Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 53, Issue 9, Pages 5195-5201Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.8b06130
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Funding
- National Natural Science Foundation of China [21707016, 51708085]
- China Postdoctoral Science Foundation [2016M600205]
- State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology [HC201705]
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Electrochemical oxidation based on SO4 center dot- and (OH)-O-center dot generated from sulfate electrolyte is a cost-effective method for degradation of persistent organic pollutants (POPs). However, sulfate activation remains a great challenge due to lack of active and robust electrodes. Herein, a B/N codoped diamond (BND) electrode is designed for electrochemical degradation of POPs via sulfate activation. It is efficient and stable for perfluorooctanoic acid (PFOA) oxidation with first-order kinetic constants of 2.4 h(-1) and total organic carbon removal efficiency of 77.4% (3 h) at relatively low current density of 4 mA cm(-2). The good activity of BND mainly originates from a B and N codoping effect. The PFOA oxidation rate at sulfate electrolyte is significantly enhanced (2.3-3.4 times) compared with those at nitrate and perchlorate electrolytes. At sulfate, PFOA oxidation rate decreases slightly in the presence of (OH)-O-center dot quencher while it declines significantly with SO4 center dot- and (OH)-O-center dot quenchers, indicate both SO4 center dot- and (OH)-O-center dot contribute to PFOA oxidation but SO4 center dot- contribution is more significant. On the basis of intermediates analysis, a proposed mechanism for PFOA degradation is that PFOA is oxidized to shorter chain perfluorocarboxylic acids gradually by SO4 center dot- and (OH)-O-center dot until it is mineralized.
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