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Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products.
Zhuang, Tao-Tao; Nam, Dae-Hyun; Wang, Ziyun; Li, Hui-Hui; Gabardo, Christine M; Li, Yi; Liang, Zhi-Qin; Li, Jun; Liu, Xiao-Jing; Chen, Bin; Leow, Wan Ru; Wu, Rui; Wang, Xue; Li, Fengwang; Lum, Yanwei; Wicks, Joshua; O'Brien, Colin P; Peng, Tao; Ip, Alexander H; Sham, Tsun-Kong; Yu, Shu-Hong; Sinton, David; Sargent, Edward H.
Afiliación
  • Zhuang TT; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Nam DH; Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Center for Excellence in Nanoscience, Department of Chemistry, University of Science and Technology of China, Hefei, An
  • Wang Z; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Li HH; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Gabardo CM; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Li Y; Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Center for Excellence in Nanoscience, Department of Chemistry, University of Science and Technology of China, Hefei, An
  • Liang ZQ; Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, ON, M5S 3G8, Canada.
  • Li J; Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Center for Excellence in Nanoscience, Department of Chemistry, University of Science and Technology of China, Hefei, An
  • Liu XJ; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Chen B; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Leow WR; Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, ON, M5S 3G8, Canada.
  • Wu R; Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Center for Excellence in Nanoscience, Department of Chemistry, University of Science and Technology of China, Hefei, An
  • Wang X; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Li F; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Lum Y; Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Center for Excellence in Nanoscience, Department of Chemistry, University of Science and Technology of China, Hefei, An
  • Wicks J; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • O'Brien CP; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Peng T; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Ip AH; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Sham TK; Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, ON, M5S 3G8, Canada.
  • Yu SH; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Sinton D; Department of Electrical and Computer Engineering, University of Toronto, 35 St George Street, Toronto, ON, M5S 1A4, Canada.
  • Sargent EH; Department of Chemistry, University of Western Ontario, 1151 Richmond Street, London, ON, N6A 5B7, Canada.
Nat Commun ; 10(1): 4807, 2019 10 22.
Article en En | MEDLINE | ID: mdl-31641126
ABSTRACT
The upgrading of CO2/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2019 Tipo del documento: Article País de afiliación: Canadá

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2019 Tipo del documento: Article País de afiliación: Canadá
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