Semi-artificial photosynthesis interfacing catalytic protein machinery with synthetic photocatalysts exhi-bits great potential in solar-to-chemical energy conversion.However,characterizing and manipulating the molecular integration structure at the biotic-abiotic interface remain a challenging task.Herein,the biointerface molecular integration details of photosystem Ⅱ(PSⅡ)-semiconductor hybrids,including the PSⅡ orientation,interfacial microdomains,and overall structure modulation,are systematically inter-rogated by lysine reactivity profiling mass spectrometry.We demonstrate the semiconductor surface bio-compatibility is essential to the PSⅡ self-assembly with uniform orientation and electroactive structure.Highly directional localization of PSⅡ onto more hydrophilic Ru/SrTiO3:Rh surface exhibits less distur-bance on PSⅡ structure and electron transfer chain,beneficial to the high water splitting activity.Further,rational modification of hydrophobic Ru2S3/CdS surface with biocompatible protamine can improve the hybrid O2-evolving activity 83.3％.Our results provide the mechanistic understanding to the structure-activity relationship of PSⅡ-semiconductor hybrids and contribute to their rational design in the future.

Min He;Wangyin Wang;Zheyi Liu;Wenxiang Zhang;Jinan Li;Wenming Tian;Ye Zhou;Yan Jin;Fangjun Wang;Can Li

CAS Key Laboratory of Separation Sciences for Analytical Chemistry,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;University of Chinese Academy of Sciences,Beijing 100049,China;State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian National Laboratory for Clean Energy,Dalian 116023,Liaoning,China;State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China

能源化学

[1]Min He;Wangyin Wang;Zheyi Liu;Wenxiang Zhang;Jinan Li;Wenming Tian;Ye Zhou;Yan Jin;Fangjun Wang;Can Li-.Characterization and manipulation of the photosystem Ⅱ-semiconductor interfacial molecular interactions in solar-to-chemical energy conversion)[J].能源化学,2022(07):437-443

rogated,Ru2S3,protamine

Characterization,manipulation,photosystem,semiconductor,interfacial,molecular,interactions,solar,chemical,energy,conversion,Semi,artificial,photosynthesis,interfacing,catalytic,protein,machinery,synthetic,photocatalysts,great,potential,However,characterizing,manipulating,integration,structure,abiotic,remain,challenging,task,Herein,biointerface,details,PS,hybrids,including,orientation,microdomains,overall,modulation,are,systematically,by,lysine,reactivity,profiling,mass,spectrometry,We,demonstrate,surface,compatibility,essential,self,assembly,uniform,electroactive,Highly,directional,localization,onto,more,hydrophilic,SrTiO3,Rh,exhibits,less,distur,bance,electron,transfer,chain,beneficial,high,water,splitting,Further,rational,modification,hydrophobic,CdS,biocompatible,can,improve,O2,evolving,Our,results,provide,mechanistic,understanding,relationship,contribute,their,design,future

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