Faculty of Agriculture, Life, and Environmental Sciences, Zhejiang University, 310058, Hangzhou, China.
Suzhou Institute for Advanced Research, University of Science and Technology of China, 215000, Suzhou, China.
Nat Commun. 2022 Dec 16;13(1):7783. doi: 10.1038/s41467-022-35502-z.
The demands for cost-effective solar fuels have triggered extensive research in artificial photosynthesis, yet the efforts in designing high-performance particulate photocatalysts are largely impeded by inefficient charge separation. Because charge separation in a particulate photocatalyst is driven by asymmetric interfacial energetics between its reduction and oxidation sites, enhancing this process demands nanoscale tuning of interfacial energetics on the prerequisite of not impairing the kinetics and selectivity for surface reactions. In this study, we realize this target with a general strategy involving the application of a core/shell type cocatalyst that is demonstrated on various photocatalytic systems. The promising HO generation efficiency validate our perspective on tuning interfacial energetics for enhanced charge separation and photosynthesis performance. Particularly, this strategy is highlighted on a BiVO system for overall HO photosynthesis with a solar-to-HO conversion of 0.73%.
对经济高效的太阳能燃料的需求促使人们在人工光合作用方面进行了广泛的研究,然而,设计高性能颗粒光催化剂的努力在很大程度上受到电荷分离效率低下的阻碍。因为颗粒光催化剂中的电荷分离是由其还原和氧化位点之间的不对称界面能驱动的,所以要增强这个过程,就需要在不损害表面反应动力学和选择性的前提下,对界面能进行纳米级的调整。在这项研究中,我们通过一种涉及应用核/壳型助催化剂的通用策略实现了这一目标,该策略已在各种光催化系统上得到验证。有希望的 HO 生成效率验证了我们对调整界面能以增强电荷分离和光合作用性能的观点。特别是,该策略在 BiVO 体系的整体 HO 光合作用中得到了强调,其太阳能到 HO 的转化率为 0.73%。