Reversible dehydrogenation and rehydrogenation of cyclohexane and methylcyclohexane by single-site platinum catalyst

Luning Chen, Pragya Verma, Kaipeng Hou, Zhiyuan Qi, Shuchen Zhang, Yi-Sheng Liu, Jinghua Guo, Vitalie Stavila, Mark D. Allendorf, Lansun Zheng, Miquel Salmeron, David Prendergast (), Gabor A. Somorjai () and Ji Su ()
Additional contact information
Luning Chen: The Molecular Foundry, Lawrence Berkeley National Laboratory
Pragya Verma: The Molecular Foundry, Lawrence Berkeley National Laboratory
Kaipeng Hou: University of California-Berkeley
Zhiyuan Qi: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Shuchen Zhang: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Yi-Sheng Liu: Advanced Light Source, Lawrence Berkeley National Laboratory
Jinghua Guo: Advanced Light Source, Lawrence Berkeley National Laboratory
Vitalie Stavila: Sandia National Laboratories
Mark D. Allendorf: Sandia National Laboratories
Lansun Zheng: Xiamen University
Miquel Salmeron: Chemical Sciences Division, Lawrence Berkeley National Laboratory
David Prendergast: The Molecular Foundry, Lawrence Berkeley National Laboratory
Gabor A. Somorjai: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Ji Su: The Molecular Foundry, Lawrence Berkeley National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Developing highly efficient and reversible hydrogenation-dehydrogenation catalysts shows great promise for hydrogen storage technologies with highly desirable economic and ecological benefits. Herein, we show that reaction sites consisting of single Pt atoms and neighboring oxygen vacancies (VO) can be prepared on CeO2 (Pt1/CeO2) with unique catalytic properties for the reversible dehydrogenation and rehydrogenation of large molecules such as cyclohexane and methylcyclohexane. Specifically, we find that the dehydrogenation rate of cyclohexane and methylcyclohexane on such sites can reach values above 32,000 molH2 molPt−1 h−1, which is 309 times higher than that of conventional supported Pt nanoparticles. Combining of DRIFTS, AP-XPS, EXAFS, and DFT calculations, we show that the Pt1/CeO2 catalyst exhibits a super-synergistic effect between the catalytic Pt atom and its support, involving redox coupling between Pt and Ce ions, enabling adsorption, activation and reaction of large molecules with sufficient versatility to drive abstraction/addition of hydrogen without requiring multiple reaction sites.

Date: 2022
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DOI: 10.1038/s41467-022-28607-y

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