Institute of Chemical Research of Catalonia (ICIQ), Barcelona Institute of Science and Technology (BIST), Avinguda Països Catalans 16, 43007 Tarragona, Spain.
Chem Soc Rev. 2017 Oct 16;46(20):6088-6098. doi: 10.1039/c7cs00248c.
Energy has been a central subject for human development from Homo erectus to date. The massive use of fossil fuels during the last 50 years has generated a large CO concentration in the atmosphere that has led to the so-called global warming. It is very urgent to come up with C-neutral energy schemes to be able to preserve Planet Earth for future generations to come and still preserve our modern societies' life style. One of the potential solutions is water splitting with sunlight (hν-WS) that is also associated with "artificial photosynthesis", since its working mode consists of light capture followed by water oxidation and proton reduction processes. The hydrogen fuel generated in this way is named as "solar fuel". For this set of reactions, the catalytic oxidation of water to dioxygen is one of the crucial processes that need to be understood and mastered in order to build up potential devices based on hν-WS. This tutorial describes the different important aspects that need to be considered to come up with efficient and oxidatively robust molecular water oxidation catalysts (Mol-WOCs). It is based on our own previous work and completed with essential contributions from other active groups in the field. We mainly aim at describing how the ligands can influence the properties of the Mol-WOCs and showing a few key examples that overall provide a complete view of today's understanding in this field.
能源一直是人类发展的核心主题,从直立人至今都是如此。在过去 50 年中,大量使用化石燃料导致大气中 CO 浓度大量增加,引发了所谓的全球变暖。非常有必要提出碳中和能源方案,以便为子孙后代保护地球,并保持我们现代社会的生活方式。潜在的解决方案之一是利用阳光(hν-WS)进行水分解,这也与“人工光合作用”有关,因为其工作模式包括光捕获,随后是水氧化和质子还原过程。这种方式产生的氢气燃料被称为“太阳能燃料”。对于这一系列反应,催化氧化水生成氧气是需要理解和掌握的关键过程之一,以便基于 hν-WS 构建潜在的设备。本教程介绍了为了设计出高效且氧化稳定的分子水氧化催化剂(Mol-WOCs)需要考虑的不同重要方面。它基于我们自己的先前工作,并结合了该领域其他活跃小组的重要贡献。我们主要旨在描述配体如何影响 Mol-WOCs 的性质,并展示一些关键示例,总体上提供了对该领域当前理解的全面了解。