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Graphitic Carbon Nitride/CdSe Quantum Dot/Iron Carbonyl Cluster Composite for Enhanced Photocatalytic Hydrogen Evolution

Li, Chuanshuai LU ; Zou, Xianshao LU ; Lin, Weihua LU ; Mourad, Hassan LU ; Meng, Jie ; Liu, Yang LU ; Abdellah, Mohamed LU ; Guo, Meiyuan LU ; Zheng, Kaibo LU and Nordlander, Ebbe LU (2021) In ACS Applied Nano Materials 4(6). p.6280-6289
Abstract

A g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite has been successfully constructed. The structure and chemical composition of the composite were investigated via, inter alia, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The ability of the assembly to act as a photocatalyst for proton reduction to form hydrogen gas was studied. With visible light irradiation for 4 h, the total H2 production catalyzed by the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite was found to be 9 times as high as a corresponding CdSe/[Fe2S2(CO)6] assembly and significantly higher than either the CdSe quantum dots or g-C3N4 alone. The g-C3N4 support/matrix was found to enhance... (More)

A g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite has been successfully constructed. The structure and chemical composition of the composite were investigated via, inter alia, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The ability of the assembly to act as a photocatalyst for proton reduction to form hydrogen gas was studied. With visible light irradiation for 4 h, the total H2 production catalyzed by the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite was found to be 9 times as high as a corresponding CdSe/[Fe2S2(CO)6] assembly and significantly higher than either the CdSe quantum dots or g-C3N4 alone. The g-C3N4 support/matrix was found to enhance the stability and efficiency of the CdSe quantum dot/iron carbonyl cluster assembly in the photocatalytic hydrogen evolution process. Results from recycling tests showed that the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite is a sustainable and robust photocatalyst, maintaining the same activity after three cycles. The photoinduced charge carrier transfer dynamics in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite system has been investigated by transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopies. The spectroscopic results indicate efficient hole transfer from the valence band of the excited CdSe quantum dots to the molecular iron carbonyl clusters and from the defect state of the quantum dots to g-C3N4 in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite, which significantly inhibits the recombination of photogenerated charge carriers in CdSe quantum dots and boosts the photocatalytic activity and stability for hydrogen evolution. Energy transfer from g-C3N4 to the CdSe quantum dot/[Fe2S2(CO)6] assembly with a time constant of 0.7 ns also contributed to the charge transfer process.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
charge transfer, energy transfer, graphitic carbon nitride, iron carbonyl cluster, photocatalytic proton reduction, quantum dot, ternary composite
in
ACS Applied Nano Materials
volume
4
issue
6
pages
10 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85110868699
ISSN
2574-0970
DOI
10.1021/acsanm.1c01096
language
English
LU publication?
yes
id
42158c1a-b6c6-4fee-acc4-7fb514aa298b
date added to LUP
2021-08-23 11:49:40
date last changed
2023-11-08 17:53:11
@article{42158c1a-b6c6-4fee-acc4-7fb514aa298b,
  abstract     = {{<p>A g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite has been successfully constructed. The structure and chemical composition of the composite were investigated via, inter alia, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The ability of the assembly to act as a photocatalyst for proton reduction to form hydrogen gas was studied. With visible light irradiation for 4 h, the total H2 production catalyzed by the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite was found to be 9 times as high as a corresponding CdSe/[Fe2S2(CO)6] assembly and significantly higher than either the CdSe quantum dots or g-C3N4 alone. The g-C3N4 support/matrix was found to enhance the stability and efficiency of the CdSe quantum dot/iron carbonyl cluster assembly in the photocatalytic hydrogen evolution process. Results from recycling tests showed that the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite is a sustainable and robust photocatalyst, maintaining the same activity after three cycles. The photoinduced charge carrier transfer dynamics in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite system has been investigated by transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopies. The spectroscopic results indicate efficient hole transfer from the valence band of the excited CdSe quantum dots to the molecular iron carbonyl clusters and from the defect state of the quantum dots to g-C3N4 in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite, which significantly inhibits the recombination of photogenerated charge carriers in CdSe quantum dots and boosts the photocatalytic activity and stability for hydrogen evolution. Energy transfer from g-C3N4 to the CdSe quantum dot/[Fe2S2(CO)6] assembly with a time constant of 0.7 ns also contributed to the charge transfer process. </p>}},
  author       = {{Li, Chuanshuai and Zou, Xianshao and Lin, Weihua and Mourad, Hassan and Meng, Jie and Liu, Yang and Abdellah, Mohamed and Guo, Meiyuan and Zheng, Kaibo and Nordlander, Ebbe}},
  issn         = {{2574-0970}},
  keywords     = {{charge transfer; energy transfer; graphitic carbon nitride; iron carbonyl cluster; photocatalytic proton reduction; quantum dot; ternary composite}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{6280--6289}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Applied Nano Materials}},
  title        = {{Graphitic Carbon Nitride/CdSe Quantum Dot/Iron Carbonyl Cluster Composite for Enhanced Photocatalytic Hydrogen Evolution}},
  url          = {{http://dx.doi.org/10.1021/acsanm.1c01096}},
  doi          = {{10.1021/acsanm.1c01096}},
  volume       = {{4}},
  year         = {{2021}},
}