Heterogeneous single-cluster catalysts(Mn3,Fe3,CO3,and MO3)supported on nitrogen-doped graphene for robust electrochemical nitrogen reduction

• 作者: Guokui Zheng Lei Li Ziqi Tian Xingwang Zhang Liang Chen
• 来源期刊: 能源化学
• 年，卷（期）: 2021,（3）
• 页码范围: 612-619
• 页数: 8页
• 语种: 英文

摘要

Electrochemical nitrogen reduction reaction(NRR)is one of the most promising alternatives to the tradi-tional Haber-Bosch process.Designing efficient electrocatalysts is still challenging.Inspired by the recent experimental and theoretical advances on single-cluster catalysts(SCCs),we systematically investigated the catalytic performance of various triple-transition-metal-atom clusters anchored on nitrogen-doped graphene for NRR through density functional theory(DFT)calculation.Among them,Mn3-N4,Fe3-N4,Co3-N4,and Mo3-N4 were screened out as electrocatalysis systems composed of non-noble metal with high activity,selectivity,stability,and feasibility.Particularly,the Co3-N4 possesses the highest activity with a limiting potential of-0.41 V through the enzymatic mechanism.The outstanding performance of Co3-N4 can be attributed to the unique electronic structure leading to strong π backdonation,which is crucial in effective N2 activation.This work not only predicts four efficient non-noble metal electrocat-alysts for NRR,but also suggest the SCCs can serve as potential candidates for other important electro-chemical reactions.