Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Chem Soc Rev. 2015 May 21;44(10):2893-939. doi: 10.1039/c5cs00064e. Epub 2015 Apr 23.
Charge kinetics is highly critical in determining the quantum efficiency of solar-to-chemical conversion in photocatalysis, and this includes, but is not limited to, the separation of photoexcited electron-hole pairs, utilization of plasmonic hot carriers and delivery of photo-induced charges to reaction sites, as well as activation of reactants by energized charges. In this review, we highlight the recent progress on probing and steering charge kinetics toward designing highly efficient photocatalysts and elucidate the fundamentals behind the combinative use of controlled synthesis, characterization techniques (with a focus on spectroscopic characterizations) and theoretical simulations in photocatalysis studies. We first introduce the principles of various processes associated with charge kinetics that account for or may affect photocatalysis, from which a set of parameters that are critical to photocatalyst design can be summarized. We then outline the design rules for photocatalyst structures and their corresponding synthetic approaches. The implementation of characterization techniques and theoretical simulations in different steps of photocatalysis, together with the associated fundamentals and working mechanisms, are also presented. Finally, we discuss the challenges and opportunities for photocatalysis research at this unique intersection as well as the potential impact on other research fields.
电荷动力学在确定光催化中的太阳能到化学转化的量子效率方面至关重要，这包括但不限于光激发电子-空穴对的分离、等离子体热载流子的利用以及光致电荷向反应位点的传递，以及通过受激电荷激活反应物。在这篇综述中，我们强调了在探测和引导电荷动力学方面的最新进展，以设计高效的光催化剂，并阐明了在光催化研究中结合使用控制合成、表征技术（重点是光谱表征）和理论模拟的基本原理。我们首先介绍了与电荷动力学相关的各种过程的原理，这些过程解释或可能影响光催化，从中可以总结出一组对光催化剂设计至关重要的参数。然后，我们概述了光催化剂结构及其相应合成方法的设计规则。还介绍了在光催化的不同步骤中实施的表征技术和理论模拟，以及相关的基本原理和工作机制。最后，我们讨论了在这个独特的交叉点进行光催化研究的挑战和机遇，以及对其他研究领域的潜在影响。
