Embedding Reverse Electron Transfer Between Stably Bare Cu Nanoparticles and Cation‐Vacancy CuWO<sub>4</sub>
Cu nanoparticles (NPs) have attracted widespread attention in electronics, energy, and catalysis. However, conventionally synthesized Cu NPs face some challenges such as surface passivation and agglomeration in applications, which impairs their functionalities in the physicochemical properties. Here, the issues above by engineering an embedded interface of stably bare Cu NPs on the cation-vacancy CuWO<sub>4</sub> support is addressed, which induces the strong metal-support interactions and reverse electron transfer. Various atomic-scale analyses directly demonstrate the unique electronic structure of the embedded Cu NPs with negative charge and anion oxygen protective layer, which mitigates the typical degradation pathways such as oxidation in ambient air, high-temperature agglomeration, and CO poisoning adsorption. Kinetics and in situ spectroscopic studies unveil that the embedded electron-enriched Cu NPs follow the typical Eley-Rideal mechanism in CO oxidation, contrasting the Langmuir-Hinshelwood mechanism on the traditional Cu NPs. This mechanistic shift is driven by the Coulombic repulsion in anion oxygen layer, enabling its direct reaction with gaseous CO to form the easily desorbed monodentate carbonate.
Authors
- Yimin A. Wu (ORCID: https://orcid.org/0000-0002-3807-8431)
- Nannan Wang
- Hua Zhou (ORCID: https://orcid.org/0000-0001-9642-8674)
- Jingyu Qian (ORCID: https://orcid.org/0000-0002-3953-5382)
- Graham King (ORCID: https://orcid.org/0000-0003-1886-7254)
- Minli Zeng
- Tom Regier (ORCID: https://orcid.org/0000-0002-0022-3509)
- Chuan Gao (ORCID: https://orcid.org/0000-0002-1165-7185)
- Carl Redshaw (ORCID: https://orcid.org/0000-0002-2090-1688)
- Yue Peng (ORCID: https://orcid.org/0000-0001-5772-3443)
- Xuefeng Chu (ORCID: https://orcid.org/0000-0003-1472-8185)
- James J. Dynes (ORCID: https://orcid.org/0000-0002-5727-530X)
- Bingsen Zhang (ORCID: https://orcid.org/0000-0002-2607-2999)
- Xia Zhong (ORCID: https://orcid.org/0009-0008-9871-682X)
- Zhen Li (ORCID: https://orcid.org/0000-0001-7871-1193)
- Xinbo Li (ORCID: https://orcid.org/0000-0002-1628-1033)
- Yanqiu Zhu (ORCID: https://orcid.org/0000-0002-0866-8852)
- Cheng‐Jun Sun (ORCID: https://orcid.org/0000-0001-9158-8337)
- Zuolong Chen
- Yinghui Pu
- Guangshe Li (ORCID: https://orcid.org/0000-0001-8592-8729)
- Xiyang Wang (ORCID: https://orcid.org/0009-0003-5329-054X)
Institutions
- Argonne National Laboratory (US)
- Guangxi University (CN)
- University of Waterloo (CA)
- University of Hull (GB)
- Jilin University (CN)
- Chinese Academy of Sciences (CN)
- State Key Laboratory of Inorganic Synthesis and Preparative Chemistry
- Canadian Light Source (Canada) (CA)
- Tsinghua University (CN)
Publication Details
- Journal
- Advanced Materials
- Published
- 2024-10-14
- DOI
- https://doi.org/10.1002/adma.202412570
- Citations
- 22
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 2.58
Funders
- U.S. Department of Energy
- Canadian Light Source
- Natural Science Foundation of Guangxi Zhuang Autonomous Region
- National Natural Science Foundation of China
- National Synchrotron Radiation Laboratory
- Office of Science
- Natural Sciences and Engineering Research Council of Canada
- Engineering and Physical Sciences Research Council
- Hefei Science Center, Chinese Academy of Sciences
- Argonne National Laboratory