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author:

Wang, R. (Wang, R..) [1] | Li, G. (Li, G..) [2] | Zong, X. (Zong, X..) [3] | Wang, J. (Wang, J..) [4] | Xu, Y. (Xu, Y..) [5] | Jin, C. (Jin, C..) [6] | Wang, M. (Wang, M..) [7] | Ma, P. (Ma, P..) [8] | Zhang, R. (Zhang, R..) [9] | Zheng, K. (Zheng, K..) [10] | Hu, J. (Hu, J..) [11] | Liao, J. (Liao, J..) [12] | Tang, Y. (Tang, Y..) [14] | Dai, Y. (Dai, Y..) [15] | Wang, S. (Wang, S..) [16]

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Scopus

Abstract:

Supported Pt catalysts often exhibit limited effectiveness in achieving complete methane oxidation, which restricts their commercial application. However, Pt catalysts are particularly attractive, especially in sulfur-containing environments, where commercial Pd catalysts are more susceptible to sulfur poisoning. Therefore, developing highly active Pt sites and gaining a deeper understanding of the intrinsic mechanisms governing methane combustion over Pt catalysts is essential. In this study, we present a highly active stannic oxide supported platinum catalyst (Pt/SnO2) for stable low-temperature methane combustion, achieving a T90 as low as 390 °C at a high gas hourly space velocity (GHSV) of 60,000 mL·gcat-1·h-1. This performance surpasses that of most other Pt catalysts as well as Pd/SnO2 and benchmark Pd/Al2O3. The superior SO2 tolerance of Pt/SnO2 was demonstrated by the stability of methane conversion at 500 °C, with only a minor reduction observed during the long-term online test. Characterization results indicate that the Pt atoms on SnO2 are electron-deficient and predominantly adopt a crowded configuration. In situ studies and density functional theory (DFT) calculations reveal that the electron-deficient, crowded Pt atoms enhance the chemisorption of CH4 molecules by withdrawing the electrons from CH4, resulting in activated CH4 with an elongated C-H bond. This work provides an in-depth understanding of the nature of Pt active sites for high-performance methane combustion, offering valuable insights for the rational design of Pt-based catalysts. © 2025 American Chemical Society.

Keyword:

crowding-atom sites electron-deficient methane combustion platinum SnO2

Community:

  • [ 1 ] [Wang R.]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian, 116023, China
  • [ 2 ] [Wang R.]State Key Laboratory of Clean and Efficient Coal Utilization, Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan, 030024, China
  • [ 3 ] [Li G.]School of Resources and Environment, Nanchang University, 999 Xuefu Road, Jiangxi, Nanchang, 330031, China
  • [ 4 ] [Zong X.]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian, 116023, China
  • [ 5 ] [Zong X.]University of Chinese Academy of Sciences, 1 Yanqihu East Rd, Beijing, 101408, China
  • [ 6 ] [Wang J.]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing, 100124, China
  • [ 7 ] [Xu Y.]Institute of Molecular Engineering Plus, Institute of Molecule Catalysis and In Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 8 ] [Jin C.]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian, 116023, China
  • [ 9 ] [Wang M.]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian, 116023, China
  • [ 10 ] [Ma P.]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing, 100124, China
  • [ 11 ] [Zhang R.]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing, 100124, China
  • [ 12 ] [Zheng K.]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing, 100124, China
  • [ 13 ] [Hu J.]State Key Laboratory of Clean and Efficient Coal Utilization, Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan, 030024, China
  • [ 14 ] [Liao J.]State Key Laboratory of Clean and Efficient Coal Utilization, Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan, 030024, China
  • [ 15 ] [Wang J.]State Key Laboratory of Clean and Efficient Coal Utilization, Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan, 030024, China
  • [ 16 ] [Tang Y.]Institute of Molecular Engineering Plus, Institute of Molecule Catalysis and In Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 17 ] [Dai Y.]Institute of Advanced Synthesis, School of Chemistry and Molecular Engineering, Nanjing Tech University, Nanjing, 211816, China
  • [ 18 ] [Wang S.]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian, 116023, China
  • [ 19 ] [Wang S.]University of Chinese Academy of Sciences, 1 Yanqihu East Rd, Beijing, 101408, China
  • [ 20 ] [Wang S.]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian, 116023, China
  • [ 21 ] [Wang S.]University of Chinese Academy of Sciences, 1 Yanqihu East Rd, Beijing, 101408, China

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Source :

Environmental Science and Technology

ISSN: 0013-936X

Year: 2025

1 0 . 9 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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