Filipov Yaroslav, Zakharchenko Andrey, Minko Sergiy, Katz Evgeny
Department of Chemistry and Biomolecular Science, Clarkson University, Potsdam, NY 13699, USA.
Nanostructured Materials Lab, University of Georgia, Athens, GA 30602, USA.
Chemphyschem. 2018 Nov 19;19(22):3035-3043. doi: 10.1002/cphc.201800851. Epub 2018 Oct 19.
Magnetic nanoparticles (MNPs) functionalized with various enzymes (amyloglucosidase, glucose oxidase and horseradish peroxidase) were used to perform biocatalytic cascades in two different states, solute suspension or aggregated, produced in the absence or presence of an external magnetic field. The biocatalytic reactions proceeded through bulk solution diffusion of intermediate substrates or substrate channeling, when the systems were dispersed or aggregated, respectively. The both pathways have shown very similar kinetics, unless the intermediate substrate was consumed by an additional biocatalytic process called "filter" for brevity. In the presence of the "filter" process, the diffusional process in the bulk solution was significantly inhibited, while the process based on the substrate channeling was still active. The systems were switched reversibly between the inhibited dispersed state and the active aggregated state by removing and applying the external magnetic field, respectively. The signal-controlled biocatalytic cascades were considered as Boolean logic circuits with the inputs consisting of biomolecules and the magnetic field on-off.
用各种酶(糖化酶、葡萄糖氧化酶和辣根过氧化物酶)功能化的磁性纳米颗粒(MNPs)用于在两种不同状态下进行生物催化级联反应,这两种状态分别是在不存在或存在外部磁场的情况下产生的溶质悬浮液或聚集体。当系统分别处于分散或聚集状态时,生物催化反应通过中间底物的本体溶液扩散或底物通道化进行。除非中间底物被一个简称为“过滤器”的额外生物催化过程消耗,否则这两种途径都显示出非常相似的动力学。在存在“过滤器”过程的情况下,本体溶液中的扩散过程受到显著抑制,而基于底物通道化的过程仍然活跃。通过分别去除和施加外部磁场,系统在受抑制的分散状态和活跃的聚集状态之间可逆地切换。信号控制的生物催化级联反应被视为布尔逻辑电路,其输入由生物分子和磁场的开/关组成。