Efficient Electrochemical Nitrate Reduction to Ammonia with Copper supported Rhodium Cluster and Single-Atom Catalysts
| Autor: | Huimin Liu, Xiuyao Lang, Chao Zhu, Janis Timoshenko, Martina Rüscher, Lichen Bai, Néstor Guijarro, Haibo Yin, Yue Peng, Junhua Li, Zheng Liu, Weichao Wang, Beatriz Roldan Cuenya, Jingshan Luo |
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| Přispěvatelé: | Universidad de Alicante. Instituto Universitario de Electroquímica, Grupo de Fotoquímica y Electroquímica de Semiconductores (GFES) |
| Jazyk: | angličtina |
| Rok vydání: | 2022 |
| Předmět: | |
| Zdroj: | Angewandte Chemie Angewandte Chemie International Edition |
| Popis: | The electrochemical nitrate reduction reaction (NITRR) provides a promising solution for restoring the imbalance in the global nitrogen cycle while enabling a sustainable and decentralized route to source ammonia. Here, we demonstrate a novel electrocatalyst for NITRR consisting of Rh clusters and single-atoms dispersed onto Cu nanowires (NWs), which delivers a partial current density of 162 mA cm−2 for NH3 production and a Faradaic efficiency (FE) of 93% at −0.2 V vs. RHE. The highest ammonia yield rate reached a record value of 1.27 mmol h−1 cm−2. Detailed investigations by electron spin resonance, in-situ infrared spectroscopy, differential electrochemical mass spectrometry and density functional theory modeling suggest that the high activity originates from the synergistic catalytic cooperation between Rh and Cu sites, whereby adsorbed hydrogen on Rh sites transfer to vicinal *NO intermediate species adsorbed on Cu promoting the hydrogenation and ammonia formation. This work is supported by the Chinese Thousand Talents Program for Young Professionals, the startup funding from Nankai University, the “111” project (Grant No. B16027), the Spanish Ministry of Science & Innovation for the “Ramon y Cajal” Program (RYC2018-023888-I), and the Singapore Ministry of Education AcRF Tier 2 (2016-T2-2-153, 2016-T2-1-131), AcRF Tier 1 (RG7/18 and RG161/19). L. Bai acknowledges the Early Postdoc Research Fellowship (P2ELP2_199800) from the Swiss National Science Foundation. XAS experiments were performed at CLAESS beamline at ALBA Synchrotron with the collaboration of ALBA staff. |
| Databáze: | OpenAIRE |
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