Abstract
Metal-support interaction plays a crucial role in governing the stability and activity of atomically dispersed platinum catalysts on ceria support. The migration and aggregation of platinum atoms during the catalytic reaction leads to the redistribution of active sites. In this study, by utilizing a multimodal characterization scheme, we observed the aggregation of platinum atoms at high temperatures under reverse water gas shift reaction conditions and the subsequent fragmentation of platinum clusters, forming “single atoms” upon cooling. Theoretical simulations of both effects uncovered the roles of carbon monoxide binding on perimeter Pt sites in the clusters and hydrogen coverage in the aggregation and fragmentation mechanisms. This study highlights the complex effects of adsorbate and supports interactions with metal sites in Pt/ceria catalysts that govern their structural transformations under in situ conditions.
| Original language | English |
|---|---|
| Pages (from-to) | 14716-14721 |
| Number of pages | 6 |
| Journal | Nanoscale |
| Volume | 16 |
| Issue number | 31 |
| DOIs | |
| State | Published - May 15 2024 |
Funding
A. I. F. and H. W. acknowledge support of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (U.S. DOE BES), Grant DE-SC0022199. Y. L.'s effort at ORNL was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. H. Y. K. acknowledges the financial support by the National Research Foundation of Korea (NRF) grant funded by the Korean government (Ministry of Science and ICT, MSIT) (2023R1A2C2008117), the Basic Science Research Program through the NRF funded by the Ministry of Education (2021R1A6A1A03043682). This research used resources of the Center for Functional Nanomaterials, which is a US DOE Office of Science Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used beamline 7-BM (QAS) of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract DESC0012704. Beamline operations were supported in part by the Synchrotron Catalysis Consortium (U.S. DOE, Office of Basic Energy Sciences, Grant DE-SC0012335). We thank S. Ehrlich, L. Ma and N. Marinkovic for help during synchrotron measurements at the QAS beamline.
| Funders | Funder number |
|---|---|
| National Research Foundation of Korea | |
| Synchrotron Catalysis Consortium | |
| Office of Science | |
| U.S. Department of Energy | DE-SC0012335 |
| U.S. Department of Energy | |
| Ministry of Science, ICT and Future Planning | 2023R1A2C2008117 |
| Ministry of Science, ICT and Future Planning | |
| Ministry of Education | 2021R1A6A1A03043682 |
| Ministry of Education | |
| Brookhaven National Laboratory | DE-SC0012704 |
| Brookhaven National Laboratory | |
| Basic Energy Sciences | DE-SC0022199 |
| Basic Energy Sciences |