Fang, Jia-Yi, Zheng, Qi-Zheng, Lou, Yao-Yin, Zhao, Kuang-Min, Hu, Sheng-Nan, Li, Guang, Akdim, Ouardia, Huang, Xiao-Yang and Sun, Shi-Gang
2022.
Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature.
Nature Communications
13
(1)
, 7899.
10.1038/s41467-022-35533-6
![]() |
Preview |
PDF
- Published Version
Available under License Creative Commons Attribution. Download (2MB) | Preview |
Abstract
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 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm−2 at −0.2 V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8 mmol cm−2 h−1 (960 mmol gcat−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.
Item Type: | Article |
---|---|
Date Type: | Published Online |
Status: | Published |
Schools: | Chemistry Cardiff Catalysis Institute (CCI) |
Publisher: | Nature Research |
Funders: | National Natural Science Foundation of China (NSFC) |
Date of First Compliant Deposit: | 12 January 2023 |
Date of Acceptance: | 8 December 2022 |
Last Modified: | 01 Jun 2023 19:03 |
URI: | https://orca.cardiff.ac.uk/id/eprint/155804 |
Actions (repository staff only)
![]() |
Edit Item |