Li, Yurou; Cao, Yueqiang; Ge, Xiaohu; Zhang, Hao; Yan, Kelin; Zhang, Jing; Qian, Gang; Jiang, Zheng; Gong, Xueqing; Li, Aoming; Zhou, Xinggui; Yuan, Weikang; Duan, Xuezhi

JOURNAL OF CATALYSIS

2022, 407, 0021-9517

Li, Yurou; Cao, Yueqiang; Ge, Xiaohu; Zhang, Hao; Yan, Kelin; Zhang, Jing; Qian, Gang; Jiang, Zheng; Gong, Xueqing; Li, Aoming; Zhou, Xinggui; Yuan, Weikang; Duan, Xuezhi

Transition metal oxides are emerging as promising catalysts for selective hydrogenations, but elaborating oxides catalysts with excellent hydrogenation activity remains challenging, especially at atomic level. Here, we report a theoretical-guided atomic design strategy with experimental verification to fabricate an excellent In2O3-based catalyst with an Pt-O-4-In2O ensemble site for acetylene semi-hydrogenation. Theoretical calculations reveal that the presence of Pt-O-4 moiety in the ensemble site increases the electron localization surrounding with the moiety and thus strengthens the frustrated Lewis pair of In-O within the In2O site adjacent to the moiety. These structure features contribute to a promoted activation of hydrogen on the ensemble site via heterolytic dissociation and enhanced acetylene semi hydrogenation on the oxygen vacancy adjacent to the Pt-O-4 moiety. The Pt-1-In2O3 catalyst featured with the ensemble site was synthesized by atomic layer deposition technology and characterized by multiple technologies, including atomic-resolution electron microscopy, X-ray absorption spectroscopy, and H-2-D-2 exchange experiments, to validate the theoretical predictions. As expected, the experimental results elucidate an enhanced activation of hydrogen, and a full conversion of acetylene with 91% of ethylene selectivity on the Pt-1-In2O3 catalyst, which is remarkably higher than those of the pristine In2O3 catalyst. (C) 2022 Elsevier Inc. All rights reserved.