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Enhancing Electrochemical Nitrate Reduction to Ammonia over Cu Nanosheets via Facet Tandem Catalysis |
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| Authors: | Yunfan Fu Shuo Wang Yi Wang Pengfei Wei Jiaqi Shao Dr. Tianfu Liu Prof. Dr. Guoxiong Wang Prof. Dr. Xinhe Bao |
| Affiliation: | 1. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China College of Energy, University of Chinese Academy of Sciences, Beijing, 100039 China These authors contributed equally to this work.;2. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China These authors contributed equally to this work.;3. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China College of Energy, University of Chinese Academy of Sciences, Beijing, 100039 China;4. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China |
| Abstract: | Electrochemical conversion of nitrate (NO3−) into ammonia (NH3) represents a potential way for achieving carbon-free NH3 production while balancing the nitrogen cycle. Herein we report a high-performance Cu nanosheets catalyst which delivers a NH3 partial current density of 665 mA cm−2 and NH3 yield rate of 1.41 mmol h−1 cm−2 in a flow cell at −0.59 V vs. reversible hydrogen electrode. The catalyst showed a high stability for 700 h with NH3 Faradaic efficiency of ≈88 % at 365 mA cm−2. In situ spectroscopy results verify that Cu nanosheets are in situ derived from the as-prepared CuO nanosheets under electrochemical NO3− reduction reaction conditions. Electrochemical measurements and density functional theory calculations indicate that the high performance is attributed to the tandem interaction of Cu(100) and Cu(111) facets. The NO2− generated on the Cu(100) facets is subsequently hydrogenated on the Cu(111) facets, thus the tandem catalysis promotes the crucial hydrogenation of *NO to *NOH for NH3 production. |
| Keywords: | Ammonia Cu Nanosheets Electrochemical Reduction Nitrate Reduction Tandem Catalysis |