Mechanism of Glucose-Fructose Isomerization over Aluminum Based Catalysts in Methanol Media
文献类型：期刊论文
| 作者 | Ju, Zhaoyang1,2; Zhang, Yuxuan1; Zhao, Tingting1; Xiao, Weihua1; Yao, Xiaoqian2 |
| 刊名 | ACS SUSTAINABLE CHEMISTRY & ENGINEERING
 |
| 出版日期 | 2019-09-03 |
| 卷号 | 7期号:17页码:14962-14972 |
| 关键词 | Glucose Fructose Aluminum-based catalysts DFT Isomerization |
| ISSN号 | 2168-0485 |
| DOI | 10.1021/acssuschemeng.9b03241 |
| 英文摘要 | The catalytic isomerization of glucose to fructose has been deemed a vital step in biorefinery, while the isomerization mechanism in alcoholic media still remains ambiguous. Hereby, density functional theory (DFT) calculations were carried out to investigate the isomerization mechanism of glucose over aluminum-based catalysts in methanol media. Al3+ was apt to coordinate with methanol and cyclic beta-D-glucose (CDG) to form various complexes. It was found that [Al-(CH3O)(2)(CH3OH)(2)](+) was the most stable one in +1 charge complexes based on the DFT calculations and ESI-MS experiments. Furthermore, the four-coordination complex [(eta(2)(O4,O6)-CDH)Al(CH3O)(2)](+) was predicted to be the most preferable. Ionic species formed between Al3+ and the solvent can further assemble with glucose to catalyze the isomerization. The isomerization proceeds mainly by three steps, including ring opening, hydride shift, and ring-closing with the migration of H from the C2-H to the O1-H bond (hydride shift) as the rate-determining step. The coordination of Al3+ with methanol showed a significant catalytic effect by shortening the proton transfer distance, which resulted in a markedly reduced overall reaction barrier for isomerization. The calculations provided a better insight into the glucose transformation in the methanol media with Al-based catalysts. |
| WOS关键词 | METHYL LEVULINATE ; BRONSTED ACID ; AB-INITIO ; CONVERSION ; LEWIS ; BIOMASS ; BOND ; COOPERATIVITY ; INSIGHTS ; ALCOHOL |
| 资助项目 | National Key R&D Program of China[2016YFE0112800] ; National Natural Science Foundation of China[31671572] ; National Natural Science Foundation of China[21776281] ; National Science Foundation of Beijing, China[2182073] |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Engineering |
| 语种 | 英语 |
| WOS记录号 | WOS:000484071600071 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Key R&D Program of China ; National Natural Science Foundation of China ; National Science Foundation of Beijing, China |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/30923]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Xiao, Weihua; Yao, Xiaoqian |
| 作者单位 | 1.China Agr Univ, Coll Engn, Engn Lab Agrobiomass & Bioproc, 17 Qinghua Donglu, Beijing 100083, Peoples R China 2.Chinese Acad Sci, CAS Key Lab Green Proc & Engn, Beijing Key Lab Ion Liquids Clean Proc, State Key Lab Multiphase Complex Syst,Inst Proc E, 1 North Second St, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Ju, Zhaoyang,Zhang, Yuxuan,Zhao, Tingting,et al. Mechanism of Glucose-Fructose Isomerization over Aluminum Based Catalysts in Methanol Media[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2019,7(17):14962-14972. |
| APA | Ju, Zhaoyang,Zhang, Yuxuan,Zhao, Tingting,Xiao, Weihua,&Yao, Xiaoqian.(2019).Mechanism of Glucose-Fructose Isomerization over Aluminum Based Catalysts in Methanol Media.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,7(17),14962-14972. |
| MLA | Ju, Zhaoyang,et al."Mechanism of Glucose-Fructose Isomerization over Aluminum Based Catalysts in Methanol Media".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 7.17(2019):14962-14972. |
入库方式： OAI收割
来源：过程工程研究所
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