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Modulating the proton transfer kinetics via Ru single atoms for highly efficient ammonia synthesis

Yu, Suxian (author)
KTH,Mikro- och nanosystemteknik,State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Zhu, Yong (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Wen, Zhibing (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
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Yu, Shengming (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Teng, Ziyue (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Liu, Guoquan (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Gao, Hua (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Zhao, Ran (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
Sun, Licheng, 1962- (author)
KTH,Organisk kemi,State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China; Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024, China; Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, 10044 Stockholm, Sweden
Li, Fei (author)
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, Dalian 116024, China
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 (creator_code:org_t)
Elsevier BV, 2023
2023
English.
In: Chem Catalysis. - : Elsevier BV. - 2667-1107 .- 2667-1093. ; 3:9
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • The electrochemical nitrate reduction reaction (eNO3RR) is an appealing technology for converting environmentally toxic NO3− to ammonia (NH3). This approach was usually obstructed by the multi-proton/electron involved process. Here, we report a catalyst with Ru single atoms supported on Co3O4 (Ru SAs-Co3O4). The as-developed Ru SAs-Co3O4 catalyst shows a remarkable NH3-evolving activity with a faradic efficiency of 94.92% ± 4.02% at the potential of −0.2 V (vs. RHE) and a generation rate of 1,843.45 ± 57.14 μmol h−1 cm−2 at the potential of −0.5 V. Further investigations revealed that the Ru SAs play a dual role in simultaneously accelerating the proton transfer and modulating the d-electron structures of the neighboring Co sites, which led to a lower energy barrier of the rate-determining step. Eventually, by combining the eNO3RR and electrosynthesis of 5,5′-azotetrazolate at a two-electrode system, an energy-saving NH3 synthesis, while simultaneously producing value-added chemicals, was successfully achieved.

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)

Keyword

coupling system
nitrate reduction reaction
proton inventory studies
proton transfer
Ru single atoms
SDG6: Clean water and sanitation
SDG7: Affordable and clean energy

Publication and Content Type

ref (subject category)
art (subject category)

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