Facile synthesis of metal-organic frameworks embedded in interconnected macroporous polymer as a dual acid-base bifunctional catalyst for efficient conversion of cellulose to 5-hydroxymethylfurfural

doi:10.1016/j.cjche.2021.06.019

中国化学工程学报 ›› 2022, Vol. 44 ›› Issue (4): 169-181.DOI: 10.1016/j.cjche.2021.06.019

Facile synthesis of metal-organic frameworks embedded in interconnected macroporous polymer as a dual acid-base bifunctional catalyst for efficient conversion of cellulose to 5-hydroxymethylfurfural

Yanan Wei¹, Yunlei Zhang¹, Bing Li¹, Wen Guan¹, Changhao Yan², Xin Li¹, Yongsheng Yan¹

1 Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212000, China;
2 Research Center of Fluid Machinery Engineering and Technology, Jiangsu University, Zhenjiang 212000, China

收稿日期:2020-09-12 修回日期:2021-06-17 出版日期:2022-04-28 发布日期:2022-06-18
通讯作者: Yunlei Zhang,E-mail:jsdxzyl@ujs.edu.cn;Yongsheng Yan,E-mail:yys@ujs.edu.cn
基金资助:
This work was financially supported by the National Natural Science Foundation of China (No. 21606100), the Natural Science Foundation of Jiangsu Province (No. BK20180850), the China Postdoctoral Science Foundation (Nos. 2019M651740 and 2019T120397) and the Young Talent Cultivate Programme of Jiangsu University.

Facile synthesis of metal-organic frameworks embedded in interconnected macroporous polymer as a dual acid-base bifunctional catalyst for efficient conversion of cellulose to 5-hydroxymethylfurfural

Yanan Wei¹, Yunlei Zhang¹, Bing Li¹, Wen Guan¹, Changhao Yan², Xin Li¹, Yongsheng Yan¹

1 Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212000, China;
2 Research Center of Fluid Machinery Engineering and Technology, Jiangsu University, Zhenjiang 212000, China

Received:2020-09-12 Revised:2021-06-17 Online:2022-04-28 Published:2022-06-18
Contact: Yunlei Zhang,E-mail:jsdxzyl@ujs.edu.cn;Yongsheng Yan,E-mail:yys@ujs.edu.cn
Supported by:
This work was financially supported by the National Natural Science Foundation of China (No. 21606100), the Natural Science Foundation of Jiangsu Province (No. BK20180850), the China Postdoctoral Science Foundation (Nos. 2019M651740 and 2019T120397) and the Young Talent Cultivate Programme of Jiangsu University.

摘要/Abstract

摘要： 5-Hydroxymethylfurfural (5-HMF), as a key platform compound for the conversion of biomass to various biomass-derived chemicals and biofuels, has been attracted extensive attention. In this research, using Pickering high internal phase emulsions (Pickering HIPEs) as template and functional metal-organic frameworks (MOFs, UiO-66-SO₃H and UiO-66-NH₂)/Tween 85 as co-stabilizers to synthesis the dual acid-base bifunctional macroporous polymer catalyst by one-pot process, which has excellent catalytic activity in the cascade reaction of converting cellulose to 5-HMF. The effects of the emulsion parameters including the amount of surfactant (ranging from 0.5% to 2.0% (mass)), the internal phase volume fraction (ranging from 75% to 90%) and the acid/base Pickering particles mass ratio (ranging from 0:6 to 6:0) on the morphology and catalytic performance of solid catalyst were systematically researched. The results of catalytic experiments suggested that the connected large pore size of catalyst can effectively improve the cellulose conversion, and the synergistic effect of acid and base active sites can effectively improve the 5-HMF yield. The highest 5-HMF yield, about 40.5%, can be obtained by using polymer/MOFs composite as catalyst (Poly-P12, the pore size of (53.3 ±11.3) μm, the acid density of 1.99 mmol·g^-1 and the base density of 1.13 mol·g^-1) under the optimal reaction conditions (130 ℃, 3 h). Herein, the polymer/MOFs composite with open-cell structure was prepared by the Pickering HIPEs templating method, which provided a favorable experimental basis and theoretical reference for achieving efficient production of high added-value product from abundant biomass.

关键词: Catalyst, Biomass, Hydrolysis, 5-Hydroxymethylfurfural, Pickering high internal phase emulsions templated polymer, Acid-base bifunctional site

Abstract: 5-Hydroxymethylfurfural (5-HMF), as a key platform compound for the conversion of biomass to various biomass-derived chemicals and biofuels, has been attracted extensive attention. In this research, using Pickering high internal phase emulsions (Pickering HIPEs) as template and functional metal-organic frameworks (MOFs, UiO-66-SO₃H and UiO-66-NH₂)/Tween 85 as co-stabilizers to synthesis the dual acid-base bifunctional macroporous polymer catalyst by one-pot process, which has excellent catalytic activity in the cascade reaction of converting cellulose to 5-HMF. The effects of the emulsion parameters including the amount of surfactant (ranging from 0.5% to 2.0% (mass)), the internal phase volume fraction (ranging from 75% to 90%) and the acid/base Pickering particles mass ratio (ranging from 0:6 to 6:0) on the morphology and catalytic performance of solid catalyst were systematically researched. The results of catalytic experiments suggested that the connected large pore size of catalyst can effectively improve the cellulose conversion, and the synergistic effect of acid and base active sites can effectively improve the 5-HMF yield. The highest 5-HMF yield, about 40.5%, can be obtained by using polymer/MOFs composite as catalyst (Poly-P12, the pore size of (53.3 ±11.3) μm, the acid density of 1.99 mmol·g^-1 and the base density of 1.13 mol·g^-1) under the optimal reaction conditions (130 ℃, 3 h). Herein, the polymer/MOFs composite with open-cell structure was prepared by the Pickering HIPEs templating method, which provided a favorable experimental basis and theoretical reference for achieving efficient production of high added-value product from abundant biomass.

Key words: Catalyst, Biomass, Hydrolysis, 5-Hydroxymethylfurfural, Pickering high internal phase emulsions templated polymer, Acid-base bifunctional site

Yanan Wei, Yunlei Zhang, Bing Li, Wen Guan, Changhao Yan, Xin Li, Yongsheng Yan. Facile synthesis of metal-organic frameworks embedded in interconnected macroporous polymer as a dual acid-base bifunctional catalyst for efficient conversion of cellulose to 5-hydroxymethylfurfural[J]. 中国化学工程学报, 2022, 44(4): 169-181.

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Facile synthesis of metal-organic frameworks embedded in interconnected macroporous polymer as a dual acid-base bifunctional catalyst for efficient conversion of cellulose to 5-hydroxymethylfurfural

Facile synthesis of metal-organic frameworks embedded in interconnected macroporous polymer as a dual acid-base bifunctional catalyst for efficient conversion of cellulose to 5-hydroxymethylfurfural

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