Graphitic Carbon Nitride/CdSe Quantum Dot/Iron Carbonyl Cluster Composite for Enhanced Photocatalytic Hydrogen Evolution
(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.
(Less)
- author
- 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
- organization
- publishing date
- 2021
- 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}}, }