Visible light-driven oxidation of non-native substrate by laccase attached on Ru-based metal-organic frameworks

IF 6.9 Q1 Environmental Science

Journal of environmental sciences Pub Date : 2024-03-01 Epub Date: 2023-03-04 DOI:10.1016/j.jes.2023.02.047

Wenguang Huang , Wentao Zhang , Guantongyi Chen , Yun Chen , Jun Ma , Dawei Huang , Qinzheng Zhao , Bingdang Wu

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引用次数: 2

Abstract

Light-induced electron transfer can broaden the substrate range of metalloenzyme. However, the efficiency of photo-enzyme coupling is limited by the poor combination of photosensitizer or photocatalyst with enzyme. Herein, we prepared the nano-photocatalyst MIL-125-NH₂@Ru(bpy) by in site embedding ruthenium pyridine-diimine complex [Ru(bpy)₃^]2+ into metal organic frameworks MIL-125-NH₂ and associated it with multicopper oxidase (MCO) laccase. Compared to [Ru(bpy)₃]²⁺, the coupling efficiency of MIL-125-NH₂@Ru(bpy)₃ for enzymatic oxygen reduction increased by 35.7%. A series of characterizations confirmed that the amino group of laccase formed chemical bonds with the surface defects or hydrophobic groups of MIL-125-NH₂@Ru(bpy)₃. Consequently, the tight binding accelerated the quenching process and electron transfer between laccase and the immobilized ruthenium pyridine-diimine complex. This work would open an avenue for the synthesis of MOFs photocatalyst towards photo-enzyme coupling.

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附着在ru基金属有机框架上的漆酶在可见光驱动下氧化非天然底物

光诱导的电子转移可以拓宽金属酶的底物范围。然而，光敏剂或光催化剂与酶的不良结合限制了光-酶偶联的效率。在此，我们制备了纳米光催化剂MIL-125-NH2@Ru通过将钌-吡啶二亚胺络合物[Ru（bpy）3]2+原位包埋到金属有机框架MIL-125-NH2中并将其与多铜氧化酶（MCO）漆酶结合。与[Ru（bpy）3]2+相比MIL-125-NH2@Ru（bpy）3的酶促氧还原活性提高了35.7%。一系列表征证实，漆酶的氨基与漆酶的表面缺陷或疏水基团形成化学键MIL-125-NH2@Ru（bpy）3.因此，紧密结合加速了漆酶和固定化的钌-吡啶-二亚胺络合物之间的猝灭过程和电子转移。这项工作将为MOFs光催化剂的合成开辟一条光酶偶联的途径。

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来源期刊

Journal of environmental sciences Environmental Science (General)

CiteScore

12.80

自引率

0.00%

发文量

审稿时长

17 days

期刊介绍： Journal of Environmental Sciences is an international peer-reviewed journal established in 1989. It is sponsored by the Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, and it is jointly published by Elsevier and Science Press. It aims to foster interdisciplinary communication and promote understanding of significant environmental issues. The journal seeks to publish significant and novel research on the fate and behaviour of emerging contaminants, human impact on the environment, human exposure to environmental contaminants and their health effects, and environmental remediation and management. Original research articles, critical reviews, highlights, and perspectives of high quality are published both in print and online.