Dynamic Intermediate Profiles of Zeolite Catalyzed Methanol to Olefins Revealed by Reactive Molecular Dynamics

doi:10.1021/acs.energyfuels.0c03796

	Dynamic Intermediate Profiles of Zeolite Catalyzed Methanol to Olefins Revealed by Reactive Molecular Dynamics
	Zheng, Mo 1,2; Li, Xiaoxia 1,2,3; Guo, Li 1,2,3; Ge, Wei 1,2,3
刊名	ENERGY & FUELS
	2021-01-21
卷号	35 期号:2 页码:1677-1690
ISSN号	0887-0624
DOI	10.1021/acs.energyfuels.0c03796
英文摘要	Taking the unique advantage of large-scale ReaxFF MD simulation in unravelling varied reaction pathways within one simulation, the process of methanol-to-olefin (MTO) was investigated by the combination of high-performance computing and cheminformatics-based reaction analysis. The initial stage model and the indirect pathway model for MTO were constructed to get a more complete scenario of the whole catalyzed process. The obtained dynamic profiles of dominant products, intermediates, and detailed reactions indicate that the MTO processes catalyzed over ZSM-5 with different acidic properties exhibit similar proceeding stages but with significant different pathways. The MTO process catalyzed by hydrated ZSM-5 with Al enhances the methane-formaldehyde route, H and CH3 transfer reactions, and oxidation reactions of surface methoxy species during the direct pathway, leading to CO2 production and CH2O consumption, which is barely taking place at the model catalyzed by zeolite without Al. Semiquantitative reaction networks with conversion ratios for C2H4 and C3H6 generation revealed that the MTO process is a product of multiple pathways with dozens of intermediates. The rich information, especially the comprehensive reaction network obtained from ReaxFF MD simulations would complement the experimental results and those of other theoretical research and be helpful for further development of highly efficient MTO processes.
资助项目	Strategic Priority Research Program of the Chinese Academy of Sciences[XDA21030700] ; Youth Innovation Promotion Association CAS
WOS研究方向	Energy & Fuels ; Engineering
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000613197300063
资助机构	Strategic Priority Research Program of the Chinese Academy of Sciences ; Youth Innovation Promotion Association CAS
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/43658]
专题	中国科学院过程工程研究所
通讯作者	Zheng, Mo; Li, Xiaoxia
作者单位	1.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China 2.Chinese Acad Sci, Innovat Acad Green Manufacture, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Zheng, Mo,Li, Xiaoxia,Guo, Li,et al. Dynamic Intermediate Profiles of Zeolite Catalyzed Methanol to Olefins Revealed by Reactive Molecular Dynamics[J]. ENERGY & FUELS,2021,35(2):1677-1690.
APA	Zheng, Mo,Li, Xiaoxia,Guo, Li,&Ge, Wei.(2021).Dynamic Intermediate Profiles of Zeolite Catalyzed Methanol to Olefins Revealed by Reactive Molecular Dynamics.ENERGY & FUELS,35(2),1677-1690.
MLA	Zheng, Mo,et al."Dynamic Intermediate Profiles of Zeolite Catalyzed Methanol to Olefins Revealed by Reactive Molecular Dynamics".ENERGY & FUELS 35.2(2021):1677-1690.