Wang Tairan, Hu Jianyu, Ouyang Runhai, Wang Yutao, Huang Yi, Hu Sulei, Li Wei-Xue
Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, iChEM, University of Science and Technology of China, Hefei, China.
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, China.
Science. 2024 Nov 22;386(6724):915-920. doi: 10.1126/science.adp6034. Epub 2024 Nov 21.
The metal-support interaction is one of the most important pillars in heterogeneous catalysis, but developing a fundamental theory has been challenging because of the intricate interfaces. Based on experimental data, interpretable machine learning, theoretical derivation, and first-principles simulations, we established a general theory of metal-oxide interactions grounded in metal-metal and metal-oxygen interactions. The theory applies to metal nanoparticles and atoms on oxide supports and oxide films on metal supports. We found that for late-transition metal catalysts, metal-metal interactions dominated the oxide support effects and suboxide encapsulation over metal nanoparticles. A principle of strong metal-metal interactions for encapsulation occurrence is formulated and substantiated by extensive experiments including 10 metals and 16 oxides. The valuable insights revealed on (strong) metal-support interaction advance the interfacial design of supported metal catalysts.
金属与载体的相互作用是多相催化中最重要的支柱之一，但由于界面复杂，建立一个基础理论一直具有挑战性。基于实验数据、可解释的机器学习、理论推导和第一性原理模拟，我们建立了一个基于金属-金属和金属-氧相互作用的金属-氧化物相互作用的通用理论。该理论适用于氧化物载体上的金属纳米颗粒和原子以及金属载体上的氧化膜。我们发现，对于晚期过渡金属催化剂，金属-金属相互作用主导了氧化物载体效应以及金属纳米颗粒上的低价氧化物包覆。通过包括10种金属和16种氧化物在内的大量实验，提出并证实了发生包覆的强金属-金属相互作用原理。关于（强）金属-载体相互作用所揭示的宝贵见解推动了负载型金属催化剂的界面设计。
