重金属碳基复合材料激活过一硫酸盐的研究
Study on Activation Peroxymonosulfate by Heavy Metal Carbon-based Composite
作者：刘杨(四川大学 建筑与环境学院, 深地科学与工程教育部重点实验室, 四川 成都 610065)；张永丽(四川大学 建筑与环境学院, 深地科学与工程教育部重点实验室, 四川 成都 610065)；郭洪光(四川大学 建筑与环境学院, 深地科学与工程教育部重点实验室, 四川 成都 610065)；程鑫(四川大学 建筑与环境学院, 深地科学与工程教育部重点实验室, 四川 成都 610065)；周鹏(四川大学 建筑与环境学院, 深地科学与工程教育部重点实验室, 四川 成都 610065)；王敬荃(四川大学 建筑与环境学院, 深地科学与工程教育部重点实验室, 四川 成都 610065)
Author：LIU Yang(Key Lab. of Deep Underground Sci. and Eng., for Minisity of Education, College of Architecture and Environment, Sichuan Univ., Chengdu 610065, China)；ZHANG Yongli(Key Lab. of Deep Underground Sci. and Eng., for Minisity of Education, College of Architecture and Environment, Sichuan Univ., Chengdu 610065, China)；GUO Hongguang(Key Lab. of Deep Underground Sci. and Eng., for Minisity of Education, College of Architecture and Environment, Sichuan Univ., Chengdu 610065, China)；CHENG Xin(Key Lab. of Deep Underground Sci. and Eng., for Minisity of Education, College of Architecture and Environment, Sichuan Univ., Chengdu 610065, China)；ZHOU Peng(Key Lab. of Deep Underground Sci. and Eng., for Minisity of Education, College of Architecture and Environment, Sichuan Univ., Chengdu 610065, China)；WANG Jingquan(Key Lab. of Deep Underground Sci. and Eng., for Minisity of Education, College of Architecture and Environment, Sichuan Univ., Chengdu 610065, China)
收稿日期：2017-12-03 年卷（期）页码：2018,50(4):214-220
期刊名称：工程科学与技术
Journal Name：Advanced Engineering Sciences
关键字：重金属;离子树脂;炭化;过一硫酸盐;有机污染物;降解
Key words：heavy metal;ion resin;carbonation;peroxymonosulfate;organic contaminates;degradation
基金项目：国家自然科学基金资助项目（51508354）；中央高校基本科研业务费专项资金资助（2012017yjsy166）
中文摘要
随着能源与环境问题的日益突出，进行重金属的回收再利用具有重要意义。为实现重金属回收后资源化利用，作者提出利用强酸性阳离子树脂将水中重金属离子回收后，经过600 ℃高温无氧炭化固定，制备含不同重金属的碳基复合材料（C-X，X=Co、Fe、Mn、Ni）。作者构建了C-X复合材料催化过一硫酸盐（PMS）降解水中有机污染物体系，研究了不同催化剂、不同氧化剂、催化剂投加量等因素对反应的影响，并验证了反应体系中存在的主要自由基种类，最后采用SEM、TEM、EDS及XPS表征手段对C-Co样品微观形貌等进行了分析。研究发现不同C-X复合材料催化激活PMS性能不同。其中，C-Co复合材料催化效率最高，且目标物降解过程符合拟一级动力学模型；C-Co复合材料对PMS、PS、H2O2均具有一定的催化作用，由高到低依次为：C-Co/PMS > C-Co/PS > C-Co/H2O2；随着催化剂投加量增加，目标物降解速率由于催化活性位点的增加而加快；3次重复利用后，C-Co复合材料催化活性仍保持在85%以上。自由基淬灭实验证明了C-Co/PMS体系中主要存在的活性物质为·OH和·SO4–。SEM和TEM表征结果显示C-Co复合材料由片状结构和针状结构拼接组装而成，Co离散分布在材料内部和表面；EDS分析表明C-Co样品中主要元素组成为C、O、S、Co、Na；XPS表征结果发现，C-Co复合材料中Co呈现价态为正2价，且Co2+是催化激活PMS的关键因素。
英文摘要
With the increasing prominence of energy and environment, the recycling of heavy metals is of great significance. To realize heavy metal recycling and resource utilization, The heavy metal-ions were recycled using strong acidic cation resin, and carbon-based metal composites (C-X, X=Co, Fe, Mn, Ni) were successfully prepared by an anaerobic carbonized method at 600 ℃. Catalytic performance of C-X composite was investigated by the activation of peroxymonosulfate(PMS) for removal of contaminants. The effect of diverse catalysts, oxidants and catalyst dosage were studied, and the main free radicals were also identified. The microscopic morphology and other characteristics of C-Co sample were characterized by SEM, TEM, EDS and XPS. The results showes that C-Co composite has a higher catalytic efficiency than others, and contaminations degradation is fitting well with the pseudo-first order kinetics model. C-Co composite also showed a different catalytic ability of PMS, PS and H2O2, and the order of catalytic efficiency was C-Co/PMS>C-Co/PS>C-Co/H2O2. In addition, with the increase of catalyst dosage, the degradation rate of target could be improved due to the increase of the catalytic activity sites. The results of the catalyst recovery experiment showed that the catalytic activity of C-Co composite remains above 85 %. The quenching study showed that main free radicals in C-Co/PMS system are·OH and·SO4-. SEM and TEM characterization analysis showed that C-Co composite is composed of piece-like and needle-like structure, and Co disperses on the catalyst interior and surface. EDS analysis showed that the main elements in C-Co sample are C, O, S, Co and Na. The results of XPS characterization showed that the cobalt in the compounds presentes a high-spin Co2+state, which was a key factor for PMS activation.
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