DEGRADATION OF METHYLENE BLUE IN WATER BY SINGLET OXYGEN GENERATED FROM FLOW-BY REACTOR BASED ON AIR DIFFUSION CATHODE
-
摘要: 构建了钛基二氧化钌(Ti/RuO2)阳极耦合空气扩散阴极(ADC)的电化学氧化体系,利用过流式反应器对亚甲基蓝(MB)进行氧化去除。结果表明:ADC阴极在200 mA电流下产生H2O2的稳定浓度达到45.33 mg/L,电流效率为65.10%。ADC-RuO2体系对有机污染物的氧化具有选择性,几乎不能氧化苯甲酸钠,但对亚甲基蓝等染料具有较强的氧化作用。且该体系在叠氮化钠和2,5二甲基呋喃等存在时氧化能力受到显著抑制,证明其主要的活性氧化物为单线态氧(~1O2)。在停留时间为2 min和电流为200 mA条件下,该体系对0.1 mmol/L MB的去除率达到99%,并且MB浓度降低90%时对应的能耗为0.25 kW·h/m3。Abstract: In this study, an electrochemical oxidation system consisting of Ti/RuO2 anode and air diffusion cathode(ADC) was constructed, to oxidative remove methylene blue(MB) in a flow-by reactor. The results showed that the stable concentration of H2O2 produced by ADC reached 45.33 mg/L under the current of 200 mA, with a current efficiency of 65.10%. The ADC-RuO2 system was selective for the oxidation of organic pollutants, since it barely oxidized sodium benzoate but showed a strong decolorizing effect on dyes such as methylene blue. In addition, the oxidizing ability was significantly inhibited in the presence of sodium azide and 2,5 dimethylfuran, suggesting the main active oxidant was singlet oxygen(~1O2). At the residence time of 2 min and 200 mA, the removal efficiency of 0.1 mmol/L MB reached 99% in the system. Furthermore, the energy consumption for reducing the MB concentration by 90% was 0.25 kW·h/m3.
-
Key words:
- electrochemical oxidation /
- air diffusion cathode /
- RuO2 anode /
- singlet oxygen /
- flow-by reactor
-
[1] BRILLAS E,SIRÉS I,OTURAN M A.Electro-Fenton process and related electrochemical technologies based on Fenton's reaction chemistry[J].Chemical Reviews,2009,109(12):6570-6631. [2] 李文刚,孙耀胜,么强,等.新型有机污染物污染现状及深度处理工艺研究进展[J].环境工程,2021,39(8):11. [3] 胡承志,刘会娟,曲久辉.电化学水处理技术研究进展[J].环境工程学报,2018,12(3):677-696. [4] CHATZISYMEON E,DIMOU A,MANTZAVINOS D,et al.Electrochemical oxidation of model compounds and olive mill wastewater over DSA electrodes:1.The case of Ti/IrO2 anode[J].Journal of Hazardous Materials,2009,167(1/2/3):268-274. [5] TZEDAKIS T,SAVALL A.Electrochemical regeneration of Ce (Ⅳ) for oxidation of p-methoxytoluene[J].Journal of Applied Electrochemistry,1997,27(5):589-597. [6] CRETIN M,OTURAN M A.Electro-Fenton Process[M].2018. [7] WANG N,ZHENG T,ZHANG G,et al.A review on Fenton-like processes for organic wastewater treatment[J].Journal of Environmental Chemical Engineering,2016,4(1):762-787. [8] KEN D S,SINHA A.Dimensionally stable anode (Ti/RuO2) mediated electro-oxidation and multi-response optimization study for remediation of coke-oven wastewater[J].Journal of Environmental Chemical Engineering,2021,9(1):105025. [9] BONOLA B,AGUILAR D,FUENTES-CAMARGO I,et al.Implications to enhance sulfamethoxazole degradation using statistical optimization of either active chlorine concentration or ORP in an electrochemical reactor[J].Journal of Environmental Chemical Engineering,2020,8(5):104179. [10] WANG C J,HOFMANN M,SAFARI A,et al.Chlorine is preferred over bisulfite for H2O2 quenching following UV-AOP drinking water treatment[J].Water Research,2019,165:115000. [11] YANG Z C,QIAN J S,YU A Q,et al.Singlet oxygen mediated iron-based Fenton-like catalysis under nanoconfinement[J].Proceedings of the National Academy Sciences of the United States of America,2019,116(14):6659-6664. [12] 田世超.电化学催化氧化降解氰化物废水研究[D].天津:河北工业大学,2015. [13] BERL E.A new cathodic process for the production of H2O2[J].Transactions of the Electrochemical Society,1939,76(1):359. [14] WANG J W,LI C L,RAUF M,et al.Gas diffusion electrodes for H2O2 production and their applications for electrochemical degradation of organic pollutants in water:a review[J].Science of the Total Environment,2021,759:143459. [15] AN J K,LI N,ZHAO Q,et al.Highly efficient electro-generation of H2O2 by adjusting liquid-gas-solid three phase interfaces of porous carbonaceous cathode during oxygen reduction reaction[J].Water Research,2019,164:114933. [16] SUN F W,CHEN T H,ZOU X H,et al.A quantitative analysis of hydroxyl radical generation as H2O2 encounters siderite:kinetics and effect of parameters[J].Applied Geochemistry,2021,126:104893. [17] ZHU S S,LI X J,KANG J,et al.Persulfate Activation on crystallographic manganese oxides:mechanism of singlet oxygen evolution for nonradical selective degradation of aqueous contaminants[J].Environmental Science& Technology,2019,53(1):307-315. [18] ENTRADAS T,WALDRON S,VOLK M.The detection sensitivity of commonly used singlet oxygen probes in aqueous environments[J].Journal of Photochemistry and Photobiology B,2020,204:111787. [19] HELD A M,HURST J K.Ambiguity associated with use of singlet oxygen trapping agents in myeloperoxidase-catalyzed oxidations[J].Biochemical and Biophysical Research Communications,1978,81(3):878-885. [20] HELD A,HALKO D,HURST J.Mechanisms of chlorine oxidation of hydrogen peroxide[J].Journal of the American Chemical Society,1978,100(18):5732-5740. [21] XIA C,XIA Y,ZHU P,et al.Direct electrosynthesis of pure aqueous H2O2 solutions up to 20% by weight using a solid electrolyte[J].Science,2019,366(6462):226-231. [22] DENG Y,ENGLEHARDT J D.Treatment of landfill leachate by the Fenton process[J].Water Research,2006,40(20):3683-3694. [23] BAÑUELOS J A,GARCÍA-RODRÍGUEZ O,EL-GHENYMY A,et al.Advanced oxidation treatment of malachite green dye using a low cost carbon-felt air-diffusion cathode[J].Journal of Environmental Chemical Engineering,2016,4(2):2066-2075. [24] BRILLAS E.A review on the degradation of organic pollutants in waters by UV photoelectro-Fenton and solar photoelectro-Fenton[J].Journal of the Brazilian Chemical Society,2014,25(3):393-417. [25] SAMSAMI S,MOHAMADI M,SARRAFZADEH M-H,et al.Recent advances in the treatment of dye-containing wastewater from textile industries:overview and perspectives[J].Process Safety and Environmental Protection,2020,143:138-163. [26] SHU Z Q,BOLTON J R,BELOSEVIC M,et al.Photodegradation of emerging micropollutants using the medium-pressure UV/H2O2 advanced oxidation process[J].Water Research,2013,47(8):2881-2889. [27] BOLTON J R,BIRCHER K G,TUMAS W,et al.Figures-of-merit for the technical development and application of advanced oxidation technologies for both electric-and solar-driven systems (IUPAC Technical Report)[J].Pure and Applied Chemistry,2001,73(4):627-637. [28] ORTS F,BONASTRE J,FERNANDEZ J,et al.Effect of chloride on the one step electrochemical treatment of an industrial textile wastewater with tin dioxide anodes.The case of trichromy procion HEXL[J].Chemosphere,2020,245:125396. [29] PEREIRA L A,de LIMA ALMEIDA D A,COUTO A B,et al.Titanium dioxide/oxidized carbon fiber electrodes electrochemically produced and their influences on Brilliant Green dye degradation[J].Materials Research Bulletin,2020,122:110642. [30] DORIA A R,PUPO M,SANTOS G O S,et al.Electrochemical oxidation of indanthrene blue dye in a filter-press flow reactor and toxicity analyses with Raphidocelis subcapitata and Lactuca sativa[J].Ecotoxicology and Environmental Safety,2020,198:110659.
点击查看大图
计量
- 文章访问数: 201
- HTML全文浏览量: 11
- PDF下载量: 3
- 被引次数: 0