Abstract
Treatment of organic contaminants in waste acid via electrochemical oxidation process has drawn sustained attention. Inspired by the electro-generation of persulfate from homogeneous sulfate (SO42-) in waste acid and the catalytic activity of heterogeneous tourmaline, this study aimed to investigate the feasibility of in-situ persulfate electro-generation and activation via utilizing homogeneous–heterogeneous hybrid catalysts system (SO42-/tourmaline) for organic contaminants removal in high chemical oxygen demand (COD) sulfate-containing waste acid. p-Aminodiphenylamine (RT-Base) was selected as a model organic contaminant to explore the mechanism of electrolysis/SO42-/tourmaline system. No RT-Base was detected after 60 min reaction in electrolysis/SO42-/tourmaline system. The formation of •OH and SO4•− in electrolysis/SO42-/tourmaline system made contributions to the RT-Base degradation. Degradation intermediates of RT-Base were identified and possible degradation pathway was proposed. Additionally, the application of electrolysis/SO42-/tourmaline system in treating the real RT-Base waste acid, which contained high COD and SO42-, was explored. Results showed that the COD removal rate was 67.94% under the optimal conditions, and the electrolysis/SO42-/tourmaline system could enhance the biodegradability of RT-Base waste acid. Furthermore, the electrolysis/SO42-/tourmaline system followed by the activated sludge process achieved a high COD removal efficiency (99.09%). Microbial DNA analysis suggested that Bacteroidetes, Proteobacteria, and Actinobacteria were the dominant bacterial phyla in the activated sludge; and metabolism was the predominant microbial function. In-situ electro-generation of persulfate/SO4•− for organics degradation achieved efficient utilization of waste sulfate. Electrochemical oxidation process with activated sludge process as a post-treatment showed great potential in the treatment of organics in high-sulfate waste acid.
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