文献类型：期刊文献

英文题名：Uniphase ruthenium-iridium alloy-based electronic regulation for electronic structure-function study in methane oxidation to methanol

作者：Yang, Le[1];Huang, Jinxu[1];Dai, Sheng[2,3];Tang, Xuan[2,3];Hu, Zhe[1];Li, Ming[4];Zeng, Hui[1];Luque, Rafael[5,6];Duan, Peigao[7];Rui, Zebao[1]

机构：[1]Sun Yat Sen Univ, Guangdong Engn Technol Res Ctr Platform Chem Mari, Sch Chem Engn & Technol, Zhuhai 519082, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Shanghai 200237, Peoples R China;[4]Univ Connecticut, Inst Mat Sci, Polymer Program, Storrs, CT 06269 USA;[5]Univ Cordoba, Dept Quim Organ, Campus Rabanales,Edificio Marie Curie C-3, E-14014 Cordoba, Spain;[6]Peoples Friendship Univ Russia RUDN Univ, 6 Miklukho Maklaya Str, Moscow 117198, Russia;[7]Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Shaanxi Key Lab Energy Chem Proc Intensificat, 28 West Xianning Rd, Xian 710049, Shaanxi, Peoples R China

年份：2020

卷号：8

期号：45

起止页码：24024

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20204909570468);WOS:【SCI-EXPANDED(收录号:WOS:000593047100029)】；

基金：The publication has been prepared with support from RUDN University, Program 5-100. This research was supported by the Fundamental Research Funds for the Central Universities (No. 20187611031610004), Guangdong Basic and Applied Basic Research Foundation (No. 2019A1515110767), National Natural Science Foundation of China (No. 22008266, 21776322, and 21576298), and Foshan Nanhai Economic and Technological Promotion Bureau Project (No. 20177611071010007 and No. 20177611071010008). Sheng Dai acknowledges the support from the Shanghai Rising-star Program (20QA1402400). Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

外文关键词：Synthesis (chemical) - Binary alloys - Chlorine compounds - Ruthenium alloys - Methane - Methanol - Iridium alloys

摘要：For the first time, we synthesize uniphase face-centered-cubic (fcc) structured Ru-Ir alloy nanoparticles (NPs) with a uniform size of similar to 2 nm over the whole composition range, using RuCl3 and IrCl4 as precursors. The electronic structure of Ir is gradually tuned by varying the composition. The consistency of the fcc structure of Ru and Ir within the RuxIr1-x alloys allows better study of the electronic structure-activity relationship without introducing unnecessary factors such as the lattice/phase effect in the case of the RuIr alloy composed of different structures of hcp-Ru and fcc-Ir. The obtained RuxIr1-x alloys were further employed as precursors for the synthesis of their corresponding oxides, RuxIr1-xO2/CuO, to probe the electronic structure-activity relationship in the methane oxidation to methanol reaction. The electronic structure of Ir4+ was able to be regulated by tuning the composition of the RuxIr1-x NP precursors. The optimum catalytic behavior was achieved over Ru0.5Ir0.5O2/CuO, where both Ru and Ir reached the highest electrophilic state, at which point the C-H cleavage capacity also reached the maximum as observed by CH4-TPR.