Energy, Environmental, and Catalysis Applications
- Rongrong Hong
Rongrong Hong
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
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- Yunshuo Wu
Yunshuo Wu
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
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- Yuetan Su*
Yuetan Su
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
*Email: [emailprotected]
More by Yuetan Su
- Eli Stavitski
Eli Stavitski
National Synchrotron Light Source II, Brookhaven National Laboratory, New York 11973, United States
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- Haiqiang Wang
Haiqiang Wang
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
More by Haiqiang Wang
- Zhongbiao Wu
Zhongbiao Wu
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
More by Zhongbiao Wu
- Xuanhao Wu*
Xuanhao Wu
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
*Email: [emailprotected]
More by Xuanhao Wu
- Xiaole Weng
Xiaole Weng
Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, P.R. China
Zhejiang Provincial Key Laboratory of Air Pollution Monitoring and Synergistic Control, Hangzhou 310058, P.R. China
ZJU-Hangzhou Global Scientific and Technological Innovation Center, Hangzhou 311200, P. R. China
More by Xiaole Weng
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ACS Applied Materials & Interfaces
Cite this: ACS Appl. Mater. Interfaces 2025, XXXX, XXX, XXX-XXX
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https://pubs.acs.org/doi/10.1021/acsami.5c00172
Published April 28, 2025
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Tailoring and stabilizing the active sites of supported noble-metal catalysts to a semioxidized state with unsaturated coordination remain a long-standing challenge in heterogeneous catalysis. Herein, we develop a reaction-atmosphere-driven evolution approach for dynamic structural tuning of semioxidized metal sites in supported Pt catalysts. N2O as an alternative oxidant is used over Pt/TiO2 in CH4 combustion to dynamically prompt the transformation of Pt0 nanoclusters into Ptδ+ (0 < δ < 2) nanoclusters. Compared to CH4 combustion with O2 that inclines to overoxidize Pt0, the catalytic activity of CH4–N2O combustion is distinctly boosted, achieving complete CH4 combustion at only 200 °C, outperforming the state-of-the-art catalysts using O2 as the oxidant. Computational and experimental studies validate that N2O triggers less electron transfer from Pt than from O2, thereby facilitating the formation and preservation of Ptδ+ species during CH4 combustion. The newly emerged semioxidized Ptδ+ species with oxygen-deficient coordination structures simultaneously enhance lattice oxygen activation and the first C–H bond dissociation of CH4, contributing to ultralow temperature activity. Our work demonstrates that modulating the reaction atmosphere to achieve the structural dynamic evolution of semioxidized metal sites can provide new strategies for designing highly efficient catalysts for low-temperature CH4 combustion.
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© 2025 American Chemical Society
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- Catalysts
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- Oxygen
- Platinum
- Redox reactions
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ACS Applied Materials & Interfaces
Cite this: ACS Appl. Mater. Interfaces 2025, XXXX, XXX, XXX-XXX
Click to copy citationCitation copied!
Published April 28, 2025
Publication History
Received
Accepted
Revised
Published
online
© 2025 American Chemical Society
Request reuse permissions
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