Abstract
Due to tunable redox properties and cost-effectiveness, copper-ceria (Cu-CeO2) materials have been investigated for a wide scope of catalytic reactions. However, accurately identifying and rationally tuning the local structures in Cu-CeO2 have remained challenging, especially for nanomaterials with inherent structural complexities involving surfaces, interfaces, and defects. Here, a nanocrystal-based atom-trapping strategy to access atomically precise Cu-CeO2 nanostructures for enhanced catalysis is reported. Driven by the interfacial interactions between the presynthesized Cu and CeO2 nanocrystals, Cu atoms migrate and redisperse onto the CeO2 surface via a solid–solid route. This interfacial restructuring behavior facilitates tuning of the copper dispersion and the associated creation of surface oxygen defects on CeO2, which gives rise to enhanced activities and stabilities catalyzing water–gas shift reaction. Combining soft and solid-state chemistry of colloidal nanocrystals provide a well-defined platform to understand, elucidate, and harness metal–support interactions. The dynamic behavior of the supported metal species can be further exploited to realize exquisite control and rational design of multicomponent nanocatalysts.
| Original language | English |
|---|---|
| Article number | 2104749 |
| Journal | Advanced Science |
| Volume | 9 |
| Issue number | 8 |
| DOIs | |
| State | Published - Mar 15 2022 |
Funding
This work 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. Use of the Advanced Photon Source was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE‐AC02‐06CH11357. Neutron total scattering measurements were conducted at the NOMAD beamline at the Spallation Neutron Source, Oak Ridge National Laboratory, which was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, U. S. Department of Energy. Electron microscopy was performed at the Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, which is a U. S. Department of Energy Office of Science User Facility. The authors thank Yujia Bian for the assistance during XAS experiments at the 10‐BM beamline at the Advanced Photon Source at Argonne National Laboratory. They also thank Minghui Zhu and Israel E. Wachs at Lehigh University for providing the CuCrFeO sample. x This work 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. Use of the Advanced Photon Source was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Neutron total scattering measurements were conducted at the NOMAD beamline at the Spallation Neutron Source, Oak Ridge National Laboratory, which was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, U. S. Department of Energy. Electron microscopy was performed at the Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, which is a U. S. Department of Energy Office of Science User Facility. The authors thank Yujia Bian for the assistance during XAS experiments at the 10-BM beamline at the Advanced Photon Source at Argonne National Laboratory. They also thank Minghui Zhu and Israel E. Wachs at Lehigh University for providing the CuCrFeOx sample.
| Funders | Funder number |
|---|---|
| U. S. Department of Energy Office of Science | |
| U.S. Department of Energy | |
| Office of Science | |
| Basic Energy Sciences | DE‐AC02‐06CH11357 |
| Argonne National Laboratory | |
| Oak Ridge National Laboratory |
Keywords
- atom-trapping
- colloidal nanocrystal
- copper-ceria
- water–gas shift reaction