Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots

Graphene quantum dot (GQD), which is the latest addition to the family of nanocarbon materials, promises a wide spectrum of novel applications. Here, we for the first time demonstrate the use of GQD and sulfonated GQDs (SGQDs) as quasi-homogenous catalysts for chemo-catalysis. Specifically, we demon...

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Main Authors: Li, Kaixin, Chen, Jie, Yan, Yibo, Min, Yonggang, Li, Haopeng, Xi, Fengna, Liu, Jiyang, Chen, Peng
Other Authors: School of Chemical and Biomedical Engineering
Format: Article
Language:English
Published: 2020
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Online Access:https://hdl.handle.net/10356/137060
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1370602023-12-29T06:46:58Z Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots Li, Kaixin Chen, Jie Yan, Yibo Min, Yonggang Li, Haopeng Xi, Fengna Liu, Jiyang Chen, Peng School of Chemical and Biomedical Engineering Engineering::Bioengineering Quasi-homogeneous Carbohydrates Graphene quantum dot (GQD), which is the latest addition to the family of nanocarbon materials, promises a wide spectrum of novel applications. Here, we for the first time demonstrate the use of GQD and sulfonated GQDs (SGQDs) as quasi-homogenous catalysts for chemo-catalysis. Specifically, we demonstrate that SGQDs are able to selectively and effectively degrade carbohydrates (eg. fructose, glucose, and cellulose) at high concentrations into 5-hydroxymethylfurfural (5-HMF). For example, dehydration of fructose (up to 20 wt% concentration) to 5-HMF with a yield of 51.7% and a conversion rate of 91.8%. SGQDs uniquely combine the merits of homogenous catalysts and heterogeneous catalysts, i.e., SGQDs resemble a homogenous catalyst in the reaction while they can be recycled just mimicking the heterogeneous catalysts. The high efficiency of SGQDs is attributed to their unique physicochemical and structural properties. The DFT calculations reveal that intra-molecular hydrogen bonded -OH groups and the adjacent -SO3H groups on SGQDs play a synergistical role in their high catalytic efficiency. This study suggests the potential of SGQD as an efficient and green carbocatalyst for one-pot biomass transformation and more generally the unique potential of functionalized GQDs as novel quasi-homogeneous catalysts for various reactions. MOE (Min. of Education, S’pore) Accepted version 2020-02-18T05:07:41Z 2020-02-18T05:07:41Z 2018 Journal Article Li, K., Chen, J., Yan, Y., Min, Y., Li, H., Xi, F., . . . Chen, P. (2018). Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots. Carbon, 136, 224-233. doi:10.1016/j.carbon.2018.04.087 0008-6223 https://hdl.handle.net/10356/137060 10.1016/j.carbon.2018.04.087 2-s2.0-85056289398 136 224 233 en Carbon © 2018 Elsevier Ltd. All rights reserved. This paper was published in Carbon and is made available with permission of Elsevier Ltd. application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Bioengineering
Quasi-homogeneous
Carbohydrates
spellingShingle Engineering::Bioengineering
Quasi-homogeneous
Carbohydrates
Li, Kaixin
Chen, Jie
Yan, Yibo
Min, Yonggang
Li, Haopeng
Xi, Fengna
Liu, Jiyang
Chen, Peng
Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
description Graphene quantum dot (GQD), which is the latest addition to the family of nanocarbon materials, promises a wide spectrum of novel applications. Here, we for the first time demonstrate the use of GQD and sulfonated GQDs (SGQDs) as quasi-homogenous catalysts for chemo-catalysis. Specifically, we demonstrate that SGQDs are able to selectively and effectively degrade carbohydrates (eg. fructose, glucose, and cellulose) at high concentrations into 5-hydroxymethylfurfural (5-HMF). For example, dehydration of fructose (up to 20 wt% concentration) to 5-HMF with a yield of 51.7% and a conversion rate of 91.8%. SGQDs uniquely combine the merits of homogenous catalysts and heterogeneous catalysts, i.e., SGQDs resemble a homogenous catalyst in the reaction while they can be recycled just mimicking the heterogeneous catalysts. The high efficiency of SGQDs is attributed to their unique physicochemical and structural properties. The DFT calculations reveal that intra-molecular hydrogen bonded -OH groups and the adjacent -SO3H groups on SGQDs play a synergistical role in their high catalytic efficiency. This study suggests the potential of SGQD as an efficient and green carbocatalyst for one-pot biomass transformation and more generally the unique potential of functionalized GQDs as novel quasi-homogeneous catalysts for various reactions.
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Li, Kaixin
Chen, Jie
Yan, Yibo
Min, Yonggang
Li, Haopeng
Xi, Fengna
Liu, Jiyang
Chen, Peng
format Article
author Li, Kaixin
Chen, Jie
Yan, Yibo
Min, Yonggang
Li, Haopeng
Xi, Fengna
Liu, Jiyang
Chen, Peng
author_sort Li, Kaixin
title Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
title_short Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
title_full Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
title_fullStr Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
title_full_unstemmed Quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
title_sort quasi-homogeneous carbocatalysis for one-pot selective conversion of carbohydrates to 5-hydroxymethylfurfural using sulfonated graphene quantum dots
publishDate 2020
url https://hdl.handle.net/10356/137060
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