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Species Abundance and Reaction Off-Rate Regulate Product Formation in Reactions Accelerated Using Isotachophoresis
Analytical Chemistry ( IF 7.4 ) Pub Date : 2021-09-07 , DOI: 10.1021/acs.analchem.1c01805
Qi Jiang 1, 2 , Ashwin Ramachandran 3 , Juan G Santiago 2
Affiliation  

We present a model for second-order and pseudo-first-order reversible chemical reactions accelerated using peak-mode isotachophoresis (ITP). In such systems, ITP preconcentrates and co-locates the reactants between the leading and trailing electrolyte zones, and this significantly accelerates chemical reactions. Our model quantifies the effects of reaction rate constants and species abundance on product formation rate. We identify two key non-dimensional parameters, which are specific groupings of reaction rate constants, species concentrations, and influx rates. We then use a regular perturbation to study the effects of reverse reaction rate and relative species abundance (and relative rates of species accumulation) on production rate. We also use this perturbation method to derive an analytical expression for the quasi-steady-state production rate achievable by ITP. Our analytical models and numerical solutions are generally applicable to a wide range of systems, which use ITP to enhance reactions. The model is also an interesting case study of the complex coupling of electric field-driven species transport and reaction kinetics.

中文翻译:

物种丰度和反应解离率调节使用等速电泳加速反应中的产物形成

我们提出了一个使用峰值模式等速电泳 (ITP) 加速的二阶和伪一阶可逆化学反应模型。在这样的系统中,ITP 将反应物预浓缩并放置在前导和后导电解质区之间,这显着加速了化学反应。我们的模型量化了反应速率常数和物种丰度对产物形成速率的影响。我们确定了两个关键的无量纲参数,它们是反应速率常数、物种浓度和流入速率的特定分组。然后,我们使用规则扰动来研究逆反应速率和相对物种丰度(以及物种积累的相对速率)对生产率的影响。我们还使用这种扰动方法推导出 ITP 可实现的准稳态生产率的解析表达式。我们的分析模型和数值解决方案通常适用于使用 ITP 来增强反应的各种系统。该模型也是电场驱动的物质传输和反应动力学复杂耦合的一个有趣的案例研究。
更新日期:2021-09-21
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