Ouyang Yu, Zhang Pu, Willner Itamar
The Institute of Chemistry, Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
Sci Adv. 2022 May 6;8(18):eabn3534. doi: 10.1126/sciadv.abn3534.
Living systems consist of complex transient cellular networks guiding structural, catalytic, and switchable functions driven by auxiliary triggers, such as chemical or light energy inputs. We introduce two different transient, dissipative, biocatalytic cascades, the coupled glucose oxidase (GOx)/horseradish peroxidase (HRP) glucose-driven oxidation of 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) to the radical anion (ABTS) and the lactate dehydrogenase (LDH)/nicotinamide adenine dinucleotide (NAD) lactate-driven reduction of NAD to NADH. The transient biocatalytic systems are driven by nucleic acid reaction modules using a nucleic acid fuel strand L' and a nicking enzyme, Nt.BbvCI, as fuel-degrading catalyst, leading to the dynamic spatiotemporal transient formation of structurally proximate biocatalysts activating the biocatalytic cascades and transient coupled processes, including the generation of chemiluminescence and the synthesis of alanine. Subjecting the mixture of biocatalysts to selective inhibitors allows the gated transient operation of the biocatalysts. The kinetics of transient biocatalytic cascades are accompanied by kinetic models and computational simulations.
生命系统由复杂的瞬态细胞网络组成，这些网络引导着由辅助触发器驱动的结构、催化和可切换功能，辅助触发器如化学或光能输入。我们介绍了两种不同的瞬态、耗散性生物催化级联反应，即耦合葡萄糖氧化酶（GOx）/辣根过氧化物酶（HRP）将2,2'-联氮双（3-乙基苯并噻唑啉-6-磺酸）（ABTS）葡萄糖驱动氧化为自由基阴离子（ABTS），以及乳酸脱氢酶（LDH）/烟酰胺腺嘌呤二核苷酸（NAD）将乳酸驱动还原为NADH。瞬态生物催化系统由核酸反应模块驱动，使用核酸燃料链L'和切口酶Nt.BbvCI作为燃料降解催化剂，导致结构上接近的生物催化剂动态时空瞬态形成，激活生物催化级联反应和瞬态耦合过程，包括化学发光的产生和丙氨酸的合成。将生物催化剂混合物置于选择性抑制剂中可实现生物催化剂的门控瞬态操作。瞬态生物催化级联反应的动力学伴随着动力学模型和计算模拟。
