Self-Assembled Protein Hybrid Nanofibrils for Photosynthetic Hydrogen Evolution  

作　　者：Weijian Chen Xiantao Hu Andi Hu Luyang Ji Yiming Huang Hao Heng Fude Feng Shu Wang 

机构地区：[1]Department of Polymer Science and Engineering,School of Chemistry and Chemical Engineering,Nanjing University,Jiangsu,Nanjing 210023 [2]Beijing National Laboratory for Molecular Sciences,Key Laboratory of Organic Solids,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190

出　　处：《CCS Chemistry》2024年第3期812-823,共12页中国化学会会刊（英文）

基　　金：the National Natural Science Foundation of China(grant nos.22077065,22021002,and 22277054);the National Key R&D Program of China(grant no.2018YFE0200700);the China Postdoctoral Science Foundation(grant no.2021M703264);the Beijing National Laboratory for Molecular Sciences for financial support.

摘　　要：In artificial photosynthesis systems,synthetic diiron complexes are popular[FeFe]-hydrogenase mimics,which are attractive for the fabrication of photocatalyst-protein hybrid structures to amplify hydrogen(H2)generation capability.However,constructing a highly bionic and efficient catalytic hybrid system is a major challenge.Notably,we designed an ideal hybrid nanofibrils system that incorporates the crucial components:(1)a[FeFe]-H2ase mimic,which has a three-arm architecture(named triFeFe)for more interaction sites and higher catalytic activity and(2)uniform hybrid nanofibrils as the biological environment in which cysteine-catalyst coordination and the hydrogen-bonding network play a vital role in both catalyst binding and hydrogen evolution reaction activity.The assembled hybrid nanofibrils achieve efficient H2 generation with a turnover number of 2.3×103,outperforming previously reported diiron catalyst-protein hybrid systems.Additionally,the hybrid nanofibrils work with photosynthetic thylakoids to produce H2,without extra photosensitizers or electron shuttle proteins,which advances the bioengineering of living systems for solar-driven biofuel production.

关 键 词：hybrid photocatalyst in situ assembly amyloid fibrils photosynthetic hydrogen evolution THYLAKOID 

分 类 号：O63[理学—高分子化学]