催化作用
化学
纳米团簇
水煤气变换反应
离解(化学)
吸附
化学物理
电子转移
多相催化
结晶学
化学工程
物理化学
有机化学
工程类
作者
Jun Yu,Xuetao Qin,Yusen Yang,Mingxin Lv,Pan Yin,Lei Wang,Zhihao Ren,Boyu Song,Qiang Li,Lirong Zheng,Song Hong,Xianran Xing,Ding Ma,Min Wei,Xue Duan
摘要
Strong metal–support interaction (SMSI) has been extensively studied in heterogeneous catalysis because of its significance in stabilizing active metals and tuning catalytic performance, but the origin of SMSI is not fully revealed. Herein, by using Pt/CeO2 as a model catalyst, we report an embedding structure at the interface between Pt and (110) plane of CeO2, where Pt clusters (∼1.6 nm) are embedded into the lattice of ceria within 3–4 atomic layers. In contrast, this phenomenon is absent in the CeO2(100) support. This unique geometric structure, as an effective motivator, triggers more significant electron transfer from Pt clusters to CeO2(110) support accompanied by the formation of interfacial structure (Ptδ+–Ov–Ce3+), which plays a crucial role in stabilizing Pt nanoclusters. A comprehensive investigation based on experimental studies and theoretical calculations substantiates that the interfacial sites serve as the intrinsic active center toward water–gas shift reaction (WGSR), featuring a moderate strength CO activation adsorption and largely decreased energy barrier of H2O dissociation, accounting for the prominent catalytic activity of Pt/CeO2(110) (a reaction rate of 15.76 molCO gPt–1 h–1 and a turnover frequency value of 2.19 s–1 at 250 °C). In addition, the Pt/CeO2(110) catalyst shows a prominent durability within a 120 h time-on-stream test, far outperforming the Pt/CeO2(100) one, which demonstrates the advantages of this embedding structure for improving catalyst stability.
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