文献类型：期刊文献

英文题名：High-density frustrated Lewis pairs based on Lamellar Nb2O5 for photocatalytic non-oxidative methane coupling

作者：Chen, Ziyu[1];Ye, Yutao[1];Feng, Xiaoyi[1];Wang, Yan[1];Han, Xiaowei[1];Zhu, Yu[1];Wu, Shiqun[1];Wang, Senyao[1];Yang, Wenda[1];Wang, Lingzhi[1];Zhang, Jinlong[1]

机构：[1]East China Univ Sci & Technol, Inst Fine Chem, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Feringa Nobel Prize Scientist Joint Res Ctr,Sch Ch, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2023

卷号：14

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000967732600014)】；

基金：This work was supported by the National Key R&D Program of China (2022YFE0107900, 2022YFB3803600, 2021YFC2103501), National Natural Science Foundation of China (22006038, 21972040), Shanghai Municipal Science and Technology Major Project (2018SHZDZX03), the Program of Introducing Talents of Discipline to Universities (B20031, B16017), Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (21ZR1417900, 20DZ2250400, 22230780200), Shanghai Sailing Program (22YF1410200) and Fundamental Research Funds for the Central Universities (222201717003).

语种：英文

摘要：To achieve efficient photocatalytic non-oxidative methane coupling, a strong polarization environment with abundant activation sites for C-H scissoring is needed. This can be created through the fabrication of high-density frustrated Lewis pairs on lamellar Nb2O5 using a thermal-reduction promoted phase-transition process. Photocatalytic methane conversion requires a strong polarization environment composed of abundant activation sites with the robust stretching ability for C-H scissoring. High-density frustrated Lewis pairs consisting of low-valence Lewis acid Nb and Lewis base Nb-OH are fabricated on lamellar Nb2O5 through a thermal-reduction promoted phase-transition process. Benefitting from the planar atomic arrangement of lamellar Nb2O5, the frustrated Lewis pairs sites are highly exposed and accessible to reactants, which results in a superior methane conversion rate of 1456 mu mol g(-1) h(-1) for photocatalytic non-oxidative methane coupling without the assistance of noble metals. The time-dependent DFT calculation demonstrates the photo-induced electron transfer from LA to LB sites enhances their intensities in a concerted way, promoting the C-H cleavage through the coupling of LA and LB. This work provides in-depth insight into designing and constructing a polarization micro-environment for photocatalytic C-H activation of methane without the assistance of noble metals.