Institutional Repository of Key Laboratory of Marine Environmental Corrosion and Bio-fouling, IOCAS
|Place of Conferral||中国科学院海洋研究所|
海洋生物污损，是人类开发利用海洋以来一直需要面对与解决的问题。因此， 亟需一种绿色、环保、有效的海洋生物污损防护技术。H2O2 作为一种强氧化性、
Marine biofouling is a problem that human beings have to face and solve since the exploitation and utilization of the ocean. Hydrogen peroxide (H2O2), as a strong oxidizing and low selectivity oxidant, has been widely used in wastewater treatment, chemical oxidation, bioligical pharmcy and antibacterial, due to its advantages of environmental friendliness and no pollution from degradation products. In situ electrochemical synthesis of H2O2 is one particularly important method and can be used in the field of antibacterial and antifouling. Herein, we use carbon-based materials as the substrate materials for electrocatalytic oxygen reduction reaction to H2O2. The production H2O2 is used for antibacterial and antifouling applications, and E. coli, S. aureus and P. aeruginosa are used as the model bacteria. In addition, the production H2O2 can be detected using the carbon-based materials as the simulated enzyme. In order to prevent the corrosion of metal by the excessive H2O2, it is further catalyzed to HXO by the haloperoxidase or to •OH according to the Fenton rection. As well we know, HXO and •OH have all strong bacterical properties, which can be used in the research on the biological protect of marine biofouling. It also has important guiding significance for development of advanced biological antifouling technology for marine biofouling. The specific research contents are as follows: (1) Electrocatalytic oxygen reduction to hydrogen peroxide by oxidized graphene aerogel supported cubic MnCO3 for antibacteria in neutral media We prepared the oxidized graphene aerogel supported cubic manganese carbonate composites (GOx/MnCO3) with different GO and MnCO3 ratio through a simple co-precipitation/in-situ coating method. The characterization results showed that the GOx/MnCO3 composites, with uniformly wrapping of GO on the surface of MnCO3 cubic, display high conductivity and abundant catalytic sites for 2-electron ORR. The G0.2M shows the best ORR catalytic performance, onset potential of 0.635 VRHE, high H2O2 production selectivity and high stability in 3.5% NaCl electrolyte. Based on this, G0.2M as oxygen reduction electrocatalyst, has good antibacterial effect at 0.55 VRHE on the stainless-steel. The antibacterial mechanism is mainly due to the electrocatalytic oxygen reaction of H2O2 and the side reaction of •OH and O2•-. This provides an impressive, effective and environmentally friendly electrochemical approach for antibacterial and antifouling applications. (2) A 3-dimensional C/CeO2 hollow nanostructure framework as a peroxidase mimetic, and its application to the colorimetric determination of hydrogen peroxide Various 3-dimensional C/CeO2 hollow nanostructure frameworks (3D C/CeO2 HNFs) were synthesized by using a polymer blowing process, which is accelerated by adding a certain amount of cerium nitrate. Polyvinylpyrrolidone was used as the polymer. The resulting 3D C/CeO2 HNFs were characterized by scanning electron microscopy, energy dispersive spectrometry, X-ray diffraction and X-ray photoelectron spectroscopy. The 3D C/CeO2 HNFs possess a large specific surface area, and the CeO2 nanocrystals consist of a single phase. The 3D C/CeO2 HNFs display intrinsic peroxidase-like activity and can catalyze the oxidation of the peroxidase substrate 3,3’,5,5’-tetramethylbenzidine in the presence of H2O2 to produce a blue product. The method was applied to the quantification of H2O2 with a 5.2 nM detection limit. The analytical range is from 10 nM to 1 μM. (3) Investigating the properties of nano core-shell CeO2@C as haloperoxidase mimicry catalyst for antifouling applications In this work, we have successfully synthesized the core-shell structure of CeO2@C by using the carbon sphere as template through a simple coprecipitation method. The as-prepared CeO2@C is characterized by scanning electron microscopy, transmission electron microscopy, energy dispersive spectrometry, X-ray diffraction, and X-ray photoelectron spectroscopy. The CeO2@C displays intrinsic haloperoxidase-like activity via catalyzing the bromination of organic signaling compoundsas well as high stability and recyclability. It can catalyze the oxidation of Br- with H2O2 to the corresponding hypobromous acid (HBrO); the produced HBrO exhibits strong antibacterial activity against Gram-negative (E. coli), Gram-positive (S. aureus) bacteria and typical marine (P. aeruginosa) bacteria. This study introduces a stable, non-poisonous and inexpensive biomimetic material for antibacterial, antifouling and disinfection applications based on novel sustainable and conservation methods. (4) C, N doped CeO2 nanoparticles as haloperoxidase mimicry for antifouling applications In this work, we have successfully synthesized the CN-CeO2 composites through a simple solid-state synthesis method. The CN-CeO2 composites are characterized by scanning electron microscopy, energy dispersive spectrometry and X-ray diffraction spectroscopy. CN-CeO2 composites display intrinsic haloperoxidase-like activity via catalyzing the bromination of organic signaling compounds, and present high stability and recyclability in catalytic reactions. On this basis, it can catalyze the oxidation of Br- with H2O2 to the corresponding hypobromous acid (HBrO), and the produced HBrO exhibits strong antibacterial activity. This study introduces a stable, green and environment friendly biomimetic material for antibacterial, antifouling and disinfection applications, which will provide a novel sustainable and conservation methods.
|王楠. 碳基催化材料的制备及抗菌防污机制的研究[D]. 中国科学院海洋研究所. 中国科学院大学,2020.|
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