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Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation.
Wen, Yunzhou; Chen, Peining; Wang, Lu; Li, Shangyu; Wang, Ziyun; Abed, Jehad; Mao, Xinnan; Min, Yimeng; Dinh, Cao Thang; Luna, Phil De; Huang, Rui; Zhang, Longsheng; Wang, Lie; Wang, Liping; Nielsen, Robert J; Li, Huihui; Zhuang, Taotao; Ke, Changchun; Voznyy, Oleksandr; Hu, Yongfeng; Li, Youyong; Goddard, William A; Zhang, Bo; Peng, Huisheng; Sargent, Edward H.
Afiliación
  • Wen Y; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Chen P; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Wang L; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Li S; Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China.
  • Wang Z; Materials and Process Simulation Center (MSC) and Joint Center for Artificial Photosynthesis (JCAP), California Institute of Technology, Pasadena, California 91125, United States.
  • Abed J; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Mao X; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Min Y; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Dinh CT; Department of Materials Science & Engineering, University of Toronto, 27 King's College Circle, Toronto, Ontario M5S 1A1, Canada.
  • Luna P; Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China.
  • Huang R; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Zhang L; Department of Chemical Engineering, Queen's University, Kingston, Ontario K7L 3N6, Canada.
  • Wang L; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Wang L; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Nielsen RJ; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Li H; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Zhuang T; State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.
  • Ke C; Materials and Process Simulation Center (MSC) and Joint Center for Artificial Photosynthesis (JCAP), California Institute of Technology, Pasadena, California 91125, United States.
  • Voznyy O; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Hu Y; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Li Y; Institute of Fuel Cell, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.
  • Goddard WA; Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario M5S 3G4, Canada.
  • Zhang B; Canadian Light Source Inc., Saskatoon, SK S7N 2 V3 Saskatchewan, Canada.
  • Peng H; Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China.
  • Sargent EH; Materials and Process Simulation Center (MSC) and Joint Center for Artificial Photosynthesis (JCAP), California Institute of Technology, Pasadena, California 91125, United States.
J Am Chem Soc ; 143(17): 6482-6490, 2021 05 05.
Article en En | MEDLINE | ID: mdl-33891414
ABSTRACT
In hydrogen production, the anodic oxygen evolution reaction (OER) limits the energy conversion efficiency and also impacts stability in proton-exchange membrane water electrolyzers. Widely used Ir-based catalysts suffer from insufficient activity, while more active Ru-based catalysts tend to dissolve under OER conditions. This has been associated with the participation of lattice oxygen (lattice oxygen oxidation mechanism (LOM)), which may lead to the collapse of the crystal structure and accelerate the leaching of active Ru species, leading to low operating stability. Here we develop Sr-Ru-Ir ternary oxide electrocatalysts that achieve high OER activity and stability in acidic electrolyte. The catalysts achieve an overpotential of 190 mV at 10 mA cm-2 and the overpotential remains below 225 mV following 1,500 h of operation. X-ray absorption spectroscopy and 18O isotope-labeled online mass spectroscopy studies reveal that the participation of lattice oxygen during OER was suppressed by interactions in the Ru-O-Ir local structure, offering a picture of how stability was improved. The electronic structure of active Ru sites was modulated by Sr and Ir, optimizing the binding energetics of OER oxo-intermediates.

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2021 Tipo del documento: Article País de afiliación: China

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2021 Tipo del documento: Article País de afiliación: China