期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 224, 期 -, 页码 772-782出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2017.09.062
关键词
Biomimetic synthesis; Hydrogenases models; Graphene; Photocatalysis; Electron transfer
资金
- National Natural Science Foundation of China [21202115]
- Research Fund for the Doctoral Program of Higher Education [20100032120070]
- Tianjin Research Program of Application Foundation and Advanced Technology [13JCQNJC06100]
- State Scholarship Fund from China Scholarship Council [201506255024]
Two novel complexes [Fe-2(mu-SC3H6S)(CO)(5)][Fc(PPh2)CHO] (3) and 5-{[Fe-2(mu-SC3H6S)(CO)(5)](PPh(2)Fc)}-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 (irriR), 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 H-2 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 H-2 production compared with the common electron donors, such as ascorbic acid (H(2)A), triethanolamine (TEOA), glucose or Na2S2O3.
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