Reversible Dehydrogenation-Rehydrogenation Using Single-Site Platinum Catalysts

Scientific Achievement

Proposed cyclohexane dehydrogenation pathway (brown arrow) on Pt₁/CeO₂ at an O vacancy (VO) involving H abstraction to the catalyst surface (as OH⁻) with associated formation of small polarons (Ce³⁺) followed by recombination and release of H₂ (green arrow).

A new catalyst consisting of single Platinum (Pt) atoms is highly efficient and reversible for the dehydrogenation and rehydrogenation of large cyclic hydrocarbons.

Significance and Impact

The new catalyst displays over 300 times higher reaction rates than commercial Pt catalysts for large molecule reactants. This will pave the way for further rational design of highly efficient catalysts for energy generation and storage.

Research Details

The research team fabricated single Pt atoms on CeO₂ and compared it to commercial 5% Pt/Al₂O₃.
By combining DRIFTS, AP-XPS, EXAFS, and DFT calculations, they showed that the Pt1/CeO₂ catalyst exhibits a super-synergistic effect, 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.

Chen, L., Verma, P., Hou, K., Qi, Z., Zhang, S., Liu, Y-S, Guo, J., Stavila, V., Allendorf, M.D., Zheng, L., Salmeron, M., Prendergast, D., Somorjai, G.A., Su, J. Nat Commun 13, 1092 (2022). 10.1038/s41467-022-28607-y

Scientific Achievement

Significance and Impact

Research Details

Chen, L., Verma, P., Hou, K., Qi, Z., Zhang, S., Liu, Y-S, Guo, J., Stavila, V., Allendorf, M.D., Zheng, L., Salmeron, M., Prendergast, D., Somorjai, G.A., Su, J. Nat Commun 13, 1092 (2022). 10.1038/s41467-022-28607-y

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