中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
High population and dispersion of pentacoordinated Al-V species on the surface of flame-made amorphous silica-alumina

文献类型:期刊论文

作者Wang, Zichun1,2,3; Jiang, Yijiao1; Yi, Xianfeng4; Zhou, Cuifeng2,3; Rawal, Aditya5; Hook, James5; Liu, Zongwen2,3; Deng, Feng4; Zheng, Anmin4; Hunger, Michael6
刊名SCIENCE BULLETIN
出版日期2019-04-30
卷号64期号:8页码:516-523
关键词Amorphous silica-alumina Pentacoordinated Al-V species Al-27 multiple quantum magic-angle-spinning NMR H/D exchange
ISSN号2095-9273
DOI10.1016/j.scib.2019.04.002
英文摘要Pentacoordinated Al (Al-V) species in silica-alumina are promising to promote the formation of acid sites or act as surface defects for tailoring single-atom catalysts. However, pentahedral coordination (Al-V) is rarely observed in conventionally prepared silica-alumina. Here, we show that high population and dispersion of Al-V species on the surface of amorphous silica-alumina (ASA) can be achieved by means of flame spray pyrolysis. High resolution TEM/EDX, high magnetic-field NMR and DFT calculations are employed to characterize the structure of as-prepared ASAs. Solid-state Al-27 multi-quantum MAS NMR experiments show that most of the Al-V species are formed independently from the alumina phase and are accessible for guest molecules on the surface. Upon water adsorption, these Al-V species are transformed to Al-VI species, structurally similar to surface Al-IV species, as confirmed by DFT calculations. The outstanding catalytic activity of as-synthesized ASA is demonstrated using the in situ H/D exchange reaction with deuterated benzene as an example. The Al-V-rich ASA provides a much lower activation energy (similar to 30 kJ/mol) than that reported for zeolite H-ZSM-5 (similar to 60 kJ/mol). The superior catalytic performance is attributed to the high Al-V content promoting the surface active sites in ASA. The knowledge gained on the synthesis of Al-V-rich ASAs and the nature of aluminum coordination in these materials could pave the way to more efficient silica-alumina based catalysts. (C) 2019 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
WOS关键词BRONSTED ACID SITES ; FRAMEWORK ALUMINUM ; NMR-SPECTROSCOPY ; H/D EXCHANGE ; AL-27 NMR ; ZEOLITES ; STATE ; MAS ; IONS ; TRANSFORMATION
资助项目Australian Research Council[DP150103842] ; Australian Research Council[DE190101618] ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; National Natural Science Foundation of China[21522310] ; National Natural Science Foundation of China[21473244] ; National Natural Science Foundation of China[21210005] ; ARC LIEF[LE0989541]
WOS研究方向Science & Technology - Other Topics
语种英语
WOS记录号WOS:000472942700009
出版者ELSEVIER SCIENCE BV
资助机构Australian Research Council ; Australian Research Council ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; ARC LIEF ; ARC LIEF ; Australian Research Council ; Australian Research Council ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; ARC LIEF ; ARC LIEF ; Australian Research Council ; Australian Research Council ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; ARC LIEF ; ARC LIEF ; Australian Research Council ; Australian Research Council ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydney ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; ARC LIEF ; ARC LIEF
源URL[http://ir.wipm.ac.cn/handle/112942/14511]  
专题中国科学院武汉物理与数学研究所
通讯作者Zheng, Anmin; Huang, Jun
作者单位1.Macquarie Univ, Dept Engn, Sydney, NSW 2109, Australia
2.Univ Sydney, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia
3.Univ Sydney, Sydney Nano Inst, Sydney, NSW 2006, Australia
4.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom Mol Phys, Wuhan 430071, Hubei, Peoples R China
5.Univ New South Wales, Mark Wainwright Analyt Ctr, Sydney, NSW 2052, Australia
6.Univ Stuttgart, Inst Chem Technol, D-70550 Stuttgart, Germany
7.Swiss Fed Inst Technol, Dept Chem & Appl Biosci, HCI, CH-8093 Zurich, Switzerland
推荐引用方式
GB/T 7714
Wang, Zichun,Jiang, Yijiao,Yi, Xianfeng,et al. High population and dispersion of pentacoordinated Al-V species on the surface of flame-made amorphous silica-alumina[J]. SCIENCE BULLETIN,2019,64(8):516-523.
APA Wang, Zichun.,Jiang, Yijiao.,Yi, Xianfeng.,Zhou, Cuifeng.,Rawal, Aditya.,...&Huang, Jun.(2019).High population and dispersion of pentacoordinated Al-V species on the surface of flame-made amorphous silica-alumina.SCIENCE BULLETIN,64(8),516-523.
MLA Wang, Zichun,et al."High population and dispersion of pentacoordinated Al-V species on the surface of flame-made amorphous silica-alumina".SCIENCE BULLETIN 64.8(2019):516-523.

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来源:武汉物理与数学研究所

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