Theoretical screening of single atoms anchored on defective graphene for electrocatalytic N2 reduction reactions: a DFT study

被引：35

作者：

Liu, Pingping ^{[1
]}

Fu, Cheng ^{[1
]}

Li, Yafei ^{[1
]}

Wei, Haiyan ^{[1
]}

机构：

[1] Nanjing Normal Univ, Sch Chem & Mat Sci, Jiangsu Key Lab NSLSCS, Jiangsu Key Lab Biofunct Mat, Nanjing 210097, Peoples R China

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2020年 / 22卷 / 17期

关键词：

NITROGEN REDUCTION; DOPED GRAPHENE; COMPLEXES BEARING; RECENT PROGRESS; AMMONIA; METAL; DINITROGEN; CATALYST; FIXATION; CONVERSION;

D O I：

10.1039/c9cp06112f

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The reduction of molecular dinitrogen (N-2) to ammonia (NH3) under mild conditions is attractive due to the wide application of ammonia. In this work, we systematically investigated a series of single metal atoms including Sc to Zn, Mo, Ru, Rh, Pd and Ag anchored on defective graphene sheets for the N-2 reduction reaction (NRR) by density functional theory computations. Our calculations revealed that single Mo embedded on nitrogen doped divacancy 555-777 graphene exhibits excellent catalytic performance for the NRR, with low overpotentials of 0.32 V for MoC1N2@555-777 graphene and 0.41 V for MoN3@555-777 graphene. In particular, the removal of produced ammonia from the catalyst surface is a rapid process with a free energy change of less than 0.50 eV. Our study provides a useful guideline for further developing highly effective SACs based on defective graphene for electrochemical reduction reactions.

引用

页码：9322 / 9329

页数：8

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