Electron penetration triggering interface activity of Pt-graphene for CO oxidation at room temperature

Yong Wang; Pengju Ren; Jingting Hu; Yunchuan Tu; Zhongmiao Gong; Yi Cui; Yanping Zheng; Mingshu Chen; Wujun Zhang; Chao Ma; Liang Yu; Fan Yang; Ye Wang; Xinhe Bao; Dehui Deng

doi:10.1038/s41467-021-26089-y

Electron penetration triggering interface activity of Pt-graphene for CO oxidation at room temperature

Nat Commun. 2021 Oct 4;12(1):5814. doi: 10.1038/s41467-021-26089-y.

Authors

Yong Wang^#^{1

2}, Pengju Ren^#^{3

4}, Jingting Hu^{1

2}, Yunchuan Tu^{1

2}, Zhongmiao Gong⁵, Yi Cui⁵, Yanping Zheng¹, Mingshu Chen¹, Wujun Zhang⁶, Chao Ma⁶, Liang Yu², Fan Yang², Ye Wang¹, Xinhe Bao², Dehui Deng^{7

8}

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, 361005, Xiamen, China.
² State Key Laboratory of Catalysis, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023, Dalian, China.
³ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, 030001, Taiyuan, China.
⁴ National Energy Center for Coal to Liquids, Synfuels China Co. Ltd., 101407, Beijing, China.
⁵ Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, 215123, Suzhou, China.
⁶ Center for High Resolution Electron Microscopy, College of Materials Science and Engineering, Hunan University, 410082, Changsha, China.
⁷ State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, 361005, Xiamen, China. dhdeng@dicp.ac.cn.
⁸ State Key Laboratory of Catalysis, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023, Dalian, China. dhdeng@dicp.ac.cn.

^# Contributed equally.

Abstract

Achieving CO oxidation at room temperature is significant for gas purification but still challenging nowadays. Pt promoted by 3d transition metals (TMs) is a promising candidate for this reaction, but TMs are prone to be deeply oxidized in an oxygen-rich atmosphere, leading to low activity. Herein we report a unique structure design of graphene-isolated Pt from CoNi nanoparticles (PtǀCoNi) for efficiently catalytic CO oxidation in an oxygen-rich atmosphere. CoNi alloy is protected by ultrathin graphene shell from oxidation and therefore modulates the electronic property of Pt-graphene interface via electron penetration effect. This catalyst can achieve near 100% CO conversion at room temperature, while there are limited conversions over Pt/C and Pt/CoNiO_x catalysts. Experiments and theoretical calculations indicate that CO will saturate Pt sites, but O₂ can adsorb at the Pt-graphene interface without competing with CO, which facilitate the O₂ activation and the subsequent surface reaction. This graphene-isolated system is distinct from the classical metal-metal oxide interface for catalysis, and it provides a new thought for the design of heterogeneous catalysts.

Abstract

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