Characterization and manipulation of the photosystem Ⅱ-semiconductor interfacial molecular interactions in solar-to-chemical energy conversion

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

来源：Journal of Energy Chemistry, 2022, 70(07): 437-443.

Semi-artificial photosynthesis interfacing catalytic protein machinery with synthetic photocatalysts exhibits 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 interrogated by lysine reactivity profiling mass spectrometry. We demonstrate the semiconductor surface biocompatibility is essential to the PSII self-assembly with uniform orientation and electroactive structure.Highly directional localization of PSII onto more hydrophilic Ru/Sr Ti O3:Rh surface exhibits less disturbance on PSII structure and electron transfer chain, beneficial to the high water splitting activity.Further, rational modification of hydrophobic Ru2S3/Cd S 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.

• 单位
  分子反应动力学国家重点实验室; 催化基础国家重点实验室; 中国科学院; 中国科学院大学