• 文献标题:   Fabrication of covalently linked graphene-mediated [FeFe]-hydrogenases biomimetic photocatalytic hydrogen evolution system in aqueous solution
  • 文献类型:   Article
  • 作  者:   LI RX, REN XT, TANG MY, CHEN MX, HUANG GB, FANG CH, LIU T, FENG ZH, YIN YB, GUO YM, MEI SK, YAN J
  • 作者关键词:   biomimetic synthesi, hydrogenases model, graphene, photocatalysi, electron transfer
  • 出版物名称:   APPLIED CATALYSIS BENVIRONMENTAL
  • ISSN:   0926-3373 EI 1873-3883
  • 通讯作者地址:   Tianjin Univ
  • 被引频次:   5
  • DOI:   10.1016/j.apcatb.2017.09.062
  • 出版年:   2018

▎ 摘  要

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.