Abstract
Based on their excellent stability, high carrier mobility, and wide photoresponse range, composites formed by embedding perovskite quantum dots (PQDs) into metal-organic frameworks (PQDs@MOF) show great development potential in the field of photocatalysis, including the toxic hexavalent chromium (Cr6+) degradation, CO2 reduction, H2 production, etc. However, the rapid recombination of photogenerated carriers is still a major obstacle to the improvement of photocatalytic performance, and the internal mechanism of photocatalysis is still unclear. In this work, we construct a novel double heterojunction photocatalyst by encapsulating CsPbBr3 PQDs in Zr-based metal-organic frameworks (UiO-67) and loading additional hole-acceptor pentylenetetrazol (PTZ). Spontaneous photoinduced charge-transfer and separation between interfaces are confirmed by time-resolved photoluminescence and transient absorption spectroscopy. Furthermore, compared with pure UiO-67, the photoactivity of CsPbBr3 PQDs@UiO-67@PTZ increased 3-fold due to the long-lived charge-separated state. Our findings provide a new guideline for the design of PQDs@MOF-based photocatalysts with long-lived photogenerated carriers and outstanding photocatalytic activity.
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