Wen Yujie, Wang Fang, Zhu Jie, Wen Qian, Xia Xiaoli, Wen Juan, Deng Changshun, Du Jia-Huan, Ke Xiaokang, Zhang Zhen, Guan Hanxi, Nie Lei, Wang Meng, Hou Wenhua, Li Wei, Tang Weiping, Ding Weiping, Chen Junchao, Peng Luming
Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China.
Department of Chemistry, Zhejiang University, Hangzhou, China.
Nat Commun. 2025 Apr 14;16(1):3537. doi: 10.1038/s41467-025-58709-2.
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 O solid-state NMR spectroscopy and DFT calculations to elucidate the detailed structural information of Pt/CeO 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 (111) surface, distinct from the original clusters and other conventionally generated Pt single atoms. The square planar Pt/CeO SAC demonstrates improved CO oxidation performance compared to Pt/CeO 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.
单原子催化剂（SACs）因其卓越且可调节的性能而备受关注，这种性能得益于通过创新合成策略实现的多样配位环境。然而，活性位点的各种局部结构给精确表征带来了重大挑战，而精确表征是建立结构-活性关系的先决条件。在此，我们结合固态核磁共振光谱和密度泛函理论计算，以阐明Pt/CeO单原子催化剂的详细结构信息及其催化行为。核磁共振数据表明，从含有水蒸气的团簇中分散出来的单个Pt原子呈现出嵌入CeO（111）表面的平面正方形几何结构，这与原始团簇和其他传统生成的Pt单原子不同。与具有八面体配位的Pt/CeO单原子催化剂相比，平面正方形Pt/CeO单原子催化剂表现出更好的CO氧化性能，这归因于适度较强的CO吸附和较低的能垒。这种方法可扩展到其他氧化物负载的单原子催化剂，实现空间分辨表征，并为其结构-活性关系提供全面的见解。
