Method, device, electronic device and storage medium for screening organic cations for electrochemical ammonia synthesis

Abstract

The present application relates to a method, apparatus, electronic device, storage medium for screening organic cations for electrochemical ammonia synthesis, and an electrolyte containing the organic cations. The method for screening organic cations for electrochemical ammonia synthesis includes: (1) constructing a primary molecular library composed of a plurality of organic cations; (2) filtering the primary molecular library based on the molecular structural characteristics of the organic cations to obtain a secondary molecular library; (3) respectively determining the quantified values of the deprotonation energy, vertical electron affinity, and hydrophobicity for the compounds in the secondary molecular library; (4) selecting the candidate organic cations from the secondary molecular library based on the quantified values. By using this method, the efficiency of screening organic cations can be effectively improved by gradually screening the characteristic parameters of the compounds, and the obtained organic cations have the ability to act as proton donors, thus contributing to improving the yield of electrochemical ammonia synthesis.

Description

Technical Field

[0001] The present application relates to the field of chemistry. Specifically, the present application relates to a method, apparatus, electronic device, storage medium for screening organic cations for electrochemical ammonia synthesis, and an electrolyte containing such organic cations. Background Art

[0002] Ammonia is one of the most important chemical commodities globally and is particularly important for the production of fertilizers for agricultural purposes. Additionally, since liquid ammonia has a higher energy density than liquid hydrogen (11.5 MJ / L vs. 8.5 MJ / L) and is also much higher than the energy density of more commonly used compressed hydrogen (4.5 MJ / L). Therefore, the application of liquid ammonia in fuel cell electric vehicles is also attractive, and the market size of liquid ammonia is expected to grow to 1.4 trillion in 2028.

[0003] Currently, the mainstream process for ammonia production is still the Haber-Bosch process (developed in 1910), that is, nitrogen and hydrogen react at high temperature and high pressure using a metal catalyst to produce ammonia. This process is very energy-consuming and emits a large amount of carbon dioxide. Generally speaking, when producing one ton of ammonia using the Haber-Bosch process, 1.87 tons of carbon dioxide need to be emitted.

[0004] One of the most ideal alternative methods for ammonia production is through electrochemical catalysis. Briefly, first, nitrogen is dissolved in the electrolyte and adsorbed onto the surface of the catalyst metal (usually Li), and the following electrochemical reaction occurs with protons at the electrode to produce NH3: N2 + 6H + + 6e - = 2NH3. However, the yield of such electrochemical reactions has been very low in the past (<1 nmol s -1 cm -2 ), which is about two orders of magnitude lower than the yield required for commercial ammonia production.

[0005] Therefore, the current process for electrochemical ammonia synthesis still needs to be improved. Summary of the Invention

[0006] Embodiments of the present application provide a method, apparatus, electronic device, storage medium for screening organic cations for electrochemical ammonia synthesis, and an electrolyte containing such organic cations. By gradually screening the characteristic parameters of compounds, the efficiency of screening organic cations can be effectively improved, and the obtained organic cations have the ability to act as proton donors, thus contributing to improving the yield of electrochemical ammonia synthesis.

[0007] In a first aspect of the present application, embodiments of the present application propose a method for screening organic cations for electrochemical ammonia synthesis, including:

[0008] (1) Construct a primary molecular library composed of multiple organic cations;

[0009] (2) Filter the primary molecular library based on the molecular structural characteristics of the organic cations to obtain a secondary molecular library;

[0010] (3) For the compounds in the secondary molecular library, determine the quantified values of deprotonation energy, vertical electron affinity, and hydrophobicity respectively;

[0011] (4) Select candidate organic cations from the secondary molecular library based on the quantified values.

[0012] In the second aspect of the present application, an embodiment of the present application provides an electrolyte for electrochemical ammonia synthesis, which is characterized by containing: an organic cation, and the organic cation is obtained by the method described in the first aspect.

[0013] In the third aspect of the present application, an embodiment of the present application provides a device for screening organic cations for electrochemical ammonia synthesis, including: a primary molecular library construction unit for constructing a primary molecular library composed of multiple organic cations; a secondary molecular library construction unit for filtering the primary molecular library based on predetermined molecular structural characteristics to obtain a secondary molecular library; a quantum chemistry analysis unit for determining the quantified values of deprotonation energy, vertical electron affinity, and hydrophobicity respectively for the compounds in the secondary molecular library; and an organic cation determination unit for selecting the candidate organic cations from the secondary molecular library based on the quantified values.

[0014] In the fourth aspect of the present application, an embodiment of the present application provides an electronic device, including:

[0015] a processor adapted to implement computer instructions; and,

[0016] a memory storing computer instructions, and the computer instructions are adapted to be loaded and executed by the processor to perform the method in the first aspect above.

[0017] In the fifth aspect of the present application, an embodiment of the present application provides a computer-readable storage medium, and the computer-readable storage medium stores computer instructions, and when the computer instructions are read and executed by the processor of the computer device, the computer device is enabled to execute the method in the first aspect above.

[0018] In the sixth aspect of the present application, an embodiment of the present application provides a computer program product or a computer program. The computer program product or the computer program includes computer instructions, and the computer instructions are stored in a computer-readable storage medium. A processor of a computer device reads the computer instructions from the computer-readable storage medium, and the processor executes the computer instructions, so that the computer device executes the method in the first aspect above.

[0019] Through the above technical solution, by filtering existing compounds based on molecular structure characteristics and screening based on quantum chemical properties, candidate organic cations can be effectively obtained. These organic cations can be used as proton donors, thereby effectively improving the efficiency of screening organic cations, and the obtained organic cations have the ability to be proton donors, thus contributing to improving the yield of electrochemical ammonia synthesis. BRIEF DESCRIPTION OF THE DRAWINGS

[0020] Figure 1 An alternative schematic diagram of a method for screening organic cations for electrochemical ammonia synthesis according to an embodiment of the present application;

[0021] Figure 2 A schematic block diagram of a device for screening organic cations for electrochemical ammonia synthesis provided by an embodiment of the present application;

[0022] Figure 3 An alternative schematic diagram of another method for screening organic cations for electrochemical ammonia synthesis according to an embodiment of the present application;

[0023] Figure 4 A schematic block diagram of an electronic device provided by an embodiment of the present application. DETAILED DESCRIPTION OF THE EMBODIMENTS

[0024] Next, the technical solutions in the embodiments of the present application will be clearly and completely described in conjunction with the accompanying drawings in the embodiments of the present application. The described embodiments should not be regarded as limitations on the present application. All other embodiments obtained by those of ordinary skill in the art without creative efforts shall fall within the scope of protection of the present application.

[0025] In the following description, the terms "first / second" involved are only used to distinguish similar objects and do not represent a specific order for the objects. It can be understood that "first / second" can be interchanged with a specific order or sequence when permitted, so that the embodiments of the present application described here can be implemented in an order other than that illustrated or described here.

[0026] Quantum chemistry focuses on electrons and reflects properties that depend on the electron distribution. It is particularly suitable for studying the formation and breakage of chemical bonds. The technical solution provided in this application can perform high-throughput screening from a vast compound database to obtain candidate organic cations that can be used for electrochemical ammonia synthesis. These organic cations have quantum chemical properties suitable for electrochemical ammonia synthesis. Using the solution provided in this application can save a large amount of time for experimental screening and improve the success rate of experimental verification.

[0027] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by those skilled in the technical field to which this application belongs. The terms used herein are only for the purpose of describing the embodiments of this application and are not intended to limit this application. Before further elaborating on the embodiments of this application, the nouns and terms involved in the embodiments of this application are first explained, and the nouns and terms involved in the embodiments of this application are applicable to the following explanations.

[0028] The term "electrochemical synthesis" used herein refers to a means of synthesizing specific chemical substances by electrocatalytic methods. In this article, electrochemical synthesis is used for ammonia synthesis. Since an electric current is used as the electron source, generally, electrochemical synthesis can avoid using toxic or dangerous reagents, protecting groups, and catalysts commonly used in organic synthesis or inorganic synthesis. In addition, electrochemical synthesis can reduce or eliminate the reactor cooling or heating process and reduce energy consumption.

[0029] The term "electrocatalysis" used herein refers to a catalytic effect that accelerates the charge transfer at the electrode-electrolyte interface. Generally speaking, an electrochemical reaction occurs at the electrode-electrolyte interface, where the electrode usually acts as both an electron donor / acceptor and a catalyst to promote the occurrence of the electrochemical reaction.

[0030] The term "electrolyte" or "electrolytic solution" used herein refers to a liquid usually used in an electrocatalytic device. The electrodes of the electrocatalytic device are arranged in the electrolyte.

[0031] The term "cation" used herein is a positively charged molecule / atom, and "anion" is a negatively charged molecule / atom. Cations or anions are usually labeled with charges such as +1, +2, -1, -2, etc., which correspond to the amount of charge held by the molecule / atom and are multiples of the electron charge e (1.602×10 -19 Coulomb). "Salt" is a compound composed of cations and anions with a total charge of 0. For example, ammonium chloride (NH4Cl) is an example of a salt, which is composed of the organic cation NH4 + and the anion Cl - combined.

[0032] The term "molecular structure feature" as used herein refers to a feature that can be determined or calculated based on the chemical composition of an organic molecule, such as including but not limited to molecular charge, molecular weight, topological polar surface area, number of heavy atoms, number of hydrogen bond donors, and atomic constitution of the molecule. Such analysis is also referred to as "chemoinformatics analysis" in this article. Usually, most of such data of compounds are also recorded in common databases, or can be obtained through some common chemoinformatics software, such as RDKit (https: / / www.rdkit.org / ).

[0033] The term "quantum chemical analysis" as used herein is a computational materials science simulation method that uses actual electron wave functions to calculate the energy levels of electrons in a molecule and the total energy of the system. This simulation method can calculate commonly used material properties such as deprotonation energy, vertical electron affinity (VEA), and LogP with high precision. Different from the aforementioned "chemoinformatics analysis", "quantum chemical analysis" requires a large amount of calculations or quantum chemical simulation experiments, and the amount of calculation and time consumed are also much greater than chemoinformatics analysis.

[0034] The term "quantum chemical simulation" as used herein is a method of numerically simulating molecular chemical reactions by computer. Through quantum mechanics, precise calculation and prediction of chemical processes (such as the formation of chemical bonds) can be carried out, opening up many new fields of chemical research. Usually, a quantum computer is used to perform the above simulation process. A quantum computer has advantages that cannot be compared with traditional computers, with powerful computing capabilities, and can realize the simulation of any complex chemical process. For a detailed introduction to quantum chemical simulation, reference can be made to SCIENCE 28 Aug 2020 Vol 369, Issue 6507 pp. 1084 - 108, or the relevant quantum chemical simulation process can be carried out using OpenFermion (https: / / quantumai.google / openfermion).

[0035] The term "deprotonation energy" as used herein is a parameter used to characterize the proton affinity of an organic cation, that is, the energy required to release a proton from an organic cation and convert it into a neutral molecule. In this article, the deprotonation energy of cation P+ is approximated by the chemical reaction P0 (P++I-→P0+HI) from the iodide salt form of the organic cation to the neutral form of the cation:

[0036] E deprotonation (P + )≈E 0 (P 0 ,gas)-E + (P + ,gas)+E 0(HI,gas)-E - (I - ,gas) These energies are calculated using quantum chemical simulations. E0, E-, and E+ correspond to the energies obtained when the total charge of the molecule is set to 0, -1, and +1, respectively, in the quantum chemical simulation. + refers to a cationic molecule in a +1 charge state, while P0 corresponds to a deprotonated cationic molecule, making it in a 0 charge state. - and HI are iodine anions and hydroiodic acid, their energies are simple constants, and they are related to the organic cation P + The choice of deprotonation energy (P + ) is larger, the cation P + The more difficult it is to release the proton in order to become a neutral molecule P 0 .

[0037] The term "vertical electron affinity (VEA)" as used herein is a parameter that characterizes the electron affinity of an organic cation, i.e., the electron addition to the organic cation P + The energy required to convert it into a typical metastable neutral molecule (with unpaired electrons in its molecular orbitals) is the energy required to convert it into a typical metastable neutral molecule (with unpaired electrons in its molecular orbitals). This addition of electrons does not change the atomic composition of the cation, but it does change the electronic state and the corresponding charge. The energy required to add electrons to the cation without changing the geometric conformation of the molecule is a key parameter because it represents the energy barrier that needs to be overcome to trigger the cascade chemical reaction on the cation. In this article, the following equation is used to approximate this value:

[0038] E VEA (P + )≈E 0 (P + ,gas)-E + (P + ,gas)

[0039] The energy values here are also calculated using quantum chemical simulations. 0 and E + correspond to the energies obtained when the total charge of the molecule is set to 0 and +1 in quantum chemistry simulations, respectively. + Refers to a cationic molecule in a +1 charge state. The higher the EVEA value, the more difficult it is for a chemical reaction to occur on the organic cation. Therefore, a cation with a higher VEA + Will be more electrochemically stable.

[0040] The term "LogP" used in this article is a parameter that characterizes the hydrophobicity of a molecule. The larger the value of LogP, the more cationic P +The less likely it is to approach water molecules. The standard method for simulating / calculating the LogP value is to compare the energy when a cation is solvated in water with the energy when it is solvated in octanol (an organic solvent). The formula is:

[0041]

[0042] According to an embodiment of the present application, the energy value here can be obtained by quantum chemical simulation calculation. E + corresponds to the energy obtained when we set the total molecular charge to +1 in the quantum chemical simulation. P + refers to a cation molecule in the +1 charge state. Octanol and water refer to the solvent models commonly used in chemical calculations. R refers to the molar gas constant (8.314 Joule K -1 mol -1 ). T refers to the temperature, and here we use room temperature T = 298.15 K.

[0043] The present application will be described in detail below with reference to the accompanying drawings.

[0044] In the first aspect of the present application, an embodiment of the present application proposes a method for screening organic cations for electrochemical ammonia synthesis. Referring to Figure 1 , the method includes:

[0045] S100: Construct a primary molecular library composed of multiple organic cations;

[0046] In this step, multiple known organic cations can be selected from a known compound database, or a series of organic cation molecules can be generated through compound design by means of AI artificial intelligence, etc. For example, based on the pre-screened candidate organic cations, by modifying their groups or changing substituents, a series of different organic compounds can be obtained. Further, through machine learning, the chemical properties of these organic compounds can be predicted, so as to select the compounds with properties meeting the requirements as members of the primary molecular library.

[0047] In addition, according to an embodiment of the present application, the ways for those skilled in the art to obtain known organic cations can be retrieved from existing compound databases, such as including but not limited to The Cambridge Crystallographic DataCentre (CCDC), ChemSpider (Search and share chemistry), ChemSub Online, ChemSynthesis, IUPAC Standards Online, PubMed, PubChem, SciFinder, ZINC, etc.

[0048] According to an embodiment of the present application, the charge number of the organic cation selected by the applicant is not more than +1. Thus, the probability of successfully screening candidate organic cations subsequently can be further increased.

[0049] According to an embodiment of the present application, the primary molecular library is determined by the following steps:

[0050] First, a plurality of organic salt compounds containing a single halogen anion are obtained. Since only a single halogen anion is contained in these organic salt compounds, the charge of the cation part thereof does not exceed +1. Those skilled in the art can understand that these plurality of organic salt compounds can be retrieved from a known database. In order to expand the screening scope, new organic salt compounds can also be generated by further performing molecular design based on artificial intelligence. According to an embodiment of the present application, when selecting a halogen anion, only organic salt compounds containing a chlorine atom, a bromine atom or an iodine atom are searched, which can improve the efficiency of constructing the primary molecular library. Additionally, according to an embodiment of the present application, the selectable organic salt compounds contain a P+ phosphonium or an N+ nitrogen hetero center, thereby further increasing the probability of finally screening an effective organic cation.

[0051] Further, after obtaining the above-mentioned organic salt compounds, the halogen anions in the obtained plurality of organic salt compounds are removed, and the remaining organic cations are combined and de-duplicated to obtain a primary molecular library.

[0052] S200: Filter the primary molecular library based on the molecular structure characteristics of the organic cation to obtain a secondary molecular library.

[0053] After obtaining the primary molecular library, before performing quantum chemical analysis, the primary molecular library can be filtered to reduce the size of its library, thereby improving the efficiency of subsequent quantum chemical analysis.

[0054] In an embodiment of the present application, the filtering criteria adopted are based on the molecular structure characteristics of the organic cation. As described above, the molecular structure characteristics are easily obtained from the information recorded in the database or determined by using conventional chemoinformatics means.

[0055] According to an embodiment of the present application, in this step, the molecular structure features that can be used for filtration include at least one selected from the following: molecular charge, molecular weight, topological polar surface area, number of heavy atoms, number of hydrogen bond donors, and atomic composition of the molecule. Considering these factors comprehensively can effectively further increase the probability of finally screening out effective organic cations. In a specific example, organic cations that meet at least one of the following conditions are selected to construct the secondary molecular library: the molecular charge does not exceed 1.0; the molecular weight does not exceed 400 daltons; the topological polar surface area does not exceed 30.0 square angstroms; the number of heavy atoms does not exceed 30; the number of hydrogen donors in the molecule does not exceed 1; the atomic composition of the molecule does not include atoms other than H, B, C, N, O, F, Si, P, S, and halogens. According to an embodiment of the present application, the term "heavy atom" mentioned here refers to an atom other than hydrogen.

[0056] In this step, performing quantum chemical analysis can be determined by conventional chemoinformatics tools or methods, and this processing step can be carried out in a high-throughput manner. According to an embodiment of the present application, after completing this step, the primary molecular library can be compressed to one-fourth, thereby significantly reducing the processing time in the subsequent quantum chemical analysis stage.

[0057] S300: For the compounds in the secondary molecular library, determine the quantitative values of deprotonation energy, vertical electron affinity, and hydrophobicity respectively; and

[0058] S400: Based on the quantitative values, select the candidate organic cations from the secondary molecular library.

[0059] After constructing the secondary molecular library through filtration under low-cost and high-throughput basic chemical conditions (molecular structure features), high-precision quantum chemical analysis processing can be carried out, that is, further screening molecules through quantum chemical calculations. The inventors, through a large amount of research work, determined the quantitative values of deprotonation energy, vertical electron affinity, and hydrophobicity as the criteria for screening organic cations. The organic cations obtained by adopting this criterion can improve the yield and long-term stability of electrochemical ammonia synthesis as electrolyte additives.

[0060] Specifically, according to an embodiment of the present application, organic cations that meet at least one of the following conditions are selected as the candidate organic cations: the quantitative value of the deprotonation energy is not lower than -1.1 eV and does not exceed -0.8 eV, preferably the quantitative value of the deprotonation energy is not lower than -1.04 eV and does not exceed -0.83 eV; the quantitative value of the vertical electron affinity is not lower than -1.23 eV; the quantitative value of the hydrophobicity LogP is greater than 0, preferably the quantitative value of the hydrophobicity LogP is not less than 0.3. According to a specific example, organic cations that fully meet the above conditions are selected as the final candidate organic cations.

[0061] Specifically, the following will provide a detailed description of the above three parameters respectively.

[0062] The deprotonation energy refers to the energy required to release a proton from a cation and convert it into a neutral molecule. The inventors of the present application found that this energy is an important reference index because it determines the ability of organic cations to capture / release protons in solution to achieve the proton shuttle phenomenon. However, the inventors also found that if this energy is too small, the cation will have difficulty in holding onto the proton, and if this energy is too large, the cation will have difficulty in releasing the proton to react with the N atom and form ammonia gas on the electrode.

[0063] The vertical electron affinity (VEA) refers to the energy required to instantaneously add an electron to an organic cation and convert it into a neutral molecule without changing the stable 3D conformation of the cation. This neutral molecule is usually unstable because it has unpaired electrons. However, as an intermediate state, this neutral molecule is a precursor for further chemical reactions and can irreversibly degrade the organic cation. Moreover, the inventors of the present application found that VEA can be an important reference for the electrochemical stability of organic cations.

[0064] LogP is a measure characterizing the hydrophobicity of organic cations. There has been no report on whether the LogP value plays a role in improving the yield and stability of electrochemical ammonia synthesis. The inventors of the present application found that if an organic cation has a certain degree of hydrophobicity, it will be more difficult for water molecules to adhere near the cation in the electrolyte. Therefore, in the present application, LogP is also used as an important reference for screening organic cations.

[0065] Verification Example

[0066] Reference Figure 3 , in this verification example, hundreds of thousands of organic compounds were obtained from PubChem, and through a series of basic chemical conditions (molecular structure) filtering and quantum chemical analysis, several organic cations that may be suitable as electrolyte additives for electrochemical ammonia synthesis were obtained, significantly shortening the time for screening target compounds from a vast compound library.

[0067] Specifically, referring to Figure 3 , in this example, first, approximately 500,000 organic salts were extracted from the PubChem database, including approximately 230,000 organic hydrochlorides (containing one chlorine anion), approximately 90,000 organic bromates (containing one bromine anion), and approximately 140,000 organic iodates (containing one iodine anion). The organic cation parts of the above organic salts were extracted and merged and de-duplicated to obtain a primary molecular library containing approximately 200,000 organic cations.

[0068] After obtaining the primary molecular library, the above primary molecular library is subjected to high-throughput and low-cost chemoinformatics analysis and filtration according to the following criteria to obtain a secondary molecular library:

[0069] 1. The charge of the molecule <= 1.0 (which means the resulting cationic charge is +1).

[0070] 2. Molecular weight <= 400.0 Dalton

[0071] 3. Topological polar surface area <= 30.0 Angstrom 2

[0072] 4. The number of heavy atoms in the molecule <= 30

[0073] 5. The number of hydrogen bond donors in the molecule <= 1

[0074] 6. LogP >= 0.0

[0075] 7. The molecule consists only of typical organic compound atoms (H, B, C, N, O, F, Si, P, S, Cl, Br, or I).

[0076] After completing the chemoinformatics molecular filtration, a secondary molecular library composed of approximately 54,000 unique organic cations was finally obtained.

[0077] After filtering through the above-mentioned eight basic chemical conditions of low cost and high throughput, the inventors performed high-precision and high-cost quantum chemical calculations to further screen the molecules. As mentioned above, through quantum chemical calculation methods, the deprotonation energy, vertical electron affinity, and hydrophobicity quantization values of each organic cation were determined as the criteria for screening organic cations, and organic cations that meet the following conditions were selected as the candidate organic cations:

[0078] The quantization value of the deprotonation energy is not less than -1.1 eV and does not exceed -0.8 eV, preferably the quantization value of the deprotonation energy is not less than -1.04 eV and does not exceed -0.83 eV;

[0079] The quantization value of the vertical electron affinity is not less than -1.23 eV;

[0080] The quantization value of hydrophobicity LogP is greater than 0, preferably the quantization value of hydrophobicity LogP is not less than 0.3.

[0081] Using the above three conditions for screening, 59 organic cations were finally obtained, which can be divided into the following categories in total:

[0082] 1. Groups containing a phosphonium P+ center.

[0083] 2. Groups containing a nitrogen hetero N+ center.

[0084] Among them, a representative organic cation of the organic cation containing a phosphonium P+ center is trihexyltetradecyl phosphonium ([P 6,6,6,14 + ). This organic cation has been reported in the literature to have relatively excellent chemical properties and can be applied to electrochemical ammonia synthesis (see B.H.R. Suryanto, et al. “Nitrogen reduction to ammonia at high efficiency and rates in a Li-mediated process based on a phosphonium proton shuttle.” In Science 372, no. 6547 (2021): 1187 - 1191.). Thus, the effectiveness of the technical solution of this application can be proved.

[0085] Of course, those skilled in the art can understand that after the above screening, other compounds containing the above organic cation (such as in the form of salts formed with halogens) can be added to the electrolyte for electrochemical synthesis through conventional electrochemical synthesis experiments to verify their chemical activity, which will not be elaborated here.

[0086] In view of this, this application also proposes the use of the candidate organic cations obtained in the first aspect in electrochemical ammonia synthesis. Specifically, in the second aspect of this application, an embodiment of this application proposes an electrolyte for electrochemical ammonia synthesis, which contains: an organic cation, and this organic cation is obtained by the method described in the first aspect. Using this electrolyte can effectively synthesize ammonia electrochemically in an electrochemical synthesis reactor. Of course, the features and advantages described for the first aspect also apply to this electrolyte, which will not be elaborated here.

[0087] In the third aspect of this application, an embodiment of this application proposes a device for screening organic cations for electrochemical ammonia synthesis, referring to Figure 2 , this device includes:

[0088] A primary molecular library construction unit 100, which is used to construct a primary molecular library composed of multiple organic cations;

[0089] A secondary molecular library construction unit 200, which is used to filter the primary molecular library based on predetermined molecular structure characteristics to obtain a secondary molecular library;

[0090] A quantum chemical analysis unit 300 for respectively determining the quantification values of the deprotonation energy, vertical electron affinity, and hydrophobicity for the compounds in the secondary molecular library; and

[0091] An organic cation determination unit 300 for selecting the candidate organic cations from the secondary molecular library based on the quantification values.

[0092] In a fourth aspect of the present application, embodiments of the present application provide an electronic device, including:

[0093] A processor adapted to implement computer instructions; and,

[0094] A memory storing computer instructions, the computer instructions being adapted to be loaded and executed by the processor to perform the method of the first aspect above.

[0095] In a fifth aspect of the present application, embodiments of the present application provide a computer-readable storage medium, the computer-readable storage medium storing computer instructions, and when the computer instructions are read and executed by a processor of a computer device, the computer device is caused to execute the method of the first aspect above.

[0096] In a sixth aspect of the present application, embodiments of the present application provide a computer program product or a computer program, the computer program product or the computer program including computer instructions, the computer instructions being stored in a computer-readable storage medium. A processor of a computer device reads the computer instructions from the computer-readable storage medium, and the processor executes the computer instructions, causing the computer device to execute the method of the first aspect above.

[0097] It should be understood that the device embodiments and the method embodiments can correspond to each other, and similar descriptions can refer to the method embodiments. To avoid repetition, it will not be elaborated here.

[0098] In the above, the devices and systems of the embodiments of the present application have been described from the perspective of functional modules. It should be understood that the functional modules can be implemented in the form of hardware, or in the form of software instructions, or in a combination of hardware and software modules. Specifically, the steps of the method embodiments in the present application can be completed by the integrated logic circuit of the hardware in the processor and / or software instructions. The steps of the method disclosed in combination with the embodiments of the present application can be directly embodied as being executed by a hardware decoding processor, or executed by a combination of the hardware and software modules in the decoding processor. Optionally, the software module can be located in a mature storage medium in the art such as a random access memory, a flash memory, a read-only memory, a programmable read-only memory, an electrically erasable programmable memory, a register, etc. The storage medium is located in the memory, and the processor reads the information in the memory and combines its hardware to complete the steps in the above method embodiments.

[0099] As Figure 4 is a schematic block diagram of the electronic device 1000 provided by an embodiment of the present application.

[0100] As Figure 4 shown, the electronic device 1000 may include:

[0101] A memory 1010 and a processor 1020. The memory 1010 is used to store a computer program and transmit the program code to the processor 1020. In other words, the processor 1020 can call and run the computer program from the memory 1010 to implement the method in the embodiment of the present application.

[0102] For example, the processor 1020 can be used to execute the steps of each execution entity in the above method 200 or method 300 according to the instructions in the computer program.

[0103] In some embodiments of the present application, the processor 1020 may include, but is not limited to:

[0104] A general-purpose processor, a digital signal processor (DSP), an application specific integrated circuit (ASIC), a field programmable gate array (FPGA), or other programmable logic devices, discrete gate or transistor logic devices, discrete hardware components, and so on.

[0105] In some embodiments of the present application, the memory 1010 includes, but is not limited to:

[0106] Volatile memory and / or non-volatile memory. Among them, the non-volatile memory can be Read-Only Memory (ROM), Programmable ROM (PROM), Erasable PROM (EPROM), Electrically Erasable PROM (EEPROM), or flash memory. The volatile memory can be Random Access Memory (RAM), which is used as an external cache. By way of example but not limitation, many forms of RAM are available, such as Static RAM (SRAM), Dynamic RAM (DRAM), Synchronous DRAM (SDRAM), Double DataRate SDRAM (DDR SDRAM), Enhanced SDRAM (ESDRAM), synch link DRAM (SLDRAM), and Direct Rambus RAM (DR RAM).

[0107] In some embodiments of the present application, the computer program may be divided into one or more modules, which are stored in the memory 1010 and executed by the processor 1020 to complete the method provided by the present application. The one or more modules may be a series of computer program instruction segments capable of performing specific functions, and the instruction segments are used to describe the execution process of the computer program in the electronic device 1000.

[0108] Optionally, the electronic device 1000 may further include:

[0109] A communication interface 1030, which can be connected to the processor 1020 or the memory 1010.

[0110] Among them, the processor 1020 can control the communication interface 1030 to communicate with other devices. Specifically, it can send information or data to other devices, or receive information or data sent by other devices. Exemplarily, the communication interface 1030 may include a transmitter and a receiver. The communication interface 1030 may further include an antenna, and the number of antennas may be one or more.

[0111] It should be understood that each component in the electronic device 1000 is connected through a bus system. Among them, the bus system includes, in addition to the data bus, a power bus, a control bus, and a status signal bus.

[0112] It should be understood that when implemented using software, it can be implemented in whole or in part in the form of a computer program product. The computer program product includes one or more computer instructions. When the computer program instructions are loaded and executed on a computer, the processes or functions according to the embodiments of the present application are generated in whole or in part. The computer can be a general-purpose computer, a special-purpose computer, a computer network, or other programmable devices. The computer instructions can be stored in a computer-readable storage medium or transmitted from one computer-readable storage medium to another. For example, the computer instructions can be transmitted from one website, computer, server, or data center to another website, computer, server, or data center in a wired manner (such as coaxial cable, optical fiber, digital subscriber line (DSL)) or a wireless manner (such as infrared, wireless, microwave, etc.). The computer-readable storage medium can be any available medium that the computer can access or a data storage device such as a server or data center that includes one or more integrated available media. The available medium can be a magnetic medium (such as a floppy disk, hard disk, magnetic tape), an optical medium (such as a digital video disc (DVD)), or a semiconductor medium (such as a solid state disk (SSD)), etc.

[0113] It should be understood that in the embodiments of the present application, "B corresponding to A" means that B is associated with A. In one implementation, B can be determined according to A. However, it should also be understood that determining B according to A does not mean determining B only according to A, and B can also be determined according to A and / or other information.

[0114] In the description of the present application, unless otherwise specified, "at least one" means one or more, and "a plurality" means two or more than two. In addition, "and / or" describes the association relationship of associated objects and indicates that three relationships can exist. For example, A and / or B can represent the cases of: A existing alone, A and B existing simultaneously, and B existing alone, where A and B can be singular or plural. The character " / " generally represents an "or" relationship between the associated objects before and after. "At least one (item)" or its similar expression refers to any combination of these items, including any combination of single item (item) or plural items (items). For example, at least one (item) of a, b, or c can represent: a, b, c, a - b, a - c, b - c, or a - b - c, where a, b, and c can be single or multiple.

[0115] It should also be understood that the first, second, etc. descriptions appearing in the embodiments of the present application are only for the purpose of indicating and distinguishing the described objects, without order, and do not represent any special limitation on the number of devices in the embodiments of the present application, and cannot constitute any limitation to the embodiments of the present application.

[0116] It should also be understood that specific features, structures, or characteristics related to the embodiments in the specification are included in at least one embodiment of the present application. In addition, these specific features, structures, or characteristics can be combined in one or more embodiments in any suitable manner.

[0117] In addition, the terms "including" and "having" and any variations thereof are intended to cover non-exclusive inclusion. For example, a process, method, system, product, or server that includes a series of steps or units does not necessarily have to be limited to those steps or units clearly listed, but may include other steps or units not clearly listed or inherent to these processes, methods, products, or devices.

[0118] It can be understood that in the specific implementation of the present application, data related to user information and the like may be involved. When the above embodiments of the present application are applied to specific products or technologies, user permission or consent needs to be obtained, and the collection, use, and processing of relevant data need to comply with relevant laws, regulations, and standards of relevant countries and regions.

[0119] Those of ordinary skill in the art can realize that the modules and algorithm steps of each example described in combination with the embodiments disclosed herein can be implemented by electronic hardware, or a combination of computer software and electronic hardware. Whether these functions are executed in a hardware or software manner depends on the specific application and design constraints of the technical solution. Professional technicians can use different methods to implement the described functions for each specific application, but such implementation should not be considered to exceed the scope of the present application.

[0120] In several embodiments provided by the present application, it should be understood that the disclosed devices, apparatuses, and methods can be implemented in other ways. For example, the apparatus embodiments described above are only illustrative. For example, the division of the modules is only a logical function division, and there can be other division methods in actual implementation. For example, multiple modules or components can be combined or integrated into another system, or some features can be ignored or not executed. Another point is that the displayed or discussed coupling or direct coupling or communication connection between each other can be through some interfaces, and the indirect coupling or communication connection of the devices or modules can be in an electrical, mechanical, or other form.

[0121] The modules described as separate components may or may not be physically separated, and the components shown as modules may or may not be physical modules, that is, they may be located in one place or distributed across multiple network units. Some or all of the modules can be selected according to actual needs to achieve the purpose of the solution of this embodiment. For example, in each embodiment of this application, each functional module can be integrated in a processing module, or each module can exist physically alone, or two or more modules can be integrated in one module.

[0122] The above are only specific embodiments of this application, but the protection scope of this application is not limited thereto. Any person skilled in the art within the technical scope disclosed in this application can easily think of changes or substitutions, which should all be covered within the protection scope of this application. Therefore, the protection scope of this application should be subject to the protection scope of the claims.

Claims

1. A method for screening organic cations for electrochemical ammonia synthesis, characterized in that Comprising: (1) Constructing a primary molecular library composed of multiple organic cations; (2) Filtering the primary molecular library based on the molecular structure characteristics of the organic cations to obtain a secondary molecular library; (3) Respectively determining the quantified values of deprotonation energy, vertical electron affinity, and hydrophobicity for the compounds in the secondary molecular library; (4) Selecting candidate organic cations from the secondary molecular library based on the quantified values.

2. The method according to claim 1, wherein Step (1) further includes: Obtaining multiple organic salt compounds containing a single halogen anion; Removing the halogen anions in the multiple organic salt compounds and merging and removing duplicates of the remaining organic cations to obtain the primary molecular library.

3. The method according to claim 2, wherein The organic salt compounds contain P+ phosphonium or N+ nitrogen hetero centers.

4. The method according to claim 1, characterized in that, In step (2), the molecular structure characteristics include at least one selected from the following: molecular charge, molecular weight, topological polar surface area, number of heavy atoms, number of hydrogen bond donors, and atomic composition of the molecule.

5. The method according to claim 4, characterized in that In step (2), selecting organic cations that meet at least one of the following conditions to construct the secondary molecular library: The molecular charge does not exceed 1.0; The molecular weight does not exceed 400 daltons; The topological polar surface area does not exceed 30.0 square angstroms; The number of heavy atoms does not exceed 30; The number of hydrogen bond donors of the molecule does not exceed 1; The atomic composition of the molecule does not include atoms other than H, B, C, N, O, F, Si, P, S, and halogens.

6. The method according to claim 1, wherein In step (4), selecting organic cations that meet at least one of the following conditions as the candidate organic cations: The quantified value of the deprotonation energy is not lower than -1.1 eV and does not exceed -0.8 eV; The quantified value of the vertical electron affinity is not lower than -1.23 eV; The quantified value of the hydrophobicity LogP is greater than 0.

7. The method according to claim 6, characterized in that, The quantified value of the hydrophobicity LogP is not less than 0.

3.

8. The method according to claim 1, wherein The quantified value of the deprotonation energy is not lower than -1.04 eV and does not exceed -0.83 eV.

9. An electrolyte for electrochemical ammonia synthesis, characterized in that, Containing: An organic cation, which is obtained by the method according to any one of claims 1 to 8.

10. An apparatus for screening organic cations for electrochemical ammonia synthesis, characterized in that, Comprising: A primary molecular library construction unit for constructing a primary molecular library composed of multiple organic cations; A secondary molecular library construction unit for filtering the primary molecular library based on predetermined molecular structure characteristics to obtain a secondary molecular library; [[ID=,28]]A quantum chemistry analysis unit for respectively determining the quantified values of deprotonation energy, vertical electron affinity, and hydrophobicity for the compounds in the secondary molecular library; An organic cation determination unit for selecting candidate organic cations from the secondary molecular library based on the quantified values.

11. An electronic device, characterized in that, Comprising a processor and a memory, wherein instructions are stored in the memory, and when the processor runs the instructions, the processor executes the method according to any one of claims 1 to 8.

12. A computer storage medium, characterized in that, Including instructions, when running on a computer, causing the computer to execute the method according to any one of claims 1 to 8.

13. A computer program product, characterized in that, Including computer program code, when the computer program code is run by an electronic device, causing the electronic device to execute the method according to any one of claims 1 to 8.

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