文献类型：期刊文献

英文题名：Design of frustrated Lewis pair in defective TiO2 for photocatalytic non-oxidative methane coupling

作者：Ma, Jiayu[1,2];Zhang, Qingqing[1,2];Chen, Ziyu[1,2];Kang, Kai[1,2];Pan, Lihan[1,2];Wu, Shiqun[1,2];Chen, Chen[1,2];Wu, Zhiqin[1,2];Zhang, Jinlong[1,2];Wang, Lingzhi[1,2]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalys, Key Lab Adv Mat, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Joint Int Res Lab Precis Chem & Mol Engn,Inst Fin, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2022

卷号：2

期号：7

起止页码：1775

外文期刊名：CHEM CATALYSIS

收录：WOS:【ESCI(收录号:WOS:000901435700008)】；

基金：This study was supported by the National Key R&D Program of China (2021YFC2103500 and SQ2019YFE011329), the National Natural Science Foundation of China (22006038 and 21972040), Shanghai Municipal Science and Technology (nos. 21ZR1417900, 2018SHZDZX03, 17520711500, and 20DZ22 50400), the Program of Introducing Talents of Discipline to Universities (nos. B16017 and B20031), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), and the Fundamental Research Funds for the Central Universities.

语种：英文

摘要：The efficient C- H polarization is the prerequisite for the low-temperature photocatalytic CH4 conversion, which is restricted by the poor C-H stretching ability of short-distance adjacent lattice atoms. Here, a frustrated Lewis pair (FLP) composed of dopedmetal in TiO2 as Lewis acid (LA) and neighboring Ti-OH as Lewis base (LB) with a long distance (0.31-0.37 nm) was designed through DFT calculation and fabricated by hydrogenation treatment of metal-doped TiO2-SiO2 with macroporous-mesoporous structure. Benefitting from the long LA-LB distance and matched acid-base intensity, hydrogenated Ga-doped composite achieves superior C-H stretching with a high photocatalytic CH4 conversion rate (139 mu mol g(-1) h(-1)). The photo-irradiation causes electron excitation from Ga to Ti-OH according to the time-dependent DFT calculation and in situ EPR analysis, which promotes the formation and coupling of .CH3. This work provides a key underpinning for regulating the characteristics of FLP for C- H activation and C-C coupling via light irradiation.