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

Abstract

The development of electrocatalysts capable of efficient reduction of nitrate (NO 3−) to ammonia (NH 3) 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 NO 2−via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO x−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 NH 3 production rate reaches a high activity of 4.8 mmol cm−2 h−1(960 mmol 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 NO 3−to NH 3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO 3 led simultaneously to high NH 3 selectivity and yield.