PbO2/Sb-SnO2/TiO2纳米管阵列电极电化学氧化降解罗丹明B

doi:10.1016/S1872-2067(19)63342-5

催化学报 ›› 2019, Vol. 40 ›› Issue (6): 917-927.DOI: 10.1016/S1872-2067(19)63342-5

PbO₂/Sb-SnO₂/TiO₂纳米管阵列电极电化学氧化降解罗丹明B

武佳^a, 朱凯^a, 徐浩^b, 延卫^b

a 西安西电开关电气有限公司, 陕西西安 710049;
b 西安交通大学环境科学与工程系, 动力工程多相流国家重点实验室, 陕西西安 710049

收稿日期:2018-11-19 修回日期:2019-03-04 出版日期:2019-06-18 发布日期:2019-04-26
通讯作者: 徐浩, 延卫
基金资助:
国家自然科学基金（21507104）；陕西省自然科学基础研究计划（2017JM2015）.

Electrochemical oxidation of rhodamine B by PbO₂/Sb-SnO₂/TiO₂ nanotube arrays electrode

Jia Wu^a, Kai Zhu^a, Hao Xu^b, Wei Yan^b

a Xi'an XD Switchgear Electric Co., Ltd., Xi'an 710049, Shaanxi, China;
b Department of Environmental Science and Engineering, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an 710049, Shaanxi, China

Received:2018-11-19 Revised:2019-03-04 Online:2019-06-18 Published:2019-04-26
Contact: S1872-2067(19)63342-5
Supported by:
This work is supported by the National Natural Science Foundation of China (21507104) and Natural Science Basic Research Plan in Shaanxi Province of China (2017JM2015).

摘要/Abstract

摘要：

罗丹明B（RhB）在印染废水中广泛存在，具有难降解和易积累等特点，严重威胁生态系统和人类健康，因此寻找一种高效、清洁、经济的处理方法引起人们的广泛关注.电化学氧化法因其操作简单、环境友好等特点而广泛应用于难处理废水或有毒废水的降解，但过多的能源消耗限制了其进一步应用.在电化学氧化过程中，电极材料的选择是影响电催化性能的重要因素之一，目前的电极材料主要有硼掺杂金刚石电极、IrO₂电极、RuO₂电极和PbO₂电极等.在这些电极材料中，PbO₂电极因价格低廉、导电性良好、化学稳定性好及析氧电位高等优点而成为具有潜力的电极材料之一.近年来，为了提高PbO₂电极的电催化活性和稳定性，研究者对其进行了一系列掺杂改性，如Cu，Bi，Ce，Fe和F等金属或非金属掺杂，以及与TiO₂，SnO₂，ZrO₂，Co₃O₄和TiN等其他化合物复合等.
相比于传统的PbO₂电极基底Ti，TiO₂纳米管阵列具有高度有序、垂直取向、表面积大及亲水性良好等优势，这些特性可使其成为一个更好的载体，关于其做基底负载电催化活性层的研究引起了人们的广泛关注.本文以TiO₂纳米管阵列作为基体，通过微波法沉积Sb-SnO₂中间层，电沉积法沉积PbO₂b表层（含α-PbO₂内层和β-PbO₂外层），制得一种复合DSA阳极材料，并将其用于处理RhB废水.通过扫描电镜（FE-SEM）、X射线衍射（XRD）和电化学测试等手段对该复合电极进行了表征，系统探讨了RhB初始浓度、电流密度、pH值、温度和氯离子浓度等因素对电化学氧化降解过程的影响，并对电极稳定性及RhB降解机理进行了深入研究.
SEM和XRD结果表明，PbO₂/Sb-SnO₂/TiO₂纳米管阵列电极表面涂层覆盖紧密，电化学测试结果表明该电极寿命达815 h.RhB电化学氧化实验结果发现，RhB降解过程遵循准一级动力学模型，且高的电流密度、中性环境、低温和氯离子的添加均有利于其降解，但电流密度过高以及人工降温均会造成能耗过大，而氯离子的加入会带来潜在的二次污染，故在实际应用中需根据实际情况进行调节.此外，通过系统研究不同参数的影响，发现该复合电极对外界环境具有较强的适应性及催化能力，而降解机理的提出有利于我们更好地研究降解过程中变化.综上可知，该复合电极较强的稳定性及催化活性使其在电化学氧化降解废水中具有较大潜在应用前景.

关键词: TiO₂纳米管阵列, 电化学氧化, 罗丹明B, 降解机理

Abstract:

A PbO₂/Sb-SnO₂/TiO₂ nanotube array composite electrode was successfully synthesized and its electrochemical oxidation properties were investigated. Field-emission scanning electron microscopy (FE-SEM) and X-ray diffraction (XRD) results showed that the PbO₂ coating was composed of an α-PbO₂ inner layer and a β-PbO₂ outer layer. Accelerated life measurement indicated that the composite electrode had a lifetime of 815 h. Rhodamine B (RhB) was employed as a model pollutant to analyze the electrocatalytic activity of the electrode. The effects of initial RhB concentration, current density, initial pH, temperature, and chloride ion concentration on the electrochemical oxidation were investigated in detail. Inductively coupled plasma atomic emission spectroscopy (ICP-AES) results suggested that the concentration of leached Pb²⁺ in the electrolyte during the electrocatalytic oxidation process can be neglected. Finally, the degradation mechanism during the electrocatalytic oxidation process was proposed based on the results of solid-phase micro-extraction-gas chromatography-mass spectrometry (SPME-GC-MS). The high electrocatalytic performance of the composite electrode makes it a promising anode for the treatment of organic pollutants in aqueous solution.

Key words: TiO₂ nanotube array, Electrochemical oxidation, Rhodamine B, Degradation mechanism

武佳, 朱凯, 徐浩, 延卫. PbO₂/Sb-SnO₂/TiO₂纳米管阵列电极电化学氧化降解罗丹明B[J]. 催化学报, 2019, 40(6): 917-927.

Jia Wu, Kai Zhu, Hao Xu, Wei Yan. Electrochemical oxidation of rhodamine B by PbO₂/Sb-SnO₂/TiO₂ nanotube arrays electrode[J]. Chinese Journal of Catalysis, 2019, 40(6): 917-927.

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PbO₂/Sb-SnO₂/TiO₂纳米管阵列电极电化学氧化降解罗丹明B

Electrochemical oxidation of rhodamine B by PbO₂/Sb-SnO₂/TiO₂ nanotube arrays electrode

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