Initial reaction mechanisms of cellulose pyrolysis revealed by ReaxFF molecular dynamics

doi:10.1016/j.fuel.2016.03.008

	Initial reaction mechanisms of cellulose pyrolysis revealed by ReaxFF molecular dynamics
	Zheng, Mo; Wang, Ze; Li, Xiaoxia; Qiao, Xianjie; Song, Wenli; Guo, Li
	2016-08-01
发表期刊	FUEL
ISSN	0016-2361
卷号	177 期号:AUG 页码:130-141
摘要	Mechanism investigation of cellulose pyrolysis is remarkably useful for efficient utilization of biomass. In this paper, a new methodology rooted in the first GPU enabled ReaxFF MD simulation program (GMD-Reax) and the unique cheminformatics based reaction analysis tool (VARxMD) was employed to investigate the initial reaction mechanism of cellulose pyrolysis. Both the overall spectrum product evolution and underlying detailed chemical reactions of cellulose pyrolysis have been revealed. A reaction scheme of cellulose pyrolysis with detailed reaction pathways for major pyrolyzates has been obtained that is not readily accessible by experiments. The simulated evolution tendencies of the major pyrolysis products (glycolaldehyde, levoglucosan and water) with temperature at 500-1400 K agrees well with the Py-GC/MS experimental observations at 673-1073 K. Compared with the large temperature discrepancy imposed by the widely used simulation strategy of artificially increased temperature in ReaxFF MD, the very close temperature range between the simulations and experiments suggests that cellulose is a good model system to validate the ReaxFF force field in predicting the behavior and chemistry events in pyrolysis of complex molecular systems. The computational approach of large model simulation facilitated by efficient computation of GMD-Reax, and chemical reaction analysis capability of VARxMD can shed new light on the detailed chemical mechanisms of pyrolysis for cellulose and other biomass. (C) 2016 Elsevier Ltd. All rights reserved.
关键词	Reaxff Md Cellulose Pyrolysis Reaction Generation Product Distribution Reaction Pathway
文章类型	Article
WOS标题词	Science & Technology ; Technology
DOI	10.1016/j.fuel.2016.03.008
收录类别	SCI
语种	英语
关键词[WOS]	DENSITY-FUNCTIONAL THEORY ; FORCE-FIELD ; RAPID PYROLYSIS ; PY-GC/MS ; SIMULATIONS ; MODEL ; CHEMISTRY ; KINETICS ; OXIDATION ; DECOMPOSITION
WOS研究方向	Energy & Fuels ; Engineering
WOS类目	Energy & Fuels ; Engineering, Chemical
项目资助者	National Natural Science Foundation of China(21373227 ; China's State Key Laboratory of Multiphase Complex Systems(MPCS-2012-A-05) ; 21073195 ; 91434105)
WOS记录号	WOS:000373061800015
引用统计	被引频次：27[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.ipe.ac.cn/handle/122111/20971
专题	多相复杂系统国家重点实验室
作者单位	Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, 1 Zhongguancun North Second St, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Zheng, Mo,Wang, Ze,Li, Xiaoxia,et al. Initial reaction mechanisms of cellulose pyrolysis revealed by ReaxFF molecular dynamics[J]. FUEL,2016,177(AUG):130-141.
APA	Zheng, Mo,Wang, Ze,Li, Xiaoxia,Qiao, Xianjie,Song, Wenli,&Guo, Li.(2016).Initial reaction mechanisms of cellulose pyrolysis revealed by ReaxFF molecular dynamics.FUEL,177(AUG),130-141.
MLA	Zheng, Mo,et al."Initial reaction mechanisms of cellulose pyrolysis revealed by ReaxFF molecular dynamics".FUEL 177.AUG(2016):130-141.

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