Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 24, Pages 9711-9718Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202002337
Keywords
ammonia synthesis; computational catalyst design; electrocatalysis; NO removal
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Funding
- China Postdoctoral Science Foundation Grant [2019M661140] Funding Source: Medline
- National Natural Science Foundation of China [91845103, 21802124, 21988101, 91945302, 21890753] Funding Source: Medline
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21010208] Funding Source: Medline
- DNL Cooperation Fund, CAS [No. DNL180201, DNL180201] Funding Source: Medline
- National Key R&D Program of China [2016YFA0204100, 2016YFA0200200] Funding Source: Medline
- Key Research Program of Frontier Sciences of the Chinese Academy of Sciences [QYZDB-SSW-JSC020] Funding Source: Medline
- LiaoNing Revitalization Talents Program [XLYC1907099] Funding Source: Medline
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NO removal from exhausted gas is necessary owing to its damage to environment. Meanwhile, the electrochemical ammonia synthesis (EAS) from N(2)suffers from low reaction rate and Faradaic efficiency (FE). Now, an alternative route for ammonia synthesis is proposed from exhaust NO via electrocatalysis. DFT calculations indicate electrochemical NO reduction (NORR) is more active than N(2)reduction (NRR). Via a descriptor-based approach, Cu was screened out to be the most active transition metal catalyst for NORR to NH(3)owing to its moderate reactivity. Kinetic barrier calculations reveal NH(3)is the most preferred product relative to H-2, N2O, and N(2)on Cu. Experimentally, a record-high EAS rate of 517.1 mu mol cm(-2) h(-1)and FE of 93.5 % were achieved at -0.9 V vs. RHE using a Cu foam electrode, exhibiting stable electrocatalytic performances with a 100 h run. This work provides an alternative strategy to EAS from exhaust NO, coupled with NO removal.
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