文献类型：期刊文献

英文题名：Exploring the Size Effect of Pt Nanoparticles on the Photocatalytic Nonoxidative Coupling of Methane

作者：Ma, Jiayu[1];Tan, Xianjun[2];Zhang, Qingqing[1];Wang, Yan[1];Zhang, Jinlong[1];Wang, Lingzhi[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalys, Sch Chem & Mol Engn, Key Lab Adv Mat & Inst Fine Chem, Shanghai 200237, Peoples R China;[2]Tsinghua Univ, Tsinghua Berkeley Shenzhen Inst, Shenzhen 518055, Peoples R China

年份：2021

卷号：11

期号：6

起止页码：3352

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20211410168269);WOS:【SCI-EXPANDED(收录号:WOS:000631434600016)】；

基金：This work was supported by the National Natural Science Foundation of China (21673073, 21972040,), the Science and Technology Commission of Shanghai Municipality (18520710200, 20DZ2250400), Shanghai Pujiang Program (18PJD012), Project supported by Shanghai Municipal S c i e n c e a n d T e c h n o l o g y M a j o r P r o j e c t (No.2018SHZDZX03), and the Program of Introducing Talents of Discipline to Universities (No. B20031, B16017).

语种：英文

外文关键词：photocatalysis; CH4 conversion; platinum nanoparticles; size effect; geometric active sites

摘要：The high inertness of the C-H bond makes the photocatalytic methane conversion a significant challenge. The platinum nanoparticle is a promising cocatalyst for CH4 activation, while the study of its structure characteristics and functionality sites remains in its infancy. Herein, the size effect of Pt( )on the photocatalytic nonoxidative methane conversion efficiency was systematically investigated over x-Pt/Ga2O3 with the particle size (x) ranging from 1.5 to 2.7 nm, where a volcano-shaped relation was observed. The smaller size is beneficial to the formation of species, which is mainly distributed on the terrace sites according to the DFT calculation. The corner Pt atom is the geometric active site for the CH4 polarization, and the terrace Pt delta+ helps promote C-H activation since the activity is decreased on reduced x-Pt/Ga2O3 with a lower Pt delta+ content. Meanwhile, Pt delta+ species favors the oxidation of adsorbed -CH3 group to center dot CH3. The volcano-shaped size effect on the NOCM activity was finally rationalized by the balance between C-H activation and C2H6 desorption from the corner sites on different sized Pt.