Chen Jinxing, Ma Qian, Li Minghua, Wu Weiwei, Huang Liang, Liu Ling, Fang Youxing, Dong Shaojun
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, PR China.
Nanoscale. 2020 Dec 8;12(46):23578-23585. doi: 10.1039/d0nr06605b.
Although nanozymes overcome a series of shortcomings of natural enzymes, their wide applications are hampered due to their limited varieties. In this work, we propose a coenzyme-dependent nanozyme, a synergistic composite comprising zeolitic imidazolate frameworks encapsulated with polyethylenimine (PEI) and functionalized with a flavin mononucleotide (PEI/ZIF-FMN). The flavin mononucleotide (FMN) plays the role of a prosthetic group, and the positively charged NH2 groups in PEI readily provide the binding affinity to nicotinamide adenine dinucleotide (NADH), which facilitates the electron transfer from NADH to FMN and terminal electron acceptors (such as O2) with a greatly enhanced (80 times) catalytic performance. The integrated nanoparticle-coenzyme composite works as an NADH oxidase mimic and couples with dehydrogenases for the tandem enzymatic reaction. PEI/ZIF-FMN also mediated the electron transfer from NADH to cytochrome c (Cyt c), thereby exhibiting Cyt c reductase-like activity.
尽管纳米酶克服了天然酶的一系列缺点，但其广泛应用却因其种类有限而受到阻碍。在这项工作中，我们提出了一种辅酶依赖性纳米酶，它是一种协同复合物，由包裹有聚乙烯亚胺（PEI）并经黄素单核苷酸功能化的沸石咪唑酯骨架（PEI/ZIF-FMN）组成。黄素单核苷酸（FMN）起到辅基的作用，PEI中带正电荷的NH2基团易于提供与烟酰胺腺嘌呤二核苷酸（NADH）的结合亲和力，这促进了电子从NADH转移到FMN和末端电子受体（如O2），催化性能大大增强（80倍）。这种整合的纳米颗粒-辅酶复合物作为一种NADH氧化酶模拟物，并与脱氢酶偶联进行串联酶促反应。PEI/ZIF-FMN还介导了电子从NADH转移到细胞色素c（Cyt c），从而表现出类似Cyt c还原酶的活性。
