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- Title
Reversible dehydrogenation and rehydrogenation of cyclohexane and methylcyclohexane by single-site platinum catalyst.
- Authors
Chen, Luning; Verma, Pragya; Hou, Kaipeng; Qi, Zhiyuan; Zhang, Shuchen; Liu, Yi-Sheng; Guo, Jinghua; Stavila, Vitalie; Allendorf, Mark D.; Zheng, Lansun; Salmeron, Miquel; Prendergast, David; Somorjai, Gabor A.; Su, Ji
- 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. Developing highly efficient and reversible hydrogenation-dehydrogenation catalysts shows great promise for hydrogen storage technologies. Here the authors develop a highly efficient and reversible de/rehydrogenation single-site platinum catalyst which exhibits great promise for hydrogen storage technologies with cyclic alkanes/aromatics as liquid organic hydrogen carriers.
- Subjects
PLATINUM catalysts; CATALYSTS; METHYL cyclohexane; CYCLOHEXANE; DEHYDROGENATION; HYDROGEN storage
- Publication
Nature Communications, 2022, Vol 13, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-022-28607-y