首页|Sp/sp2 carbon ratio-driven high-throughput screening of electrocatalytic nitrogen reduction performance on transition metal single-atom catalysts
Sp/sp2 carbon ratio-driven high-throughput screening of electrocatalytic nitrogen reduction performance on transition metal single-atom catalysts
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Single-atom catalysts(SACs)have been widely utilized in electrochemical nitrogen reduction reactions(NRR)due to their high atomic utilization and selectivity.Owing to the unique sp/sp2 co-hybridization,graphyne materials can offer stable adsorption sites for single metal atoms.To investigate the influence of the sp/sp2 hybrid carbon ratio on the electrocatalytic NRR performance of graphyne,a high-throughput screening of 81 catalysts,with 27 transition metals loaded on graphyne(GY1),graphdiyne(GY2),and graphtriyne(GY3),was conducted using first-principles calculations.The results of the screening revealed that Ti@GY3 exhibits the lowest energy barrier for the rate-determining step(0.32 eV)in NRR.Further,to explore the impact of different sp/sp2-hybridized carbon ratios on the catalytic activity of SACs,the mechanism of nitrogen(N2)adsorption,activation,and the comprehen-sive pathway of NRR on Ti@GY1,Ti@GY2,and Ti@GY3 was systematically investigated.It was found that the ratio of sp/sp2-hybridized carbon can significantly modulate the d-band center of the metal,thus affecting the energy barrier of the rate-determining step in NRR,decreasing from Ti@GY1(0.59 eV)to Ti@GY2(0.49 eV),and further to Ti@GY3(0.32 eV).Additionally,the Hall conductance was found to increase with the bias voltage in the range of 0.4-1 V,as calculated by Nanodcal software,demonstrating an improvement in the conduc-tivity of the SAC.In summary,this work provides theo-retical guidance for modulating the electrocatalytic nitrogen reduction activity of SACs by varying the ratio of sp/sp2 hybrid carbon,with Ti@GY3 showing potential as an excellent NRR catalyst.
Nitrogen reduction reactionsSingle-atom catalystsGraphyneRatio of sp/sp2 hybrid carbonHigh-throughput screening
State Key Laboratory of Marine Resource Utilization in South China Sea,School of Materials Science and Engineering,Hainan University,Haikou 570100,China
School of Materials Science and Engineering,Tianjin Key Laboratory of Composite and Functional Materials,Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education),Tianjin University,Tianjin 300072,China
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