Selective photocatalytic oxidation of benzyl alcohol to benzaldehyde or C-C coupled products by visible-light-absorbing quantum dots

Kevin P. McClelland; Emily A. Weiss

doi:10.1021/acsaem.8b01652

Selective photocatalytic oxidation of benzyl alcohol to benzaldehyde or C-C coupled products by visible-light-absorbing quantum dots

Kevin P. McClelland, Emily A. Weiss^*

^*Corresponding author for this work

Chemistry

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

105 Scopus citations

Abstract

This Forum Article describes the photocatalytic oxidation of benzyl alcohol by visible-light-absorbing colloidal CdS quantum dots (QDs), with 99% selectivity for benzaldehyde or 91% selectivity for C-C coupled products (primarily hydrobenzoin). The selectivity is tuned through the number of low-valent Cd atoms photodeposited on the surfaces of the QDs in situ; this deposition is enhanced by addition of a Cd²⁺ salt and suppressed by addition of an electron scavenger, anthroquinone-2-sulfonate, to the reaction mixture. In both cases, the external quantum efficiency (number of oxidative equivalents extracted from the QDs per incident photon) of the system is ∼1%.

Original language	English (US)
Pages (from-to)	92-96
Number of pages	5
Journal	ACS Applied Energy Materials
Volume	2
Issue number	1
DOIs	https://doi.org/10.1021/acsaem.8b01652
State	Published - Jan 28 2019

Funding

This work was supported as part of the Center for Light Energy Activated Redox Processes (LEAP), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award No. DESC0001059. K.P.M. acknowledges a graduate fellowship through the National Science Foundation (Award No. DGE-1324585). This work made use of the Keck-II facility of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. The authors would like to thank Shichen Lian and Mohamad Kodaimati for helpful discussions.

Keywords

Electron scavenger
Phosphonate ligands
Photodeposition
Product selectivity
Semiconductor nanocrystals

ASJC Scopus subject areas

Chemical Engineering (miscellaneous)
Energy Engineering and Power Technology
Electrochemistry
Materials Chemistry
Electrical and Electronic Engineering

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10.1021/acsaem.8b01652

Cite this

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title = "Selective photocatalytic oxidation of benzyl alcohol to benzaldehyde or C-C coupled products by visible-light-absorbing quantum dots",

abstract = "This Forum Article describes the photocatalytic oxidation of benzyl alcohol by visible-light-absorbing colloidal CdS quantum dots (QDs), with 99% selectivity for benzaldehyde or 91% selectivity for C-C coupled products (primarily hydrobenzoin). The selectivity is tuned through the number of low-valent Cd atoms photodeposited on the surfaces of the QDs in situ; this deposition is enhanced by addition of a Cd2+ salt and suppressed by addition of an electron scavenger, anthroquinone-2-sulfonate, to the reaction mixture. In both cases, the external quantum efficiency (number of oxidative equivalents extracted from the QDs per incident photon) of the system is ∼1%.",

keywords = "Electron scavenger, Phosphonate ligands, Photodeposition, Product selectivity, Semiconductor nanocrystals",

author = "McClelland, {Kevin P.} and Weiss, {Emily A.}",

note = "Funding Information: This work was supported as part of the Center for Light Energy Activated Redox Processes (LEAP), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award No. DESC0001059. K.P.M. acknowledges a graduate fellowship through the National Science Foundation (Award No. DGE-1324585). This work made use of the Keck-II facility of Northwestern University{\textquoteright}s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. The authors would like to thank Shichen Lian and Mohamad Kodaimati for helpful discussions. Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

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N2 - This Forum Article describes the photocatalytic oxidation of benzyl alcohol by visible-light-absorbing colloidal CdS quantum dots (QDs), with 99% selectivity for benzaldehyde or 91% selectivity for C-C coupled products (primarily hydrobenzoin). The selectivity is tuned through the number of low-valent Cd atoms photodeposited on the surfaces of the QDs in situ; this deposition is enhanced by addition of a Cd2+ salt and suppressed by addition of an electron scavenger, anthroquinone-2-sulfonate, to the reaction mixture. In both cases, the external quantum efficiency (number of oxidative equivalents extracted from the QDs per incident photon) of the system is ∼1%.

AB - This Forum Article describes the photocatalytic oxidation of benzyl alcohol by visible-light-absorbing colloidal CdS quantum dots (QDs), with 99% selectivity for benzaldehyde or 91% selectivity for C-C coupled products (primarily hydrobenzoin). The selectivity is tuned through the number of low-valent Cd atoms photodeposited on the surfaces of the QDs in situ; this deposition is enhanced by addition of a Cd2+ salt and suppressed by addition of an electron scavenger, anthroquinone-2-sulfonate, to the reaction mixture. In both cases, the external quantum efficiency (number of oxidative equivalents extracted from the QDs per incident photon) of the system is ∼1%.

KW - Electron scavenger

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KW - Photodeposition

KW - Product selectivity

KW - Semiconductor nanocrystals

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Selective photocatalytic oxidation of benzyl alcohol to benzaldehyde or C-C coupled products by visible-light-absorbing quantum dots

Abstract

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Keywords

ASJC Scopus subject areas

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