文献类型：期刊文献

英文题名：Atomic Insights into the Cu Species Supported on Zeolite for Direct Oxidation of Methane to Methanol via Low-Damage HAADF-STEM

作者：Tang, Xuan[1,2];Ye, Jiajie[2];Guo, Lisheng[1];Pu, Tiancheng[3];Cheng, Lu[2];Cao, Xiao-Ming[2];Guo, Yanglong[2];Wang, Li[2];Guo, Yun[2];Zhan, Wangcheng[2];Dai, Sheng[1,2]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Lehigh Univ, Dept Chem & Biomol Engn, Bethlehem, PA 18015 USA

年份：2023

卷号：35

期号：25

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20231914061231);WOS:【SCI-EXPANDED(收录号:WOS:000978567800001)】；

基金：X.T. and J.Y. contributed equally to this work. This work was supported by the National Key Research and Development Program of China (2016YFC0204300), the National Natural Science Foundation of China (U21A20326 and 21976057), the Fundamental Research Funds for the Central Universities, China Postdoctoral Science Foundation (2022M721144), Shanghai Municipal Science and Technology Major Project (grant 2018SHZDZX03), Shanghai Rising-star Program (20QA1402400), the Science and Technology Commission of Shanghai Municipality (22ZR1415700), and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center. The authors thank Dr. Yafeng Cai for the fruitful discussion. The authors also thank the Research Center of Analysis and Test at ECUST for technique support.

语种：英文

外文关键词：beam sensitive; copper; direct oxidation of methane; transmission electron microscopy; zeolites

摘要：Precise determination of the structure-property relationship of zeolite-based metal catalysts is critical for the development toward practical applications. However, the scarcity of real-space imaging of zeolite-based low-atomic-number (LAN) metal materials due to the electron-beam sensitivity of zeolites has led to continuous debates regarding the exact LAN metal configurations. Here, a low-damage high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) imaging technique is employed for direct visualization and determination of LAN metal (Cu) species in ZSM-5 zeolite frameworks. The structures of the Cu species are revealed based on the microscopy evidence and also proved by the complementary spectroscopy results. The correlation between the characteristic Cu size in Cu/ZSM-5 catalysts and their direct oxidation of methane to methanol reaction properties is unveiled. As a result, the mono-Cu species stably anchored by Al pairs inside the zeolite channels are identified as the key structure for higher C1 oxygenates yield and methanol selectivity for direct oxidation of methane. Meanwhile, the local topological flexibility of the rigid zeolite frameworks induced by the Cu agglomeration in the channels is also revealed. This work exemplifies the combination of microscopy imaging and spectroscopy characterization serves as a complete arsenal for revealing structure-property relationships of the supported metal-zeolite catalysts.