Co-reporter:Weiqiang Yu;Qianqian Huang;Rui Lu;Shuai Chen;Jie Xu
Green Chemistry (1999-Present) 2017 vol. 19(Issue 14) pp:3327-3333
Publication Date(Web):2017/07/17
DOI:10.1039/C7GC00659D
Etherification of ethylene glycol with methanol provides a sustainable route for the production of widely used dimethoxyethane; dimethoxyethane is a green solvent and reagent that is applied in batteries and used as a potential diesel fuel additive. SAPO-34 zeolite was found to be an efficient and highly selective catalyst for this etherification via a continuous flow experiment. It achieved up to 79.4% selectivity for dimethoxyethane with around 96.7% of conversion. The relationship of the catalyst's structure and the dimethoxyethane selectivity was established via control experiments. The results indicated that the pore structure of SAPO-34 effectively limited the formation of 1,4-dioxane from activated ethylene glycol, enhanced the reaction of the activated methanol with ethylene glycol in priority, and thus resulted in high selectivity for the desired products. The continuous flow technology used in the study could efficiently promote the complete etherification of EG with methanol to maintain high selectivity for dimethoxyethane.
Co-reporter:Xiaoqin Si;Jiazhi Chen;Rui Lu;Qianqian Huang;Huifang Jiang;Esben Taarning;Jie Xu
Green Chemistry (1999-Present) 2017 vol. 19(Issue 20) pp:4849-4857
Publication Date(Web):2017/10/16
DOI:10.1039/C7GC02492D
Efficient fractionation of woody biomass provides an opportunity to separate and then upgrade each of the cellulose, hemicellulose and lignin fractions. The current processes for the fractionation of biomass target high-quality cellulose or lignin solely. Here, we developed a simple and efficient strategy for achieving high-quality cellulose and lignin simultaneously from woody biomass. Solvent thermal treatment was used to release the lignin and hemicellulose fragments from beech sawdust. 92.8% cellulose was retained in cellulose pulp with the purity of cellulose as high as 93.5% and a highly crystalline structure, using tetrahydrofurfuryl alcohol (THFA) and water as the solvent. In addition, 77.4% pure lignin powder was recovered. A linear correlation between the lignin monomer yield and the percentage of total β-O-4 or condensed linkages was observed during the lignin depolymerization process. Our strategy offers a possibility for the high-value utilization of whole biomass.
Co-reporter:Rui Lu;Dr. Fang Lu;Jiazhi Chen;Dr. Weiqiang Yu;Qianqian Huang;Junjie Zhang;Dr. Jie Xu
Angewandte Chemie International Edition 2016 Volume 55( Issue 1) pp:249-253
Publication Date(Web):
DOI:10.1002/anie.201509149
Abstract
We report a cascade synthetic route to directly obtain diethyl terephthalate, a replacement for terephthalic acid, from biomass-derived muconic acid, ethanol, and ethylene. The process involves two steps: First, a substituted cyclohexene system is built through esterification and Diels–Alder reaction; then, a dehydrogenation reaction provides diethyl terephthalate. The key esterification reaction leads to improved solubility and modulates the electronic properties of muconic acid, thus promoting the Diels–Alder reaction with ethylene. With silicotungstic acid as the catalyst, nearly 100 % conversion of muconic acid was achieved, and the cycloadducts were formed with more than 99.0 % selectivity. The palladium-catalyzed dehydrogenation reaction preferentially occurs under neutral or mildly basic conditions. The total yield of diethyl terephthalate reached 80.6 % based on the amount of muconic acid used in the two-step synthetic process.
Co-reporter:Rui Lu;Dr. Fang Lu;Jiazhi Chen;Dr. Weiqiang Yu;Qianqian Huang;Junjie Zhang;Dr. Jie Xu
Angewandte Chemie 2016 Volume 128( Issue 1) pp:257-261
Publication Date(Web):
DOI:10.1002/ange.201509149
Abstract
We report a cascade synthetic route to directly obtain diethyl terephthalate, a replacement for terephthalic acid, from biomass-derived muconic acid, ethanol, and ethylene. The process involves two steps: First, a substituted cyclohexene system is built through esterification and Diels–Alder reaction; then, a dehydrogenation reaction provides diethyl terephthalate. The key esterification reaction leads to improved solubility and modulates the electronic properties of muconic acid, thus promoting the Diels–Alder reaction with ethylene. With silicotungstic acid as the catalyst, nearly 100 % conversion of muconic acid was achieved, and the cycloadducts were formed with more than 99.0 % selectivity. The palladium-catalyzed dehydrogenation reaction preferentially occurs under neutral or mildly basic conditions. The total yield of diethyl terephthalate reached 80.6 % based on the amount of muconic acid used in the two-step synthetic process.
Co-reporter:Penghua Che, Fang Lu, Xin Nie, Yizheng Huang, Yanliang Yang, Feng Wang and Jie Xu
Chemical Communications 2015 vol. 51(Issue 6) pp:1077-1080
Publication Date(Web):24 Nov 2014
DOI:10.1039/C4CC08467E
An excellent linear correlation between lnδ (OH chemical shift) and 1/T (temperature) is discovered for the first time for hydroxyl compounds. The derived slope (A) provides information as an index not only for distinguishing different types of H-bonds, but also for predicting their reactivities. This finding can be extended to other H-bond-containing molecules.
Co-reporter:Penghua Che, Fang Lu, Xiaoqin Si and Jie Xu
RSC Advances 2015 vol. 5(Issue 31) pp:24139-24143
Publication Date(Web):27 Feb 2015
DOI:10.1039/C4RA15919E
1,2-Dimethoxyethane is explored for the first time as etherification agent for the acid-catalyzed synthesis of methyl ethers from biomass-derived hydroxyl compounds. H3PW12O40 catalyst can provide the formation of isosorbide methyl ethers with 80% GC yield from isosorbide. The acid catalyst type and acid amount are of critical importance in improving etherification reactivities of hydroxyl groups with 1,2-dimethoxyethane.
Co-reporter:Jiazhi Chen, Fang Lu and Jie Xu
RSC Advances 2015 vol. 5(Issue 7) pp:5068-5071
Publication Date(Web):11 Dec 2014
DOI:10.1039/C4RA13959C
Monodispersed Al, Sn, Fe, Nb, Ti-doped hollow nanocages (approx. 120 nm) with MCM-41 molecular sieve structures were synthesized by reacting nanosized MCM-41 silica seeds with in situ coated heteroatomic species. The Al-doped hollow MCM-41 nanocages have significantly improved accessible acid sites, which show enhanced activity in catalytic hydrolysis of cellobiose.
Co-reporter:Jiazhi Chen;Dr. Fang Lu;Junjie Zhang;Weiqiang Yu; Feng Wang; Jin Gao; Jie Xu
ChemCatChem 2013 Volume 5( Issue 10) pp:2822-2826
Publication Date(Web):
DOI:10.1002/cctc.201300316
Co-reporter:Penghua Che, Fang Lu, Xin Nie, Yizheng Huang, Yanliang Yang, Feng Wang and Jie Xu
Chemical Communications 2015 - vol. 51(Issue 6) pp:NaN1080-1080
Publication Date(Web):2014/11/24
DOI:10.1039/C4CC08467E
An excellent linear correlation between lnδ (OH chemical shift) and 1/T (temperature) is discovered for the first time for hydroxyl compounds. The derived slope (A) provides information as an index not only for distinguishing different types of H-bonds, but also for predicting their reactivities. This finding can be extended to other H-bond-containing molecules.
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