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![]() |
刊名 | SCIENCE BULLETIN
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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 |
DOI | 10.1016/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. |
入库方式: OAI收割
来源:武汉物理与数学研究所
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