Fabrication of a stable Ti/Pb-TiOxNWs/PbO2 anode and its application in benzoquinone degradation

Fabrication of a stable Ti/Pb-TiOxNWs/PbO2 anode and its application in benzoquinone degradation
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稳定Ti/Pb-TiOxNWs/PbO2阳极的制备及其在苯醌降解中的应用

DOI:
10.1016/j.electacta.2020.137532
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发表时间:
2020-12
影响因子:
6.6
通讯作者:
Yingjuan Guo
Yingjuan Guo
中科院分区:
材料科学2区
文献类型:
--
作者:
Lihua Yu;Juanqin Xue;Lihua Zhang;Changbin Tang;Yingjuan Guo

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摘要为了延缓钛基体的钝化以及提高PbO 2涂层与钛基体的结合力,采用碱腐蚀、离子置换和高温煅烧等方法在多孔钛表面原位形成了钛-铅复合氧化物纳米线(Pb-TiOxNWs)中间层。同时制备了以多孔钛为基体的Ti/PbO 2和Ti/TiO 2纳米线/PbO 2电极,并进行了对比。采用扫描电子显微镜(SEM)、X射线衍射(XRD)和X射线光电子能谱(XPS)对制备的中间层和PbO 2涂层的表面结构和形貌进行了表征。通过循环伏安法(CV)、线性扫描伏安法(LSV)和交流阻抗谱(EIS)分析了复合氧化物中间层对PbO 2电极电化学性能的影响。对具有和不具有不同中间层的电极进行加速寿命测试。结果表明,PbOx被引入到二氧化钛的三维网络结构中,形成Pb-TiOxNW。Ti/Pb-TiOxNWs/PbO 2电极的表面由于PbO 2的粒径较小而更致密。在Ti/Pb-TiOxNW上沉积的PbO 2具有β(110)择优取向。Ti/Pb-TiOxNW/PbO 2的析氧电位达到最大值2.19V。加速寿命试验表明,与Ti/PbO 2和Ti/TiO 2纳米线/PbO 2相比,Ti/Pb-TiOxNW/PbO 2电极寿命分别提高了91.7%和35.3%。因此,可以得出结论,通过添加Pb-TiOxNW中间层,钛基PbO 2电极实现了显著改善的形貌和电化学性能。特别地,PbO 2涂层电极的电化学稳定性通过Pb-TiOxNWs中间层显著改善。将该电极用于100 mg/L废水中苯醌的电化学氧化。结果表明,氯离子在提高电氧化降解电流效率方面起着至关重要的作用。在相同条件下,NaCl存在下的COD去除率比硫酸盐存在下的COD去除率高45%。中间产物的HPLC分析结果表明,氯离子电生成的氧化剂比硫酸根电生成的氧化剂具有更强的开环和矿化能力。
Abstract To delay passivation of a titanium (Ti) substrate as well as enhance adhesion between an electrodeposited PbO2 coating and the Ti substrate, a titanium-lead composite oxide nanowire (Pb-TiOxNWs) intermediate layer was formed in situ on the surface of porous Ti by alkali etching, ion substitution, and high-temperature calcination. At the same time, Ti/PbO2 and Ti/TiO2NWs/PbO2 electrodes with porous Ti as a matrix were prepared for comparison. The surface structure and morphology of the prepared intermediate layer and the PbO2 coating were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The influences of the composite oxide intermediate layer on the electrochemical performance of the PbO2 electrode were analyzed by cyclic voltammetry (CV), linear sweep voltammetry (LSV), and AC impedance spectroscopy (EIS). Accelerated lifetime tests were performed for electrodes with and without different intermediate layers. The results showed that PbOx was incorporated into the titanium dioxide three-dimensional network structure, resulting in formation of Pb-TiOxNWs. The surface of the Ti/Pb-TiOxNWs/PbO2 electrode was denser due to the smaller particle size of PbO2. The preferred crystal orientation of β(110) was observed for PbO2 deposited on Ti/Pb-TiOxNWs. The oxygen evolution potential reached a maximum of 2.19V for Ti/Pb-TiOxNWs/PbO2. Accelerated life tests showed that compared with Ti/PbO2 and Ti/TiO2NWs/PbO2, the electrode life of Ti/Pb-TiOxNWs/PbO2 was increased by 91.7% and 35.3%, respectively. Therefore, it can be concluded that significantly improved morphology and electrochemical performance were achieved for titanium-based PbO2 electrodes by the addition of a Pb-TiOxNWs intermediate layer. In particular, the electrochemical stability of the PbO2 coating electrodes was improved markedly by the Pb-TiOxNWs intermediate layer. The electrodes were used for electrochemical oxidation of benzoquinone in wastewater (100mg/L). It was found that chloride ions played a critical role in improving the current efficiency of electro-oxidative degradation. Under the same conditions, the COD removal rate in the presence of NaCl was 45% higher than in the presence of sulfate. The results of HPLC analysis of the intermediate products indicated that the oxidants electro-generated by chloride ions had stronger ring-opening and mineralization capabilities than those electro-generated by sulfate ions.
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发表时间: 2016-05
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发表时间: 1995-12
影响因子: 4
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发表时间: 2013
期刊: Electrocatalysis
影响因子: 3.1
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通讯作者: Alan H. Degaki;Gabriel F. Pereira;R. Rocha‐Filho;N. Bocchi;S. Biaggio
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影响因子: 8.6
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发表时间: 2020-01
影响因子: 6.6
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