School of Chemistry and Materials Science , University of Science and Technology of China , Jinzhai Road 96 , Hefei 230026 , China.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Zhongshan Road 457 , Dalian 116023 , China.
J Am Chem Soc. 2018 Mar 7;140(9):3250-3256. doi: 10.1021/jacs.7b10662. Epub 2018 Jan 27.
It has been anticipated that learning from nature photosynthesis is a rational and effective way to develop artificial photosynthesis system, but it is still a great challenge. Here, we assembled a photoelectrocatalytic system by mimicking the functions of photosystem II (PSII) with BiVO semiconductor as a light harvester protected by a layered double hydroxide (NiFeLDH) as a hole storage layer, a partially oxidized graphene (pGO) as biomimetic tyrosine for charge transfer, and molecular Co cubane as oxygen evolution complex. The integrated system exhibited an unprecedentedly low onset potential (0.17 V) and a high photocurrent (4.45 mA cm), with a 2.0% solar to hydrogen efficiency. Spectroscopic studies revealed that this photoelectrocatalytic system exhibited superiority in charge separation and transfer by benefiting from mimicking the key functions of PSII. The success of the biomimetic strategy opened up new ways for the rational design and assembly of artificial photosynthesis systems for efficient solar-to-fuel conversion.
人们一直期望通过模仿光合作用来开发人工光合作用系统，但这仍然是一个巨大的挑战。在这里，我们通过使用 BiVO 半导体作为光收集器，层状双氢氧化物（NiFeLDH）作为空穴存储层，部分氧化石墨烯（pGO）作为仿生酪氨酸用于电荷转移，以及分子 Co 立方烷作为氧析出复合物，模拟光合作用系统 II（PSII）的功能来组装光电催化系统。该集成系统表现出前所未有的低起始电位（0.17 V）和高光电流（4.45 mA cm），太阳能到氢气的效率为 2.0%。光谱研究表明，通过模拟 PSII 的关键功能，该光电催化系统在电荷分离和转移方面表现出优越性。仿生策略的成功为高效太阳能到燃料转化的人工光合作用系统的合理设计和组装开辟了新途径。
