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作 者:杨丙衡 安路阳 张立涛 宋迪慧 刘合鑫 YANG Bingheng;AN Luyang;ZHANG Litao;SONG Dihui;LIU Hexin(Sinosteel Anshan Research Institute of Thermo-energy Company Limited,Anshan 114000,Liaoning,China;Engineering Research Center for Iron and Steel Industry Wastewater Advanced Treatment Technology of Liaoning Province,Anshan 114000,Liaoning,China;Environmental Engineering Academician Experts Workstation,Anshan 114000,Liaoning,China)
机构地区:[1]中钢集团鞍山热能研究院,辽宁鞍山114000 [2]辽宁省钢铁行业废水深度处理技术工程研究中心,辽宁鞍山114000 [3]环境工程院士工作站,辽宁鞍山114000
出 处:《化工进展》2020年第10期4256-4267,共12页Chemical Industry and Engineering Progress
基 金:辽宁省重点研发计划指导计划(2018230004)。
摘 要:电催化技术深度处理焦化废水仍受极板导电性和催化活性制约而无法广泛应用。本文在以掺杂锑的二氧化锡的钛网(Ti/SnO2-Sb)为底层、以掺杂铈的二氧化铅(PbO2-Ce)为顶层的二维结构之间插入良好导电性的非离子型高聚化合物聚吡咯(PPy),形成具有三维结构的Ti/SnO2-Sb/PPy/PbO2-Ce电极能够增加电流效率,提高催化活性。分别通过X射线衍射图谱、高分辨率透射电子显微镜、X射线光电子能谱和热重分析来表征电极的结构、元素的化学状态和热稳定性,通过线性扫描伏安法和循环伏安法测试电极的电化学表面行为。分析表明,铈的掺杂使极板羟基自由基(·OH)产生量有较大增幅;PPy中间层的插入增强了电极热稳定性,使电流效率提升至7.55%。电化学分析表明Ti/SnO2-Sb/PPy/PbO2-Ce电极具有较高的活性表面积和析氧电位。为使极板达到最佳应用条件,通过响应面法得到一组预测优化参数:电流密度161.18A/m2,电解质浓度5.90g/L,极板间距1.58cm,初始pH为9.05。在最优条件下,对焦化废水的降解效率达到90.47%,能耗为0.787kW·h/g,并据此对可能得催化氧化原理提供预测。The advanced treatment of coking wastewater by electrocatalytic technology is still limited bythe insufficient conductivity and catalytic activity of the plates and cannot be widely used. Nonconductivepolypyrrole(PPy) with good conductivity was inserted into the two-dimensional structure with antimony-doped tin dioxide(Ti/SnO2-Sb) as the bottom layer and cerium-doped lead dioxide(PbO2-Ce) as the toplayer, to form a three-dimensional Ti/SnO2-Sb/PPy/PbO2-Ce electrode that can increase the currentefficiency and improve the catalytic activity. The structure of the electrode, the chemical state of theelement, and the thermal stability were characterized by X-ray diffraction patterns, high-resolutiontransmission electron microscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis,respectively. Electrochemical surface behavior of the electrodes was tested by linear scanning voltammetryand cyclic voltammetry. The analysis showed that the doping of cerium significantly increased the amountof hydroxyl radicals(·OH) on the plate and the insertion of PPy into the intermediate layer improved theelectrode’s thermal stability and increased the current efficiency to 7.55%. Electrochemical analysisshowed that the Ti/SnO2-Sb/PPy/PbO2-Ce electrode had high active surface area and oxygen evolutionpotential. In order to achieve the best performance for the plates, a set of optimal operation parameterswere predicted by using the response surface method as current density 161.18 A/m2, electrolyteconcentration 5.90 g/L, plate spacing 1.58 cm, and initial pH 9.05. Under the optimal conditions, thedegradation efficiency of coking wastewater reached 90.47%, and the energy consumption was 0.787 kW·h/g.Based on the results, the possible catalytic oxidation principles was provided.
关 键 词:电化学 焦化废水 二氧化铅电极 响应面法 环境 催化
分 类 号:X703.1[环境科学与工程—环境工程]
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