Photogenerated Charge Separation in a CdSe Nanocluster Encapsulated in a Metal-Organic Framework for Improved Photocatalysis

Indrani Choudhuri; Donald G. Truhlar

doi:10.1021/acs.jpcc.0c00007

Photogenerated Charge Separation in a CdSe Nanocluster Encapsulated in a Metal-Organic Framework for Improved Photocatalysis

Indrani Choudhuri, Donald G. Truhlar

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	8504-8513
Number of pages	10
Journal	Journal of Physical Chemistry C
Volume	124
Issue number	16
DOIs	https://doi.org/10.1021/acs.jpcc.0c00007
State	Published - Apr 23 2020

Bibliographical note

Funding 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.

Publisher Copyright:
© 2020 American Chemical Society.

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title = "Photogenerated Charge Separation in a CdSe Nanocluster Encapsulated in a Metal-Organic Framework for Improved Photocatalysis",

abstract = "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.",

author = "Indrani Choudhuri and Truhlar, {Donald G.}",

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AU - Choudhuri, Indrani

AU - Truhlar, Donald G.

N1 - Funding 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. Publisher Copyright: © 2020 American Chemical Society.

PY - 2020/4/23

Y1 - 2020/4/23

N2 - 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.

AB - 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.

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Photogenerated Charge Separation in a CdSe Nanocluster Encapsulated in a Metal-Organic Framework for Improved Photocatalysis

Abstract

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