Graduate School of Engineering, Nagoya University, Nagoya, 464-8603, Japan.
Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Katsura, Kyoto, 615-8520, Japan.
Angew Chem Int Ed Engl. 2017 Dec 11;56(50):15993-15997. doi: 10.1002/anie.201709124. Epub 2017 Nov 15.
The particle size effect of Pd nanoparticles supported on alumina with various crystalline phases on methane combustion was investigated. Pd/θ, α-Al O with weak metal-support interaction showed a volcano-shaped dependence of the catalytic activity on the size of Pd particles, and the catalytic activity of the strongly interacted Pd/γ-Al O increased with the particle size. Based on a structural analysis of Pd nanoparticles using CO adsorption IR spectroscopy and spherical aberration-corrected scanning/transmission electron microscopy, the dependence of catalytic activity on Pd particle size and the alumina crystalline phase was due to the fraction of step sites on Pd particle surface. The difference in fraction of the step site is derived from the particle shape, which varies not only with Pd particle size but also with the strength of metal-support interaction. Therefore, this interaction perturbs the particle size effect of Pd/Al O for methane combustion.
研究了不同晶相氧化铝负载钯纳米粒子的粒径效应对甲烷燃烧的影响。具有较弱金属-载体相互作用的 Pd/θ、α-Al2O3 表现出 Pd 粒子尺寸对催化活性的火山形依赖性,而强相互作用的 Pd/γ-Al2O3 的催化活性随粒子尺寸的增加而增加。基于 CO 吸附红外光谱和球差校正扫描/透射电子显微镜对 Pd 纳米粒子的结构分析,催化活性对 Pd 粒子尺寸和氧化铝晶相的依赖性归因于 Pd 粒子表面台阶位的分数。台阶位分数的差异源于颗粒形状,它不仅随 Pd 粒子尺寸而变化,而且随金属-载体相互作用的强度而变化。因此,这种相互作用干扰了 Pd/Al2O3 对甲烷燃烧的粒径效应。