Hou Zhiquan, Lu Yue, Liu Yuxi, Liu Ning, Hu Jingcong, Wei Lu, Li Zeya, Tian Xinrong, Gao Ruyi, Yu Xiaohui, Feng Yuan, Wu Linke, Deng Jiguang, Wang Dingsheng, Sui Manling, Dai Hongxing, Li Yadong
Key Laboratory of Beijing on Regional Air Pollution Control, Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Advanced Functional Materials, Education Ministry of China, Faculty of Environment and Life Science, Beijing University of Technology, Beijing 100124, China.
Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China.
J Am Chem Soc. 2023 Jul 26;145(29):15869-15878. doi: 10.1021/jacs.3c02909. Epub 2023 Jul 14.
Designing new synthesis routes to fabricate highly thermally durable precious metal single-atom catalysts (SACs) is challenging in industrial applications. Herein, a general strategy is presented that starts from dual-metal nanocrystals (NCs), using bimetallic NCs as a facilitator to spontaneously convert a series of noble metals to single atoms on aluminum oxide. The metal single atoms are captured by cation defects formed on the surface of the inverse spinel (ABO) structure, which process provides numerous anchoring sites, thus facilitating generation of the isolated metal atoms that contributes to the extraordinary thermodynamic stability. The Pd/AlCoO-AlO shows not only improved low-temperature activity but also unprecedented (hydro)thermal stability for CO and propane oxidation under harsh aging conditions. Furthermore, our strategy exhibits a small scaling-up effect by the simple physical mixing of commercial metal oxide aggregates with AlO. The good regeneration between oxidative and reductive atmospheres of these ionic palladium species makes this catalyst system of potential interest for emissions control.
设计新的合成路线以制备具有高耐热性的贵金属单原子催化剂(SACs)在工业应用中具有挑战性。在此,提出了一种通用策略,该策略从双金属纳米晶体(NCs)开始,使用双金属NCs作为促进剂,将一系列贵金属自发转化为氧化铝上的单原子。金属单原子被在反尖晶石(ABO)结构表面形成的阳离子缺陷捕获,该过程提供了大量的锚定位点,从而促进了孤立金属原子的生成,这有助于实现非凡的热力学稳定性。Pd/AlCoO-AlO不仅显示出改善的低温活性,而且在苛刻的老化条件下对CO和丙烷氧化表现出前所未有的(水)热稳定性。此外,我们的策略通过将商业金属氧化物聚集体与AlO简单物理混合表现出较小的放大效应。这些离子钯物种在氧化和还原气氛之间良好的再生性能使得该催化剂体系在排放控制方面具有潜在的应用价值。