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Biomolecular Release from Alginate‐modified Electrode Triggered by Chemical Inputs Processed through a Biocatalytic Cascade – Integration of Biomolecular Computing and Actuation
Electroanalysis ( IF 3 ) Pub Date : 2017-12-29 , DOI: 10.1002/elan.201700810
Andrey V. Okhokhonin 1, 2 , Sergii Domanskyi 3 , Yaroslav Filipov 1, 3 , Maria Gamella 1 , Alisa N. Kozitsina 2 , Vladimir Privman 3 , Evgeny Katz 1
Affiliation  

Biocatalytic cascades involving more than one or two enzyme‐catalyzed step are inefficient inside alginate hydrogel prepared on an electrode surface. The problem originates from slow diffusion of intermediate products through the hydrogel from one enzyme to another. However, enzyme activity can be improved by surface immobilization. We demonstrate that a complex cascade of four consecutive biocatalytic reactions can be designed, with the enzymes immobilized in an LBL‐assembled polymeric layer at the alginate‐modified electrode surface. The product, hydrogen peroxide, then induces dissolution of iron‐cross‐linked alginate, which results in release process of entrapped biomolecular species, here fluorescently marked oligonucleotides, denoted F‐DNA. The enzymatic cascade can be viewed as a biocomputing network of concatenated AND gates, activated by combinations of four chemical input signals, which trigger the release of F‐DNA. The reactions, and diffusion/release processes were investigated by means of theoretical modeling. A bottleneck reaction step associated with one of the enzymes was observed. The developed system provides a model for biochemical actuation triggered by a biocomputing network of reactions.

中文翻译:

通过生物催化级联处理的化学输入触发的藻酸盐修饰电极释放生物分子–生物分子计算和驱动的集成

在电极表面制备的藻酸盐水凝胶内部,生物催化级联反应涉及一个或两个以上的酶催化步骤,效率低下。问题源于中间产物通过水凝胶从一种酶缓慢扩散到另一种酶。但是,通过表面固定可以提高酶的活性。我们证明了可以设计出四个连续的生物催化反应的复杂级联,将酶固定在藻酸盐修饰的电极表面的LBL组装的聚合物层中。过氧化氢产物然后诱导铁交联藻酸盐的溶解,从而导致被包裹的生物分子物质(此处为荧光标记的寡核苷酸,称为F‐DNA)的释放过程。酶联级联可以看作是串联AND门的生物计算网络,通过四个化学输入信号的组合激活,从而触发F‐DNA的释放。通过理论模型研究了反应和扩散/释放过程。观察到与一种酶相关的瓶颈反应步骤。开发的系统提供了由生物反应网络触发的生化驱动模型。
更新日期:2017-12-29
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