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Origin and Structural Characteristics of Tri-coordinated Extra-framework Aluminum Species in Dealuminated Zeolites

文献类型：期刊论文

作者Yi, Xianfeng3,7; Liu, Kangyu4; Chen, Wei3,7; Li, Junjie5; Xu, Shutao6; Li, Chengbin3; Xiao, Yao3,7; Liu, Haichao4; Guo, Xinwen5; Liu, Shang-Bin1
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2018-08-29
卷号140期号:34页码:10764-10774
ISSN号0002-7863
DOI10.1021/jacs.8b04819
英文摘要Post-synthetic dealumination treatment is a common tactic adopted to improve the catalytic performance of industrialized zeolitic catalysts through enhancements in acidity and stability. However, among the possible extra-framework aluminum (EFAL) species in dealuminated zeolites such as Al3+, Al(OH)(2+), Al(OH)(2)(+), AlO+, AlOOH, and Al(OH)(3), the presence of tri-coordinated EFAL-Al3+ species, which exhibit large quadrupolar effect due to the lack of hydrogen-bonding species, was normally undetectable by conventional one- and two-dimensional H-1 and/or Al-27 solid-state nuclear magnetic resonance (SSNMR) techniques. By combining density functional theory (DFT) calculations with experimental P-31 SSNMR using trimethylphosphine (TMP) as the probe molecule, we report herein a comprehensive study to certify the origin, fine structure, and possible location of tri-coordinated EFAL-Al3+ species in dealuminated HY zeolite. The spatial proximities and synergies between the Bronsted and various Lewis acid sites were clearly identified, and the origin for the observed EFAL-Al3+ species with ultra-strong Lewis acidity was deduced to be at the expense of adjacent Bronsted acid sites. The excellent performance of such tri-coordinated EFAL species was furthermore confirmed by glucose isomerization reactions.
WOS关键词SOLID-STATE NMR ; BRONSTED/LEWIS ACID SYNERGY ; C-13 CHEMICAL-SHIFT ; P-31 NMR ; THEORETICAL CALCULATION ; GLUCOSE ISOMERIZATION ; NONFRAMEWORK ALUMINUM ; LEWIS ACIDITY ; H/D EXCHANGE ; SPECTROSCOPY
资助项目National Natural Science Foundation of China[21522310] ; National Natural Science Foundation of China[21473244] ; National Natural Science Foundation of China[91645112] ; Natural Science Foundation of Hubei Province of China[2018CFA009] ; Key Research Program of Frontier Sciences, CAS[QYZDB-SSW-SLH026] ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund[U1501501] ; Sinopec Corp.[417012-4]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000443654400024
出版者AMER CHEMICAL SOC
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund ; Sinopec Corp. ; Sinopec Corp.
源URL[http://ir.wipm.ac.cn/handle/112942/13096]  
专题中国科学院武汉物理与数学研究所
通讯作者Zheng, Anmin
作者单位1.Acad Sinica, Inst Atom & Mol Sci, Taipei 10617, Taiwan
2.Wuhan Oxford Joint Catalysis Lab, Wuhan 430071, Hubei, Peoples R China
3.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Key Lab Magnet Resonance Biol Syst,Wuhan Inst Phy, Wuhan 430071, Hubei, Peoples R China
4.Peking Univ, Coll Chem & Mol Engn, BNLMS, State Key Lab Struct Chem Stable & Unstable Speci, Beijing 100871, Peoples R China
5.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China
6.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China
7.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714		 Yi, Xianfeng,Liu, Kangyu,Chen, Wei,et al. Origin and Structural Characteristics of Tri-coordinated Extra-framework Aluminum Species in Dealuminated Zeolites[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2018,140(34):10764-10774.
APA Yi, Xianfeng.,Liu, Kangyu.,Chen, Wei.,Li, Junjie.,Xu, Shutao.,...&Zheng, Anmin.(2018).Origin and Structural Characteristics of Tri-coordinated Extra-framework Aluminum Species in Dealuminated Zeolites.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,140(34),10764-10774.
MLA Yi, Xianfeng,et al."Origin and Structural Characteristics of Tri-coordinated Extra-framework Aluminum Species in Dealuminated Zeolites".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 140.34(2018):10764-10774.

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来源：武汉物理与数学研究所

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