Fabrication of covalently linked graphene-mediated [FeFe]-hydrogenases biomimetic photocatalytic hydrogen evolution system in aqueous solution

[Display omitted] •Graphene-mediated biomimetic photocatalytic system is fabricated in water.•Organic photosensitizer and organometallic catalyst are covalently linked to GO.•Effects of electron-transfer-pathway on H2 production efficiency are analyzed.•Two novel bionic H-cluster models are synthesi...

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Published inApplied catalysis. B, Environmental Vol. 224; pp. 772 - 782
Main Authors Li, Rui-Xia, Ren, Xiang-Ting, Tang, Ming-Yi, Chen, Ming-Xi, Huang, Guan-Bo, Fang, Chang-Hui, Liu, Ting, Feng, Zhan-Heng, Yin, Yi-Bing, Guo, Ya-Mei, Mei, Shun-Kang, Yan, Jing
Format Journal Article
LanguageEnglish
Published Amsterdam Elsevier B.V 01.05.2018
Elsevier BV
Subjects
Aqueous solutions
Ascorbic acid
Biomimetic synthesis
Biomimetics
Catalysis
Cystine
Efficiency
Electron microscopy
Electron transfer
Emission analysis
Fabrication
Fluorescence
Fourier transforms
Graphene
Hydrogen evolution
Hydrogen production
Hydrogenases
Hydrogenases models
Inductively coupled plasma
Infrared analysis
Infrared spectroscopy
Photocatalysis
Sodium thiosulfate
Spectrometry
Transmission electron microscopy
Triethanolamine
Electron transfer
Graphene
Biomimetic synthesis
Photocatalysis
Hydrogenases models
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Abstract [Display omitted] •Graphene-mediated biomimetic photocatalytic system is fabricated in water.•Organic photosensitizer and organometallic catalyst are covalently linked to GO.•Effects of electron-transfer-pathway on H2 production efficiency are analyzed.•Two novel bionic H-cluster models are synthesized and characterized successfully.•Positive result is earned by introducing cystine into photocatalytic system. Two novel complexes [Fe2(μ-SC3H6S)(CO)5][Fc(PPh2)CHO] (3) and 5-{[Fe2(μ-SC3H6S)(CO)5](PPh2Fc)}-10, 15, 20-triphenylporphyrin (4), which contain ferrocene-based ligand to simulate the role of the active site of [FeFe]-hydrogenases (H-Cluster), are synthesized and characterized successfully. A graphene-mediated [FeFe]-hydrogenases biomimetic nanohybrid (TPP-NHCO-GO-[3Fe2S]) 6 is fabricated by linking organic photosensitizer tetraphenylporphyrin (TPP) and complex 3 to graphene oxide (GO) via the covalent bond. The new nanohybrid 6 is characterized by elemental analysis, Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM) and inductively coupled plasma atomic emission spectrometry (ICP-AES). By comparing the ultraviolet-visible (UV-vis) absorption, fluorescence emission and time-resolved fluorescence, it can be found the efficiency of electron transfer has been obviously improved with the presence of GO, and the efficiency of electron transfer in intramolecular system is higher than that in intermolecular system. These results are also supported by the photo-induced H2 production experiments with corresponding catalytic systems in water. Besides, the cystine is used as the sacrificial electron donor for light catalytic reaction in aqueous solution, which improves the efficiency of photocatalytic H2 production compared with the common electron donors, such as ascorbic acid (H2A), triethanolamine (TEOA), glucose or Na2S2O3.
AbstractList Two novel complexes [Fe2(µ-SC3H6S)(CO)5][Fc(PPh2)CHO] (3) and 5-{[Fe2(µ-SC3H6S)(CO)5](PPh2Fc)}-10, 15, 20-triphenylporphyrin (4), which contain ferrocene-based ligand to simulate the role of the active site of [FeFe]-hydrogenases (H-Cluster), are synthesized and characterized successfully. A graphene-mediated [FeFe]-hydrogenases biomimetic nanohybrid (TPP-NHCO-GO-[3Fe2S]) 6 is fabricated by linking organic photosensitizer tetraphenylporphyrin (TPP) and complex 3 to graphene oxide (GO) via the covalent bond. The new nanohybrid 6 is characterized by elemental analysis, Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM) and inductively coupled plasma atomic emission spectrometry (ICP-AES). By comparing the ultraviolet-visible (UV-vis) absorption, fluorescence emission and time-resolved fluorescence, it can be found the efficiency of electron transfer has been obviously improved with the presence of GO, and the efficiency of electron transfer in intramolecular system is higher than that in intermolecular system. These results are also supported by the photo-induced H2 production experiments with corresponding catalytic systems in water. Besides, the cystine is used as the sacrificial electron donor for light catalytic reaction in aqueous solution, which improves the efficiency of photocatalytic H2 production compared with the common electron donors, such as ascorbic acid (H2A), triethanolamine (TEOA), glucose or Na2S2O3.
[Display omitted] •Graphene-mediated biomimetic photocatalytic system is fabricated in water.•Organic photosensitizer and organometallic catalyst are covalently linked to GO.•Effects of electron-transfer-pathway on H2 production efficiency are analyzed.•Two novel bionic H-cluster models are synthesized and characterized successfully.•Positive result is earned by introducing cystine into photocatalytic system. Two novel complexes [Fe2(μ-SC3H6S)(CO)5][Fc(PPh2)CHO] (3) and 5-{[Fe2(μ-SC3H6S)(CO)5](PPh2Fc)}-10, 15, 20-triphenylporphyrin (4), which contain ferrocene-based ligand to simulate the role of the active site of [FeFe]-hydrogenases (H-Cluster), are synthesized and characterized successfully. A graphene-mediated [FeFe]-hydrogenases biomimetic nanohybrid (TPP-NHCO-GO-[3Fe2S]) 6 is fabricated by linking organic photosensitizer tetraphenylporphyrin (TPP) and complex 3 to graphene oxide (GO) via the covalent bond. The new nanohybrid 6 is characterized by elemental analysis, Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM) and inductively coupled plasma atomic emission spectrometry (ICP-AES). By comparing the ultraviolet-visible (UV-vis) absorption, fluorescence emission and time-resolved fluorescence, it can be found the efficiency of electron transfer has been obviously improved with the presence of GO, and the efficiency of electron transfer in intramolecular system is higher than that in intermolecular system. These results are also supported by the photo-induced H2 production experiments with corresponding catalytic systems in water. Besides, the cystine is used as the sacrificial electron donor for light catalytic reaction in aqueous solution, which improves the efficiency of photocatalytic H2 production compared with the common electron donors, such as ascorbic acid (H2A), triethanolamine (TEOA), glucose or Na2S2O3.
Author Guo, Ya-Mei
Yin, Yi-Bing
Feng, Zhan-Heng
Chen, Ming-Xi
Yan, Jing
Li, Rui-Xia
Ren, Xiang-Ting
Huang, Guan-Bo
Tang, Ming-Yi
Fang, Chang-Hui
Liu, Ting
Mei, Shun-Kang
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  givenname: Jing
  surname: Yan
  fullname: Yan, Jing
  email: jingyan@tju.edu.cn
  organization: Department of Chemistry, School of Science, Tianjin University, Tianjin 300072, China
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Hydrogenases models
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Snippet [Display omitted] •Graphene-mediated biomimetic photocatalytic system is fabricated in water.•Organic photosensitizer and organometallic catalyst are...
Two novel complexes [Fe2(µ-SC3H6S)(CO)5][Fc(PPh2)CHO] (3) and 5-{[Fe2(µ-SC3H6S)(CO)5](PPh2Fc)}-10, 15, 20-triphenylporphyrin (4), which contain ferrocene-based...
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elsevier
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SubjectTerms Aqueous solutions
Ascorbic acid
Biomimetic synthesis
Biomimetics
Catalysis
Cystine
Efficiency
Electron microscopy
Electron transfer
Emission analysis
Fabrication
Fluorescence
Fourier transforms
Graphene
Hydrogen evolution
Hydrogen production
Hydrogenases
Hydrogenases models
Inductively coupled plasma
Infrared analysis
Infrared spectroscopy
Photocatalysis
Sodium thiosulfate
Spectrometry
Transmission electron microscopy
Triethanolamine
Title Fabrication of covalently linked graphene-mediated [FeFe]-hydrogenases biomimetic photocatalytic hydrogen evolution system in aqueous solution
URI https://dx.doi.org/10.1016/j.apcatb.2017.09.062
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