CAS OpenIR
Concentration fluctuation due to reaction-diffusion coupling near an isolated active site on catalyst surfaces
Li, Yanping1,2,3; Zhao, Mingcan2,4; Li, Chengxiang2,5; Ge, Wei2,3,4
2019-10-01
Source PublicationCHEMICAL ENGINEERING JOURNAL
ISSN1385-8947
Volume373Pages:744-754
AbstractThe coupling of reaction and diffusion processes on catalytic surfaces leads to spatio-temporal heterogeneity in concentration. Understanding of this phenomenon is very important for better catalyst design and higher reaction efficiency. In this work, molecular dynamics simulations combing hard-sphere and pseudo-particle modeling are carried out to investigate the coupling between the reaction and diffusion near an isolated active site in 2D pores with a simple reaction model. The local fluctuation in concentration caused mainly by the reaction-diffusion coupling is observed and proved to be non-stochastic using quantitative parameters proposed in this work. The reaction factor R and diffusion factor D are defined to quantitatively characterize the reaction and diffusion performance, respectively. The results show that the fluctuation is weak when the process is reaction-limited (e. g., R/D is very small) or diffusion-limited (e. g., R/D is very large). When R/D is within a certain range, the strongest fluctuation appears. Besides, the diffusion factor D has a relatively larger effect on the fluctuation than the reaction factor R. Similarly, it is found that the highest overall yield of the pore is obtained only when R/D is within a specific range due to the reaction and diffusion coupling. It is also found that the local fluctuation must be considered when studying complex reaction processes with different reaction orders. The results are expected to be helpful for understanding the reaction and diffusion coupling and the complex reaction kinetics at the atomic scale, as well as for the design of catalysts and the improvement of catalytic efficiency.
KeywordMolecular dynamics simulation Reaction-diffusion coupling Isolated active sites Concentration fluctuation Hard sphere model
DOI10.1016/j.cej.2019.05.052
Language英语
WOS KeywordMOLECULAR-DYNAMICS ; PHASE-TRANSITIONS ; CHEMICAL DIFFUSION ; DIRECT CONVERSION ; SIMULATION ; COKE ; ZEOLITE ; MECHANISM ; H-ZSM-5 ; MODEL
Funding Project"Transformational Technologies for Clean Energy and Demonstration" ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDA21030700] ; Key Research Program of Frontier Sciences, Chinese Academy of Sciences[QYZDJ-SSW-JSC029] ; Science Challenge Project[TZ2016001] ; SINOPEC-CAS[418028]
WOS Research AreaEngineering
WOS SubjectEngineering, Environmental ; Engineering, Chemical
Funding Organization"Transformational Technologies for Clean Energy and Demonstration" ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Key Research Program of Frontier Sciences, Chinese Academy of Sciences ; Science Challenge Project ; SINOPEC-CAS
WOS IDWOS:000471682900071
PublisherELSEVIER SCIENCE SA
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/30077
Collection中国科学院过程工程研究所
Corresponding AuthorLi, Chengxiang; Ge, Wei
Affiliation1.Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
3.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
4.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
5.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
Recommended Citation
GB/T 7714
Li, Yanping,Zhao, Mingcan,Li, Chengxiang,et al. Concentration fluctuation due to reaction-diffusion coupling near an isolated active site on catalyst surfaces[J]. CHEMICAL ENGINEERING JOURNAL,2019,373:744-754.
APA Li, Yanping,Zhao, Mingcan,Li, Chengxiang,&Ge, Wei.(2019).Concentration fluctuation due to reaction-diffusion coupling near an isolated active site on catalyst surfaces.CHEMICAL ENGINEERING JOURNAL,373,744-754.
MLA Li, Yanping,et al."Concentration fluctuation due to reaction-diffusion coupling near an isolated active site on catalyst surfaces".CHEMICAL ENGINEERING JOURNAL 373(2019):744-754.
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