Polarization Effects on the Cellulose Dissolution in Ionic Liquids:   Molecular Dynamics Simulations with Polarization Model and Integrated   Tempering Enhanced Sampling Method

doi:10.1021/acs.jpcb.6b12647

CORC > 北京大学 > 化学与分子工程学院

	Polarization Effects on the Cellulose Dissolution in Ionic Liquids: Molecular Dynamics Simulations with Polarization Model and Integrated Tempering Enhanced Sampling Method
	Kan, Zigui ; Zhu, Qang ; Yang, Lijiang ; Huang, Zhixiong ; Jin, Biaobing ; Ma, Jing
刊名	JOURNAL OF PHYSICAL CHEMISTRY B
	2017
关键词	1,3-DIMETHYLIMIDAZOLIUM CHLORIDE GLUCOSE SOLVATION FORCE-FIELDS SOLVENTS WATER NMR DEFINITION POLAR
DOI	10.1021/acs.jpcb.6b12647
英文摘要	Conformation of cellulose with various degree of polymerization of n = 1-12 in ionic liquid 1,3-dimethylimidazolium chloride ([C(1)mim]CI) and the intermolecular interaction between them was studied by means of molecular dynamics (MD) simulations with fixed-charge and charge variable polarizable force fields, respectively. The integrated tempering enhanced sampling method was also employed in the simulations in order to improve the sampling efficiency. Cellulose undergoes significant conformational changes from a gaseous right-hand helical twist along the long axis to a flexible conformation in ionic liquid. The intermolecular interactions between cellulose and ionic liquid were studied by both infrared spectrum measurements and theoretical simulations. Designated by their puckering parameters, the pyranose rings of cellulose oligomers are mainly arranged in a chair conformation. With the increase in the degree of polymerization of cellulose, the boat and skew-boat conformations of cellulose appear in the MD simulations, especially in the simulations with polarization model. The number and population of hydrogen bonds between the cellulose and the chloride anions show that chloride anion is prone to form HBs whenever it approaches the hydroxyl groups of cellulose and, thus, each hydroxyl group is fully hydrogen bonded to the chloride anion. MD simulations with polarization model presented more abundant conformations than that with nonpolarization model. The application of the enhanced sampling method further enlarged the conformational spaces that could be visited by facilitating the system escaping from the local minima. It was found that the electrostatics interactions between the cellulose and ionic liquid contribute more to the total interaction energies than the van der Waals interactions. Although the interaction energy between the cellulose and anion is about 2.9 times that between the cellulose and cation, the role of cation is non-negligible. hi contrast, the interaction energy between the cellulose and water is too weak to dissolve cellulose in water.; National Natural Science Foundation of China [21290192, 21273102, 21673111, 21373016, U1430237]; SCI(E); ARTICLE; 17; 4319-+; 121
语种	英语
内容类型	期刊论文
源URL	[http://ir.pku.edu.cn/handle/20.500.11897/473496]
专题	化学与分子工程学院
推荐引用方式 GB/T 7714	Kan, Zigui,Zhu, Qang,Yang, Lijiang,et al. Polarization Effects on the Cellulose Dissolution in Ionic Liquids: Molecular Dynamics Simulations with Polarization Model and Integrated Tempering Enhanced Sampling Method[J]. JOURNAL OF PHYSICAL CHEMISTRY B,2017.
APA	Kan, Zigui,Zhu, Qang,Yang, Lijiang,Huang, Zhixiong,Jin, Biaobing,&Ma, Jing.(2017).Polarization Effects on the Cellulose Dissolution in Ionic Liquids: Molecular Dynamics Simulations with Polarization Model and Integrated Tempering Enhanced Sampling Method.JOURNAL OF PHYSICAL CHEMISTRY B.
MLA	Kan, Zigui,et al."Polarization Effects on the Cellulose Dissolution in Ionic Liquids: Molecular Dynamics Simulations with Polarization Model and Integrated Tempering Enhanced Sampling Method".JOURNAL OF PHYSICAL CHEMISTRY B (2017).