Department of Materials Science and Metallurgy, University of Cambridge, 27 Charles Babbage Road, Cambridge, CB3 0FS, UK.
Department of Earth Sciences, University of Cambridge, Downing Street, Cambridge, CB2 3EQ, UK.
Nanoscale. 2023 Apr 27;15(16):7420-7429. doi: 10.1039/d3nr00745f.
Bimetallic Pd-Mg nanoparticles were synthesized by partial galvanic replacement of plasmonic Mg nanoparticles, and their catalytic and photocatalytic properties in selective hydrogenation of acetylene have been investigated. Electron probe studies confirm that the Mg-Pd structures mainly consist of metallic Mg and sustain several localized plasmon resonances across a broad wavelength range. We demonstrate that, even without light excitation, the Pd-Mg nanostructures exhibit an excellent catalytic activity with selectivity to ethylene of 55% at 100% acetylene conversion achieved at 60 °C. With laser excitation at room temperature over a range of intensities and wavelengths, the initial reaction rate increased up to 40 times with respect to dark conditions and a 2-fold decrease of the apparent activation energy was observed. A significant wavelength-dependent change in hydrogenation kinetics strongly supports a catalytic behavior affected by plasmon excitation. This report of coupling between Mg's plasmonic and Pd's catalytic properties paves the way for sustainable catalytic structures for challenging, industrially relevant selective hydrogenation processes.
双金属 Pd-Mg 纳米颗粒通过等离子体 Mg 纳米颗粒的部分电置换合成，并研究了它们在乙炔选择性加氢中的催化和光催化性能。电子探针研究证实，Mg-Pd 结构主要由金属 Mg 组成，并在很宽的波长范围内维持几个局域等离子体共振。我们证明，即使没有光激发，Pd-Mg 纳米结构在 60°C 下达到 100%乙炔转化率时，表现出优异的催化活性，对乙烯的选择性达到 55%。在室温下，在一系列强度和波长的激光激发下，初始反应速率相对于暗条件增加了 40 倍，并且观察到表观活化能降低了 2 倍。加氢动力学的显著波长依赖性强烈支持受等离子体激发影响的催化行为。本报告中 Mg 的等离子体和 Pd 的催化性能的耦合为具有挑战性的、工业相关的选择性加氢过程的可持续催化结构铺平了道路。
