Huang Weixin, Xu Hao, Deng Yang, Lin Shih-Wei, Pham Hien N, Zhang Rui, Jiang Dong, Zhang Zihao, DeLaRiva Andrew, Feng Shuxuan, Li Yixiao, Zhang Xinrui, Datye Abhaya K, Chen Chih-Jung, Wang Yong
The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, USA.
Department of Chemistry, University of North Dakota, Grand Forks, ND, USA.
Nat Commun. 2025 Aug 7;16(1):7274. doi: 10.1038/s41467-025-62447-w.
Activation of surface lattice oxygen and chemisorbed oxygen on catalyst surfaces constitutes a pivotal step in heterogeneous oxidative catalysis. Herein, we report a strategy for enhancing oxygen activation by rational design of catalysts with single-atom promoters. Single-site Zr species in CeO (Zr-CeO) are synthesized using the atom-trapping method. The Zr-CeO-supported Pt catalyst exhibits enhanced catalytic performance over the CeO-supported Pt catalyst in the oxidation of CO, CH, and CH, achieving significantly lower T values (temperature required to reach 50% conversion). This enhanced catalytic activity is attributed to the formation of an asymmetric Zr-O-Pt structure, which favors the activation of the adjacent surface lattice oxygen and chemisorbed molecular oxygen. This work exemplifies that incorporating single-site atoms into oxide support facilitates oxygen activation, providing new insights into the role of atomically dispersed promoters in heterogeneous catalysis.
催化剂表面晶格氧和化学吸附氧的活化是多相氧化催化中的关键步骤。在此，我们报告了一种通过合理设计具有单原子促进剂的催化剂来增强氧活化的策略。采用原子捕获法合成了CeO（Zr-CeO）中的单原子Zr物种。Zr-CeO负载的Pt催化剂在CO、CH和CH的氧化反应中表现出比CeO负载的Pt催化剂更高的催化性能，实现了显著更低的T值（达到50%转化率所需的温度）。这种增强的催化活性归因于形成了不对称的Zr-O-Pt结构，这有利于相邻表面晶格氧和化学吸附分子氧的活化。这项工作例证了将单原子掺入氧化物载体有助于氧活化，为原子分散促进剂在多相催化中的作用提供了新的见解。
