Enhancing Built‐in Electric Fields for Efficient Photocatalytic Hydrogen Evolution by Encapsulating C60 Fullerene into Zirconium‐Based Metal‐Organic Frameworks

Abstract 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 C60 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 C60@NU‐901. The direct consequence is a robust built‐in electric field, which tends to be 10.7 times higher in C60@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−1 h−1 for C60@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.