Wang Haodong, Choi Hyuk, Shimogawa Ryuichi, Li Yuanyuan, Zhang Lihua, Kim Hyun You, Frenkel Anatoly I
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794, USA.
Department of Materials Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea.
Nanoscale. 2024 Aug 13;16(31):14716-14721. doi: 10.1039/d4nr01396d.
Metal-support interaction plays a crucial role in governing the stability and activity of atomically dispersed platinum catalysts on ceria support. The migration and aggregation of platinum atoms during the catalytic reaction leads to the redistribution of active sites. In this study, by utilizing a multimodal characterization scheme, we observed the aggregation of platinum atoms at high temperatures under reverse water gas shift reaction conditions and the subsequent fragmentation of platinum clusters, forming "single atoms" upon cooling. Theoretical simulations of both effects uncovered the roles of carbon monoxide binding on perimeter Pt sites in the clusters and hydrogen coverage in the aggregation and fragmentation mechanisms. This study highlights the complex effects of adsorbate and supports interactions with metal sites in Pt/ceria catalysts that govern their structural transformations under conditions.
金属-载体相互作用在决定原子分散在二氧化铈载体上的铂催化剂的稳定性和活性方面起着关键作用。催化反应过程中铂原子的迁移和聚集导致活性位点的重新分布。在本研究中，通过采用多模态表征方案，我们观察到在逆水煤气变换反应条件下高温时铂原子的聚集以及随后铂簇的碎片化，冷却后形成“单原子”。对这两种效应的理论模拟揭示了一氧化碳在簇边缘铂位点上的吸附以及氢覆盖度在聚集和碎片化机制中的作用。这项研究突出了吸附质和载体与铂/二氧化铈催化剂中金属位点相互作用的复杂效应，这些效应决定了它们在特定条件下的结构转变。
