Theoretical Investigations of Electrochemical Nitrogen Reduction on Single Transition Metal Atom Catalysts Supported by 1T-MoSe2
The search for stable and efficient single-atom catalysts(SACs)for the electrocatalytic nitrogen reduction reaction(eNRR)has garnered signif-icant theoretical interest.In this study,we evaluate the eNRR perfor-mance of eighteen two-dimensional 1T-MoSe2-supported transition met-al single-atom catalysts(TM@1T-MoSe2,TM=V,Cr,Mn,Fe,Co,Ni,Nb,Mo,Tc,Ru,Rh,Pd,Ta,W,Re,Os,Ir,and Pt)using density func-tional theory calculations.We as-sess the stability of each TM@1T-MoSe2,as well as the limiting potential of eNRR and the ammonia selectivity on each stable TM@1T-MoSe2.Our results show that W@1T-MoSe2 is the most promising single-atom catalyst for eNRR,with a limiting potential of-0.23 V via the distal pathway starting from three co-adsorbed nitrogen molecules.Furthermore,the mul-ti-adsorption of N2 on W@1T-MoSe2 effectively suppress the hydrogen evolution reaction,thus enhancing the selectivity of the eNRR.This research provides a promising avenue for the development of a new class of 1T-MoSe2-based single-atom catalysts for electrocatalytic am-monia synthesis.
Density functional theorySingle-atom catalystElectrochemical nitrogen re-ductionSelectivityActivity
孙阿强、秦明鑫、朱少通、周颖、白志强、张文华
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中国科学技术大学精准智能化学重点实验室,合肥 230026
中国科学技术大学合肥微尺度物质科学国家研究中心,合肥 230026
河南师范大学物理学院,新乡 453007
密度泛函理论 单原子催化剂 氮气电还原 选择性 活性
国家重点研发计划国家重点研发计划国家自然科学基金CAS Project for Young Scientists in Basic ResearchInnovation Program for Quantum Science and TechnologyUSTC Tang Scholarship
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