Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 37, Pages 14515-14519Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b06482
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Funding
- National Natural Science Foundation of China [21673215, 21533007, U1632263]
- Fundamental Research Funds for the Central Universities [WK2060030029, WK3430000005]
- Users with Excellence Program of Hefei Science Center CAS [2019HSC-UE016]
- Max -Planck Partner Group
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Developing an active and stable metal single-atom catalyst (SAC) is challenging due to the high surface free energy of metal atoms. In this work, we report that tailoring of the 5d state of Pt-1 single atoms on Co3O4 through strong electronic metal-support interactions (EMSIs) boosts the activity up to 68-fold higher than those on other supports in dehydrogenation of ammonia borane for room-temperature hydrogen generation. More importantly, this catalyst also exhibits excellent stability against sintering and leaching, in sharp contrast to the rapid deactivation observed on other Pt single-atom and nanoparticle catalysts. Detailed spectroscopic characterization and theoretical calculations revealed that the EMSI tailors the unoccupied 5d state of Pt-1 single atoms, which modulates the adsorption of ammonia borane and facilities hydrogen desorption, thus leading to the high activity. Such extraordinary electronic promotion was further demonstrated on Pd-1/Co3O4 and in hydrogenation reactions, providing a new promising way to design advanced SACs with high activity and stability.
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