Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, Sichuan 610054, China.
Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208, United States.
Nano Lett. 2021 Jul 14;21(13):5620-5626. doi: 10.1021/acs.nanolett.1c01124. Epub 2021 Jun 25.
The development of highly selective and active catalysts to catalyze an industrially important semihydrogenation reaction remains an open challenge. Here, we report the design of a bimetallic Pd/Cu(111) catalyst with Pd rafts confined in a Cu nanosheet, which exhibits desirable catalytic performance for acetylene semihydrogenation to ethylene with the selectivity of >90%. Theory calculations show that Pd atoms replacing neighboring Cu atoms in Cu(111) can improve the catalytic activity by reducing the energy barrier of the semihydrogenation reaction, as compared to unsubstituted Cu(111), and can improve the selectivity by weakening the adsorption of CH, as compared to a Pd(111) surface. The presence of Pd rafts confined in Cu nanosheets effectively turns on Cu nanosheets for semihydrogenation of acetylene with high activity and selectivity under mild reaction conditions. This work offers a well-defined nanostructured Pd/Cu(111) model catalyst that bridges the pressure and materials' gap between surface-science catalysis and practical catalysis.
开发高选择性和高活性的催化剂以催化工业上重要的半氢化反应仍然是一个开放的挑战。在这里，我们报告了一种双金属 Pd/Cu(111)催化剂的设计，其中 Pd 筏限制在 Cu 纳米片中，该催化剂在乙炔半氢化生成乙烯的反应中表现出理想的催化性能，选择性>90%。理论计算表明，与未取代的 Cu(111)相比，Pd 原子取代 Cu(111)中的相邻 Cu 原子可以降低半氢化反应的能垒，从而提高催化活性，与 Pd(111)表面相比，它可以通过削弱 CH 的吸附来提高选择性。限制在 Cu 纳米片中的 Pd 筏的存在可以在温和的反应条件下有效地开启 Cu 纳米片用于乙炔的半氢化反应，从而具有高活性和选择性。这项工作提供了一种明确定义的纳米结构 Pd/Cu(111)模型催化剂，它在表面科学催化和实际催化之间的压力和材料差距之间架起了桥梁。
