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用于增强臭氧催化降解双酚 A 活性的三维 MnO 多孔空心微球。

Three-dimensional MnO porous hollow microspheres for enhanced activity as ozonation catalysts in degradation of bisphenol A.

机构信息

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China.

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China; Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Guangzhou, 510275, China.

出版信息

J Hazard Mater. 2017 Jan 5;321:162-172. doi: 10.1016/j.jhazmat.2016.09.013. Epub 2016 Sep 5.

DOI:10.1016/j.jhazmat.2016.09.013
PMID:27619962
Abstract

Three-dimensional (3D) MnO porous hollow microspheres (δ- and α- MnO PHMSs), with high adsorption and catalytic ozonation performance, were synthesized by a self-template (MnCO microspheres) process at room temperature. The synthesized MnO PHMSs were characterized by X-ray diffraction (XRD), scanning electronic microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and Brunauer-Emmett-Teller (BET) surface area. The results showed that PHMSs exhibit the excellent adsorption ability and catalytic activity owning to their hollow spherical structure, mesoporous shell and well-defined interior voids, leading to the strong adsorption for bisphenol A (BPA) and the retention of O molecules on catalyst. Moreover, the catalytic performance of α-MnO PHMSs was better than that of δ-MnO PHMSs which was attributed to the richer lattice oxygen of α-MnO PHMSs to accelerate O decomposition by producing more reactive oxidative species. The degradation efficiency of BPA using 3D α-MnO PHMSs was more than 90% in the presence of ozone within 30min reaction time. The probe tests for reactive oxidative species (ROSs) displayed that BPA degradation by catalytic ozonation is dominated by O and OH in our present study. Furthermore, the organic compounds as intermediates of the degradation process were identified by LC/MS.

摘要

三维(3D)MnO 多孔空心微球(δ-MnO 和 α-MnO PHMSs),具有高吸附和催化臭氧化性能,通过室温下的自模板(MnCO 微球)工艺合成。合成的 MnO PHMSs 通过 X 射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X 射线光电子能谱(XPS)和 Brunauer-Emmett-Teller(BET)表面积进行了表征。结果表明,PHMSs 由于其空心球形结构、介孔壳和明确的内部空隙,表现出优异的吸附能力和催化活性,对双酚 A(BPA)具有很强的吸附能力,并保持催化剂上的 O 分子。此外,α-MnO PHMSs 的催化性能优于 δ-MnO PHMSs,这归因于 α-MnO PHMSs 中更丰富的晶格氧通过产生更多的活性氧化物种来加速 O 的分解。在 30min 的反应时间内,在臭氧存在下,使用 3Dα-MnO PHMSs 对 BPA 的降解效率超过 90%。活性氧化物种(ROSs)的探针测试表明,在本研究中,催化臭氧化降解 BPA 主要由 O 和 OH 主导。此外,通过 LC/MS 鉴定了降解过程中有机化合物作为中间产物。

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