Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal–Support Interaction

Siwei Li(Peking University), Yao Xu(Peking University), Yifu Chen(Peking University), Weizhen Li(Peking University), Lili Lin(Peking University), Mengzhu Li(Peking University), Yuchen Deng(Peking University), Xiaoping Wang(Syngenta (China)), Binghui Ge(Chinese Academy of Sciences), Ce Yang(Peking University), Siyu Yao(Peking University), Jinglin Xie(Peking University), Yongwang Li(Syngenta (China)), Xi Liu(Syngenta (China)), Ding Ma(Peking University)
Angewandte Chemie International Edition
July 10, 2017
Cited by 513

Abstract

Abstract A one‐step ligand‐free method based on an adsorption–precipitation process was developed to fabricate iridium/cerium oxide (Ir/CeO 2 ) nanocatalysts. Ir species demonstrated a strong metal–support interaction (SMSI) with the CeO 2 substrate. The chemical state of Ir could be finely tuned by altering the loading of the metal. In the carbon dioxide (CO 2 ) hydrogenation reaction it was shown that the chemical state of Ir species—induced by a SMSI—has a major impact on the reaction selectivity. Direct evidence is provided indicating that a single‐site catalyst is not a prerequisite for inhibition of methanation and sole production of carbon monoxide (CO) in CO 2 hydrogenation. Instead, modulation of the chemical state of metal species by a strong metal–support interaction is more important for regulation of the observed selectivity (metallic Ir particles select for methane while partially oxidized Ir species select for CO production). The study provides insight into heterogeneous catalysts at nano, sub‐nano, and atomic scales.


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