Selective Electrocatalytic Degradation of Odorous Mercaptans Derived from S-Au Bond Recongnition on a Dendritic Gold/Boron-Doped Diamond Composite Electrode

被引:45
作者
Chai, Shouning [1 ,2 ]
Wang, Yujing [3 ]
Zhang, Ya-nan [1 ]
Liu, Meichuan [1 ]
Wang, Yanbin [1 ]
Zhao, Guohua [1 ]
机构
[1] Tongji Univ, Shanghai Key Lab Chem Assessment & Sustainabil, Sch Chem Sci & Engn, Shanghai 200092, Peoples R China
[2] Xian Univ Architecture & Technol, Coll Sci, Xian 710055, Shaanxi, Peoples R China
[3] Xian Technol Univ, Sch Mat & Chem Engn, Xian 710032, Shaanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
TRACE ORGANIC CONTAMINANTS; GOLD NANOPARTICLES; METHYL MERCAPTAN; ELECTROCHEMICAL TRANSFORMATION; MOLECULAR RECOGNITION; HYDROXYL RADICALS; FLUORESCENT-PROBE; WASTE-WATER; REMOVAL; ADSORPTION;
D O I
10.1021/acs.est.7b00393
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
To improve selectivity of electrocatalytic degradation of toxic, odorous mercaptans, the fractal-structured dendritic Au/BDD (boron-doped diamond) anode with molecular recognition is fabricated through a facile replacement method. SEM and TEM characterizations show that the gold dendrites are single crystals and have high population of the Au (111) facet. The distinctive structure endows the electrode with advantages of low resistivity, high active surface area, and prominent electrocatalytic activity. To evaluate selectivity, the dendritic Au/BDD is applied in degrading two groups of synthetic wastewater containing thiophenol/2-mercaptobenzimidazole (targets) and phenol/2-hydroxybenzimidazole (interferences), respectively. Results show that targets removals reach 91%/94%, while interferences removals are only 58%/48% in a short time. The corresponding degradation kinetic constants of targets are 3.25 times and 4.1 times that of interferences in the same group, demonstrating modification of dendritic gold on BDD could effectively enhance electrocatalytic target-selectivity. XPS and EXAFS further reveal that the selective electrocatalytic degradation derives from preferential recognition and fast adsorption to thiophenol depending on strong Au-S bond. The efficient, selective degradation is attributed to the synergetic effects between accumulative behavior and outstanding electrochemical performances. This work provides a new strategy for selective electrochemical degradation of contaminants for actual wastewater treatment.
引用
收藏
页码:8067 / 8076
页数:10
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