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Can Hammett indicators accurately measure the acidity of zeolite catalysts with confined space? Insights into the mechanism of coloration

文献类型：期刊论文

作者Chen, Wei2,4; Yi, Xianfeng4; Huang, Ling4; Liu, Wentao1; Li, Guangchao2,4; Acharya, Dinesh2,4; Sun, Xianyong4; Zheng, Anmin1,3,4
刊名CATALYSIS SCIENCE & TECHNOLOGY
出版日期2019-09-21
卷号9期号:18页码:5045-5057
ISSN号2044-4753
DOI10.1039/c9cy01392j
英文摘要The acidic properties of zeolite catalysts play a crucial role in governing catalytic performances, which makes the acidity characterization an important subject in the field of zeolite catalysis. So far, Hammett titration has been a conventional method to determine the acidic strength of liquid and solid acids, however, the reliability of this titration method to measure the acidity of acidic sites inside zeolites is in debate. It is necessary to unveil the origin of the coloration of Hammett indicators adsorbed inside zeolite channels and cages. Herein, by employing an advanced computational method, the adsorbed structures and electronic properties of a series of Hammett indicators with various pK(a) (from -0.29 to -14.52) values have been investigated, concerning the interaction with the Bronsted acidic sites inside H-ZSM-5, H-MOR and H-Y zeolites. On the basis of the theoretical results, the intimate relationship between the coloration (traditionally corresponding to the protonation of Hammett indicators) and HOMO-LUMO gap has been established by DFT and time-dependent (TD) DFT calculations for the first time. Furthermore, not only the Bronsted acidity, but also the pore confinement derived from the zeolite framework could also render the coloration by effectively reducing the HOMO-LUMO gaps, which can be differentiated by the diverse shapes and sizes of zeolite cages. Therefore, one should be cautious in the utilization of Hammett titration for the acidity determination of porous zeolite catalysts and other solid acids, and other more accurate approaches are needed in the future.
WOS关键词MOLECULAR-ORBITAL METHODS ; C-13 CHEMICAL-SHIFT ; TD-DFT ; STRENGTH ; PROBE ; QUANTIFICATION ; ADSORPTION ; BENCHMARKS ; TITRATION ; SURFACES
资助项目National Natural Science Foundation of China[91645112] ; National Natural Science Foundation of China[21802164] ; National Natural Science Foundation of China[21902180] ; Key Research Program of Frontier Sciences, CAS[QYZDB-SSW-SLH026] ; Natural Science Foundation of Hubei Province of China[2018CFA009] ; SINOPEC Shanghai Research Institute of Petrochemical Technology[417012-4]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000487788800018
出版者ROYAL SOC CHEMISTRY
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; SINOPEC Shanghai Research Institute of Petrochemical Technology ; SINOPEC Shanghai Research Institute of Petrochemical Technology
源URL[http://ir.wipm.ac.cn/handle/112942/21431]  
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.Zhengzhou Univ, Sch Mat Sci & Engn, Zhengzhou 450052, Henan, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Hubei, Peoples R China
4.Chinese Acad Sci, Key Lab Magnet Resonance Biol Syst, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math,State Key Lab Magnet Reson, Wuhan 430071, Hubei, Peoples R China
推荐引用方式
GB/T 7714		 Chen, Wei,Yi, Xianfeng,Huang, Ling,et al. Can Hammett indicators accurately measure the acidity of zeolite catalysts with confined space? Insights into the mechanism of coloration[J]. CATALYSIS SCIENCE & TECHNOLOGY,2019,9(18):5045-5057.
APA Chen, Wei.,Yi, Xianfeng.,Huang, Ling.,Liu, Wentao.,Li, Guangchao.,...&Zheng, Anmin.(2019).Can Hammett indicators accurately measure the acidity of zeolite catalysts with confined space? Insights into the mechanism of coloration.CATALYSIS SCIENCE & TECHNOLOGY,9(18),5045-5057.
MLA Chen, Wei,et al."Can Hammett indicators accurately measure the acidity of zeolite catalysts with confined space? Insights into the mechanism of coloration".CATALYSIS SCIENCE & TECHNOLOGY 9.18(2019):5045-5057.

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来源：武汉物理与数学研究所

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