Zeolite-Encaged Isolated Platinum Ions Enable Heterolytic Dihydrogen Activation and Selective Hydrogenations

作者：Xin Deng, Bin Qin, Runze Liu, Xuetao Qin, Weili Dai, Guangjun Wu, Naijia Guan, Ding Ma, Landong Li · 发表于：Journal of the American Chemical Society · 年份：2021 · DOI：10.1021/jacs.1c09535 · 被引用次数：196 · 研究领域：Asymmetric Hydrogenation and Catalysis、Nanomaterials for catalytic reactions、Catalysis and Hydrodesulfurization Studies

Understanding the unique behaviors of atomically dispersed catalysts and the origin thereof is a challenging topic. Herein, we demonstrate a facile strategy to encapsulate Pt δ+ species within Y zeolite and reveal the nature of selective hydrogenation over a Pt@Y model catalyst. The unique configuration of Pt@Y, namely atomically dispersed Pt δ+ stabilized by the surrounding oxygen atoms of six-membered rings shared by sodalite cages and supercages, enables the exclusive heterolytic activation of dihydrogen over Pt δ+ ···O 2– units, resembling the well-known classical Lewis pairs. The charged hydrogen species, i.e., H + and H δ−, are active reagents for selective hydrogenations, and therefore, the Pt@Y catalyst exhibits remarkable performance in the selective hydrogenation of α,β-unsaturated aldehydes to unsaturated alcohols and of nitroarenes to arylamines.