Journal Home Online First Current Issue Archive For Authors Journal Information 中文版

Engineering >> 2022, Volume 9, Issue 2 doi: 10.1016/j.eng.2021.11.017

Electrochemical Removal of Chlorophenol Pollutants by Reactive Electrode Membranes: Scale-up Strategy for Engineered Applications

a State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
b State Key Laboratory of NBC Protection for Civilian, Beijing 102205, China

Received: 2021-07-14 Revised: 2021-08-24 Accepted: 2021-11-23 Available online: 2022-01-10

Next Previous

Abstract

Chlorophenols (CPs) are significant refractory pollutants that are highly toxic to humans and other organisms. Reactive electrode membranes (REMs) show considerable potential in the electrochemical removal of refractory pollutants by allowing flow-through operations with convection-enhanced mass transfer. However, relevant studies are commonly performed on the laboratory scale, and there is no straightforward method that guarantees success in scaling up engineered REM reactors. In this study, we demonstrated that a tubular concentric electrode (TCE) configuration with a titanium suboxide ceramic anode and a stainless-steel cathode is suitable for large-scale CPs removal. Both theoretical and experimental results showed that the TCE configuration not only allows the electrode surface to be orthogonal to electric field lines everywhere, but also has an ohmic resistance that is inversely proportional to the length of the electrode. In addition, the TCE configuration can be operated in either the anode-to-cathode (AC) or the cathode-to-anode (CA) mode based on the flow direction, creating adjustable conditions for selective degradation of CPs. This was confirmed by 98% removal of 2,4-dichlorophenol (2,4-DCP) and 72.5% removal of chemical oxygen demand (COD) in the CA mode, in which the kinetic constant was one order of magnitude higher than that for the AC mode under flow-through single-pass operations. This can be explained by the lower activation energy and free energy in the CA mode, as revealed by theoretical calculations and experimental measurements. The TCE configuration is also suitable for a numbering-up strategy to scale up the electrochemical reactor without increasing the ohmic resistance or decreasing the specific electrode area, achieving 99.4% removal of 2,4-DCP with an energy consumption of 1.5 kW·h·m−3 when three TCE modules were employed. This study presents a suitable electrode design configuration for the REM reactor, offering effective strategies to bridge the “Valley of Death” encountered when scaling up the electrochemical removal of CP pollutants.

SupplementaryMaterials

Figures

Fig. 1

Fig. 2

Fig. 3

Fig. 4

Fig. 5

References

[ 1 ] Moreira FC, Boaventura RAR, Brillas E, Vilar VJP. Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters. Appl Catal B 2017;202:217–61. link1

[ 2 ] Radjenovic J, Sedlak DL. Challenges and opportunities for electrochemical processes as next-generation technologies for the treatment of contaminated water. Environ Sci Technol 2015;49(19):11292–302. link1

[ 3 ] Zhu L, Santiago-Schübel B, Xiao H, Hollert H, Kueppers S. Electrochemical oxidation of fluoroquinolone antibiotics: mechanism, residual antibacterial activity and toxicity change. Water Res 2016;102:52–62. link1

[ 4 ] Guo L, Jing Y, Chaplin BP. Development and characterization of ultrafiltration TiO2 Magnéli phase reactive electrochemical membranes. Environ Sci Technol 2016;50(3):1428–36. link1

[ 5 ] Lin H, Peng H, Feng X, Li X, Zhao J, Yang K, et al. Energy-efficient for advanced oxidation of bio-treated landfill leachate effluent by reactive electrochemical membranes (REMs): laboratory and pilot scale studies. Water Res 2021;190:116790. link1

[ 6 ] Zaky AM, Chaplin BP. Porous substoichiometric TiO2 anodes as reactive electrochemical membranes for water treatment. Environ Sci Technol 2013;47 (12):6554–63. link1

[ 7 ] Ma J, Ma J, Zhang C, Song J, Dong W, Waite TD. Flow-electrode capacitive deionization (FCDI) scale-up using a membrane stack configuration. Water Res 2020;168:115186. link1

[ 8 ] Sun M, Wang X, Winter LR, Zhao Y, Ma W, Hedtke T, et al. Electrified membranes for water treatment applications. ACS EST Eng 2021;1(4):725–52. link1

[ 9 ] Noël T, Cao Y, Laudadio G. The fundamentals behind the use of flow reactors in electrochemistry. Acc Chem Res 2019;52(10):2858–69. link1

[10] Sulaymon AH, Abbar AH. Scale-up of electrochemical reactors. In: Kleperis J, Linkov V, editors. Electrolysis. London: IntechOpen Ltd.; 2012. p. 189–202. link1

[11] Goodridge F, Scott K. Electrochemical process engineering. New York: Springer Publishing Co.; 1995. link1

[12] Walsh F, Reade G. Design and performance of electrochemical reactors for efficient synthesis and environmental treatment. Part 2. Typical reactors and their performance. Analyst 1994;119(5):797–803. link1

[13] Walsh FC, Ponce de León C. Progress in electrochemical flow reactors for laboratory and pilot scale processing. Electrochim Acta 2018;280:121–48. link1

[14] Ni XY, Liu H, Wang C, Wang WL, Xu ZB, Chen Z, et al. Comparison of carbonized and graphitized carbon fiber electrodes under flow-through electrode system (FES) for high-efficiency bacterial inactivation. Water Res 2020;168:115150. link1

[15] Wang J, Zhi D, Zhou H, He X, Zhang D. Evaluating tetracycline degradation pathway and intermediate toxicity during the electrochemical oxidation over a Ti/Ti4O7 anode. Water Res 2018;137:324–34. link1

[16] Pourmahmoud N, Sadeghifar H, Torkavannejad A. A novel, state-of-the-art tubular architecture for polymer electrolyte membrane fuel cells: performance enhancement, size and cost reduction. Int J Heat Mass Transf 2017;108(Pt A):577–84. link1

[17] Rabuni MF, Li T, Punmeechao P, Li K. Electrode design for direct-methane micro-tubular solid oxide fuel cell (MT-SOFC). J Power Sources 2018;384:287–94. link1

[18] Ressel S, Laube A, Fischer S, Chica A, Flower T, Struckmann T. Performance of a vanadium redox flow battery with tubular cell design. J Power Sources 2017;355:199–205. link1

[19] You S, Liu B, Gao Y, Wang Y, Tang CY, Huang Y, et al. Monolithic porous Magnéli-phase Ti4O7 for electro-oxidation treatment of industrial wastewater. Electrochim Acta 2016;214:326–35. link1

[20] Gayen P, Chen C, Abiade JT, Chaplin BP. Electrochemical oxidation of atrazine and clothianidin on Bi-doped SnO2–TinO2n–1 electrocatalytic reactive electrochemical membranes. Environ Sci Technol 2018;52(21):12675–84. link1

[21] Pei S, You S, Ma J, Chen X, Ren N. Electron spin resonance evidence for electrogenerated hydroxyl radicals. Environ Sci Technol 2020;54(20):13333–43. link1

[22] Cˇorovic´ S, Pavlin M, Miklavcˇicˇ D. Analytical and numerical quantification and comparison of the local electric field in the tissue for different electrode configurations. Biomed Eng Online 2007;6:37. link1

[23] Hankin A, Bedoya-Lora FE, Ong CK, Alexander JC, Petter F, Kelsall GH. From millimetres to metres: the critical role of current density distributions in photo-electrochemical reactor design. Energy Environ Sci 2017;10:346–60. link1

[24] Zhou J, Wang T, Xie X. Rationally designed tubular coaxial-electrode copper ionization cells (CECICs) harnessing non-uniform electric field for efficient water disinfection. Environ Int 2019;128:30–6. link1

[25] Zhou J, Wang T, Xie X. Locally enhanced electric field treatment (LEEFT) promotes the performance of ozonation for bacterial inactivation by disrupting cell membrane. Environ Sci Technol 2020;54(21):14017–25. link1

[26] Sun L, Wang X, Li M, Zhang S, Wang Q. Anodic titania nanotubes grown on titanium tubular electrodes. Langmuir 2014;30(10):2835–41. link1

[27] Perry SC, Ponce de León C, Walsh FC. Review—the design, performance and continuing development of electrochemical reactors for clean electrosynthesis. J Electrochem Soc 2020;167(15):155525. link1

[28] Ahn Y, Hatzell MC, Zhang F, Logan BE. Different electrode configurations to optimize performance of multi-electrode microbial fuel cells for generating power or treating domestic wastewater. J Power Sources 2014;249:440–5. link1

[29] Jaramillo-Gutiérrez MI, Carreño-Lizcano MI, Ruiz-Lizarazo JO, Pedraza-Avella JA, Rivero EP, Cruz-Díaz MR. Design, mathematical modelling, and numerical simulation of a novel tubular photoelectrochemical reactor and experimental validation by residence time distribution and mass transfer coefficients. Chem Eng J 2020;386:123895. link1

[30] Lei Y, Zhan Z, Saakes M, van der Weijden RD, Buisman CJN. Electrochemical recovery of phosphorus from wastewater using tubular stainless-steel cathode for a scalable long-term operation. Water Res 2021;199:117199. link1

[31] Wang AJ, Wang HC, Cheng HY, Liang B, Liu WZ, Han JL, et al. Electrochemistrystimulated environmental bioremediation: development of applicable modular electrode and system scale-up. Environ Sci Ecotech 2020;3:100050. link1

[32] Wang G, Liu Y, Ye J, Lin Z, Yang X. Electrochemical oxidation of methyl orange by a Magnéli phase Ti4O7 anode. Chemosphere 2020;241:125084. link1

[33] Deborde M, von Gunten U. Reactions of chlorine with inorganic and organic compounds during water treatment—kinetics and mechanisms: a critical review. Water Res 2008;42(1–2):13–51. link1

[34] Cheng X, Guo H, Li W, Yang B, Wang J, Zhang Y, et al. Metal-free carbocatalysis for persulfate activation toward nonradical oxidation: enhanced singlet oxygen generation based on active sites and electronic property. Chem Eng J 2020;396:125107. link1

[35] Ma Y, Gu Y, Jiang D, Mao X, Wang D. Degradation of 2,4-DCP using persulfate and iron/E-carbon micro-electrolysis coupling system. J Hazard Mater 2021;413:125381. link1

[36] Guo H, Kim Y. Scalable multi-electrode microbial electrolysis cells for high electric current and rapid organic removal. J Power Sources 2018;391:67–72. link1

[37] Martínez-Huitle CA, Rodrigo MA, Sirés I, Scialdone O. Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants: a critical review. Chem Rev 2015;115(24):13362–407. link1

[38] He W, Dong Y, Li C, Han X, Liu G, Liu J, et al. Field tests of cubic-meter scale microbial electrochemical system in a municipal wastewater treatment plant. Water Res 2019;155:372–80. link1

Related Research