Nanoclusters encapsulated in a metal-organic framework (MOF) are the subject of intense interest because of their high promise for photocatalysis. We show computationally that a CdSe nanocluster incorporated into NU-1000 (Cd6Se6@NU-1000) allows electron transfer from a visible-light photo-excited organic linker to the lowest unoccupied crystal orbital of the inorganic cluster, which can lead to charge separation. Substituents on the linker can be used to tune the band position and the band gap of the whole composite (Cd6Se6@NU-1000), and this makes it possible to perform the water splitting reaction under visible light. The achievement of charge separation within the MOF leads to longer life of the excited states, and as a result, it can enhance the photocatalytic activity of the system.
Bibliographical noteFunding Information:
The authors are grateful to Laura Gagliardi for many stimulating discussions. This research was supported as part of the Nanoporous Materials Genome Center by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under award DE-FG02-17ER16362.
© 2020 American Chemical Society.