Abstract
Single-atom site catalysts can improve the rates and selectivity of many catalytic reactions. We have modified Pt1/CeO2 single sites by combining them with molecular groups and with oxygen vacancies of the support. The new sites include hydrided (Pt2+-Ce3+Hδ−) and hydroxylated (Pt2+-Ce3+OH) sites that exhibit higher reactivity and selectivity to previous single sites for several reactions, including a ninefold increase in the reaction rate for carbon monoxide oxidation and a 2.3-fold improvement of propylene selectivity for oxidative dehydrogenation of propane. The atomic structure and reaction steps of these sites were determined with in situ and ex situ spectroscopy techniques and theoretical methods.
| Original language | English |
|---|---|
| Pages (from-to) | 514-519 |
| Number of pages | 6 |
| Journal | Science |
| Volume | 388 |
| Issue number | 6746 |
| DOIs | |
| State | Published - May 1 2025 |
Funding
Funding: This work was funded by the following: US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, under contract DE-AC02-05CH11231, FWP CH030201 (Catalysis Research Program); Work by J.Y., L.J.F., P.Y., and X.Z. was performed as part of User Projects at the Molecular Foundry of the Lawrence Berkeley National Laboratory under contract DE-AC02-05CH11231. L.J.F. acknowledges support from the Alexander von Humboldt Foundation, Bonn, Germany. P.Y., D.P., and J.S. acknowledge support from the Hydrogen Materials Advanced Research Consortium (HyMARC), established as part of the Energy Materials Network by the US DOE, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, under contract DE-AC02-05CH11231.Y.G. acknowledges support from the National Natural Science Foundation of China under grant 22376075 and the Central China Normal University project (CCNU24JCPT017). Z.W. was supported by the US DOE, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract DE-AC02-05CH11231. The XANES work was supported by National Science and Technology Council of Taiwan under grant NSTC 113-2112-M-213-008. B.Y. and Q.H. acknowledge support from Singapore National Research Foundation under award NRF-NRFF11-2019-0002 and Singapore Low-Carbon Energy Research Funding Initiative hosted under A*STAR (awards U2102d2006; U2305d4003). This research used resources of the National Energy Research Scientific Computing Center, which is supported by the US DOE, Office of Science, under contract DE-AC02-05CH11231. This research used the Lawrencium computational cluster resource provided by the IT Division at the Lawrence Berkeley National Laboratory (supported by US DOE, Office of Science, Office of Basic Energy Sciences, under contract DE-AC02-05CH11231). This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Author contributions: Conceptualization: J.Y., M.S., J.S. Methodology: J.Y., L.J.F., D.P., Y.G., J.L., M.S., J.S. Investigation: J.Y., L.J.F., S.Y., B.Z., P.V., L.D., Y.C., Z.W., X.Z., S.Z., S.C., J.L.C., B.Y., S.T., Q.H., S.N. Visualization: J.Y., L.J.F., S.Y., B.Z., P.V., L.D., B.Y. Funding acquisition: M.S., J.S., Y.G., D.P., L.J.F., Z.W., Q.H., B.Y. Project administration: J.Y., M.S., J.S. Supervision: J.S., M.S., J.L., Y.G., D.P. Writing – original draft: J.Y., L.J.F., S.Y., B.Z., P.V. Writing – review & editing: J.Y., J.S., M.S., J.L., Y.G., D.P., Z.W. Competing interests: Authors declare that they have no competing interests. Data and materials availability: All data are available in the main text or the SM, including data S1 to S11, or have been deposited at Zenodo (37). License information: Copyright © 2025 the authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original US government works. https://www.science.org/about/science-licenses-journal-article-reuse This work was funded by the following: US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, under contract DE-AC02-05CH11231, FWP CH030201 (Catalysis Research Program); Work by J.Y., L.J.F., P.Y., and X.Z. was performed as part of User Projects at the Molecular Foundry of the Lawrence Berkeley National Laboratory under contract DE-AC02-05CH11231. L.J.F. acknowledges support from the Alexander von Humboldt Foundation, Bonn, Germany. P.Y., D.P., and J.S. acknowledge support from the Hydrogen Materials Advanced Research Consortium (HyMARC), established as part of the Energy Materials Network by the US DOE, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, under contract DE-AC02-05CH11231. Y.G. acknowledges support from the National Natural Science Foundation of China under grant 22376075 and the Central China Normal University project (CCNU24JCPT017). Z.W. was supported by the US DOE, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract DE-AC02-05CH11231. The XANES work was supported by National Science and Technology Council of Taiwan under grant NSTC 113-2112-M-213-008. B.Y. and Q.H. acknowledge support from Singapore National Research Foundation under award NRF-NRFF11-2019-0002 and Singapore Low-Carbon Energy Research Funding Initiative hosted under A*STAR (awards U2102d2006; U2305d4003). This research used resources of the National Energy Research Scientific Computing Center, which is supported by the US DOE, Office of Science, under contract DE-AC02-05CH11231. This research used the Lawrencium computational cluster resource provided by the IT Division at the Lawrence Berkeley National Laboratory (supported by US DOE, Office of Science, Office of Basic Energy Sciences, under contract DE-AC02-05CH11231). This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.