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- W4283213246 endingPage "121651" @default.
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- W4283213246 abstract "Electrocatalytic nitrogen reduction reaction (NRR) is an appealing strategy for green ammonia synthesis. Despite tremendous efforts, current NRR performances of most catalysis systems remain far below the targets for practical applications. Herein, a highly active and selective NRR catalysis system is reported by using an Rh single-atom catalyst in water-in-salt electrolytes (WISE). The developed single-atomic Rh on MnO 2 (Rh 1 /MnO 2 ) catalyst in 9 m K 2 SO 4 presents a superior NH 3 yield of 271.8 μg h −1 mg −1 and Faradaic efficiency of 73.3%, far exceeding that in dilute electrolyte and representing one of the best NRR performances on record. Multiple operando XAS, in situ FTIR/Raman spectroscopic characterizations together with the theoretical calculations unravel that WISE enables Rh 1 /MnO 2 to exhibit suppressed H 2 evolution, increased N 2 enrichment on catalyst surface, and enhanced N 2 activation/hydrogenation on active Rh sites. A record-high NRR performance (271.8 μg h −1 mg −1 , 73.3%) was achieved over an Rh single-atom catalyst (Rh 1 /MnO 2 ) in water-in-salt electrolytes (WISE). Combined theoretical computations and operando/in situ spectroscopic characterizations revealed that WISE endowed Rh 1 /MnO 2 with suppressed H 2 evolution, increased N 2 enrichment on catalyst surface, and enhanced N 2 activation/hydrogenation on active Rh sites. • We combine catalyst and electrolyte engineering to achieve an ultra-efficiency nitrogen reduction reaction (NRR). • A record-high NH 3 yield of 271.8 μg h −1 mg −1 and FE of 73.3% is achieved in this new catalysis system. • Multiple operando characterizations and theoretical calculations are adopted to profoundly understand the NRR mechanism." @default.
- W4283213246 created "2022-06-22" @default.
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- W4283213246 date "2022-11-01" @default.
- W4283213246 modified "2023-10-17" @default.
- W4283213246 title "Ultra-efficient N2 electroreduction achieved over a rhodium single-atom catalyst (Rh1/MnO2) in water-in-salt electrolyte" @default.
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- W4283213246 doi "https://doi.org/10.1016/j.apcatb.2022.121651" @default.
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