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Cu-Al2O3中骨架铜类芬顿催化去除水中有机污染物
摘要点击 2056  全文点击 717  投稿时间:2016-08-09  修订日期:2016-10-09
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中文关键词  Cu-Al2O3  类芬顿催化剂  骨架铜  有机污染物  活性物种
英文关键词  Cu-Al2O3  Fenton-like catalyst  framework Cu  organic pollutants  active species
作者单位E-mail
徐丹 大连理工大学食品与环境学院, 盘锦 124221 1552599143@qq.com 
张丽丽 中国科学院生态环境研究中心, 北京 100085 llzhang@rcees.ac.cn 
柳丽芬 大连理工大学食品与环境学院, 盘锦 124221  
中文摘要
      为解决传统铁基芬顿催化剂在水体通常酸碱(pH>6)条件下活性低的问题,采用简单共沉淀法制备了Cu掺杂的Al2O3类芬顿催化剂.通过X射线衍射(XRD)、X射线光电子能谱(XPS)和紫外可见(UV-vis)吸收光谱分析表明,Cu-Al2O3中铜掺杂的质量分数低于4.77%时,催化剂中铜主要以Cu2+和Cu+的形式共存于Al2O3的骨架结构中,形成Al-O-Cu键;过量的铜掺杂会导致外骨架铜物种如铜氧化物团簇的存在.以难降解有机污染物2-氯苯酚(2-chlorophenol,2-CP)和染料罗丹明B(Rhodamine B,RhB)为目标污染物,对Cu-Al2O3的类芬顿催化性能进行了详细地研究.结果表明,骨架铜物种在中性温和条件下对2-CP和RhB显示出很高的催化去除效率和稳定性,反应2 h,Cu-Al2O3(Cu质量分数4.77%)对2-CP的去除率达到54%,相应的TOC去除率达到49%,而铜离子溶出浓度仅为0.0255 mg·L-1,而Cu-Al2O3(Cu质量分数7.58%)由于外骨架铜的存在导致催化活性增加缓慢和稳定性下降.ESR测试结果表明,·OH和HO2-/O2是反应中主要的活性物种.
英文摘要
      To address the problem of low activity for Fe-based Fenton-like catalysts at neutral pH, Cu-Al2O3 Fenton-like catalyst was prepared by a simple co-precipitation method. The samples were characterized by means of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and diffuse reflectance UV-vis spectra (UV-vis DRS). The results showed that both Cu2+ and Cu+mainly existed in the bulk framework of Al2O3 for Cu-Al2O3 with appropriate Cu doping (lower than 4.77% Cu), forming the bond of Al-O-Cu, while excessive Cu doping in Al2O3 (e. g. 7.58% Cu) could result in the occurrence of extraframework Cu species. The Fenton-like catalytic performance of the prepared samples was evaluated by the degradation of 2-chlorophenol (2-CP) and Rhodamine B (RhB). The results showed that the catalyst with framework Cu species had high catalytic activity and stability for the degradation of 2-CP and RhB. After reaction for 2 h, the degradation rate of 2-CP reached up to 54% over Cu-Al2O3(4.77% Cu) in the presence of H2O2, the corresponding TOC removal reached 49%, and the Cu release concentration was only 0.0255 mg·L-1. However, the existence of extraframework Cu in Al2O3 would lead to the reduction of the catalytic performance. ESR analysis showed that·OH and HO2-/O2 were the primary active species.

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