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author:

Ahmad, Munir (Ahmad, Munir.) [1] | Hussain, Muhammad Bilal (Hussain, Muhammad Bilal.) [2] | Chen, Jiahui (Chen, Jiahui.) [3] | Yang, Yang (Yang, Yang.) [4] | Wu, Xuexian (Wu, Xuexian.) [5] | Chen, Hao (Chen, Hao.) [6] | Afzal, Shahzad (Afzal, Shahzad.) [7] | Raza, Waseem (Raza, Waseem.) [8] | Zeng, Zhengxin (Zeng, Zhengxin.) [9] | Ye, Fei (Ye, Fei.) [10] | Zhao, Xueyang (Zhao, Xueyang.) [11] | Zhang, Jiujun (Zhang, Jiujun.) [12] | Feng, Renfei (Feng, Renfei.) [13] | Fu, Xian-Zhu (Fu, Xian-Zhu.) [14] | Luo, Jing-Li (Luo, Jing-Li.) [15]

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EI

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:

Atoms Binary alloys Carbon dioxide Density functional theory Direct methanol fuel cells (DMFC) Doping (additives) Electrocatalysts Methanol Methanol fuels Molecules Organometallics Platinum Porous materials Reaction intermediates Ruthenium alloys

Community:

  • [ 1 ] [Ahmad, Munir]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, Munir]Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo; 315100, China
  • [ 3 ] [Hussain, Muhammad Bilal]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, Jiahui]School of Materials Science and Hydrogen Energy, Foshan University, Foshan; 528200, China
  • [ 5 ] [Yang, Yang]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, Xuexian]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, Hao]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, Shahzad]Department of Environmental Engineering, China Jiliang University, Zhejiang, Hangzhou; 310018, China
  • [ 9 ] [Raza, Waseem]Institute for Advanced Study, Shenzhen University, Shenzhen; 518060, China
  • [ 10 ] [Zeng, Zhengxin]College of Environmental Sciences, Sichuan Agricultural University, Chengdu; 625014, China
  • [ 11 ] [Ye, Fei]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, Xueyang]School of Environmental Science and Technology, Dalian University of Technology, Dalian; 116024, China
  • [ 13 ] [Zhang, Jiujun]College of Materials Science and Engineering, Fuzhou University, Fuzhou; 350108, China
  • [ 14 ] [Zhang, Jiujun]Institute for Sustainable Energy, College of Sciences, Shanghai University, Shanghai; 200444, China
  • [ 15 ] [Feng, Renfei]Canadian Light Source Inc., Saskatoon; SK; S7N 0X4, Canada
  • [ 16 ] [Fu, Xian-Zhu]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, Jing-Li]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

Year: 2024

Issue: 12

Volume: 14

Page: 9134-9143

1 1 . 7 0 0

JCR@2023

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SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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