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author:

Ahmad, M. (Ahmad, M..) [1] | Hussain, M.B. (Hussain, M.B..) [2] | Chen, J. (Chen, J..) [3] | Yang, Y. (Yang, Y..) [4] | Wu, X. (Wu, X..) [5] | Chen, H. (Chen, H..) [6] | Afzal, S. (Afzal, S..) [7] | Raza, W. (Raza, W..) [8] | Zeng, Z. (Zeng, Z..) [9] | Ye, F. (Ye, F..) [10] | Zhao, X. (Zhao, X..) [11] | Zhang, J. (Zhang, J..) [12] | Feng, R. (Feng, R..) [13] | Fu, X.-Z. (Fu, X.-Z..) [14] | Luo, J.-L. (Luo, J.-L..) [15]

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Scopus

Abstract:

Bottlenecks in direct methanol fuel cells (DMFCs) with conventional noble metals as anode catalysts involve the formation of valueless byproducts and carbon dioxide (CO2) emissions. Carbon-supported Pt single atoms have demonstrated high performance in DMFCs. However, the adsorbed intermediates (COads) strongly bind to Pt single-atom sites, resulting in complete methanol oxidation to CO2 and low power densities. Herein, we have developed a DMFC for CO2-emission-free coproduction of electricity and valuable formate using metal organic framework (MOF)-derived N-doped porous carbon-supported PtRu single-atom (referred to as PtRuSA/NPC) catalysts. The DMFC produces current and power densities of 657 mA cm-2 and 97.4 mW cm-2, respectively, at a potential of 0.65 V with a 98.4% Faraday efficiency for formate at 80 °C. Density functional theory (DFT) calculations show that CH3OH molecules preferentially adsorb onto the PtRu single atoms, but their oxidation to CO2 molecules on PtRuSA/NPC is kinetically unfavorable due to the large energy barrier. This study offers a pathway to developing high-performance and CO2-emission-free electrocatalysts for DMFCs. © 2024 American Chemical Society.

Keyword:

CO2-emission-free DMFCs electrocatalysts formate production PtRu single atoms

Community:

  • [ 1 ] [Ahmad M.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China
  • [ 2 ] [Ahmad M.]Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100, China
  • [ 3 ] [Hussain M.B.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China
  • [ 4 ] [Chen J.]School of Materials Science and Hydrogen Energy, Foshan University, Foshan, 528200, China
  • [ 5 ] [Yang Y.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China
  • [ 6 ] [Wu X.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China
  • [ 7 ] [Chen H.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China
  • [ 8 ] [Afzal S.]Department of Environmental Engineering, China Jiliang University, Zhejiang, Hangzhou, 310018, China
  • [ 9 ] [Raza W.]Institute for Advanced Study, Shenzhen University, Shenzhen, 518060, China
  • [ 10 ] [Zeng Z.]College of Environmental Sciences, Sichuan Agricultural University, Chengdu, 625014, China
  • [ 11 ] [Ye F.]Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China
  • [ 12 ] [Zhao X.]School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China
  • [ 13 ] [Zhang J.]College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 14 ] [Zhang J.]Institute for Sustainable Energy, College of Sciences, Shanghai University, Shanghai, 200444, China
  • [ 15 ] [Feng R.]Canadian Light Source Inc., Saskatoon, S7N 0X4, SK, Canada
  • [ 16 ] [Fu X.-Z.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China
  • [ 17 ] [Luo J.-L.]Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518055, China

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Source :

ACS Catalysis

ISSN: 2155-5435

Year: 2024

Issue: 12

Volume: 14

Page: 9134-9143

1 1 . 7 0 0

JCR@2023

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 3

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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