, but are not limited to, one or more of silver, copper, gold, aluminum, and platinum. The carbon materials include one or more of graphite, graphene, and carbon nanotubes.

[0669] In some embodiments, the perovskite solar cell 10 further includes a substrate layer, which is a rigid substrate layer or a flexible substrate layer; further, the rigid substrate layer is transparent glass; the material of the flexible substrate layer includes an organic polymer material; further, the material of the flexible substrate layer may be one or more of the following materials mixed in different proportions: including but not limited to polyvinyl alcohol (PVA), polyester (PET), polyimide (PI), polyethylene naphthalate (PEN), polydimethylsiloxane (PDMS), etc.

[0670] The perovskite solar cell 10 can be a nip structure or a pin structure.

[0671] In the case where the perovskite solar cell 10 includes a hole transport layer 13 and an electron transport layer 15, the perovskite solar cell 10 comprises a first electrode 11, a hole transport layer 13, a functional layer 12, a perovskite light-absorbing layer 14, an electron transport layer 15, and a second electrode 16, which are sequentially stacked along its thickness direction M. Optionally, a buffer layer, a passivation layer, or other functional layer structures may be further included between the transport layer and the perovskite light-absorbing layer 14. Figure 3 The image shown is an inverted perovskite solar cell 10; Figure 3 The middle arrow indicates the direction of the incident light.

[0672] like Figure 4 As shown, the perovskite solar cell 10 includes a second electrode 16, an electron transport layer 15, a perovskite light-absorbing layer 14, a functional layer 12, a hole transport layer 13, and a first electrode 11, which are sequentially stacked along its thickness direction M. Optionally, a buffer layer, a passivation layer, or other functional layer structures may be further included between the transport layer and the perovskite light-absorbing layer 14. Figure 4 The image shown is of the formal structure of a perovskite solar cell 10; Figure 4 The middle arrow indicates the direction of the incident light.

[0673] In the case where the perovskite solar cell 10 does not include the hole transport layer 13

[0674] like Figure 5 As shown, the perovskite solar cell 10 includes a first electrode 11, a functional layer 12, a perovskite light-absorbing layer 14, an electron transport layer 15, and a second electrode 16, which are sequentially stacked along its thickness direction M. Optionally, a buffer layer, passivation layer, or other functional layer structures may be further included between the transport layer and the perovskite light-absorbing layer 14. Figure 5 The image shown is an inverted perovskite solar cell 10; Figure 5 The middle arrow indicates the direction of the incident light.

[0675] like Figure 6As shown, the perovskite solar cell 10 includes a second electrode 16, an electron transport layer 15, a perovskite light-absorbing layer 14, a functional layer 12, and a first electrode 11, which are sequentially stacked along its thickness direction M. Optionally, a buffer layer, passivation layer, or other functional layer structure may be further included between the transport layer and the perovskite light-absorbing layer 14. Figure 6 The image shown is of the formal structure of a perovskite solar cell 10; Figure 6 The middle arrow indicates the direction of the incident light.

[0676] In the embodiments of this application, the thickness of each film layer in the perovskite solar cell 10 can be detected using equipment and methods known in the art, such as using an ellipsometer to detect the film thickness, and the test method can refer to the standard test.

[0677] Photovoltaic module 1

[0678] Sixthly, the present application also provides a photovoltaic module 1.

[0679] like Figure 7 As shown, the photovoltaic module 1 includes a perovskite solar cell 10 according to any embodiment of the first aspect of this application.

[0680] In some embodiments, the photovoltaic module 1 may include at least one perovskite solar cell 10. For example, the photovoltaic module 1 may include one perovskite solar cell 10, or it may include multiple perovskite solar cells 10. When the photovoltaic module 1 includes multiple perovskite solar cells 10, the multiple perovskite solar cells 10 can be connected in series, parallel, or mixed configurations. A mixed configuration means that the multiple perovskite solar cells 10 are divided into multiple groups of cells, each group is internally connected in series, and then adjacent groups are connected in parallel; or each group is internally connected in parallel, and then adjacent groups are connected in series. Figure 7 As shown, the photovoltaic module 1 includes at least one perovskite solar cell 10.

[0681] In some embodiments, the photovoltaic module 1 includes a single-junction perovskite cell made of the perovskite cell described above, or a tandem cell including the perovskite cell described above.

[0682] The aforementioned tandem solar cell, by connecting a wide-bandgap cell and a narrow-bandgap cell in series, can more rationally utilize photons across the entire spectrum and reduce energy loss. Specifically, the tandem solar cell includes a bottom cell and a top cell. The bottom cell has a relatively narrow bandgap and can be a silicon cell, or it can be a perovskite solar cell 10. The top cell has a relatively wide bandgap and can be a perovskite solar cell 10. Exemplarily, the tandem solar cell can include one or more of a crystalline silicon perovskite tandem solar cell or a full perovskite solar cell 10. Exemplarily, the aforementioned crystalline silicon perovskite tandem solar cell can include a crystalline silicon bottom cell and a perovskite top cell arranged in sequence, wherein the aforementioned perovskite solar cell 10 can be used as the perovskite top cell in the crystalline silicon perovskite tandem solar cell. Exemplarily, the aforementioned full perovskite solar cell 10 can include a first perovskite cell and a second perovskite cell arranged in sequence, wherein both the first perovskite cell and the second perovskite cell can be the perovskite solar cell 10 of this application.

[0683] Power generation unit

[0684] In a seventh aspect, the present application also provides a power generation device, including a photovoltaic module 1 according to any embodiment of the sixth aspect of the present application. By using the photovoltaic module 1, the transparency of the power generation device can be guaranteed, and the power generation device can have a high photoelectric conversion efficiency, which can be applied to application scenarios that require both transparency and conductivity.

[0685] Electrical appliances

[0686] Eighthly, this application also provides an electrical device 2.

[0687] like Figure 8 As shown, the electrical device 2 includes a photovoltaic module 1 according to any embodiment of the sixth aspect of this application.

[0688] Photovoltaic module 1 can be used as a power source for electrical device 2, or it can be used as an energy storage unit for photovoltaic module 1. Electrical device 2 can be, but is not limited to, mobile devices (such as mobile phones, laptops, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf carts, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc.

[0689] Figure 8 This is a schematic diagram of an example electrical device 2. The electrical device 2 is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle, etc. The electrical device 2 includes a photovoltaic module 1.

[0690] As another example, the electrical device 2 can be a mobile phone, tablet, laptop, etc.

[0691] Example

[0692] The following embodiments describe the disclosure of this application in more detail. These embodiments are merely illustrative, as various modifications and variations will be apparent to those skilled in the art within the scope of the disclosure of this application. Unless otherwise stated, all parts, percentages, and ratios reported in the following embodiments are based on weight, and all reagents used in the embodiments are commercially available or synthesized by conventional methods and can be used directly without further processing, and the instruments used in the embodiments are commercially available.

[0693] Preparation of the compound shown in Formula I1-2:

[0694] Step 1:

[0695] In a reaction vessel, add a mixture of (4-(bis([1,1'-biphenyl]-4-yl)amino)phenyl)boronic acid (0.42 mmol), 2,1,3-benzothiadiazole-4-carboxylic acid-7-bromo-methyl ester (0.5 mmol), tetra(triphenylphosphine)palladium Pd(PPh3)4 (15 mg, 0.021 mmol), and potassium carbonate (87 mg, 0.63 mmol) in tetrahydrofuran (THF) (14 mL) and water (2 mL) and heat under reflux overnight. After cooling to room temperature, extract the mixture with CH2Cl2 and dry the combined organic layers with anhydrous Na2SO4. After evaporating the solvent, purify the residue by column chromatography (silica gel, petroleum ether:CH2Cl2 = 1:1 as eluent) to a yield of 57%, as a dark red solid.

[0696] The reaction process is as follows:

[0697]

[0698] Step 2: This process involves heating the product from Step 1 with a mixture of potassium hydroxide (KOH) (1 mmol) in tetrahydrofuran (THF) (5 mL) and methanol (MeOH) at 70°C overnight. After cooling to room temperature, an equal volume of water is added, followed by the addition of 2 mol / L HCl (aqueous solution) to neutralize the mixture. Most of the methanol is removed by rotary evaporation, followed by extraction with dichloroisocyanurate, and the removal of water from the organic phase by adding anhydrous magnesium sulfate. The mixture is then filtered, concentrated, and purified by rapid column chromatography (silica gel, CH2Cl2:methanol volume ratio 10:1 as eluent) to obtain a yellow liquid in 80% yield, which is the reaction product. Figure 9 and Figure 10 The image shows the NMR spectrum of the reaction product. The horizontal axis represents the chemical shift in ppm, and the vertical axis represents the signal intensity. The peak positions and intensities reflect the characteristic information of the product.

[0699] The reaction process is as follows:

[0700]

[0701] Preparation of compounds represented by formula I1-3:

[0702] Step 1:

[0703] In a reaction vessel, add a mixture of 2-(diethoxyphosphoryl)pyridine-5-boronic acid pinacol ester (1 eq), 1,4-phenylenediamine, N1-(4-bromophenyl)-N1,N4,N4-triphenyl (CAS: 585540-48-3) (1 eq), tetra(triphenylphosphine)palladium Pd(PPh3)4 (0.04 eq), and potassium carbonate (2 eq) in tetrahydrofuran (THF) and water (7 / 1, v / v) and heat under reflux overnight. After cooling to room temperature, extract the mixture with CH2Cl2 and dry the combined organic layers with anhydrous Na2SO4. After evaporating the solvent, purify the residue by column chromatography (silica gel, petroleum ether:CH2Cl2 = 1:1 as eluent) to a yield of 70%, a yellow oily liquid.

[0704] The reaction process is as follows:

[0705]

[0706] Step 2:

[0707] Take a reaction vessel and dissolve the product (1 eq) from step 1 in 1,4-dioxane, then add trimethylbromosilane (10 eq) dropwise. Stir the reaction at 25°C for 22 hours under an argon atmosphere. Then, add methanol and continue stirring for 3 hours. Finally, add distilled water dropwise until the solution becomes opaque and stir overnight. If no solid precipitates, distill under reduced pressure until the liquid becomes turbid and add distilled water until solid precipitates. Filter the product, dissolve it in tetrahydrofuran, precipitate with n-hexane, wash the filtered product with n-hexane, filter and dry to give a light green solid, yield 50%. Figure 11 and Figure 12 The NMR spectrum of the reaction products is shown.

[0708] The reaction process is as follows:

[0709]

[0710] Preparation of the compound shown in Formula I2-1:

[0711] Step 1:

[0712] In a reaction vessel, add a mixture of 1,4-phenylenediamine, N1,N1,N4-triphenyl-N4-[4-(4,4,5,5-tetramethyl-1,3,2-dioxoboron-2-yl)phenyl]-(CAS1325614-39-8) (1 eq), diethyl (E)-2-(4-bromophenyl)vinylphosphonate (CAS:60585-76-4) (1 eq), tetra(triphenylphosphine)palladium Pd(PPh3)4 (0.04 eq), and potassium carbonate (2 eq) in tetrahydrofuran (THF) and water (7 / 1, v / v) and heat under reflux overnight. After cooling to room temperature, extract the mixture with CH2Cl2 and dry the combined organic layers with anhydrous Na2SO4. After evaporating the solvent, purify the residue by column chromatography (silica gel, petroleum ether:CH2Cl2 = 1:1 as eluent) to a yield of 80%, a yellow oily liquid.

[0713] The reaction process is as follows:

[0714]

[0715] Step 2:

[0716] The reaction steps are as shown in step 2 of the preparation of the compound in formula I1-3, and will not be repeated here; Figure 13 and Figure 14 The NMR spectrum of the reaction products is shown.

[0717]

[0718] Preparation of the compound shown in Formula I2-3:

[0719] Step 1:

[0720] Take a reaction vessel and add dibenzo[a,j]acridine, 7,14-dihydro (1 eq, CAS: 31054-34-9), methyl 2-(4-bromophenyl)quinoline-6-carboxylic acid (1 eq, CAS: 1204473-26-6), tris(dibenzylene-BASEacetone)dipalladium(0)Pd2(dba)3 (0.02 eq), tritert-butylphosphine (1M toluene solution, 0.1 eq), and cesium carbonate (2 eq). Add toluene to replace the air in the flask with Ar. The starting materials react overnight in toluene at 110°C for 12 h. After cooling to room temperature, extract the mixture with CH2Cl2 and dry the combined organic layers with anhydrous Na2SO4. After evaporating the solvent, purify the residue by column chromatography (silica gel, ethyl acetate: petroleum ether = 1:2 as eluent), yielding 52% as a yellow oily liquid.

[0721] The reaction process is as follows:

[0722]

[0723] Step 2:

[0724] The reaction steps are as shown in step 2 of the preparation of the compound in formula I1-3, and will not be repeated here; Figure 15 and Figure 16 The NMR spectrum of the reaction products is shown.

[0725] The reaction process is as follows:

[0726]

[0727] Preparation of the compound shown in Formula I3-2:

[0728] Step 1:

[0729] Take a reaction vessel and add 10,15-dihydro-5H-diindolo[3,2-A:3',2'-C]carbazole (CAS109005-10-9) (1 eq), (E)-2-(4-bromophenyl)vinylphosphonate diethyl ester (CAS:60585-76-4) (1 eq), tris(dibenzylacetone)dipalladium (0.02 eq), tritert-butylphosphine (0.08 eq), cesium carbonate (2 eq), and an appropriate amount of toluene. Purge the gas three times to create an inert atmosphere. Heat to 110°C and react overnight. The obtained product is extracted with saturated brine and water. The oil phase is dried over anhydrous magnesium sulfate, filtered, and concentrated. The final product is separated by column chromatography (CH...

[0730] 2Cl2 / EA = 3:1 (v / v), rotary evaporated, the final product was placed in an oven and vacuum dried at 70℃ for 12 h to obtain a yellow oily liquid with a yield of 50%.

[0731] The reaction process is as follows:

[0732]

[0733] Step 2:

[0734] The reaction steps are as shown in step 2 of the preparation of the compound in formula I1-3, and will not be repeated here; Figure 17 and Figure 18 The NMR spectrum of the reaction products is shown.

[0735] The reaction process is as follows:

[0736]

[0737] Preparation of the compound shown in Formula I3-1:

[0738] Step 1:

[0739] Take a reaction vessel and add ethyl 5-(4-bromophenyl)thiophene-2-carboxylate (2 eq, CAS: 19282-41-8), 5,7-dihydroindole[2,3-b]carbazole (1 eq, CAS: 111296-90-3), tris(dibenzylene-BASEacetone)dipalladium(0)Pd2(dba)3 (0.05 eq), tritert-butylphosphine (1M toluene solution, 0.2 eq), and cesium carbonate (4 eq). Add toluene to replace the air in the flask with Ar. The reactants are reacted overnight in toluene at 110°C for 12 h. After cooling to room temperature, the mixture is extracted with CH2Cl2, and the combined organic layers are dried with anhydrous Na2SO4. After evaporating the solvent, the residue is purified by column chromatography (silica gel, ethyl acetate: petroleum ether = 1:4 as eluent), yielding 60%, a deep yellow paste.

[0740] The reaction process is as follows:

[0741]

[0742] Step 2: The reaction steps are as shown in step 2 of the preparation of the compound represented by formula I1-3, and will not be repeated here; Figure 19 and Figure 20 The NMR spectrum of the reaction products is shown.

[0743] The reaction process is as follows:

[0744]

[0745] Preparation of the compound shown in Formula I4-1:

[0746] Step 1:

[0747] The synthesis process is the same as the first step of Formula I3-1, except that ethyl 5-(4-bromophenyl)thiophene-2-carboxylic acid is replaced with ethyl 4-[5-(4-chlorophenyl)-2-thiophene]benzoate (CAS: 480390-66-7);

[0748] The reaction process is as follows:

[0749]

[0750] Step 2:

[0751] The reaction steps are as shown in step 2 of the preparation of the compound in formula I1-3, and will not be repeated here; Figure 21 and Figure 22 The NMR spectrum of the reaction products is shown.

[0752] The reaction process is as follows:

[0753]

[0754] Preparation of the compound shown in Formula I4-2:

[0755] Step 1:

[0756] Diethyl (E)-2-(4-bromophenyl)vinylphosphonate (CAS: 60585-76-4) (1 eq) was dissolved in tetrahydrofuran and stirred at -78°C for 0.5 h under an argon atmosphere. Then, butyllithium (2.5 eq) was slowly added dropwise to the above system, and stirring was continued for 1 h after the addition. 2-Isopropoxy-4,4,5,5-tetramethyl-1,3,2-dioxaborane (4 eq) was added dropwise, and the reaction was carried out at -78°C for 1 h. Then, the temperature was raised to room temperature, and the product was poured into deionized water. It was then extracted three times with chloroform, and the organic phase was collected. The organic phases were combined, and water was removed by anhydrous magnesium sulfate. The solvent was removed by rotary evaporation. The product was recrystallized from isopropanol, and the precipitate was dissolved in chloroform and precipitated with methanol to obtain a yellow oily liquid with a yield of 82%.

[0757] The reaction process is as follows:

[0758]

[0759] Step 2:

[0760] Take a reaction vessel and add p-bromoiodobenzene (1 eq), the product of step 1 (1 eq), tetrakis(triphenylphosphine)palladium Pd(PPh3)4 (0.04 eq), and potassium carbonate (2 eq) in a mixture of tetrahydrofuran (THF) and water (7 / 1, v / v). Heat under reflux overnight. After cooling to room temperature, extract the mixture with CH2Cl2 and dry the combined organic layers with anhydrous Na2SO4. After evaporating the solvent, purify the residue by column chromatography (silica gel, ethyl acetate:CH2Cl2 = 1:3 as eluent) to a yield of 85%, as a yellow oily liquid.

[0761] The reaction process is as follows:

[0762]

[0763] Step (3): Referring to step (1) of formula I3-1, it will not be repeated here. The reaction process is as follows:

[0764]

[0765] Step (4): The hydrolysis process is referenced from step 2 of formula I-3, and will not be repeated here. The reaction process is as follows:

[0766]

[0767] Figure 23 and Figure 24 The NMR spectrum of the reaction products is shown.

[0768] Comparative Example 1:

[0769] (4-(3,6-dimethyl-9H-carbazole-9-yl)butyl)phosphonic acid Me-4PACz, CAS: 2747959-96-0, is represented by the compound shown in formula D-1, and its structural formula is as follows:

[0770]

[0771] Example: Fabrication of perovskite solar cells

[0772] (1) First electrode

[0773] One-third of a 1.5m×1.5cm FTO layer (FTO layer thickness of 500nm) was etched away using zinc powder and 1mol / L hydrochloric acid. The layer was then ultrasonically cleaned multiple times with acetone and isoacetone, immersed in deionized water and ultrasonically cleaned for 10 minutes, and finally dried with nitrogen gas for later use. The layer was then further cleaned in an ultraviolet ozone generator and used as the first electrode.

[0774] (2) Nickel oxide (NiO) x Preparation of hole transport layer

[0775] Nickel oxide (NiO) was spin-coated onto the surface of the first electrode at a speed of 5000 rpm. x The precursor of the nanoparticles (10 mg / mL, water as solvent) was then transferred to a constant temperature hot stage and heated at 100 °C for 15 min. After cooling to room temperature, a hole transport layer with a thickness of 20 nm was formed.

[0776] (3) Preparation of functional layers

[0777] An ethanol solution of 1 mg / mL self-assembled molecules was spin-coated onto the surface of the hole transport layer at a speed of 4000 rpm. The layer was then transferred to a constant temperature hot plate and heated at 100 °C for 10 min. After cooling to room temperature, a functional layer was formed.

[0778] (4) Preparation of perovskite light-absorbing layer

[0779] A precursor solution of 1.5 mol / L methylammonium lead iodide (CH3NH3PbI3, MAPbI3) was spin-coated onto the surface of the functional layer at a speed of 4000 rpm, with N,N-dimethylformamide (DMF) as the solvent. The layer was then transferred to a constant temperature hot plate and heated at 100 °C for 30 min. After cooling to room temperature, a perovskite light-absorbing layer with a thickness of 500 nm was formed.

[0780] (5) Fabrication of electron transport layer and second electrode

[0781] A 30 nm C60 layer, a 7 nm BCP layer, and a 60 nm Cu electrode (as the second electrode) were sequentially deposited on the perovskite light-absorbing layer at a deposition rate of 0.1 A / s to obtain a perovskite solar cell device.

[0782] After the perovskite solar cell device is prepared, a layer of encapsulating adhesive can be applied around the device and on its surface. The encapsulating adhesive is a colorless and transparent epoxy resin adhesive. A glass backing layer is then covered on the encapsulating adhesive and pressed together. After standing for 2 hours, the encapsulating adhesive is cured, and the perovskite solar cell is obtained.

[0783] Among them, the self-assembled molecules of Examples 1 to 8 are made of different materials, and the functional layers of Examples 1, 9 and 10 are made of different thicknesses.

[0784] Comparative Example 1

[0785] Perovskite solar cells were prepared using a method similar to that of Example 1, except that the material of the functional layer was adjusted.

[0786] Comparative Example 2

[0787] Perovskite solar cells were prepared using a method similar to that in Example 1. However, unlike Example 1, no functional layer was provided; instead, a perovskite light-absorbing layer was directly deposited on the surface of the hole transport layer.

[0788] Examples 11 and 12

[0789] Perovskite solar cells were fabricated using a method similar to that of Example 1, except that a nickel oxide hole transport layer was not included. The fabrication steps of the perovskite solar cells include:

[0790] (1) First electrode

[0791] One-third of a 1.5m×1.5cm FTO layer (FTO layer thickness of 500nm) was etched away using zinc powder and 1mol / L hydrochloric acid. The layer was then ultrasonically cleaned multiple times with acetone and isoacetone, immersed in deionized water and ultrasonically cleaned for 10 minutes, and finally dried with nitrogen gas for later use. The layer was then further cleaned in an ultraviolet ozone generator and used as the first electrode.

[0792] (2) Preparation of functional layers

[0793] An ethanol solution of 1 mg / mL self-assembled molecules was spin-coated onto the surface of the hole transport layer at a speed of 4000 rpm. The layer was then transferred to a constant temperature hot plate and heated at 100 °C for 10 min. After cooling to room temperature, a functional layer was formed.

[0794] (3) Preparation of perovskite light-absorbing layer

[0795] A precursor solution of 1.5 mol / L methylammonium lead iodide (CH3NH3PbI3, MAPbI3) was spin-coated onto the surface of the functional layer at a speed of 4000 rpm, with DMF as the solvent. The layer was then transferred to a constant temperature hot plate and heated at 100 °C for 30 min. After cooling to room temperature, a perovskite light-absorbing layer with a thickness of 500 nm was formed.

[0796] (4) Fabrication of electron transport layer and second electrode

[0797] A 30 nm C60 layer, a 7 nm BCP layer, and a 60 nm Cu electrode (as the second electrode) were sequentially deposited on the perovskite light-absorbing layer at a deposition rate of 0.1 A / s to obtain a perovskite solar cell device.

[0798] After the perovskite solar cell device is prepared, a layer of encapsulating adhesive can be applied around the device and on its surface. The encapsulating adhesive is a colorless and transparent epoxy resin adhesive. A glass backing layer is then covered on the encapsulating adhesive and pressed together. After standing for 2 hours, the encapsulating adhesive is cured, and the perovskite solar cell is obtained.

[0799] The self-assembled molecules in Examples 11 and 12 are made of different materials.

[0800] Performance testing

[0801] 1. Photoelectric conversion efficiency

[0802] Under normal temperature and pressure, a standard AM1.5G solar light source, conforming to the national standard IEC61215, was used for testing. Crystalline silicon solar cells were used to correct the light intensity to achieve a solar intensity. A four-channel digital source meter (Keithley 2440) was used to measure the current-voltage characteristic curve of the solar cells under illumination, obtaining the open-circuit voltage Voc, short-circuit current density Jsc, fill factor FF, and photoelectric conversion efficiency Eff. The photoelectric conversion efficiency is calculated as follows:

[0803] Eff = Pout / Pin × 100%, where Pout and Pin are the operating output power and incident light power of the perovskite solar cell, respectively, and the incident light power is 100mW / cm². 2 .

[0804] The photoelectric conversion efficiency obtained from the test is used as the initial efficiency.

[0805] 2. Device stability determination

[0806] After the photoelectric conversion efficiency test, the perovskite solar cell was placed in an atmospheric environment (relative humidity 65-85%, ambient temperature approximately 15-40℃) and left in the dark for 500 hours. The photoelectric conversion efficiency was then tested again (each test continued until forward and reverse scans showed no hysteresis, and the photoelectric conversion efficiency was recorded). The ratio of the photoelectric conversion efficiency of the perovskite solar cell after 500 hours of atmospheric exposure to the initial efficiency was calculated and used as the normalized efficiency of the solar cell after 500 hours of exposure.

[0807] Initial normalized efficiency = retest efficiency / initial efficiency * 100%.

[0808] The test results are shown in Table 1.

[0809] Table 1

[0810]

[0811] In Comparative Example 2, no functional layer was set between the hole transport layer and the perovskite light-absorbing layer. Side reactions may occur at the interface between the hole transport layer and the perovskite light-absorbing layer, and the perovskite material in the perovskite light-absorbing layer may decompose, resulting in poor device stability and photoelectric conversion efficiency of the perovskite solar cell.

[0812] Compared to Comparative Example 2, Comparative Example 1 has a functional layer between the hole transport layer and the perovskite light-absorbing layer. The functional layer includes Me-4PACz. The Me-4PACz has poor conductivity, which results in poor passivation effect and carrier migration performance, thus limiting the improvement in device stability and photoelectric conversion efficiency of the perovskite solar cell.

[0813] The self-assembled molecules provided in the functional layer of this application embodiment also include conjugated groups, which make the electron cloud distributed throughout the molecule, thereby improving the conductivity and intrinsic stability of the self-assembled molecules. When applied to perovskite solar cells, this can improve device stability and photoelectric conversion efficiency.

[0814] Experiments have shown that using self-assembled molecules of different materials can effectively improve the device stability and photoelectric conversion efficiency of perovskite solar cells. Furthermore, functional layer thicknesses ranging from 0.1 nm to 20 nm all effectively improve the device stability and photoelectric conversion efficiency of perovskite solar cells.

[0815] Furthermore, the functional layer in this embodiment also has hole transport function and can be used as a hole transport layer. When the thickness of the functional layer is 1nm to 30nm, it can effectively improve the device stability and photoelectric conversion efficiency of perovskite solar cells.

[0816] Although illustrative embodiments have been demonstrated and described, those skilled in the art should understand that the above embodiments should not be construed as limiting the implementation of the present application, and that changes, substitutions and modifications can be made to the embodiments without departing from the spirit, principles and scope of the implementation of the present application.

Claims

1. A perovskite solar cell comprising a first electrode, a functional layer, a perovskite light-absorbing layer, and a second electrode, which are stacked in a thickness direction of the perovskite solar cell, the functional layer comprising a self-assembled molecule, the self-assembled molecule comprising one or more of a structural formula represented by Formula I1, a structural formula represented by Formula I2, a structural formula represented by Formula I3, or a structural formula represented by Formula I4. wherein The self-assembled molecule comprises a structural formula represented by Formula I1. In Formula I1, Ar1 represents a hole-extracting group having 10 to 30 ring-forming atoms. D1 includes a substituted or unsubstituted heteroarylene group, or a substituted or unsubstituted alkenylene group. E1 represents an oxygen-containing group. n1 represents the number of linking sites of D1 and Ar1, and n1 is any positive integer of 1 to 8. The self-assembled molecule comprises a structural formula represented by Formula I2. In Formula I2, Ar2 represents a hole-extracting group having 10 to 30 ring-forming atoms. E2 represents an oxygen-containing group. D 21 and D 22 one of which comprises a substituted or unsubstituted arylene group, or a substituted or unsubstituted arylheterocycle group;D 21 and D 22 the other of which comprises a substituted or unsubstituted arylheterocycle group, or a substituted or unsubstituted alkenylene group; The self-assembled molecule comprises a structural formula represented by Formula I3. n2 represents D 21 the number of attachment sites of Ar2, n2, is any positive integer from 1 to 8; In Formula I3, Ar3 represents a hole-extracting group having 31 to 60 ring-forming atoms. D3 includes a substituted or unsubstituted arylene group, a substituted or unsubstituted heteroarylene group, or a substituted or unsubstituted alkenylene group. E3 represents an oxygen-containing group. n3 represents the number of linking sites of D3 and Ar3, and n3 is any positive integer of 2 to 8. The self-assembled molecule comprises a structural formula represented by Formula I4. In Formula I4, Ar4 represents a hole-extracting group having 31 to 60 ring-forming atoms. E4 represents an oxygen-containing group. D 41 and D 42 each independently comprises a substituted or unsubstituted arylene group, a substituted or unsubstituted heteroarylene group, or a substituted or unsubstituted alkenylene group; n4 represents D 41 the number of attachment sites of Ar4and n4 is any positive integer from 2 to 8; The hole-extracting group having 10 to 30 ring-forming atoms includes a substituted or unsubstituted aniline group having 10 to 30 ring-forming atoms, a substituted or unsubstituted acridine group having 10 to 30 ring-forming atoms, 2. The perovskite solar cell of claim 1, wherein, In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. The substituted or unsubstituted aniline group having 10 to 30 ring-forming atoms includes a structure represented by Formula A1, 3. The perovskite solar cell of claim 2, wherein, In Formula A1, In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. M 11 and M 12 each independently comprises a substituted or unsubstituted aromatic group having a ring-forming atom number of C5 to C15; M 13 comprising a substituted or unsubstituted arylene group having a ring-forming atom number of C5 to C15; In the formula, 4. The perovskite solar cell of claim 3, wherein, The substituted or unsubstituted aniline-based group having a ring-forming atom number of C10 to C30 includes a substituted or unsubstituted formula A 1-1 one or more of the structures shown to a substituted or unsubstituted formula A 1-5 one or more of the structures shown to a substituted or unsubstituted formula A s1, s2, s3, and s4 are any integer of 0 to 3, and s1, s2, s3, and s4 are not simultaneously 0 in the same structural formula. * denotes the linking site of the hole-extracting group to D1, or * denotes the linking site of the hole-extracting group to D 21 ; The substituted or unsubstituted acridine group having 10 to 30 ring-forming atoms includes a structure represented by Formula A2, 5. The perovskite solar cell of claim 2, wherein, In Formula A2, In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. M 21 comprises a single bond, a substituted or unsubstituted C6to C15arylene group, or a substituted or unsubstituted C5to C15heteroarylene group; M 22 and M 23 each independently comprises a substituted or unsubstituted C6 to C15 aromatic hydrocarbon group, or a substituted or unsubstituted C6 to C15 aromatic heterocyclic group; In the formula, 6. The perovskite solar cell of claim 5, wherein, The substituted or unsubstituted acridine-based group having a ring-forming atom number of C10 to C30 includes a substituted or unsubstituted formula A 2-1 one or more of the structures shown to a substituted or unsubstituted formula A 2-3 one or more of the structures shown to a substituted or unsubstituted formula A s1, s2 are any integer of 0 to 3, and s1, s2 are not simultaneously 0 in the same structural formula. * denotes the linking site of the hole-extracting group to D1, or * denotes the linking site of the hole-extracting group to D 21 ; The hole-extracting group having 31 to 60 ring-forming atoms includes a substituted or unsubstituted carbazole group having 31 to 60 ring-forming atoms, 7. The perovskite solar cell according to any one of claims 1 to 6, wherein ​ In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group.

8. The perovskite solar cell of claim 7, wherein, The substituted or unsubstituted carbazole group having a ring-forming atom number of C31 to C60 includes a structure represented by Formula B1, In Formula B1, S 20 comprises a single bond, a substituted or unsubstituted C6 to C30 arylene group, or a substituted or unsubstituted C5 to C30 heteroarylene group; S 21 and S 22 each independently comprises a substituted or unsubstituted C6 to C30 aromatic hydrocarbon group, or a substituted or unsubstituted C6 to C30 nitrogen-containing aromatic heterocyclic group; In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group.

9. The perovskite solar cell according to claim 8, wherein, The substituted or unsubstituted carbazolyl group having a ring-forming atom number of C31 to C60 includes a substituted or unsubstituted formula B 1-1 one or more of the structures shown to a substituted or unsubstituted formula B 1-6 one or more of the structures shown to a substituted or unsubstituted formula B In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. * denotes the site of attachment of the hole-extracting group to D3, or * denotes the site of attachment of the hole-extracting group to D 41 ; s1, s2, s3, s4, s5, and s6 are any one of 0 to 3, and s1, s2, s3, s4, s5, and s6 are not simultaneously 0 in the same structural formula.

10. The perovskite solar cell according to any one of claims 1 to 9, wherein D1 includes a substituted or unsubstituted aromatic heterocyclic group; or D 21 and one of D 22 includes a substituted or unsubstituted arylene group, or a substituted or unsubstituted heteroarylene group;D 21 and the other of D 22 includes a substituted or unsubstituted heteroarylene group; or D3 includes a substituted or unsubstituted aromatic hydrocarbon group, or a substituted or unsubstituted aromatic heterocyclic group; or D 41 and D 42 each independently comprises a substituted or unsubstituted arylene group, or a substituted or unsubstituted heteroarylene group.

11. The perovskite solar cell according to any one of claims 1 to 10, wherein D 21 , D 22 , D3, D 41 and D 42 each independently comprises a substituted or unsubstituted arylene group comprising a substituted or unsubstituted arylene group having a ring-forming atom count of C6to C15.

12. The perovskite solar cell of claim 11, wherein, The substituted or unsubstituted arylene group having a ring-forming atom number of C6to C15includes a substituted or unsubstituted formula G 1-1 one or more of the structures shown 1-3 one or more of the structures shown wherein * indicates D 21 , D3, D 41 one of R1, R2, R3, R4, R5, R6, R7, R8, R9, R10, R11, R12, R13, R14, R15, R16, R17, R18, R19, R20, # represents D 22 , D3, D 42 one of which is the point of attachment to the oxygen-containing group.

13. The perovskite solar cell according to any one of claims 1 to 12, wherein, D1, D 21 , D 22 , D3, D 41 and D 42 each independently includes a substituted or unsubstituted aromatic heterocyclic group, the substituted or unsubstituted aromatic heterocyclic group including a substituted or unsubstituted aromatic heterocyclic group having a ring-forming atom number of C5 to C15, the ring-forming atom in the substituted or unsubstituted aromatic heterocyclic group having a ring-forming atom number of C5 to C15 further including one or more atoms of nitrogen, oxygen, sulfur.

14. The perovskite solar cell according to claim 13, wherein The ring-forming atom in the substituted or unsubstituted aromatic heterocyclic group having a ring-forming atom number of C5 to C15 includes a nitrogen atom, The substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 includes substituted or unsubstituted formula G. 2-1 The structure shown is used for substituted or unsubstituted formula G. 2-9 One or more of the structures shown, In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. * indicates the connecting site of one of D1, D 21 , D3, D 41 and the hole-extracting group; # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group; and / or The ring-forming atom in the substituted or unsubstituted aromatic heterocyclic group having a ring-forming atom number of C5 to C15 includes an oxygen atom, The substituted or unsubstituted aromatic heterocyclic group having a cyclic number of C5 to C15 includes substituted or unsubstituted formula G. 3-1 The structure shown is used for substituted or unsubstituted formula G. 3-3 One or more of the structures shown, In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. * indicates the connecting site of one of D1, D 21 , D3, D 41 and the hole-extracting group; # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group; and / or The ring-forming atom in the substituted or unsubstituted aromatic heterocyclic group having a ring-forming atom number of C5 to C15 includes a nitrogen, oxygen, sulfur atom, The substituted or unsubstituted heteroaromatic ring group having a ring atom number of C5 to C15 includes a substituted or unsubstituted formula G 4-1 one or more of the structures shown below to a substituted or unsubstituted formula G 4-3 one or more of the structures shown below to a substituted or unsubstituted formula G In the case where the above group is substituted, the substituent group includes one or more of an amine group, a halogen group, an alkylthio group, an oxygen-containing substituent group, or a C1 to C5 alkyl group. * indicates the connecting site of one of D1, D 21 , D3, D 41 and the hole-extracting group; # indicates D1, D 22 D3, D 42 One of them is the connection site with the oxygen-containing group; The substituted or unsubstituted C2 to C6 chain alkenylene group includes a vinylene group, a propenylene group, or a butenylene group. The oxygen-containing group includes one or more of a carboxylic acid group, a phosphorous acid group, a phosphoric acid group, a sulfonic acid group, a silicic acid group, a siloxane group, a boronic acid group, a carboxylate group, a phosphonate group, a sulfonate group, a silicate group, a borate group, a carboxylate, a phosphite, a phosphate, a borate, or a silicate. The substituted or unsubstituted heteroaromatic ring group having a ring atom number of C5 to C15 includes a substituted or unsubstituted formula G 5-1 one or more of the structures shown to a substituted or unsubstituted formula G 5-7 one or more of the structures shown to a substituted or unsubstituted formula G The oxygen-containing group includes one or more of a carboxylic acid group, a phosphoric acid group, a boronic acid group, a carboxylate, a phosphate, or a borate. * indicates the connecting site of one of D1, D 21 , D3, D 41 and the hole-extracting group; represents one of D1, D 22 , D3, D 42 one of which is the point of attachment to the oxygen-containing group.

15. The perovskite solar cell according to any one of claims 1 to 14, wherein, D1, D 21 , D 22 , D3, D 41 and D 42 each independently includes a substituted or unsubstituted alkenylene group including a substituted or unsubstituted C2to C6chain alkenylene group, or a substituted or unsubstituted cyclic alkenylene group having a ring atom number of C5to C15, The self-assembled molecule includes one or more of a compound represented by Formula I1-1 to a compound represented by Formula I4-2, 16. The perovskite solar cell of claim 15, wherein, The functional layer is disposed on the first electrode, and is in contact with at least a part of a surface of the first electrode.

17. The perovskite solar cell according to any one of claims 1 to 16, wherein, The thickness of the functional layer is 1 nm to 30 nm.

18. The perovskite solar cell of claim 17, wherein, 22. The perovskite solar cell according to any one of claims 1 to 19, further comprising a hole transport layer, the functional layer being between the hole transport layer and the perovskite light-absorbing layer.

19. The perovskite solar cell according to any one of claims 1 to 18, wherein, The thickness of the functional layer is 0.1 nm to 20 nm.

20. The perovskite solar cell according to any one of claims 1 to 19, wherein, The hole transport layer includes a hole transport material, 21. The perovskite solar cell of claim 20, wherein, ​ ​ 23. The perovskite solar cell of claim 22, wherein, ​ 24. The perovskite solar cell of claim 22 or 23, wherein, ​ The hole transport material includes a hole transport organic material, the hole transport organic material includes one or more of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], poly(3,4-ethylenedioxythiophene)-polystyrene sulfonic acid, 2,2',7,7'-tetrakis[N,N-bis(4-methoxyphenyl)amino]-9,9'-spirobifluorene, poly-3-hexylthiophene, methoxytriphenylamine-fluoromethylformamide, triptycene-core triphenylamine, 3,4-ethylenedioxythiophene-methoxytriphenylamine, N-4-anilinocarbazole-spirobifluorene, polythiophene, phosphonic acid-based monomer, carboxylic acid-based monomer, carbazolyl-based monomer, sulfonic acid-based monomer, triphenylamine-based monomer, aromatic-based monomer; and / or The hole transport layer includes a hole transport inorganic material, the hole transport inorganic material includes one or more of metal oxide, cuprous iodide, and cuprous thiocyanate.

25. The perovskite solar cell according to any one of claims 1 to 24, wherein, The perovskite light-absorbing layer includes a perovskite material, the perovskite material includes one or more of a compound of a molecular formula of ABX3 or M2CDN6, A and M each independently comprise one or more of Li + , Na + , K + , Rb + , Cs + , a methylamine cation, an ethylamine cation, a propylamine cation, a butylamine cation, a pentylamine cation, a hexylamine cation, a formamidinium cation, or an imidazolium cation; B comprises one or more of the cations Ca 2+ , Sr 2+ , Cd 2+ , Cu 2+ , Ni 2+ , Mn 2+ , Fe 2+ , Co 2+ , Pd 2+ , Ge 2+ , Sn 2+ , Pb 2+ , Sn 2+ , Yb 2+ , and Eu 2+ . X and N each independently comprise one or more of F - , Cl - , Br - , or I - ; C comprises Cs + , Ag + , K + or Ru + one or more. D comprises one or more of Bi 3+ , Ni 3+ , Fe 3+ , Sb 3+ , In 3+ , or Cu 3+ .

26. The perovskite solar cell of any one of claims 1 to 25, further comprising an electron transport layer between the perovskite light-absorbing layer and the second electrode.

27. A photovoltaic module comprising one or more perovskite solar cells of any one of claims 1 to 26.

28. A power generation apparatus comprising the photovoltaic module of claim 27.

29. An electric device comprising the photovoltaic module of claim 27.

30. A self-assembled molecule, the self-assembled molecule includes one or more of a structural formula of Formula I1, a structural formula of Formula I2, a structural formula of Formula I3, a structural formula of Formula I4, The self-assembled molecule includes a structural formula of Formula I1, In Formula I1, Ar1 represents a hole extraction group having a ring atom number of C10 to C30; D1 includes a substituted or unsubstituted heteroarylene group, or a substituted or unsubstituted alkenylene group; E1 represents an oxygen-containing group; n1 represents a number of connection sites of D1 and Ar1, n1 is any positive integer from 1 to 8; The self-assembled molecule includes a structural formula of Formula I2, In Formula I2, Ar2 represents a hole extraction group having a ring atom number of C10 to C30; D 21 and D 22 one of R1and R2comprises a substituted or unsubstituted arylene group, or a substituted or unsubstituted aromatic heterocyclic group;D 21 and D 22 the other of R1and R2comprises a substituted or unsubstituted aromatic heterocyclic group, or a substituted or unsubstituted alkenyl group; E2 represents an oxygen-containing group; n2 represents D 21 the number of attachment sites of Ar2, n2, is any positive integer from 1 to 8; The self-assembled molecule includes a structural formula of Formula I3, In Formula I3, Ar3 represents a hole extraction group having a ring atom number of C31 to C60; D3 includes a substituted or unsubstituted aralkylene group, a substituted or unsubstituted heteroarylene group, or a substituted or unsubstituted alkenylene group; E3 represents an oxygen-containing group; n3 represents a number of connection sites of D3 and Ar3, n3 is any positive integer from 2 to 8; The self-assembled molecule includes a structural formula of Formula I4, In Formula I4, Ar4 represents a hole extraction group having a ring atom number of C31 to C60; D 41 and D 42 each independently comprises a substituted or unsubstituted arylene group, a substituted or unsubstituted heteroarylene group, or a substituted or unsubstituted alkenylene group; n4 represents D 41 the number of attachment sites of Ar4and n4 is any positive integer from 2 to 8; E4 represents an oxygen-containing group.

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