Concentration fluctuation due to reaction-diffusion coupling near an isolated active site on catalyst surfaces
文献类型：期刊论文
| 作者 | Li, Yanping1,2,3; Zhao, Mingcan2,4; Li, Chengxiang2,5; Ge, Wei2,3,4 |
| 刊名 | CHEMICAL ENGINEERING JOURNAL
 |
| 出版日期 | 2019-10-01 |
| 卷号 | 373页码:744-754 |
| ISSN号 | 1385-8947 |
| 关键词 | Molecular dynamics simulation Reaction-diffusion coupling Isolated active sites Concentration fluctuation Hard sphere model |
| DOI | 10.1016/j.cej.2019.05.052 |
| 英文摘要 | The 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. |
| WOS关键词 | MOLECULAR-DYNAMICS ; PHASE-TRANSITIONS ; CHEMICAL DIFFUSION ; DIRECT CONVERSION ; SIMULATION ; COKE ; ZEOLITE ; MECHANISM ; H-ZSM-5 ; MODEL |
| 资助项目 | "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研究方向 | Engineering |
| 语种 | 英语 |
| 出版者 | ELSEVIER SCIENCE SA |
| WOS记录号 | WOS:000471682900071 |
| 资助机构 | "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 |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/30076]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Li, Chengxiang; Ge, Wei |
| 作者单位 | 1.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 |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：过程工程研究所
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