Peng Dang, Dandan Ren, Zhengxing Lv, Qingqing Gu, Jiaxin Lin, Ruiying Li, Wentao Zheng, Zhe Gao, Lixia Ling, Weixin Huang, Xiaodong Wen, Zhenhua Zhang
Strong metal–support interaction (SMSI) is not only a fundamental concept in heterogeneous catalysis but also emerging as an effective strategy for designing advanced catalysts. Here, we present a facile approach to construct an SMSI over Ru/CeO 2 catalysts by simply altering the precursor types of supported Ru species. Under the same preparation conditions, when using Ru(NO)(NO 3 ) 3 as the precursor (Ru(N)/CeO 2 ), the residual N species located at the Ru–N–Ce interfaces weaken the Ce–O bonds in ceria, promoting the surface migration of CeO 2– x species to generate SMSI together with increasing surface oxygen vacancy concentrations, whereas this process does not occur when RuCl 3 is employed (Ru(Cl)/CeO 2 ). Catalytic performance of the Ru/CeO 2 catalysts in CO 2 hydrogenation sensitively depends on the structures of the supported Ru species. The Ru(Cl)/CeO 2 catalyst with exposed Ru atoms exhibits better H 2 activation and H-spillover capacities, efficiently driving CO 2 hydrogenation to CH 4 via combined Mars–van Krevelen (MvK) and H 2 -assisted associated mechanisms. However, the hydrogenation process is seriously impeded over the Ru(N)/CeO 2 catalyst with encapsulated Ru structures, resulting in the CO production through an MvK mechanism. This finding offers an innovative approach for tailoring catalyst structures for targeted CO 2 conversion via the SMSI effect.