Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia

Wenhui He, Jian Zhang, Stefan Dieckhöfer, Swapnil Varhade, Ann Cathrin Brix, Anna Lielpetere, Sabine Seisel, João R. C. Junqueira and Wolfgang Schuhmann ()
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Wenhui He: Ruhr University Bochum
Jian Zhang: Ruhr University Bochum
Stefan Dieckhöfer: Ruhr University Bochum
Swapnil Varhade: Ruhr University Bochum
Ann Cathrin Brix: Ruhr University Bochum
Anna Lielpetere: Ruhr University Bochum
Sabine Seisel: Ruhr University Bochum
João R. C. Junqueira: Ruhr University Bochum
Wolfgang Schuhmann: Ruhr University Bochum

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: Abstract Electrocatalytic recycling of waste nitrate (NO3−) to valuable ammonia (NH3) at ambient conditions is a green and appealing alternative to the Haber−Bosch process. However, the reaction requires multi-step electron and proton transfer, making it a grand challenge to drive high-rate NH3 synthesis in an energy-efficient way. Herein, we present a design concept of tandem catalysts, which involves coupling intermediate phases of different transition metals, existing at low applied overpotentials, as cooperative active sites that enable cascade NO3−-to-NH3 conversion, in turn avoiding the generally encountered scaling relations. We implement the concept by electrochemical transformation of Cu−Co binary sulfides into potential-dependent core−shell Cu/CuOx and Co/CoO phases. Electrochemical evaluation, kinetic studies, and in−situ Raman spectra reveal that the inner Cu/CuOx phases preferentially catalyze NO3− reduction to NO2−, which is rapidly reduced to NH3 at the nearby Co/CoO shell. This unique tandem catalyst system leads to a NO3−-to-NH3 Faradaic efficiency of 93.3 ± 2.1% in a wide range of NO3− concentrations at pH 13, a high NH3 yield rate of 1.17 mmol cm−2 h−1 in 0.1 M NO3− at −0.175 V vs. RHE, and a half-cell energy efficiency of ~36%, surpassing most previous reports.

Date: 2022
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DOI: 10.1038/s41467-022-28728-4

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