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

Hao Chen; Zhenzhen Yang; Honggen Peng; Kecheng Jie; Peipei Li; Shunmin Ding; Wei Guo; Xian Suo; Jixing Liu; Ran Yan; Wenming Liu; Chi Linh Do-Thanh; Hongming Wang; Zhendong Wang; Lu Han; Weimin Yang; Sheng Dai

doi:10.1016/j.chempr.2021.08.022

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

Hao Chen, Zhenzhen Yang, Honggen Peng, Kecheng Jie, Peipei Li, Shunmin Ding, Wei Guo, Xian Suo, Jixing Liu, Ran Yan, Wenming Liu, Chi Linh Do-Thanh, Hongming Wang, Zhendong Wang, Lu Han, Weimin Yang, Sheng Dai

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

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, and rapid mass transfer ensured by the rigid porous architecture.

Original language	English
Pages (from-to)	3340-3358
Number of pages	19
Journal	Chem
Volume	7
Issue number	12
DOIs	https://doi.org/10.1016/j.chempr.2021.08.022
State	Published - Dec 9 2021

Funding

H.C., Z.Y., W.G., and S.D. were supported financially by the US Department of Energy , Office of Science , Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division , Catalysis Science program . H.P. was supported financially by the National Natural Science Foundation of China ( 21976078 and 21773106 ), the National Key R&D Program of China ( 2016YFC0205900 ), and the Natural Science Foundation of Jiangxi Province ( 20201BAB203024 ).

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
National Natural Science Foundation of China	21773106, 21976078
Natural Science Foundation of Jiangxi Province	20201BAB203024
National Key Research and Development Program of China	2016YFC0205900

Keywords

SDG12: Responsible consumption and production
antagonistic cascade catalysis
bifunctional
ionic liquid
porous liquid
zeolite

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10.1016/j.chempr.2021.08.022

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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, and rapid mass transfer ensured by the rigid porous architecture.",

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author = "Hao Chen and Zhenzhen Yang and Honggen Peng and Kecheng Jie and Peipei Li and Shunmin Ding and Wei Guo and Xian Suo and Jixing Liu and Ran Yan and Wenming Liu and Do-Thanh, {Chi Linh} and Hongming Wang and Zhendong Wang and Lu Han and Weimin Yang and Sheng Dai",

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doi = "10.1016/j.chempr.2021.08.022",

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T1 - A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis

AU - Chen, Hao

AU - Yang, Zhenzhen

AU - Peng, Honggen

AU - Jie, Kecheng

AU - Li, Peipei

AU - Ding, Shunmin

AU - Guo, Wei

AU - Suo, Xian

AU - Liu, Jixing

AU - Yan, Ran

AU - Liu, Wenming

AU - Do-Thanh, Chi Linh

AU - Wang, Hongming

AU - Wang, Zhendong

AU - Han, Lu

AU - Yang, Weimin

AU - Dai, Sheng

PY - 2021/12/9

Y1 - 2021/12/9

N2 - 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, and rapid mass transfer ensured by the rigid porous architecture.

AB - 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, and rapid mass transfer ensured by the rigid porous architecture.

KW - SDG12: Responsible consumption and production

KW - antagonistic cascade catalysis

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

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