Revealing the structure-activity relationship of Pt1/CeO2 with 17O solid-state NMR spectroscopy and DFT calculations
Single-atom catalysts (SACs) have attracted significant interest due to their exceptional and tunable performance, enabled by diverse coordination environments achieved through innovative synthetic strategies. However, various local structures of active sites pose significant challenges for precise characterization, a prerequisite for developing structure-activity relationships. Here, we combine <sup>17</sup>O solid-state NMR spectroscopy and DFT calculations to elucidate the detailed structural information of Pt/CeO<sub>2</sub> SACs and their catalytic behaviors. The NMR data reveal that single Pt atoms, dispersed from clusters with water vapor, exhibit a square planar geometry embedded in CeO<sub>2</sub> (111) surface, distinct from the original clusters and other conventionally generated Pt single atoms. The square planar Pt/CeO<sub>2</sub> SAC demonstrates improved CO oxidation performance compared to Pt/CeO<sub>2</sub> SAC with octahedral coordination, due to moderately strong CO adsorption and low energy barriers. This approach can be extended to other oxide-supported SACs, enabling spatially resolved characterization and offering comprehensive insights into their structure-activity relationships.
Authors
- Weiping Ding (ORCID: https://orcid.org/0000-0002-8034-5740)
- Juan Wen (ORCID: https://orcid.org/0000-0003-0049-5333)
- Jia‐Huan Du (ORCID: https://orcid.org/0000-0003-2408-0060)
- Zhen Zhang (ORCID: https://orcid.org/0000-0003-2435-1916)
- Fang Wang (ORCID: https://orcid.org/0000-0003-0595-5095)
- Hanxi Guan (ORCID: https://orcid.org/0000-0003-4746-1907)
- Lei Nie (ORCID: https://orcid.org/0000-0003-4359-3451)
- Meng Wang (ORCID: https://orcid.org/0000-0002-3380-3534)
- Luming Peng (ORCID: https://orcid.org/0000-0003-1935-1620)
- Xiaoli Xia
- Yujie Wen (ORCID: https://orcid.org/0000-0002-7105-0465)
- Changshun Deng (ORCID: https://orcid.org/0000-0001-7250-9074)
- Weiping Tang (ORCID: https://orcid.org/0000-0002-0039-3196)
- Wei Li (ORCID: https://orcid.org/0000-0001-7801-3643)
- Jie Zhu (ORCID: https://orcid.org/0000-0003-2073-8021)
- Junchao Chen (ORCID: https://orcid.org/0000-0002-7601-5458)
- Wenhua Hou
- Xiaokang Ke
- Qian Wen
Institutions
- University of Science and Technology of China (CN)
- Nanjing University of Chinese Medicine (CN)
- Nanjing Tech University (CN)
- Shanghai Jiao Tong University (CN)
- Tiangong University (CN)
- Peking University (CN)
- Hefei National Center for Physical Sciences at Nanoscale (CN)
- Beijing National Laboratory for Molecular Sciences (CN)
- Quzhou University (CN)
- Ministry of Education and Child Care (CA)
- Zhejiang University (CN)
- Nanjing University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-04-14
- DOI
- https://doi.org/10.1038/s41467-025-58709-2
- Citations
- 11
- Primary Topic
- Advanced NMR Techniques and Applications
- Type
- article
- Field-Weighted Citation Impact
- 8.32
Funders
- Salt Science Research Foundation
- National Natural Science Foundation of China
- Radboud Universiteit
- Nanjing University
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Natural Science Foundation of Zhejiang Province