Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature

被引：506

作者：

Fang, Jia-Yi ^{[1
]}

Zheng, Qi-Zheng ^{[1
]}

Lou, Yao-Yin ^{[1
,2
,3
]}

Zhao, Kuang-Min ^{[1
]}

Hu, Sheng-Nan ^{[1
]}

Li, Guang ^{[1
]}

Akdim, Ouardia ^{[3
]}

Huang, Xiao-Yang ^{[1
,3
]}

Sun, Shi-Gang ^{[1
,3
]}

机构：

[1] Xiamen Univ, Dept Chem, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China

[2] Soochow Univ, Sch Chem & Environm Engn, Coll Chem Chem Engn & Mat Sci, Suzhou 215123, Jiangsu, Peoples R China

[3] Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales

来源：

NATURE COMMUNICATIONS | 2022年 / 13卷 / 01期

基金：

中国国家自然科学基金; 中国博士后科学基金;

关键词：

ELECTRONIC-STRUCTURE; NITRATE REDUCTION; COPPER; NITROGEN; ENERGY; GAS; ELECTRODEPOSITION; ELECTROOXIDATION; SPECTROSCOPY; ADSORPTION;

D O I：

10.1038/s41467-022-35533-6

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

The development of electrocatalysts capable of efficient reduction of nitrate (NO3-) to ammonia (NH3) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO2- via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NOx- adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 1001% Faradaic efficiency at an ampere-level current density of 1035mAcm(-2) at -0.2V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8mmolcm(-2) h(-1) (960mmol g(cat)(-1) h(-1)). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO3- to NH3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO3 led simultaneously to high NH3 selectivity and yield.

引用

页数：13

共 69 条

[1] AN INFRARED STUDY OF NO ADSORPTION AT DEFECT SITES ON PT(111) [J].