Fu Xin-Pu, Wu Cui-Ping, Wang Wei-Wei, Jin Zhao, Liu Jin-Cheng, Ma Chao, Jia Chun-Jiang
Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, 250100, Jinan, China.
Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering & National Institute for Advanced Materials, Nankai University, 300350, Tianjin, China.
Nat Commun. 2023 Oct 27;14(1):6851. doi: 10.1038/s41467-023-42577-9.
Dual-interfacial structure within catalysts is capable of mitigating the detrimentally completive adsorption during the catalysis process, but its construction strategy and mechanism understanding remain vastly lacking. Here, a highly active dual-interfaces of CeO/CoO/Co is constructed using the pronounced interfacial interaction from surrounding small CeO islets, which shows high activity in catalyzing the water-gas shift reaction. Kinetic evidence and in-situ characterization results revealed that CeO modulates the oxidized state of Co species and consequently generates the dual active CeO/CoO/Co interface during the WGS reaction. A synergistic redox mechanism comprised of independent contribution from dual functional interfaces, including CeO/CoO and CoO/Co, is authenticated by experimental and theoretical results, where the CeO/CoO interface alleviates the CO poison effect, and the CoO/Co interface promotes the H formation. The results may provide guidance for fabricating dual-interfacial structures within catalysts and shed light on the mechanism over multi-component catalyst systems.
催化剂内部的双界面结构能够减轻催化过程中有害的竞争性吸附，但其构建策略和机理认识仍极为匮乏。在此，利用周围小氧化铈小岛显著的界面相互作用构建了具有高活性的CeO/CoO/Co双界面，其在催化水煤气变换反应中表现出高活性。动力学证据和原位表征结果表明，氧化铈调节了钴物种的氧化态，从而在水煤气变换反应过程中产生了双活性CeO/CoO/Co界面。实验和理论结果证实了由CeO/CoO和CoO/Co双功能界面独立贡献组成的协同氧化还原机理，其中CeO/CoO界面减轻了一氧化碳中毒效应，CoO/Co界面促进了氢的形成。这些结果可为催化剂内部双界面结构的构建提供指导，并为多组分催化剂体系的机理研究提供启示。
