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author:

Wang, Ran (Wang, Ran.) [1] | Li, Guobo (Li, Guobo.) [2] | Zong, Xupeng (Zong, Xupeng.) [3] | Wang, Jiaxing (Wang, Jiaxing.) [4] | Xu, Yuanjie (Xu, Yuanjie.) [5] | Jin, Chengwen (Jin, Chengwen.) [6] | Wang, Mingzhe (Wang, Mingzhe.) [7] | Ma, Peijie (Ma, Peijie.) [8] | Zhang, Rui (Zhang, Rui.) [9] | Zheng, Kun (Zheng, Kun.) [10] | Hu, Jiangliang (Hu, Jiangliang.) [11] | Liao, Junjie (Liao, Junjie.) [12] | Wang, Jiancheng (Wang, Jiancheng.) [13] | Tang, Yu (Tang, Yu.) [14] | Dai, Yihu (Dai, Yihu.) [15] | Wang, Shudong (Wang, Shudong.) [16] | Wang, Sheng (Wang, Sheng.) [17]

Indexed by:

EI

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:

Aluminum compounds Atoms Benchmarking Catalyst activity Catalyst poisoning Catalyst supports Chemical bonds Combustion Density functional theory Design for testability Electrons Methane Palladium compounds Platinum Platinum compounds Sulfur

Community:

  • [ 1 ] [Wang, Ran]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian; 116023, China
  • [ 2 ] [Wang, Ran]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, Guobo]School of Resources and Environment, Nanchang University, 999 Xuefu Road, Jiangxi, Nanchang; 330031, China
  • [ 4 ] [Zong, Xupeng]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian; 116023, China
  • [ 5 ] [Zong, Xupeng]University of Chinese Academy of Sciences, 1 Yanqihu East Rd, Beijing; 101408, China
  • [ 6 ] [Wang, Jiaxing]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing; 100124, China
  • [ 7 ] [Xu, Yuanjie]Institute of Molecular Engineering Plus, Institute of Molecule Catalysis and In Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
  • [ 8 ] [Jin, Chengwen]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian; 116023, China
  • [ 9 ] [Wang, Mingzhe]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian; 116023, China
  • [ 10 ] [Ma, Peijie]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing; 100124, China
  • [ 11 ] [Zhang, Rui]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing; 100124, China
  • [ 12 ] [Zheng, Kun]Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing; 100124, China
  • [ 13 ] [Hu, Jiangliang]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, Junjie]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, Jiancheng]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, Yu]Institute of Molecular Engineering Plus, Institute of Molecule Catalysis and In Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
  • [ 17 ] [Dai, Yihu]Institute of Advanced Synthesis, School of Chemistry and Molecular Engineering, Nanjing Tech University, Nanjing; 211816, China
  • [ 18 ] [Wang, Shudong]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian; 116023, China
  • [ 19 ] [Wang, Shudong]University of Chinese Academy of Sciences, 1 Yanqihu East Rd, Beijing; 101408, China
  • [ 20 ] [Wang, Sheng]Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Rd, Dalian; 116023, China
  • [ 21 ] [Wang, Sheng]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

Issue: 24

Volume: 59

Page: 12121-12131

1 0 . 9 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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