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Issue 9, 2018
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ZnSe quantum dots modified with a Ni(cyclam) catalyst for efficient visible-light driven CO2 reduction in water

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Abstract

A precious metal and Cd-free photocatalyst system for efficient CO2 reduction in water is reported. The hybrid assembly consists of ligand-free ZnSe quantum dots (QDs) as a visible-light photosensitiser combined with a phosphonic acid-functionalised Ni(cyclam) catalyst, NiCycP. This precious metal-free photocatalyst system shows a high activity for aqueous CO2 reduction to CO (Ni-based TONCO > 120), whereas an anchor-free catalyst, Ni(cyclam)Cl2, produced three times less CO. Additional ZnSe surface modification with 2-(dimethylamino)ethanethiol (MEDA) partially suppresses H2 generation and enhances the CO production allowing for a Ni-based TONCO of > 280 and more than 33% selectivity for CO2 reduction over H2 evolution, after 20 h visible light irradiation (λ > 400 nm, AM 1.5G, 1 sun). The external quantum efficiency of 3.4 ± 0.3% at 400 nm is comparable to state-of-the-art precious metal photocatalysts. Transient absorption spectroscopy showed that band-gap excitation of ZnSe QDs is followed by rapid hole scavenging and very fast electron trapping in ZnSe. The trapped electrons transfer to NiCycP on the ps timescale, explaining the high performance for photocatalytic CO2 reduction. With this work we introduce ZnSe QDs as an inexpensive and efficient visible light-absorber for solar fuel generation.

Graphical abstract: ZnSe quantum dots modified with a Ni(cyclam) catalyst for efficient visible-light driven CO2 reduction in water

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Article information


Submitted
12 Oct 2017
Accepted
24 Jan 2018
First published
24 Jan 2018

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2018,9, 2501-2509
Article type
Edge Article

ZnSe quantum dots modified with a Ni(cyclam) catalyst for efficient visible-light driven CO2 reduction in water

M. F. Kuehnel, C. D. Sahm, G. Neri, J. R. Lee, Katherine L. Orchard, A. J. Cowan and E. Reisner, Chem. Sci., 2018, 9, 2501
DOI: 10.1039/C7SC04429A

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