中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
首页 机构 成果 学者
  
  1. CAS IR Grid
  2. 过程工程研究所
  3. 中国科学院过程工程研究所
Reaction-Controlled Phase-Transfer Process of Polyoxometalate-Based Catalyst for Cellulose Esterification: A Molecular Dynamics Study

文献类型：期刊论文

作者Liu, Yubing2; Yao, Xiaoqian1; Liu, Xiaomin1; Chen, Wei2; Song, Yu-Fei2
刊名JOURNAL OF PHYSICAL CHEMISTRY C
出版日期2021-11-25
卷号125期号:46页码:25478-25487
ISSN号1932-7447
DOI10.1021/acs.jpcc.1c05561
英文摘要The solution dynamics behavior of polyoxometalates (POMs) is essential to understand their catalytic mechanism under real conditions. Herein, the phase-transfer process of a novel catalyst PVDB-VBC-IM-PW12 (copolymer of divinylbenzene with 4-vinyl-benzyl chloride as the support, imidazole methyl as the linker, and alpha-PW12O403- as catalytic active sites) for cellulose esterification was studied for the first time by molecular dynamics simulations. The simulation results show that the synergistic effect of the polymer support and the ionic liquid can overcome the electrostatic repulsion of the POM anions, and the catalyst can be synthesized firmly in an aqueous solution. The catalyst structure becomes loose in the acid solution, exposing the active sites of PW12 to catalyze cellulose. After the esterification is completed, the cellulose ester without hydroxyl groups loses the H-bond with PW12 and is separated from the catalyst. At the same time, PW12 is reloaded on the support. In addition, it was also found that the active site of PW12 is mainly the bridging oxygen Ob1 instead of the outermost terminal oxygen Ot. This is due to the formation of stronger hydrogen bonds between Ob1 and the hydroxyl group on the cellulose. These findings reveal the dynamic behavior mechanism of POMs in catalytic reactions at the molecular level, which is very helpful for the design of efficient POM-based catalysts.
WOS关键词ACETATE PROPIONATE CAP ; IONIC LIQUIDS ; FORCE-FIELD ; MESOPOROUS POLYMER ; SULFONIC-ACID ; KEGGIN ANIONS ; BUTYRATE CAB ; SIMULATIONS ; EPOXIDATION ; MANUFACTURE
资助项目National Key Research and Development Program of China[2017YFB0307303] ; National Natural Science Foundation of China[21776281] ; Fundamental Research Funds for the Central Universities[XK1802-6] ; Fundamental Research Funds for the Central Universities[XK1803-05] ; Fundamental Research Funds for the Central Universities[XK1902]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
语种英语
WOS记录号WOS:000731169200006
出版者AMER CHEMICAL SOC
资助机构National Key Research and Development Program of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities
源URL[http://ir.ipe.ac.cn/handle/122111/51447]  
专题中国科学院过程工程研究所
通讯作者Yao, Xiaoqian; Chen, Wei; Song, Yu-Fei
作者单位1.Chinese Acad Sci, Beijing Key Lab Ionic Liquids Clean Proc, Inst Proc Engn, CAS Key Lab Green Proc & Engn,State Key Lab Multi, Beijing 100190, Peoples R China
2.Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
推荐引用方式
GB/T 7714		 Liu, Yubing,Yao, Xiaoqian,Liu, Xiaomin,et al. Reaction-Controlled Phase-Transfer Process of Polyoxometalate-Based Catalyst for Cellulose Esterification: A Molecular Dynamics Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2021,125(46):25478-25487.
APA Liu, Yubing,Yao, Xiaoqian,Liu, Xiaomin,Chen, Wei,&Song, Yu-Fei.(2021).Reaction-Controlled Phase-Transfer Process of Polyoxometalate-Based Catalyst for Cellulose Esterification: A Molecular Dynamics Study.JOURNAL OF PHYSICAL CHEMISTRY C,125(46),25478-25487.
MLA Liu, Yubing,et al."Reaction-Controlled Phase-Transfer Process of Polyoxometalate-Based Catalyst for Cellulose Esterification: A Molecular Dynamics Study".JOURNAL OF PHYSICAL CHEMISTRY C 125.46(2021):25478-25487.

入库方式： OAI收割

来源：过程工程研究所

浏览0
下载0
收藏0
其他版本

除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。