Method for predicting and screening monatomic nitrogen reduction catalyst with high activity and selectivity based on coulomb-like descriptor
By constructing a three-stage screening strategy based on coulomb descriptors and coordination environment correction, the problems of physical interpretation and high-throughput screening for predicting the nitrogen reduction reaction performance of single-atom catalysts were solved, achieving efficient and accurate prediction of catalyst activity and selectivity.
Patent Information
- Application Number
- CN202511419054.6
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-09-30
- Publication Date
- 2026-02-24
AI Technical Summary
In the existing technology, the prediction of nitrogen reduction reaction performance of single-atom catalysts lacks physically interpretable descriptors. Traditional methods have low computational efficiency and limited model universality, making it difficult to achieve high-throughput screening. Furthermore, the two-step strategy is prone to missing the true rate-determining step, leading to biased activity prediction.
By calculating the first and last hydrogenation free energy changes of single-atom nitrogen reduction catalysts, a volcanic relationship between a coulombic descriptor and the hydrogenation limiting potential is established. Deviations from the structure are identified and the rate-determining step is corrected. Combined with coordination environment correction extended descriptors, high-throughput screening of highly active and selective single-atom catalysts is achieved.
It achieves efficient and accurate prediction of the activity and selectivity of single-atom catalysts, reducing the amount of density functional theory calculations by 70%. It is applicable to d-block, p-block and various coordination structures, with a correlation coefficient R2 value exceeding 0.83, and the prediction results are consistent with the experimental results.
Smart Images
Figure CN121565281A_ABST
Abstract
Description
Technical Field
[0001] This invention belongs to the field of nitrogen reduction catalyst technology, specifically relating to a method for predicting and screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor-like prediction. Background Technology
[0002] In existing technologies, the prediction of nitrogen reduction reaction performance of single-atom catalysts lacks physically interpretable descriptors. Traditional descriptors, such as d-band centers and p-band centers, rely on density functional theory calculations, which have limited applicability, such as failing to cover p-region metals, and are difficult to explain the physical nature of catalytic activity. Furthermore, the modulating effects of different coordination structures (such as M-N4 and M-CN3) on catalytic activity are not systematically incorporated into the descriptors, limiting the model's universality. While density functional theory calculations of the entire process require significant computational resources, making high-throughput screening difficult, machine learning methods, although more efficient, lack physical interpretability and therefore cannot guide catalyst design principles. On the other hand, the "two-step strategy" commonly used in existing technologies, which only considers the first and final hydrogenation steps, easily overlooks the true rate-determining step, leading to biases in catalyst activity prediction.
[0003] Therefore, there is an urgent need to develop a method for rapidly predicting the activity and selectivity of single-atom catalysts. Summary of the Invention
[0004] The purpose of this section is to outline some aspects of embodiments of the present invention and to briefly describe some preferred embodiments. Simplifications or omissions may be made in this section, as well as in the abstract and title of this application, to avoid obscuring the purpose of these documents; however, such simplifications or omissions should not be construed as limiting the scope of the invention.
[0005] In view of the problems existing in the above and / or prior art, the present invention is proposed.
[0006] Therefore, the purpose of this invention is to overcome the shortcomings of the prior art and provide a method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction.
[0007] To solve the above-mentioned technical problems, the present invention provides the following technical solution:
[0008] Calculate the free energy change ΔG1 for the first hydrogenation step and ΔG2 for the last hydrogenation step in a single-atom nitrogen reduction catalyst, and calculate the hydrogenation limiting potential U. L A coulomb descriptor Φ and the hydrogenation limiting potential U were established through linear fitting. L The volcanic relationship will be related to the limiting potential deviation ΔU of the volcanic relationship curve. L Structures with a voltage greater than 0.25V are marked as deviating structures;
[0009] Wherein, the coulombic descriptor Φ represents the interaction between the metal active center of the single-atom nitrogen reduction catalyst and the nitrogen reduction reaction intermediate, and is defined by equation (1);
[0010] Φ=N e M N e N / (R M +R N (1);
[0011] In equation (1), N e M N is the number of valence electrons at the center of the catalyst metal atom; e N R represents the number of valence electrons of the nitrogen atom in the nitrogen reduction reaction intermediate. M R is the atomic radius of the metal; N The radius of a nitrogen atom;
[0012] Calculate the Gibbs free energy curve deviating from the structurally intact nitrogen reduction reaction pathway, identify the true rate-determining step, and correct the hydrogenation limiting potential to U' using the free energy change of the true rate-determining step. L Establish the relationship between Φ and U' through linear fitting. L The volcanic relationship allows for accurate prediction of the activity of catalysts deviating from their structural design;
[0013] The extended descriptor is obtained by correcting the coulombic descriptor Φ according to the coordination environment.
[0014] in, α is the average electronegativity of the coordinating atoms, and α is the coupling factor of the reaction coordination environment, α = x / 2, where x is the number of coordinating N atoms;
[0015] Based on the fact that the number of valence electrons in metals is in the range of 0 to 10, and the atomic radius is... For single-atom nitrogen reduction catalysts within a given range, high-throughput predictions of the activity of pre-designed single-atom catalysts are performed using extended descriptors, while simultaneously calculating the hydrogen evolution free energy change ΔG. H And calculate the hydrogen evolution limiting potential U. H , satisfy U' L >-0.98V and (U' L -U H The -0.5V standard is the predicted single-atom nitrogen reduction catalyst that combines high activity and high selectivity.
[0016] As a preferred embodiment of the method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction according to the present invention, the single-atom nitrogen reduction catalyst includes one or more of the following: metal phthalocyanine molecules, two-dimensional metal phthalocyanine COF structures, and nitrogen-doped graphene-supported single-atom catalysts.
[0017] As a preferred embodiment of the method for predictively screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptors as described in this invention, wherein: the metal active center of the single-atom nitrogen reduction catalyst includes the metals Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Ru, Rh, Pd, Ag, Ta, W, Re, Os, Ir, Pt, Au, Al, Ga, In, and Ge.
[0018] As a preferred embodiment of the method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction according to the present invention, wherein: the coordinating atom is an atom that is directly bonded to a metal atom.
[0019] As a preferred embodiment of the method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in this invention, wherein: the hydrogenation limiting potential U L It is obtained by calculation using equation (2);
[0020] U L =-(ΔG1, ΔG2) max / e (2);
[0021] Where ΔG1 is the free energy change of the first hydrogen addition step, and ΔG2 is the free energy change of the last hydrogen addition step, (ΔG1, ΔG2) max It is the maximum value among ΔG1 and ΔG2.
[0022] As a preferred embodiment of the method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in this invention, wherein: the limiting potential is corrected using the true rate-determining step free energy change as U' L It is obtained by calculation using equation (3);
[0023] U' L =-ΔG 真实 / e(3);
[0024] Wherein, ΔG 真实 The free energy variation of the real velocity step.
[0025] As a preferred embodiment of the method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in this invention, wherein: the calculation of the hydrogen evolution limiting potential U...H It is obtained by calculation using equation (4);
[0026] U H =-ΔG H / e (4);
[0027] Wherein, ΔG H This is the change in the free energy of hydrogen evolution.
[0028] Beneficial effects of this invention:
[0029] (1) Physical interpretability: The Coulomb-like descriptor constructed by this invention based on the inherent properties of atoms (number of valence electrons, radius, electronegativity) clearly reflects the essence of the interaction between the metal center and the intermediate, overcoming the "black box" defect of machine learning;
[0030] (2) Efficient screening: Based on the constructed Coulomb descriptor, a three-stage screening is performed, which reduces the DFT full-path computation by more than 70% and achieves efficient high-throughput screening (1000+ configurations / week);
[0031] (3) Accuracy: After correcting for the effects of the rate-determining step and coordination environment, the correlation coefficient R 2 A value exceeding 0.83 indicates high accuracy in the prediction results;
[0032] (4) Universality: The prediction method of this invention is applicable to d-block, p-block, and s-block metals and various coordination structures (M-N4, M-CN3, etc.), providing a general framework for the design of novel catalysts;
[0033] (5) Selectivity optimization: This invention can simultaneously predict the inhibition ability of the hydrogen evolution reaction (HER) and screen for highly selective and highly active catalysts, such as VPc, whose (U' L -U H =0.08V. Attached Figure Description
[0034] To more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings used in the description of the embodiments will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort. Wherein:
[0035] Figure 1 The diagram shows the correlation curves (a) between the number of valence electrons of a metal center and the limiting potential during the construction of the coulombic descriptor of this invention, (b) the correlation curves (c) between the atomic radius and the limiting potential of metal centers with the same number of valence electrons, and (c) a schematic diagram of the coulombic interaction between the catalytic metal center and the nitrogen reduction reaction intermediate.
[0036] Figure 2 This is a schematic diagram of the overall process of the prediction method in Embodiment 1 of the present invention.
[0037] Figure 3 The free energy change ΔG1 for the first hydrogenation step and ΔG2 for the last hydrogenation step in Example 1 of this invention are given by different catalysts. The pentagram is used to calculate the limiting potential U. L The hydrogenation step with the highest reaction energy barrier.
[0038] Figure 4 For Embodiment 1 of the present invention, the coulomb descriptor Φ and the limiting potential U are... L The volcanic relationship curve (a), the Gibbs free energy curve of the complete nitrogen reduction reaction pathway (b), and the Coulomb descriptor Φ and the corrected U' L The volcano relationship curve (c).
[0039] Figure 5 This is a comparison diagram of coordination environment correction before and after in Embodiment 1 of the present invention.
[0040] Figure 6 This is a diagram illustrating the high-throughput screening and verification process in Embodiment 1 of the present invention. Detailed Implementation
[0041] To make the above-mentioned objects, features and advantages of the present invention more apparent and understandable, the specific embodiments of the present invention will be described in detail below with reference to the examples in the specification.
[0042] Many specific details are set forth in the following description in order to provide a full understanding of the invention. However, the invention may also be practiced in other ways different from those described herein, and those skilled in the art can make similar extensions without departing from the spirit of the invention. Therefore, the invention is not limited to the specific embodiments disclosed below.
[0043] Secondly, the term "one embodiment" or "embodiment" as used herein refers to a specific feature, structure, or characteristic that may be included in at least one implementation of the present invention. The phrase "in one embodiment" appearing in different places in this specification does not necessarily refer to the same embodiment, nor is it a single or selective embodiment that is mutually exclusive with other embodiments.
[0044] The construction process of the class Coulomb descriptor Φ in this invention is as follows: Figure 1 As shown, firstly, the correlation between the number of valence electrons of a metal center and the limiting potential is established. Secondly, for metal centers with the same number of valence electrons, the correlation between their atomic radius and the limiting potential is established. Finally, the Coulomb-like interaction between the catalytic metal center and the nitrogen reduction reaction intermediate is obtained.
[0045] Example 1
[0046] like Figure 2As shown, this embodiment provides a rapid prediction method for highly active and selective single-atom nitrogen reduction catalysts based on coulomb descriptors, specifically as follows:
[0047] All single-atom nitrogen reduction catalysts predicted in this embodiment include metal phthalocyanine molecules (MPc), two-dimensional metal phthalocyanine COF structures (MPc-COF), and nitrogen-doped graphene-supported single-atom catalysts (M@N4, M@C2N2, M@C3N, M@CN3), where metal M refers to Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Ru, Rh, Pd, Ag, Ta, W, Re, Os, Ir, Pt, Au, Al, Ga, In, and Ge.
[0048] (1) Preliminary screening: Calculate the free energy change ΔG1 of the first hydrogen addition step (*N2→*NNH) and the free energy change ΔG2 of the last hydrogen addition step (*NH2→*NH3), and the results are as follows. Figure 3 As shown; calculate the hydrogenation limiting potential U according to equation (1). L ;
[0049] U L =-(ΔG1, ΔG2) max / e (1);
[0050] Where, (ΔG1, ΔG2) max It is the maximum value among ΔG1 and ΔG2.
[0051] A coulomb descriptor Φ and the hydrogenation limiting potential U were established through linear fitting. L The volcanic relationship was obtained, and the limiting potentials of MPC, MPC-COF, and M@N4 were compared with the volcanic relationship curves of the descriptors, as shown in the figure. Figure 4 As shown in (a), the limiting potential deviation ΔU of the relationship curve with the volcano is... L Structures with a voltage greater than 0.25V were marked as off-center structures. The following off-center structures were obtained through screening: VPc, TiPc, MoPc, TiPc-COF, MoPc-COF, Ti@N4, and V@N4.
[0052] Among them, the coulombic descriptor Φ represents the interaction between the catalyst metal active center and the nitrogen reduction reaction *N2 intermediate in the form of end-group adsorption configuration;
[0053] Φ=N e M N e N / (R M +R N (2);
[0054] In equation (2), N e MThe number of valence electrons at the center of a catalyst metal atom represents the number of d electrons for d-block metals and the number of s+p electrons for p-block metals. 10 The number of s electrons taken by the metal; N e N R represents the number of valence electrons of the nitrogen atom in the NRR intermediate; M R is the atomic radius of the metal; N Where is the radius of a nitrogen atom.
[0055] (2) Rate-determining step verification: The Gibbs free energy curves of the complete nitrogen reduction reaction pathways of the off-structure catalysts VPc, TiPc, MoPc, TiPc-COF, MoPc-COF, Ti@N4, and V@N4 were calculated using PBE functional analysis and D3 dispersion correction. The results are as follows: Figure 4 As shown in (b).
[0056] (3) Accurate prediction: Based on the full path analysis, the true rate-determining step of the above-mentioned deviation structure is the *NH3 desorption step. According to equation (3), the hydrogenation limiting potential U is... L Corrected to U' L ;
[0057] U' L =-ΔG PDS / e(3);
[0058] In equation (3), ΔG PDS The free energy change for the *NH3 desorption step;
[0059] A Coulomb-like descriptor Φ and the corrected U' are established through linear fitting. L The volcano relationship curve, such as Figure 4 As shown in (c), the activity of the above-mentioned deviated catalysts is accurately predicted.
[0060] (4) Extended descriptor:
[0061] Descriptor Φ correction was performed on M@N4, M@C2N2, M@C3N, and M@CN3 under different coordination environments to obtain extended descriptors: The results are as follows Figure 5 As shown, where, The electronegativity of the coordinating atoms is represented by the Pauling scale, with N atoms having an electronegativity of 3.04 and C atoms having an electronegativity of 2.55. α is the coupling factor of the reaction coordination environment, α = x / 2, where x is the number of coordinated N atoms. Coordinating atoms refer to atoms that directly bond with metal M, quantifying the modulating effect of the coordination environment on activity. N4 represents 4 N atoms coordinated with M, C2N2 represents 2 N atoms and 2 C atoms coordinated with M, C3N represents 1 N atom and 3 C atoms coordinated with M, and CN3 represents 3 N atoms and 1 C atom coordinated with M.
[0062] (5) High-throughput prediction and validation:
[0063] Based on the fact that the number of valence electrons in metals is in the range of 0 to 10, and the atomic radius is... For single-atom nitrogen reduction catalysts within the specified range, high-throughput predictions were performed on all single-atom nitrogen reduction catalysts in this embodiment using extended descriptors, and the hydrogen evolution free energy change ΔG was calculated simultaneously. H And calculate the hydrogen evolution limiting potential U according to equation (4). H ;
[0064] U H =-ΔG H / e (4);
[0065] Take U' L >-0.98V and (U' L -U H Using -0.5V as the standard, it was predicted that MoPc, VPc, MoPc-COF, and VPc-COF possess both high activity and high selectivity.
[0066] Figure 2 The diagram below illustrates the overall flow of the prediction method in Example 1, where (a) shows the construction of a coulombic descriptor for nitrogen reduction reaction activity; (b) provides an overview of the three-stage screening strategy, namely, the first stage is a preliminary screening based on a "two-step approximation," the second stage verifies the rate-determining step through full-path analysis of outliers, and the third stage uses the corrected limiting potential for prediction optimization; (c) shows the correction through coordination environment, to... By incorporating coordination effects to optimize the universality of descriptors, the nitrogen reduction reaction activity of single-atom catalysts with different coordination structures can be accurately predicted.
[0067] Comparative Example 1
[0068] The difference between this comparative example and Example 1 is that the hydrogenation limiting potential U in step (3) is not performed. L The modifications are the same as in Example 1.
[0069] contrast Figure 4 (a) and (c) show that the limiting potentials of VPc, TiPc, and MoPc before correction were -0.26V, -0.80V, and -0.33V, respectively, and after correction were -0.97V, -1.41V, and -0.52V, respectively, showing a significant difference. After correction, the correlation coefficients R of VPc, TiPc, and MoPc deviating from the structure... L 2 The value increased from 0.74 to 0.87, and the correlation coefficient R of TiPc-COF, MoPc-COF, Ti@N4, and V@N4 increased. L 2The value increased from 0.60 to 0.78, and the correlation between the limiting potential and the descriptor was significantly improved.
[0070] Comparative Example 2
[0071] The difference between this comparative example and Example 1 is that the correction and expansion of the descriptor Φ in step (4) is not performed; otherwise, it is the same as Example 1.
[0072] Figure 5 The figures for Example 1 are before and after correction based on the coordination environment. (a) shows schematic diagrams of different coordination structures of the nitrogen-doped graphene-supported single-atom catalyst (M-N4, M-C2N2, M-C3N, M-CN3); (b) shows volcano plots of the limiting potential versus descriptor Φ for the nitrogen-doped graphene-supported single-atom catalysts with different coordination structures; and (c) shows the limiting potential versus extended descriptor Φ for the nitrogen-doped graphene-supported single-atom catalysts with different coordination structures. A map of a volcano.
[0073] contrast Figure 5 In (b) and (c), it can be observed that before coordination environment correction, the limiting potentials of single-atom catalysts in different coordination environments exhibit different volcano-shaped curves with respect to the descriptor Φ. However, after coordination environment correction, the limiting potentials of single-atom catalysts in different coordination environments and their correlation with the extended descriptor Φ are different. The presence of the same volcano-shaped curve indicates an expanded descriptor. The description of the activity of single-atom catalysts with different coordination environments is universal, and the correlation coefficient R0 is also applicable. L 2 The value reached 0.83.
[0074] Figure 6 The results of high-throughput screening and validation in Example 1 are shown in the figure. (a) shows the limiting potential and extended descriptor after coordination environment correction. (a) is a volcano plot, where the blue dashed line represents the limiting potential = -0.98V; (b) is a graph showing the corrected limiting potential—the relationship between the corrected limiting potential and the hydrogen evolution potential difference, where the orange dashed line represents the difference between the corresponding limiting potential and the hydrogen evolution potential of the metal-based reference, approximately –0.5V. Combined with... Figure 6 (a) and (b) clearly show that the single-atom nitrogen reduction catalysts MoPc, VPc, MoPc-COF, and VPc-COF possess both high activity and high selectivity.
[0075] Figure 6 (c) represents the yield of ammonia (NH3) in actual experiments with a single-atom catalyst and the extended descriptor of this invention. The correlation between NH3 yield and the extended descriptor of this invention can be observed. There is a clear linear relationship, indicating that the prediction method provided by this invention is consistent with the experimental trend and the prediction results are highly reliable.
[0076] In summary, this invention constructs a physically interpretable descriptor to quantitatively characterize the interaction strength between single-atom catalysts and nitrogen reduction reaction intermediates, avoiding excessive reliance on density functional theory calculations; it develops an efficient three-stage screening strategy to accurately identify the rate-determining step of the nitrogen reduction reaction, reducing the overall computational cost and achieving high-throughput catalyst screening; it introduces a coordination environment correction term to expand the universality of the descriptor, making it applicable to single-atom catalysts with different coordination structures such as M-N4, M-CN3, and M-C2N2; and it achieves simultaneous prediction of catalyst activity (limiting potential) and selectivity (inhibition of hydrogen evolution reaction), screening high-performance nitrogen reduction reaction catalysts that are consistent with actual experimental trends and have high reliability.
[0077] It should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and are not intended to limit it. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can be made to the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention, and all such modifications or substitutions should be covered within the scope of the claims of the present invention.
Claims
1. A method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor-like prediction, characterized in that: include, Calculate the free energy change ΔG1 for the first hydrogenation step and ΔG2 for the last hydrogenation step in a single-atom nitrogen reduction catalyst, and calculate the hydrogenation limiting potential U. L A coulomb descriptor Φ and the hydrogenation limiting potential U were established through linear fitting. L The volcanic relationship will be related to the limiting potential deviation ΔU of the volcanic relationship curve. L Structures with a voltage greater than 0.25V are marked as deviating structures; Wherein, the coulombic descriptor Φ represents the interaction between the metal active center of the single-atom nitrogen reduction catalyst and the nitrogen reduction reaction intermediate, and is defined by equation (1); Φ=N e M N e N / (R M +R N ) (1); In equation (1), N e M N is the number of valence electrons at the center of the catalyst metal atom; e N R represents the number of valence electrons of the nitrogen atom in the nitrogen reduction reaction intermediate. M R is the atomic radius of the metal; N The radius of a nitrogen atom; Calculate the Gibbs free energy curve deviating from the structurally intact nitrogen reduction reaction pathway, identify the true rate-determining step, and correct the limiting potential to U' using the free energy change of the true rate-determining step. L Establish the relationship between Φ and U' through linear fitting. L The volcanic relationship allows for accurate prediction of the activity of catalysts deviating from their structural design; The extended descriptor is obtained by correcting the coulombic descriptor Φ according to the coordination environment. in, α is the average electronegativity of the coordinating atoms, and α is the coupling factor of the reaction coordination environment, α = x / 2, where x is the number of coordinating N atoms; Based on the fact that the number of valence electrons in metals is in the range of 0 to 10, and the atomic radius is... For single-atom nitrogen reduction catalysts within a given range, high-throughput predictions of the activity of pre-designed single-atom catalysts are performed using extended descriptors, while simultaneously calculating the hydrogen evolution free energy change ΔG. H And calculate the hydrogen evolution limiting potential U. H , satisfy U' L >-0.98V and (U' L -U H The -0.5V standard is the predicted single-atom nitrogen reduction catalyst that combines high activity and high selectivity.
2. The method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in claim 1, characterized in that: The single-atom nitrogen reduction catalyst includes one or more of the following: metal phthalocyanine molecules, two-dimensional metal phthalocyanine COF structures, and nitrogen-doped graphene-supported single-atom catalysts.
3. The method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in claim 1 or 2, characterized in that: The metal active center of the single-atom nitrogen reduction catalyst includes metals such as Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Ru, Rh, Pd, Ag, Ta, W, Re, Os, Ir, Pt, Au, Al, Ga, In, and Ge.
4. The method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in claim 1, characterized in that: The coordinating atom is an atom that directly bonds with a metal atom.
5. The method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in claim 1, characterized in that: The hydrogenation limiting potential U L It is obtained by calculation using equation (2); U L =-(ΔG1,ΔG2) max / e (2); Where ΔG1 is the free energy change of the first hydrogen addition step, and ΔG2 is the free energy change of the last hydrogen addition step, (ΔG1, ΔG2) max It is the maximum value among ΔG1 and ΔG2.
6. The method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in claim 1, characterized in that: The hydrogenation limiting potential is corrected using the real rate-determining step free energy change as U' L It is obtained by calculation using equation (3); U’ L =-ΔG 真实 / e(3); Wherein, ΔG 真实 The free energy variation of the real velocity step.
7. The method for screening single-atom nitrogen reduction catalysts with high activity and selectivity based on coulomb descriptor prediction as described in claim 1, characterized in that: The calculation of the hydrogen evolution limiting potential U H It is obtained by calculation using equation (4); U H =-ΔG H / e (4); Wherein, ΔG H This is the change in the free energy of hydrogen evolution.