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Recent advances in the electrochemical oxidation water treatment: Spotlight on byproduct control

Yang Yang

《环境科学与工程前沿(英文)》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1264-7

摘要: Abstract • Byproduct formation mechanisms during electrochemical oxidation water treatment. • Control byproduct formation by quenchers. • Process optimization to suppress byproduct formation. Electrochemical oxidation (EO) is a promising technique for decentralized wastewater treatment, owing to its modular design, high efficiency, and ease of automation and transportation. The catalytic destruction of recalcitrant, non-biodegradable pollutants (per- and poly-fluoroalkyl substances (PFAS), pharmaceuticals, and personal care products (PPCPs), pesticides, etc.) is an appropriate niche for EO. EO can be more effective than homogeneous advanced oxidation processes for the degradation of recalcitrant chemicals inert to radical-mediated oxidation, because the potential of the anode can be made much higher than that of hydroxyl radicals (EOH = 2.7 V vs. NHE), forcing the direct transfer of electrons from pollutants to electrodes. Unfortunately, at such high anodic potential, chloride ions, which are ubiquitous in natural water systems, will be readily oxidized to chlorine and perchlorate. Perchlorate is a to-be-regulated byproduct, and chlorine can react with matrix organics to produce organic halogen compounds. In the past ten years, novel electrode materials and processes have been developed. However, spotlights were rarely focused on the control of byproduct formation during EO processes in a real-world context. When we use EO techniques to eliminate target contaminants with concentrations at μg/L-levels, byproducts at mg/L-levels might be produced. Is it a good trade-off? Is it possible to inhibit byproduct formation without compromising the performance of EO? In this mini-review, we will summarize the recent advances and provide perspectives to address the above questions.

关键词: Electrochemical water treatment     Byproducts     Perchlorate    

Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

《环境科学与工程前沿(英文)》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1345-7

摘要: Abstract • Electrode fouling is characterized by non-destructive characterization. • Electrode fouling is highly dependent on electrochemical process. • Active chlorine can prevent the formation of polymeric fouling film. Electrode fouling is a problem that commonly occurs during electro-oxidation water purification. This study focused on identifying the fouling behavior of Pt electrode associated with the formation of polymeric layer during electro-oxidation of phenol. The in situ electrochemical measurements and non-destructive observation of the electrode morphology were reported. The results demonstrated that the electrode fouling was highly dependent on thermodynamic process of electrode that was controlled by anode potential. At anode potential lower than 1.0 V vs SHE, the direct electro-oxidation caused the electrode fouling by the formation of polymeric film. The fouling layer decreased the electrochemically active surface area from 8.38 cm2 to 1.57 cm2, indicated by the formation of polymeric film with thickness of 2.3 mm, increase in mass growing at a rate of 3.26 μg/cm2/min. The degree to which the anode was fouled was independent of anion in the electrolyte. In comparison, at anode potential higher than 2.7 V vs SHE, the anions (e.g., chloride) could exert a major influence to the behavior of electrode fouling. The presence of chloride was shown to mitigate the fouling of electrode significantly through preventing the formation of polymeric film by active chlorine (e.g., Cl• and Cl2) produced from anodic oxidation of chloride. Since chloride is the most abundant anionic species existing in both natural and engineered water system, this study not only offers a deep insight into the mechanism of electrode fouling, but also suggests strategies for anti-fouling in the presence of chloride in electro-oxidation process.

关键词: Electro-oxidation     Electrode fouling     Polymeric film     Chloride ions    

Electrochemical oxidation of humic acid at the antimony- and nickel-doped tin oxide electrode

TANG Chengli,YAN Wei,ZHENG Chunli

《环境科学与工程前沿(英文)》 2014年 第8卷 第3期   页码 337-344 doi: 10.1007/s11783-013-0545-9

摘要: This work investigated the degradation of humic acid (HA) in aqueous solution by electrochemical oxidation with Antimony- and Nickel-doped Tin oxide electrode (Ni-Sb-SnO /Ti electrode) as the anode. Initial concentrations of HA ranged from 3 to 9 mg·L . Under such a concentration scope, the degradation of HA was a mass transfer controlled process. Degradation rate increased with the increase of HA initial concentration. Test on the effect of tert-butanol revealed that ·OH played an important role in the oxidation of HA. The absence of cation Ca was beneficial to HA degradation, which suggested that both indirect and direct electrolyze happened during the whole electrochemical oxidation process. Alkaly (pH= 12) and neutral (pH= 7) conditions were benefical to HA degradation.

关键词: electrochemical oxidation     humic acid (HA)     natural water     Ni-Sb-SnO2/Ti electrode    

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

《环境科学与工程前沿(英文)》 2022年 第16卷 第4期 doi: 10.1007/s11783-021-1476-5

摘要:

• MES was constructed for simultaneous ammonia removal and acetate production.

关键词: Biocathode     Carbon dioxide     Electrochemical oxidation     Graphite anode     Boron-doped diamond    

An electrochemical process that uses an Fe

Chaojie Jiang, Lifen Liu, John C. Crittenden

《环境科学与工程前沿(英文)》 2016年 第10卷 第4期 doi: 10.1007/s11783-016-0860-z

摘要: A bio-electrochemical fuel cell reactor with cathodic Fe /TiO generates electricity. It destroys recalcitrant pollutants in cathode chamber without photocatalysis. Fe /TiO generates reactive oxygenated species in the dark or under photocatalysis. Cathodic produced ROS (hydroxy radical/superoxide radical) can degrade tetracycline or dyes. Electricity generation is enhanced by semiconductor catalyzed cathodic degradation of pollutants. In this study, a new water treatment system that couples (photo-) electrochemical catalysis (PEC or EC) in a microbial fuel cell (MFC) was configured using a stainless-steel (SS) cathode coated with Fe /TiO . We examined the destruction of methylene blue (MB) and tetracycline. Fe /TiO was prepared using a chemical reduction-deposition method and coated onto an SS wire mesh (500 mesh) using a sol technique. The anode generates electricity using microbes (bio-anode). Connected via wire and ohmic resistance, the system requires a short reaction time and operates at a low cost by effectively removing 94% MB (initial concentration 20 mg·L ) and 83% TOC/TOC under visible light illumination (50 W; 1.99 mW·cm for 120 min, MFC-PEC). The removal was similar even without light irradiation (MFC-EC). The of the MFC-PEC system was approximately 0.675 kWh·m ·order , whereas that of the MFC-EC system was zero. The system was able to remove 70% COD in tetracycline solution (initial tetracycline concentration 100 mg·L ) after 120 min of visible light illumination; without light, the removal was 15% lower. The destruction of MB and tetracycline in both traditional photocatalysis and photoelectrocatalysis systems was notably low. The electron spin-resonance spectroscopy (ESR) study demonstrated that ·OH was formed under visible light, and ·O was formed without light. The bio-electricity-activated O and ROS (reactive oxidizing species) generation by Fe /TiO effectively degraded the pollutants. This cathodic degradation improved the electricity generation by accepting and consuming more electrons from the bio-anode.

关键词: Bio-anode     Photocatalytic cathode     Fe0/TiO2     ESR     Dye and antibiotics     Advanced oxidation    

Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized

Yang Li, Yixin Zhang, Guangshen Xia, Juhong Zhan, Gang Yu, Yujue Wang

《环境科学与工程前沿(英文)》 2021年 第15卷 第1期 doi: 10.1007/s11783-020-1293-2

摘要: Abstract • Gas diffusion electrode (GDE) is a suitable setup for practical water treatment. • Electrochemical H2O2 production is an economically competitive technology. • High current efficiency of H2O2 production was obtained with GDE at 5–400 mA/cm2. • GDE maintained high stability for H2O2 production for ~1000 h. • Electro-generation of H2O2 enhances ibuprofen removal in an E-peroxone process. This study evaluated the feasibility of electrochemical hydrogen peroxide (H2O2) production with gas diffusion electrode (GDE) for decentralized water treatment. Carbon black-polytetrafluoroethylene GDEs were prepared and tested in a continuous flow electrochemical cell for H2O2 production from oxygen reduction. Results showed that because of the effective oxygen transfer in GDEs, the electrode maintained high apparent current efficiencies (ACEs,>80%) for H2O2 production over a wide current density range of 5–400 mA/cm2, and H2O2 production rates as high as ~202 mg/h/cm2 could be obtained. Long-term stability test showed that the GDE maintained high ACEs (>85%) and low energy consumption (<10 kWh/kg H2O2) for H2O2 production for 42 d (~1000 h). However, the ACEs then decreased to ~70% in the following 4 days because water flooding of GDE pores considerably impeded oxygen transport at the late stage of the trial. Based on an electrode lifetime of 46 days, the overall cost for H2O2 production was estimated to be ~0.88 $/kg H2O2, including an electricity cost of 0.61 $/kg and an electrode capital cost of 0.27 $/kg. With a 9 cm2 GDE and 40 mA/cm2 current density, ~2–4 mg/L of H2O2 could be produced on site for the electro-peroxone treatment of a 1.2 m3/d groundwater flow, which considerably enhanced ibuprofen abatement compared with ozonation alone (~43%–59% vs. 7%). These findings suggest that electrochemical H2O2 production with GDEs holds great promise for the development of compact treatment technologies for decentralized water treatment at a household and community level.

关键词: Advanced oxidation process     Electro-peroxone     Gas diffusion electrode     Hydrogen peroxide     Oxygen reduction    

Enhancement of the electrocatalytic oxidation of antibiotic wastewater over the conductive black carbon-PbO

Xiangyu Wang, Yu Xie, Guizhen Yang, Jiming Hao, Jun Ma, Ping Ning

《环境科学与工程前沿(英文)》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1201-9

摘要: • A novel conductive carbon black modified lead dioxide electrode is synthesized. • The modified PbO2 electrode exhibits enhanced electrochemical performances. • BBD method could predict optimal experiment conditions accurately and reliably. • The modified electrode possesses outstanding reusability and safety. The secondary pollution caused by modification of an electrode due to doping of harmful materials has long been a big concern. In this study, an environmentally friendly material, conductive carbon black, was adopted for modification of lead dioxide electrode (PbO2). It was observed that the as-prepared conductive carbon black modified electrode (C-PbO2) exhibited an enhanced electrocatalytical performance and more stable structure than a pristine PbO2 electrode, and the removal efficiency of metronidazole (MNZ) and COD by a 1.0% C-PbO2 electrode at optimal conditions was increased by 24.66% and 7.01%, respectively. Results revealed that the electrochemical degradation of MNZ wastewater followed pseudo-first-order kinetics. This intimates that the presence of conductive carbon black could improve the current efficiency, promote the generation of hydroxyl radicals, and accelerate the removal of MNZ through oxidation. In addition, MNZ degradation pathways through a C-PbO2 electrode were proposed based on the identified intermediates. To promote the electrode to treat antibiotic wastewater, optimal experimental conditions were predicted through the Box-Behnken design (BBD) method. The results of this study suggest that a C-PbO2 electrode may represent a promising functional material to pretreat antibiotic wastewaters.

关键词: Conductive carbon black     PbO2 electrode     Metronidazole     Electrochemical oxidation     Box-Behnken design-response surface method    

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要: Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词: catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

《环境科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 428-434 doi: 10.1007/s11783-013-0517-0

摘要: This work describes the environmentally friendly technology for oxidation of ammonia (NH ) to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation (SCO) over a nanosized Pt-Rh/γ-Al O catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid (H PtCl ) and rhodium (III) nitrate (Rh(NO ) ) with γ-Al O in a tubular fixed-bed flow quartz reactor (TFBR). The characterization of catalysts were thoroughly measured using transmission electron microscopy (TEM), three-dimensional excitation-emission fluorescent matrix (EEFM) spectroscopy, UV-Vis absorption, dynamic light-scattering (DLS), zeta potential meter, and cyclic voltammetry (CV). The results demonstrated that at a temperature of 673K and an oxygen content of 4%, approximately 99% of the NH was removed by catalytic oxidation over the nanosized Pt-Rh/γ-Al O catalyst. N was the main product in NH -SCO process. Further, it reveals that the oxidation of NH was proceeds by the over-oxidation of NH into NO, which was conversely reacted with the NH to yield N . Therefore, the application of nanosized Pt-Rh/γ-Al O catalyst can significantly enhance the catalytic activity toward NH oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-Al O catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.

关键词: ammonia (NH3)     nanosized Pt-Rh/γ-Al2O3 catalyst     excitation-emission fluorescent matrix (EEFM)     selective catalytic oxidation (SCO)     tubular fixed-bed reactor (TFBR)    

Recent advances in electrochemical decontamination of perfluorinated compounds from water: a review

《环境科学与工程前沿(英文)》 2023年 第17卷 第2期 doi: 10.1007/s11783-023-1618-z

摘要:

● Recent advances in the electrochemical decontamination of PFAS are reviewed.

关键词: Perfluorinated compounds     Electrochemical approach     Working mechanisms     Impacting factor     Coupled process    

Research progress in tribo-electrochemistry and tribo-electrochemical polishing

ZHAI Wenjie

《机械工程前沿(英文)》 2007年 第2卷 第4期   页码 463-467 doi: 10.1007/s11465-007-0080-0

摘要: In this paper, the status quo and recent progress in the research on tribo-electrochemistry in aqueous and non-aqueous media, respectively, are reviewed. Much more attention has been paid to the tribo-electrochemical mechanisms for the control of friction and wear. Based on a summary of the conventional polishing principles of hard and brittle materials, the tribo-electrochemical polishing method is proposed. The results of the preliminary test show that tribo-electrochemical polishing is promising to become a critical technology in the high efficient polishing and planarization of microelectronic materials.

关键词: tribo-electrochemical mechanisms     planarization     non-aqueous     tribo-electrochemistry     summary    

Enhanced electrochemical performance of CoNiS@TiCT electrode material through doping of cobalt element

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1440-1449 doi: 10.1007/s11705-023-2333-9

摘要: The composite electrode of CoNiSx and Ti3C2Tx MXene was successfully prepared using a one-step hydrothermal method under the in-situ doping of the cobalt element. The effects of in-situ doping of the cobalt element on the micromorphology and electrochemical performance of the electrodes were investigated. After in-situ doping of the cobalt element, NiS with a needle-like structure was converted into a CoNiSx with petal-like structure. The petal-like CoNiSx with a rough surface was very dense and evenly wrapped on the surface and interlamination of Ti3C2Tx, which helped increase the specific surface area and pore volume of the electrode. Under the identical test conditions, CoNiSx@Ti3C2Tx had a higher specific capacitance and capacitance retention than NiS@Ti3C2Tx. This result indicated that the in-situ doping of the cobalt element promoted the electrochemical performance of the electrode. The energy density of the CoNiSx@Ti3C2Tx/nickel foam (NF)//activated carbon (AC)/NF asymmetric supercapacitor device was 59.20 Wh·kg–1 at a power density of 826.73 W·kg–1, which was much higher than that of NiS@Ti3C2Tx/NF//AC/NF. Three CoNiSx@Ti3C2Tx/NF//AC/NF in series were able to illuminate the light emitting diode lamp for about 10 min, which was higher than the 5 min of three NiS@Ti3C2Tx/NF//AC/NF in series under the same condition. The CoNiSx@Ti3C2Tx/NF//AC/NF with high energy density had better application potential in energy storage than the NiS@Ti3C2Tx/NF//AC/NF.

关键词: MXene     supercapacitor     cobalt doping     structure characterization     electrochemical performance    

Effect of denitrifying bacteria on the electrochemical reaction of activated carbon fiber in electrochemical

YING Diwen, JIA Jinping, ZHANG Lehua

《环境科学与工程前沿(英文)》 2007年 第1卷 第3期   页码 305-310 doi: 10.1007/s11783-007-0051-z

摘要: An electrochemical-activated denitrifying biofilm system consisting of activated carbon fiber electrodes immobilized with denitrifying bacteria film as cathode was studied. A revised model for an electrochemical-activated denitrifying biofilm was developed and validated by electrochemical analysis of cathodal polarization curves and nitrate consumption rate. The cathodal polarization curve and nitrate consumption rate were introduced to verify the rate of electrochemical reaction and the activity of denitrifying bacteria, respectively. It was shown that the denitrification process effectively strengthened the electrochemical reaction while the electron also intensified denitrification activity. Electron was transferred between electrochemical process and biological process not only by hydrogen molecule but also by new produced active hydrogen atom. Additionally, a parameter of apparent exchange current density was deprived from the cathodal polarization curve with high overpotential, and a new bio-effect current density was defined through statistical analysis, which was linearly dependent to the activity of denitrification bacteria. Activated carbon fiber (ACF) electrode was also found to be more suitable to the electrochemical denitrifying system compared with graphite and platinum.

关键词: ACF     apparent exchange     hydrogen molecule     activated     biological process    

Special issue on electrochemical conversion and utilization of hydrogen energy

《能源前沿(英文)》 2024年 第18卷 第3期   页码 263-264 doi: 10.1007/s11708-024-0944-6

摘要: Special issue on electrochemical conversion and utilization of hydrogen energy

关键词: hydrogen energy    

Emerging electrochemical processes for materials recovery from wastewater: Mechanisms and prospects

Lingchen Kong, Xitong Liu

《环境科学与工程前沿(英文)》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1269-2

摘要: Abstract • Mechanisms for selective recovery of materials in electrochemical processes are discussed. • Wastewaters that contain recoverable materials are reviewed. • Application prospects are discussed from both technical and non-technical aspects. Recovering valuable materials from waste streams is critical to the transition to a circular economy with reduced environmental damages caused by resource extraction activities. Municipal and industrial wastewaters contain a variety of materials, such as nutrients (nitrogen and phosphorus), lithium, and rare earth elements, which can be recovered as value-added products. Owing to their modularity, convenient operation and control, and the non-requirement of chemical dosage, electrochemical technologies offer a great promise for resource recovery in small-scale, decentralized systems. Here, we review three emerging electrochemical technologies for materials recovery applications: electrosorption based on carbonaceous and intercalation electrodes, electrochemical redox processes, and electrochemically induced precipitation. We highlight the mechanisms for achieving selective materials recovery in these processes. We also present an overview of the advantages and limitations of these technologies, as well as the key challenges that need to be overcome for their deployment in real-world systems to achieve cost-effective and sustainable materials recovery.

关键词: Materials recovery     Electrosorption     Capacitive deionization     Redox processes     Electrochemical precipitation    

标题 作者 时间 类型 操作

Recent advances in the electrochemical oxidation water treatment: Spotlight on byproduct control

Yang Yang

期刊论文

Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

期刊论文

Electrochemical oxidation of humic acid at the antimony- and nickel-doped tin oxide electrode

TANG Chengli,YAN Wei,ZHENG Chunli

期刊论文

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

期刊论文

An electrochemical process that uses an Fe

Chaojie Jiang, Lifen Liu, John C. Crittenden

期刊论文

Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized

Yang Li, Yixin Zhang, Guangshen Xia, Juhong Zhan, Gang Yu, Yujue Wang

期刊论文

Enhancement of the electrocatalytic oxidation of antibiotic wastewater over the conductive black carbon-PbO

Xiangyu Wang, Yu Xie, Guizhen Yang, Jiming Hao, Jun Ma, Ping Ning

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

期刊论文

Recent advances in electrochemical decontamination of perfluorinated compounds from water: a review

期刊论文

Research progress in tribo-electrochemistry and tribo-electrochemical polishing

ZHAI Wenjie

期刊论文

Enhanced electrochemical performance of CoNiS@TiCT electrode material through doping of cobalt element

期刊论文

Effect of denitrifying bacteria on the electrochemical reaction of activated carbon fiber in electrochemical

YING Diwen, JIA Jinping, ZHANG Lehua

期刊论文

Special issue on electrochemical conversion and utilization of hydrogen energy

期刊论文

Emerging electrochemical processes for materials recovery from wastewater: Mechanisms and prospects

Lingchen Kong, Xitong Liu

期刊论文