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作 者:邱江源 肖碧源 覃方红 张美婷 万婷 刘锦萍 陈建华[3] 黄在银 QIU Jiang-Yuan;QIN Fang-Hong;XIAO Bi-Yuan;ZHANG Mei-Ting;WAN Ting;LIU Jin-Ping;CHEN Jian-Hua;HUANG Zai-Ying(College of Chemistry and Chemical Engineering, Guangxi University for Nationalities, Nanning 530006, China;The Sixth Geological Brigade of Hubei Geological Bureau, Xiaogan, Hubei 432000, China;School of Resources, Environment and Materials, Innovation Center for Metal Resources Utilization and Environment Protection, and Guangxi Key Laboratory of Processing for Non-ferrous Metal and Featured Materials, Guangxi University, Nanning 530004, China)
机构地区:[1]广西民族大学化学化工学院,南宁530006 [2]湖北地质局第六支队,孝感432000 [3]广西大学环境与资源学院,广西金属资源利用和环境保护中心,广西有色金属和特色材料加工重点实验室,南宁530004
出 处:《无机化学学报》2019年第9期1665-1677,共13页Chinese Journal of Inorganic Chemistry
基 金:the financial support from the National Natural Science Foundation of China (Grants No.21273050, 21573048, 21873022, 51574092)~~
摘 要:纯Fe2O3表面活性位点较少具有较低的催化活性限制了其在多相芬顿催化体系中的应用。通常采用元素掺杂、贵金属负载以及与其它化合物质复合等改性措施来提升催化活性,然而这些措施存在催化剂制备复杂,制备成本高以及催化剂的精细结构难以精准控制等问题。因此,本文提出在α-Fe2O3表面引入氧空位缺陷构筑双活性位点(Fe^2+和氧空位)用于促进H2O2分解提高降解污染物降解效率。实验结果发现α-Fe2O3-x-330/H2O2体系具有较宽的pH使用范围(pH=2~10)。当pH=4时,罗丹明B的降解速率常数为0.834 h^-1,而且催化剂具有磁性,易回收重复使用。催化机理研究表明氧空位缺陷α-Fe2O3-x催化剂的氧空位和Fe2+两种活性位点均可促进H2O2分解,而且氧空位的引入有利于污染物在催化剂表面的吸附进一步提高催化性能。Intrinsically poor reactivity restricts hematite (α-Fe2O3) from heterogeneous Fenton systems. Usually, metal ion doping, noble metal loading, and compounding with other compounds to enhance their catalytic activity are necessary, making them complex, expensive, and difficult to control. Here a surface-electronic-state-modulation-based concept applied to hematite is presented. This concept enables hematite with dual reaction sites as highly reactive and reusable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics, via activation of H2O2 and without any extra energy input. The rhodamine B degradation rate constants for α-Fe2O3-x-330/H2O2 systems were 0.834 h-1, when pH=4, and have a much wider pH working window (pH=2~10) than traditional Fenton systems. Meanwhile, the used catalyst can be easily recovered by magnetic separation. Oxygen vacancy and Fe(Ⅱ) on defective α-Fe2O3-x surfaces have been confirmed as the active sites for H2O2 activation while the adjacent vacancy oxygens site adsorbs organic molecules and thus improves the Fenton-like catalytic performance. These findings may not only extend the environment applications of pure transition metal oxide but also stimulate new opportunities for the same as many other transition metal oxides by surface electronic-state modulation.
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