Charged Substrate and Product Together Contribute Like a Nonreactive Species to the Overall Electrostatic Steering in Diffusion-Reaction Processes

doi:10.1021/acs.jpcb.6b01393

	Charged Substrate and Product Together Contribute Like a Nonreactive Species to the Overall Electrostatic Steering in Diffusion-Reaction Processes
	Xu, Jingjie 1; Xie, Yan 2; Lu, Benzhuo2 ; Zhang, Linbo 2
	2016-08-25
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY B
ISSN	1520-6106
卷号	120 期号:33 页码:8147-8153
摘要	The Debye-Huckel limiting law is used to study the binding kinetics of substrate-enzyme system as well as to estimate the reaction rate of a electrostatically steered diffusion-controlled reaction process. It is based on a linearized Poisson-Boltzmann model and known for its accurate predictions in dilute solutions. However, the substrate and product particles are in nonequilibrium states and are possibly charged, and their contributions to the total electrostatic field cannot be. explicitly studied in the Poisson-Boltzmann model. Hence the influences of substrate and product on reaction rate coefficient were not known. In this work, we consider all the charged species, including the charged substrate, product, and mobile salt ions in a Poisson-Nernst-Planck model, and then compare the results with previous work The results indicate that both the charged substrate and product can significantly influence the reaction rate coefficient with different behaviors under different setups of computational conditions. It is interesting to find that when substrate and product are both considered, under an overall neutral boundary condition for all the bulk charged species, the,computed reaction rate kinetics recovers a similar Debye-Huckel limiting law again. This phenomenon implies that the charged product counteracts the influence of charged substrate on reaction rate coefficient. Our analysis, discloses the fact that the total charge concentration of substrate and product, though in a nonequilihrium state individually; obeys an equilibrium Boltzmann distribution, and therefore contributes as a normal charged ion species to ionic strength. This explains why the Debye-Huckel limiting law still works in a considerable range of conditions even though the effects of charged substrate and product particles are not specifically and explicitly considered in the theory.
DOI	10.1021/acs.jpcb.6b01393
语种	英语
资助项目	China NSF[91430215] ; China NSF[91530323] ; China NSF[11321061] ; China NSF[21573274] ; China NSF[91530102] ; National Center for Mathematics and Interdisciplinary Sciences (NCMIS) of Chinese Academy of Sciences (CAS) ; NCMIS of CAS
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:000382180200010
出版者	AMER CHEMICAL SOC
引用统计
文献类型	期刊论文
条目标识符	http://ir.amss.ac.cn/handle/2S8OKBNM/23350
专题	计算数学与科学工程计算研究所
通讯作者	Lu, Benzhuo
作者单位	1.Univ Sci & Technol China, Sch Math Sci, Hefei, Peoples R China 2.Chinese Acad Sci, Acad Math & Syst Sci, State Key Lab Sci & Engn Comp, Beijing, Peoples R China
推荐引用方式 GB/T 7714	Xu, Jingjie,Xie, Yan,Lu, Benzhuo,et al. Charged Substrate and Product Together Contribute Like a Nonreactive Species to the Overall Electrostatic Steering in Diffusion-Reaction Processes[J]. JOURNAL OF PHYSICAL CHEMISTRY B,2016,120(33):8147-8153.
APA	Xu, Jingjie,Xie, Yan,Lu, Benzhuo,&Zhang, Linbo.(2016).Charged Substrate and Product Together Contribute Like a Nonreactive Species to the Overall Electrostatic Steering in Diffusion-Reaction Processes.JOURNAL OF PHYSICAL CHEMISTRY B,120(33),8147-8153.
MLA	Xu, Jingjie,et al."Charged Substrate and Product Together Contribute Like a Nonreactive Species to the Overall Electrostatic Steering in Diffusion-Reaction Processes".JOURNAL OF PHYSICAL CHEMISTRY B 120.33(2016):8147-8153.