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

Journal of the American Chemical Society

4 years ago

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

Yu Wang, Wenxing Chen, Hailiang Zhu, Jun Li, Yuxi Liu, Dongsheng He, Lin Gu, Juncai Dong, Yadong Li, Quanchen Feng, Shu Zhao, Dingsheng Wang, Jun Yang, Zhi Li, Rong Yu, Yuanmin Zhu

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.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b01471

DOI: 10.1021/jacs.7b01471