Ag-Co3O4-CoOOH-Nanowires Tandem Catalyst for Efficient Electrocatalytic Conversion of Nitrate to Ammonia at Low Overpotential via Triple Reactions

被引：44

作者：

Wu, Shilu ^{[1
]}

Jiang, Yingyang ^{[1
]}

Luo, Wenjie ^{[1
]}

Xu, Peng ^{[1
]}

Huang, Longlong ^{[1
]}

Du, Yiwen ^{[1
]}

Wang, Hui ^{[1
]}

Zhou, Xuemei ^{[1
]}

Ge, Yongjie ^{[1
]}

Qian, Jinjie ^{[1
]}

Nie, Huagui ^{[1
]}

Yang, Zhi ^{[1
]}

机构：

[1] Wenzhou Univ, Coll Chem & Mat Engn, Key Lab Carbon Mat Zhejiang, Wenzhou 325035, Peoples R China

来源：

ADVANCED SCIENCE | 2023年 / 10卷 / 33期

基金：

美国国家科学基金会;

关键词：

Ag/Co3O4/CoOOH NWs; ammonia; electrocatalysis; nitrate reduction; tandem catalysis; triple reactions; OXYGEN EVOLUTION REACTION; SILVER NANOWIRES; REDUCTION; NANOPARTICLES; ELECTRODES; KINETICS; GROWTH; CO3O4; RAMAN;

D O I：

10.1002/advs.202303789

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The electrocatalytic conversion of nitrate (NO3-) to NH3 (NO3RR) offers a promising alternative to the Haber-Bosch process. However, the overall kinetic rate of NO3RR is plagued by the complex proton-assisted multiple-electron transfer process. Herein, Ag/Co3O4/CoOOH nanowires (i-Ag/Co3O4 NWs) tandem catalyst is designed to optimize the kinetic rate of intermediate reaction for NO3RR simultaneously. The authors proved that NO3-. ions are reduced to NO2-. preferentially on Ag phases and then NO2-. to NO on Co3O4 phases. The CoOOH phases catalyze NO reduction to NH3 via NH2OH intermediate. This unique catalyst efficiently converts NO3-. to NH3 through a triple reaction with a high Faradaic efficiency (FE) of 94.3% and a high NH3 yield rate of 253.7 mu mol h(-1) cm(-2) in 1 M KOH and 0.1 M KNO3 solution at.0.25 V versus RHE. The kinetic studies demonstrate that converting NH2OH into NH3 is the rate-determining step (RDS) with an energy barrier of 0.151 eV over i-Ag/Co3O4 NWs. Further applying i-Ag/Co3O4 NWs as the cathode material, a novel Zn-nitrate battery exhibits a power density of 2.56 mW cm(-2) and an FE of 91.4% for NH3 production.

引用

页数：12

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