Burke Rebeckah, Bren Kara L, Krauss Todd D
Department of Chemistry, University of Rochester, Rochester, New York 14627, USA.
J Chem Phys. 2021 Jan 21;154(3):030901. doi: 10.1063/5.0032172.
Colloidal semiconducting nanocrystals (NCs) are powerful elements of a photocatalytic system useful for enabling a variety of chemical transformations owing to their strong light-absorbing properties and high degree of size-, shape-, and composition-tunability. Key to their utility is our understanding of the photoinduced charge transfer processes required for these photochemical transformations. This Perspective will focus on the implementation of semiconductor NCs for photochemical fuel formation. Three general system designs for photocatalytic proton reduction using semiconductor NCs will be reviewed: metal-semiconductor heterostructures, NC photosensitizers with molecular catalysts, and hydrogenase-based systems. Other relevant reactions toward solar fuel targets, such as CO and N reductions with NCs, will also be highlighted. Illustrating the versatile roles that NCs can play in light-driven chemical reactions, advances made toward NC-catalyzed organic transformations will be discussed. Finally, we will share a few concluding thoughts and perspectives on the future of the field, with a focus on goals toward improving and implementing NC-based technologies for solar fuel development.
胶体半导体纳米晶体（NCs）是光催化系统的重要组成部分，由于其强大的光吸收性能以及高度的尺寸、形状和组成可调性，可用于实现多种化学转化。其效用的关键在于我们对这些光化学转化所需的光致电荷转移过程的理解。本综述将聚焦于半导体NCs在光化学燃料形成方面的应用。将回顾三种使用半导体NCs进行光催化质子还原的一般系统设计：金属 - 半导体异质结构、具有分子催化剂的NC光敏剂以及基于氢化酶的系统。还将重点介绍其他与太阳能燃料目标相关的反应，例如使用NCs进行的CO和N还原反应。为说明NCs在光驱动化学反应中可以发挥的多种作用，将讨论在NC催化的有机转化方面取得的进展。最后，我们将分享一些关于该领域未来的总结性思考和观点，重点是改进和实施基于NCs的太阳能燃料开发技术目标。
