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Title: A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis

Abstract

The emergence of porous liquids (PLs) opened opportunities to form unique antagonistic systems capable of fulfilling cascade reactions promoted by incompatible active sites in one pot, which is a long-term challenging subject in catalysis. Herein, unique bifunctional type III PL-based systems were facilely fabricated via assembly of zeolite nanosheets with ionic liquids. Rational structural design afforded PLs that feature high zeolite concentration, stable dispersion after 2 years, abundant cavity distribution, and involvement of antagonistic groups (acid and base sites) in separated and active form via steric hindrance control and electronic repulsion regulation. These unique properties worked cooperatively to fulfill the cascade deacetalization-Knoevenagel/Aldol condensation in one pot with superior catalytic efficiency outperforming the traditional systems. The key to success lies in the formation of bifunctional composites, transformation of zeolite from heterogeneous to homogeneous via surface modification, as well as rapid mass transfer ensured by the rigid porous architecture.

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [4];  [5];  [1];  [3];  [6];  [5];  [5];  [3];  [5];  [5];  [7];  [8]; ORCiD logo [4]
  1. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Nanchang Univ. (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Nanchang Univ. (China)
  6. Jiangsu University, Zhenjiang (China)
  7. Tongji Unversity, Shanghai (China)
  8. Sinopec Shanghai Research Institute of Petrochemical Technology, Shanghai (China)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1830136
Alternate Identifier(s):
OSTI ID: 1869352
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Chem
Additional Journal Information:
Journal Volume: 7; Journal Issue: 12; Journal ID: ISSN 2451-9294
Publisher:
Cell Press, Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; porous liquid; ionic liquid; zeolite; bifunctional; antagonistic cascade catalysis

Citation Formats

Chen, Hao, Yang, Zhenzhen, Peng, Honggen, Jie, Kecheng, Li, Peipei, Ding, Shunmin, Guo, Wei, Suo, Xian, Liu, Jixing, Yan, Ran, Liu, Wenming, Do-Thanh, Chi-Linh, Wang, Hongming, Wang, Zhendong, Han, Lu, Yang, Weimin, and Dai, Sheng. A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis. United States: N. p., 2021. Web. doi:10.1016/j.chempr.2021.08.022.
Chen, Hao, Yang, Zhenzhen, Peng, Honggen, Jie, Kecheng, Li, Peipei, Ding, Shunmin, Guo, Wei, Suo, Xian, Liu, Jixing, Yan, Ran, Liu, Wenming, Do-Thanh, Chi-Linh, Wang, Hongming, Wang, Zhendong, Han, Lu, Yang, Weimin, & Dai, Sheng. A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis. United States. https://doi.org/10.1016/j.chempr.2021.08.022
Chen, Hao, Yang, Zhenzhen, Peng, Honggen, Jie, Kecheng, Li, Peipei, Ding, Shunmin, Guo, Wei, Suo, Xian, Liu, Jixing, Yan, Ran, Liu, Wenming, Do-Thanh, Chi-Linh, Wang, Hongming, Wang, Zhendong, Han, Lu, Yang, Weimin, and Dai, Sheng. Wed . "A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis". United States. https://doi.org/10.1016/j.chempr.2021.08.022. https://www.osti.gov/servlets/purl/1830136.
@article{osti_1830136,
title = {A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis},
author = {Chen, Hao and Yang, Zhenzhen and Peng, Honggen and Jie, Kecheng and Li, Peipei and Ding, Shunmin and Guo, Wei and Suo, Xian and Liu, Jixing and Yan, Ran and Liu, Wenming and Do-Thanh, Chi-Linh and Wang, Hongming and Wang, Zhendong and Han, Lu and Yang, Weimin and Dai, Sheng},
abstractNote = {The emergence of porous liquids (PLs) opened opportunities to form unique antagonistic systems capable of fulfilling cascade reactions promoted by incompatible active sites in one pot, which is a long-term challenging subject in catalysis. Herein, unique bifunctional type III PL-based systems were facilely fabricated via assembly of zeolite nanosheets with ionic liquids. Rational structural design afforded PLs that feature high zeolite concentration, stable dispersion after 2 years, abundant cavity distribution, and involvement of antagonistic groups (acid and base sites) in separated and active form via steric hindrance control and electronic repulsion regulation. These unique properties worked cooperatively to fulfill the cascade deacetalization-Knoevenagel/Aldol condensation in one pot with superior catalytic efficiency outperforming the traditional systems. The key to success lies in the formation of bifunctional composites, transformation of zeolite from heterogeneous to homogeneous via surface modification, as well as rapid mass transfer ensured by the rigid porous architecture.},
doi = {10.1016/j.chempr.2021.08.022},
journal = {Chem},
number = 12,
volume = 7,
place = {United States},
year = {Wed Sep 22 00:00:00 EDT 2021},
month = {Wed Sep 22 00:00:00 EDT 2021}
}

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