Enhanced Interfacial Electron Transfer in Photocatalyst‐Natural Enzyme Coupled Artificial Photosynthesis System: Tuning Strategies and Molecular Simulations

Author:

Lou Xiaoxuan1,Zhang Chen1ORCID,Xu Zhiyong2,Ge Shengbo3,Zhou Jian2ORCID,Qin Deyu1,Qin Fanzhi1,Zhang Xin4,Guo Zhanhu5,Wang Chongchen6

Affiliation:

1. College of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education) Hunan University Changsha 410082 P. R. China

2. School of Chemistry and Chemical Engineering and Guangdong Provincial Key Lab for Green Chemical Product Technology South China University of Technology Guangzhou 510640 P. R. China

3. Co‐Innovation Center of Efficient Processing and Utilization of Forestry Resources College of Materials Science and Engineering Nanjing Forestry University Nanjing 210037 P. R. China

4. Physical & Computational Science Directorate Pacific Northwest National Laboratory Washington 99354 USA

5. Department of Mechanical and Construction Engineering Northumbria University Newcastle Upon Tyne NE1 8ST UK

6. School of Environmental and Energy Engineering and Beijing Key Laboratory of Functional Materials for Building Structure and Environment Remediation Beijing University of Civil Engineering and Architecture Beijing 100044 China

Abstract

AbstractLaccase is capable of catalyzing a vast array of reactions, but its low redox potential limits its potential applications. The use of photocatalytic materials offers a solution to this problem by converting absorbed visible light into electrons to facilitate enzyme catalysis. Herein, MIL‐53(Fe) and NH2‐MIL‐53(Fe) serve as both light absorbers and enzyme immobilization carriers, and laccase is employed for solar‐driven chemical conversion. Electron spin resonance spectroscopy results confirm that visible light irradiation causes rapid transfer of photogenerated electrons from MOF excitation to T1 Cu(II) of laccase, significantly increasing the degradation rate constant of tetracycline (TC) from 0.0062 to 0.0127 min−1. Conversely, there is only minimal or no electron transfer between MOF and laccase in the physical mixture state. Theoretical calculations demonstrate that the immobilization of laccase's active site and its covalent binding to the metal‐organic framework surface augment the coupled system's activity, reducing the active site accessible from 27.8 to 18.1 Å. The constructed photo‐enzyme coupled system successfully combines enzyme catalysis’ selectivity with photocatalysis's high reactivity, providing a promising solution for solar energy use.

Funder

National Natural Science Foundation of China

Fundamental Research Funds for the Central Universities

Natural Science Foundation of Hunan Province

Publisher

Wiley

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