Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes

Journal of the American Chemical Society
Quanchen FengYadong Li

Abstract

Improving the catalytic selectivity of Pd catalysts is of key importance for various industrial processes and remains a challenge so far. Given the unique properties of single-atom catalysts, isolating contiguous Pd atoms into a single-Pd site with another metal to form intermetallic structures is an effective way to endow Pd with high catalytic selectivity and to stabilize the single site with the intermetallic structures. Based on density functional theory modeling, we demonstrate that the (110) surface of Pm3̅m PdIn with single-atom Pd sites shows high selectivity for semihydrogenation of acetylene, whereas the (111) surface of P4/mmm Pd3In with Pd trimer sites shows low selectivity. This idea has been further validated by experimental results that intermetallic PdIn nanocrystals mainly exposing the (110) surface exhibit much higher selectivity for acetylene hydrogenation than Pd3In nanocrystals mainly exposing the (111) surface (92% vs 21% ethylene selectivity at 90 °C). This work provides insight for rational design of bimetallic metal catalysts with specific catalytic properties.

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Citations

Mar 21, 2018·Chemical Communications : Chem Comm·Yu XiongYadong Li
Jul 28, 2018·Advanced Materials·Max J HülseyNing Yan
Nov 30, 2018·Chemistry : a European Journal·Jingjie GeYadong Li
Jun 20, 2020·Chemical Communications : Chem Comm·Chenliang YeYadong Li
Sep 2, 2020·Chemical Society Reviews·Lulu LiJinlong Gong
Oct 10, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Yuan TaoFeng Luo
Jul 10, 2019·Advanced Materials·Xuning LiBin Liu
Sep 25, 2020·Nanoscale·Benjamin P WilliamsChia-Kuang Tsung
Nov 25, 2020·Nature Nanotechnology·Sharon MitchellJavier Pérez-Ramírez
Feb 23, 2021·Chemical Communications : Chem Comm·Fengjuan Qin, Wenxing Chen
Feb 26, 2021·Science and Technology of Advanced Materials·Marc Armbrüster
Mar 17, 2021·Journal of the American Chemical Society·Kunlong LiuNanfeng Zheng

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