Zhang Lina, Wan Shaolong, Du Congcong, Wan Qiang, Pham Hien, Zhao Jiafei, Ding Xingyu, Wei Diye, Zhao Wei, Li Jiwei, Zheng Yanping, Xie Hui, Zhang Hua, Chen Mingshu, Zhang Kelvin H L, Wang Shuai, Lin Jingdong, Huang Jianyu, Lin Sen, Wang Yong, Datye Abhaya K, Wang Ye, Xiong Haifeng
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry & Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China.
Nat Commun. 2024 Feb 9;15(1):1234. doi: 10.1038/s41467-024-45483-w.
Identification of active sites in catalytic materials is important and helps establish approaches to the precise design of catalysts for achieving high reactivity. Generally, active sites of conventional heterogeneous catalysts can be single atom, nanoparticle or a metal/oxide interface. Herein, we report that metal/oxide reverse interfaces can also be active sites which are created from the coordinated migration of metal and oxide atoms. As an example, a Pd/CeO single-atom catalyst prepared via atom trapping, which is otherwise inactive at 30 °C, is able to completely oxidize formaldehyde after steam treatment. The enhanced reactivity is due to the formation of a CeO-Pd nanoparticle domain interface, which is generated by the migration of both Ce and Pd atoms on the atom-trapped Pd/CeO catalyst during steam treatment. We show that the generation of metal oxide-metal interfaces can be achieved in other heterogeneous catalysts due to the coordinated mobility of metal and oxide atoms, demonstrating the formation of a new active interface when using metal single-atom material as catalyst precursor.
确定催化材料中的活性位点很重要，有助于建立精确设计催化剂以实现高反应活性的方法。通常，传统多相催化剂的活性位点可以是单原子、纳米颗粒或金属/氧化物界面。在此，我们报道金属/氧化物反向界面也可以是活性位点，它是由金属和氧化物原子的协同迁移产生的。例如，通过原子捕获制备的Pd/CeO单原子催化剂，在30°C时原本无活性，但经过蒸汽处理后能够完全氧化甲醛。反应活性增强是由于形成了CeO-Pd纳米颗粒域界面，这是在蒸汽处理过程中，Ce和Pd原子在原子捕获的Pd/CeO催化剂上迁移而产生的。我们表明，由于金属和氧化物原子的协同迁移，在其他多相催化剂中也可以实现金属氧化物-金属界面的生成，这证明了使用金属单原子材料作为催化剂前体时会形成新的活性界面。
