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Wenhui He, Jian Zhang, Stefan Dieckhöfer, Swapnil Varhade, Ann Cathrin Brix, Anna Lielpētere, Sabine Seisel, João R. C. Junqueira, Wolfgang W. Schuhmann
Electrocatalytic recycling of waste nitrate (NO 3 − ) to valuable ammonia (NH 3 ) 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 NH 3 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 NO 3 − -to-NH 3 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/CuO x and Co/CoO phases. Electrochemical evaluation, kinetic studies, and in−situ Raman spectra reveal that the inner Cu/CuO x phases preferentially catalyze NO 3 − reduction to NO 2 − , which is rapidly reduced to NH 3 at the nearby Co/CoO shell. This unique tandem catalyst system leads to a NO 3 − -to-NH 3 Faradaic efficiency of 93.3 ± 2.1% in a wide range of NO 3 − concentrations at pH 13, a high NH 3 yield rate of 1.17 mmol cm −2 h −1 in 0.1 M NO 3 − at −0.175 V vs. RHE, and a half-cell energy efficiency of ~36%, surpassing most previous reports.
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He, W., Zhang, J., Dieckhöfer, S., Varhade, S., Brix, A. C., Lielpētere, A., Seisel, S., Junqueira, J. R. C., & Schuhmann, W. W. (2022). Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia. Nature Communications, 13(1), 1129. https://doi.org/10.1038/s41467-022-28728-4
He, Wenhui, et al. "Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia." Nature Communications, vol. 13, no. 1, 2022, pp. 1129, https://doi.org/10.1038/s41467-022-28728-4.
He, Wenhui, Jian Zhang, Stefan Dieckhöfer, Swapnil Varhade, Ann Cathrin Brix, Anna Lielpētere, Sabine Seisel, João R. C. Junqueira, and Wolfgang W. Schuhmann. "Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia." Nature Communications 13, no. 1 (2022): 1129. https://doi.org/10.1038/s41467-022-28728-4.
He W., Zhang J., Dieckhöfer S. [и др.] Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia // Nature Communications. — 2022. — Vol. 13, № 1. — P. 1129. — URL: https://doi.org/10.1038/s41467-022-28728-4
@article{he2022splicing,
title = {{Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia}},
author = {Wenhui He and Jian Zhang and Stefan Dieckhöfer and Swapnil Varhade and Ann Cathrin Brix and Anna Lielpētere and Sabine Seisel and João R. C. Junqueira and Wolfgang W. Schuhmann},
journal = {Nature Communications},
year = {2022},
volume = {13},
number = {1},
pages = {1129},
doi = {10.1038/s41467-022-28728-4},
url = {https://doi.org/10.1038/s41467-022-28728-4}
}TY - JOUR AU - He, Wenhui AU - Zhang, Jian AU - Dieckhöfer, Stefan AU - Varhade, Swapnil AU - Brix, Ann Cathrin AU - Lielpētere, Anna AU - Seisel, Sabine AU - Junqueira, João R. C. AU - Schuhmann, Wolfgang W. TI - Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia JO - Nature Communications VL - 13 IS - 1 SP - 1129 PY - 2022 DA - 2022/03/02 DO - 10.1038/s41467-022-28728-4 UR - https://doi.org/10.1038/s41467-022-28728-4 ER -
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