Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, Republic of Korea.
Department of Chemistry, School of Natural Science, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, Republic of Korea.
ACS Appl Mater Interfaces. 2017 Nov 22;9(46):40151-40161. doi: 10.1021/acsami.7b09416. Epub 2017 Nov 13.
Artificial photosynthesis is considered one of the most promising solutions to modern energy and environmental crises. Considering that it is enabled by multiple components through a series of photoelectrochemical processes, the key to successful development of a photosynthetic device depends not only on the development of novel individual components but also on the rational design of an integrated photosynthetic device assembled from them. However, most studies have been dedicated to the development of individual components due to the lack of a general and simple method for the construction of the integrated device. In the present study, we report a versatile and simple method to prepare an efficient and stable photoelectrochemical device via controlled assembly and integration of functional components on the nanoscale using the layer-by-layer (LbL) assembly technique. As a proof of concept, we could successfully build a photoanode for solar water oxidation by depositing a thin film of diverse cationic polyelectrolytes and anionic polyoxometalate (molecular metal oxide) water oxidation catalysts on the surface of various photoelectrode materials (e.g., FeO, BiVO, and TiO). It was found that the performance of photoanodes was significantly improved after the deposition in terms of stability as well as photocatalytic properties, regardless of types of photoelectrodes and polyelectrolytes employed. Considering the simplicity and versatile nature of LbL assembly techniques, our approach can contribute to the realization of artificial photosynthesis by enabling the design of novel photosynthetic devices.
人工光合作用被认为是解决现代能源和环境危机最有前途的方法之一。考虑到它是通过一系列光电化学过程由多个组件实现的，成功开发光合作用装置的关键不仅取决于新型单个组件的开发，还取决于从它们组装的集成光合作用装置的合理设计。然而，由于缺乏构建集成设备的通用和简单方法，大多数研究都致力于单个组件的开发。在本研究中，我们报告了一种通用且简单的方法，通过使用层层（LbL）组装技术在纳米尺度上控制组装和集成功能组件，来制备高效稳定的光电化学器件。作为概念验证，我们可以通过在各种光电电极材料（例如 FeO、BiVO 和 TiO）表面上沉积各种阳离子聚电解质和阴离子多金属氧酸盐（分子金属氧化物）水氧化催化剂，成功构建用于太阳能水氧化的光阳极。研究发现，无论使用哪种光电电极和聚电解质，沉积后光阳极的性能在稳定性和光催化性能方面都得到了显著提高。考虑到 LbL 组装技术的简单性和通用性，我们的方法可以通过设计新型光合作用装置为人工光合作用的实现做出贡献。
