Liu Liping, Meng Haibing, Chai Yongqiang, Chen Xianjie, Xu Jingyi, Liu Xiaolong, Liu Weixu, Guldi Dirk M, Zhu Yongfa
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
College of Chemistry, Taiyuan University of Technology, Taiyuan, 030024, P. R. China.
Angew Chem Int Ed Engl. 2023 Mar 6;62(11):e202217897. doi: 10.1002/anie.202217897. Epub 2023 Feb 6.
High-efficiency photocatalysts based on metal-organic frameworks (MOFs) are often limited by poor charge separation and slow charge-transfer kinetics. Herein, a novel MOF photocatalyst is successfully constructed by encapsulating C into a nano-sized zirconium-based MOF, NU-901. By virtue of host-guest interactions and uneven charge distribution, a substantial electrostatic potential difference is set-up in C @NU-901. The direct consequence is a robust built-in electric field, which tends to be 10.7 times higher in C @NU-901 than that found in NU-901. In the catalyst, photogenerated charge carriers are efficiently separated and transported to the surface. For example, photocatalytic hydrogen evolution reaches 22.3 mmol g h for C @NU-901, which is among the highest values for MOFs. Our concept of enhancing charge separation by harnessing host-guest interactions constitutes a promising strategy to design photocatalysts for efficient solar-to-chemical energy conversion.
基于金属有机框架（MOF）的高效光催化剂常常受到电荷分离不佳和电荷转移动力学缓慢的限制。在此，通过将碳封装到纳米尺寸的锆基金属有机框架NU-901中，成功构建了一种新型MOF光催化剂。借助主客体相互作用和电荷分布不均，在C@NU-901中建立了显著的静电势差。直接结果是形成了强大的内建电场，其在C@NU-901中的强度往往比在NU-901中高10.7倍。在该催化剂中，光生电荷载流子被有效分离并传输到表面。例如，C@NU-901的光催化析氢量达到22.3 mmol g⁻¹ h⁻¹，这是MOF中的最高值之一。我们利用主客体相互作用增强电荷分离的概念构成了一种有前景的策略，用于设计高效太阳能到化学能转换的光催化剂。
