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

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

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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

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