新型Ti/TiOxHy/Sb-SnO2电极上苯胺电化学氧化反应

doi:10.1016/S1872-2067(16)62555-X

催化学报 ›› 2016, Vol. 37 ›› Issue (11): 1860-1870.DOI: 10.1016/S1872-2067(16)62555-X

新型Ti/TiO_xH_y/Sb-SnO₂电极上苯胺电化学氧化反应

李晓良, 徐浩, 延卫

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:2016-07-29 修回日期:2016-09-19 出版日期:2016-11-25 发布日期:2016-11-25
通讯作者: Hao Xu,Tel.:+86-15829780706; Fax:+86-29-82664731; E-mail:xuhao@xjtu.edu.cn;Wei Yan, E-mail:yanwei@xjtu.edu.cn
基金资助:
国家自然科学基金（21507104）；中央高校基础研究基金.

Electrochemical oxidation of aniline by a novel Ti/TiO_xH_y/Sb-SnO₂ electrode

Xiaoliang Li, Hao Xu, Wei Yan

Department of Environmental Science and Engineering, State Key Laboratory of Multiphase flow in Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, Shan'xi, China

Received:2016-07-29 Revised:2016-09-19 Online:2016-11-25 Published:2016-11-25
Contact: Hao Xu,Tel.:+86-15829780706; Fax:+86-29-82664731; E-mail:xuhao@xjtu.edu.cn;Wei Yan, E-mail:yanwei@xjtu.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (21507104) and the Fundamental Research Funds for the Central Universities of China.

摘要/Abstract

摘要：

苯胺是一种重要的化工原料，广泛应用于印染、制药、造纸、橡胶等领域.随着化工行业的迅速发展，苯胺的需求量越来越大.然而，苯胺毒性高，大量使用势必造成水体中苯胺浓度的升高，给人类健康及生态环境造成危害.因此，急需一种高效、洁净、经济的方法处理含苯胺废水.
电化学氧化法比较新颖，相比传统废水处理方法，它具有高效、简单、清洁等优点，因此被应用于很多废水处理当中，但过多的能耗限制了其进一步广泛应用.阳极作为电化学氧化技术的核心部件，直接影响到电化学氧化反应性能.因此开发出一种高效、经济的阳极材料很有必要.此外，对苯胺降解条件的优化也同样重要.
关于苯胺电化学氧化，已有的研究包括Pt电极、PbO₂电极和石墨电极等阳极材料.比较而言，Ti/Sb-SnO₂电极具有制备工艺简单，析氧过电位较高，材料廉价和电催化性能较强等优点.然而，它的稳定性仍有待提高.因此本文制备了一种高稳定性的Ti/TiO_xH_y/Sb-SnO₂电极，并用于处理苯胺废水.较为系统地研究了电流密度、苯胺初始浓度、pH、NaCl投加量及反应器类型对苯胺电催化氧化性能的影响，同时采用扫描电镜（SEM）、X射线衍射（XRD）和电化学测试对该电极进行了表征，并应用紫外-可见光谱、化学需氧量、电流效率及能耗对不同参数进行评定和优化.
SEM及XRD结果表明，Ti/TiO_xH_y/Sb-SnO₂电极涂层覆盖比较完全、紧实，未出现裂缝的发生，因而有利于提高电极稳定性.循环伏安测试结果表明，此电极具备较高的析氧过电位（2.0 V vs Ag/AgCl）及电化学孔隙度（76.31%），因此有利于电极催化性能的提高.苯胺电化学氧化实验结果发现，该反应符合准一级动力学模型，且高电流密度、酸性环境、适当NaCl投加量（0.2 wt%）更有利于苯胺的降解.另外，Ti/TiO_xH_y/Sb-SnO₂电极在三维反应器中对苯胺的处理效果要远远好于在二维反应器中.可以看出，Ti/TiO_xH_y/Sb-SnO₂电极具有较好的处理苯胺性能，可为苯胺废水处理的应用提供了一定的理论指导.

关键词: 苯胺, Ti/TiO_xH_y/Sb-SnO₂电极, 电化学氧化, 氯离子, 三维反应器

Abstract:

Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiO_xH_y/Sb-SnO₂ electrode prepared by the electrodeposition method. Scanning electron micros-copy, X-ray diffraction, and electrochemical measurements were used to characterize its morphol-ogy, crystal structure, and electrochemical properties. Removal of aniline by the Ti/TiO_xH_y/Sb-SnO₂ electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand (COD) analysis under different conditions, including current densities, initial concentrations of aniline, pH values, concentrations of chloride ions, and types of reactor. It was found that a higher current den-sity, a lower initial concentration of aniline, an acidic solution, the presence of chloride ions (0.2 wt% NaCl), and a three-dimensional (3D) reactor promoted the removal efficiency of aniline. Elec-trochemical degradation of aniline followed pseudo-first-order kinetics. The aniline (200 mL of 100 mg·L^-1) and COD removal efficiencies reached 100% and 73.5%, respectively, at a current density of 20 mA·cm^-2, pH of 7.0, and supporting electrolyte of 0.5 wt% Na₂SO₄ after 2 h electrolysis in a 3D reactor. These results show that aniline can be significantly removed on the Ti/TiO_xH_y/Sb-SnO₂ electrode, which provides an efficient way for elimination of aniline from aqueous solution.

Key words: Aniline, Ti/TiO_xH_y/Sb-SnO₂ electrode, Electrochemical oxidation, Chloride ions, Three-dimensional reactor

李晓良, 徐浩, 延卫. 新型Ti/TiO_xH_y/Sb-SnO₂电极上苯胺电化学氧化反应[J]. 催化学报, 2016, 37(11): 1860-1870.

Xiaoliang Li, Hao Xu, Wei Yan. Electrochemical oxidation of aniline by a novel Ti/TiO_xH_y/Sb-SnO₂ electrode[J]. Chinese Journal of Catalysis, 2016, 37(11): 1860-1870.

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新型Ti/TiO_xH_y/Sb-SnO₂电极上苯胺电化学氧化反应

Electrochemical oxidation of aniline by a novel Ti/TiO_xH_y/Sb-SnO₂ electrode

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