ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Ling Cheng,Tao Jiang,Kai Yan,Jianyu Gong,Jingdong Zhang
When photoelectrocatalysis (PEC) couples with electroenzymatic catalysis (EEC), effective utilization of electrons from PEC process for yield of H 2 O 2 plays an important role in the enzymatic catalysis. In the present work, we designed a novel dual-cathode PEC-EEC system for pollutant removal. In this system, BiVO 4 photoanode was prepared by electrodeposition for visible light-driven PEC process while carbon cloth was used as the first cathode for electrogeneration of H 2 O 2 and hemin/Cu prepared by electrophoretic deposition acted as the second cathode for enzymatic catalysis. The performances of the constructed dual-cathode PEC-EEC system were evaluated by decoloring Rhodamine B (RhB), which showed high decoloration percentage with acceptable stability and reusability. Further, the system was applied to degradation of tetracycline (TC), indicating that about 93.6% of TC was removed after 2-h treatment. A pathway for TC degradation in such a dual-cathode PEC-EEC system was proposed based on the intermediates determined by liquid chromatography coupled to mass spectrometry in tandem (LC-ESI-MS/MS).
研究领域:
环境科学
·
光催化
·
电化学
✓ 已验证
DOI
高影响因子
Joule
·
2022
·
IF 46.048
Qing Han,Wei Guo,Xiaofeng He,Tongchao Liu,Xiao Liu,Xuebing Zhu,Tengfei Bian,Lei Jiang,Jun Lu,Yong Zhao
Aprotic lithium-oxygen (Li-O 2 ) batteries have attracted extensive attention due to their ultrahigh theoretical energy density. However, slow and undesired electron transfer during cathodic reactions causes low cyclic stability in these batteries. Here, we demonstrate that O 2 mass transport and electron transfer for cathodic reactions in Li-O 2 batteries could be decoupled by a double-cathode structure that efficiently enables stable electron transfer between the cathode and Li 2 O 2 /O 2 . This resolves various side reactions and slow Li 2 O 2 reaction kinetics issues in conventional Li-O 2 batteries, leading to stable operation of the cell for nearly 2 months at a capacity of 0.2 and 5 mAh cm −2 , with more than 4- and 10-fold increases in cycle life when compared with single-cathode batteries. These remarkable improvements in the cyclic stability of Li-O 2 batteries with double cathodes provide an interesting concept for improving the operational stability of other metal-rechargeable batteries with conversion-type chemistry.
研究领域:
电化学
·
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yandi Rao,Aoqi Li,Yuxin Zhang,Fuxi Wang,Tianhu Zhang,Yiping Sheng,Tifeng Jiao
A composite electrochemical oxidation system combined with Electro-Fenton and persulfate (PS) was proposed to degrade metronidazole. The CoFe 2 O 4 -PTFE (CFOP) electrode was used in parallel with the acetylene black-PTFE electrode (ABP) as the dual-cathode of Electro-Fenton. Then the Electro-Fenton was coupled with PS to degrade metronidazole in wastewater synergistically. The self-produce of H 2 O 2 , in-situ circulation of Co(II)/ Co(III) and Fe(III)/ Fe(II), and activation of persulfate were simultaneously conducted. After 120 min, the removal rate of metronidazole reached 90.6% by ABP/CFOP/PS system. The influence of operation parameters (dosage of PS, initial pH, current density, temperature) on the removal of metronidazole was analyzed. The catalyst exhibited good stability and recyclability for five consecutive cycles. The radical quenching and EPR tests reveal that both OH and SO 4 − · are identified responsible for the degradation of metronidazole. The possible decomposition pathway of metronidazole was proposed by HPLC-MS analysis. The toxicity analysis indicates that heterogeneous Electro-Fenton could reduce the toxicity of metronidazole.
研究领域:
环境科学
·
废水处理技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qizhan Zhang,Haoran Yin,Pei Su,Wenyang Fu,Ge Song,Minghua Zhou
An improved dual-cathode peroxi-coagulation (PC) process using natural air diffusion electrode (NADE) and HNO 3 modified carbon felt (MCF) was first proposed to improve the removal efficiency of organic pollutants in neutral and alkaline wastewater and reduce the formation of iron sludge. The improved PC process does not require any additional oxidants or catalysts, nor does it need to adjust the pH of the wastewater in advance but can directly treat actual wastewater, achieving a target pollutant (C 12 H 14 N 4 O 2 S, sulfamethazine) removal of 87%-100% within 60 min and TOC removal of 46–76% within 240 min with the corresponding energy consumption below 0.02 kWh gTOC -1 . Compared with the conventional PC process, this improved process could produce hydroxyl radical ( • OH) and superoxide radical (O 2 •- ) more efficiently, which greatly increased the SMT removal rate constant by 3–4 times and oxidative removal proportion of organic pollutants from 42 ∼ 47% to 85 ∼ 90%. Thanks to the Fe(II) regeneration capacity of MCF to promote iron circulation, the yield of • OH was 4.1 times higher while the iron sludge production was less than a quarter when compared with that of conventional PC. The improved PC process illustrated better purification performance and lower energy consumption for actual wastewaters such as pharmaceutical wastewater, surface water and rural decentralized domestic sewage than the conventional PC process. Our work elucidated the mechanism of promoting Fe(II) regeneration through MCF cathode under alkaline conditions to enhance • OH production and O 2 •- oxidation, showing a good environmental application prospect.
研究领域:
环境科学
·
污水处理
·
电化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chen Shu,Bin Chen,Weihu Zhang,Lele Cui,Wenheng Jing
Renewable electricity-driven hydrogen peroxide (H 2 O 2 ) electrosynthesis technology has recently emerged as a multidisciplinary research frontier as its distributed deployment capability can provide enhanced versatility for various potential niche applications. Despite significant progress in screening advanced electrocatalysts and fundamental understanding of microscopic reaction mechanisms, industrially viable electrolysis devices suitable for this technology are still lacking due to technical challenges such as low space/electrode utilisation and single-pass yield as well as poor operability. Here, we demonstrate a membrane-free dual-cathode stack reactor featuring compactness (inter-electrode distance configured to flow field plate thickness) and ideal electrode utilisation (two cathodes paired with one anode). Structurally discontinuous carbon films with self-sustained aeration are assembled as cathodes, which enables open air-fed O 2 -to-H 2 O 2 conversion and thus effectively simplifies operation. Even with low electrolyte concentrations (0.05 M Na 2 SO 4 ), this design demonstrates efficient H 2 O 2 production from bench- to industrial-scale operating current densities (75–200 mA cm −2 ) at relatively low cell voltages (5.9–11.0 V). Impressive single-pass H 2 O 2 accumulations of 959.6–2332.1 mg L −1 with current efficiencies of 55.1 %–90.7 % can be achieved at low hydraulic retention times of 15–60 s. The practicality and reliability of the device can be further elucidated by its robustness in decentralized wastewater remediation scenarios. This all-material/components-commercial design paves the way for advancing the technology readiness level of H 2 O 2 electrosynthesis processes.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Haifang Tang,Zuoyan Zhu,Qian Shang,Yanhong Tang,Danyu Zhang,Yi Du,Meijun Liu,Kai Yin,Chengbin Liu
A simple, efficient, and environmentally friendly electro-Fenton (EF) process is highly demanded for EF practical application. Herein, a highly practical double-cathode EF system has been developed: (1) KOH-activated graphite felt (AGF) for H2O2 production and (2) FeOCl-modified carbon cloth (FeOCl/CC) for H2O2 activation. The H2O2 production at the AGF cathode reaches 3.4 mmol/L in 60 min (pH 3, −0.6 V vs Ag/AgCl), and the FeOCl/CC cathode shows an excellent H2O2 activation performance where the removal percentage of tetracycline (TC, a rising refractory organic pollutant) reaches 98.2% in 5 min ([H2O2] = 1.0 mmol/L, C0 = 10.0 mg/L, pH 3, and −0.8 V vs Ag/AgCl). The double-cathode EF system is proved by TC degradation. The removal percentage of TC achieves 96% in 20 min and total organic carbon (TOC) removal percentage reaches 92% in 2 h (C0 = 10.0 mg/L, pH 5, and −0.6 V vs Ag/AgCl) in a static system. Furthermore, the system is highly effective in a wide pH range from 3 to 7. Significantly, in the continuous-flow system, the TC degradation percentage reaches 95% within 1.5 h, the mineralization reaches 88% within 4 h (C0 = 10.0 mg/L, v = 4 mL/min, pH 5, and −0.6 V vs Ag/AgCl), and the performance remains highly stable even after prolonging for 15 h. The system has a high oxidative flux (1510 mg/(min m2)) and low energy consumption (45 kWh/(kg TOC)). Encouragingly, such a small-scale reactor (V = 100 mL, 4 mL/min) can treat 5.76 L of TC wastewater in one day. The toxicity of TC solution is remarkably reduced after EF treatment. This study would advance the practical application of an EF treatment process.
研究领域:
环境科学
·
化学工程
·
水处理技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Qizhan Zhang,Minghua Zhou,Xuedong Du,Pei Su,Wenyang Fu,Ge Song
To simultaneously improve the H 2 O 2 electrosynthesis, Fe(II) regeneration and pH application range in EF process, a highly efficient dual-cathode electro-Fenton (EF) process using easily available Fe(III) as catalysts for the treatment of organic wastewater at a wide pH range was first proposed, in which natural air diffusion electrode (NADE) was designed as one cathode for H 2 O 2 production without aeration and the modified carbon felt (MCF) was acted as the other cathode mainly for Fe(II) regeneration. Nitric acid modification significantly enhanced the electrochemical properties of CF and introduced more oxygen-containing functional groups. The Fe(II) regeneration rate of MCF with higher electroactive surface area was 4.7 times that of CF cathode at pH 7. It was found that as the homogeneous Fe(III) was hydrolyzed into solid hydroxides, the accompanying H + decreased the solution pH and MCF not only accelerated the dissolved Fe(III)/Fe(II) cycle but also reduced the adsorbed solid iron to ≡Fe(II) on the cathode surface. This simultaneously promoted the homogeneous and heterogeneous Fenton reactions and enhanced the efficiency of EF degradation process. For bronopol, 2,4-dichlorophenoxyacetic acid, sulfamethazine and phenol (100 mg L −1 ), the process had TOC removal of 48%−72% within 60 min with the corresponding mineralization current efficiency of 16.5%−56.2%, and the electrical energy consumption <0.225 kWh (gTOC) −1 , which all greatly advantaged over that of the conventional EF. Therefore, this process is efficient and low-cost, being very promising for the treatment of organic wastewater.
研究领域:
环境科学
·
污水处理
·
电化学技术
✓ 已验证
DOI
高影响因子
Journal of CO2 Utilization
·
2021
·
IF 7.132
Danqing Shu,Miao Wang,Fengyu Tian,Honglei Zhang,Chuang Peng
Electroreduction of CO 2 to high value-added products such as hydrocarbons provides a promising way to create a carbon neutral circular economy. Copper (Cu) is the most effective metal catalyst with selectivity towards hydrocarbons but Cu catalyst alone generally produces hydrocarbons at low selectivity and yield. Operando surface enhanced infrared absorption spectroscopic (SEIRAS) analysis reveals that the low hydrocarbon yield is attributed to the poor ability of Cu to produce carbon monoxide (CO), which is a crucial intermediate for hydrocarbon formation. In the current study, an Ag-Cu dual-cathode CO 2 RR device is developed, which allows separate control of electrode potential. This dual-cathode cell shows increased hydrocarbon yield (83 % for methane and 106 % for ethylene) and a 200 mV lower onset potential for C 2 H 4 , compared to electrolysis with a single Cu cathode. The CO produced by the Ag cathode transfers to Cu and increase its CO coverage, facilitating methane formation as well as promoting C C coupling to form ethylene. This study also reveals a mismatch of optimum electrode potential between Ag and Cu, which results in compromised performance of the two components in an Ag-Cu bimetallic electrocatalyst, but poses no challenge in the dual-cathode cell. To optimize the performance of the dual-cathode cell, we propose the use of a single-pass dual-gas-diffusion-cathode reactor with enhanced mass transfer for maximum hydrocarbon production. This work verifies that splitting the complex CO 2 RR process into two separate steps is a feasible method to improve the overall efficiency and rate of advanced products while reducing the energy input.
研究领域:
能源化学
·
电催化
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chuan Cao,Yanjun Guo,Dadi Chen,Jun Cui,Xiang Hu
Conventional heterogeneous iron-based catalysts face challenges such as insufficient catalytic activity, sluggish Fe(Ⅲ)/Fe(Ⅱ) cycle, and hindered electron transfer during Fenton catalytic reactions. Herein, Fe 3 O 4 /Fe 0 /Fe 3 C-2-600, obtained by calcining MIL-88B (Fe) in-situ growth on stainless-steel mesh at varying temperatures, was served as a catalytic electrode in a dual-cathode electro-Fenton system. The catalytic mechanism was elucidated by density functional theory (DFT) calculations. Based on the calculations, the presence of Fe 0 could induce electron transfer to Fe(Ⅲ), accelerating the Fe(Ⅲ)/Fe(Ⅱ) cycle. Simultaneously, Fe 0 was functioned as an electron transfer station, rapidly exporting electrons from the internal Fe 3 O 4 core to the surface graphite layer, further activating H 2 O 2 . Due to the rapid electron transfer, the Fe 3 O 4 /Fe 0 /Fe 3 C-2-600 cathodes demonstrated remarkable catalytic activity, achieving a 97.7 % degradation of tetracycline (TC) within 12 min. According to electron spin resonance tests and quenching experiments, hydroxyl radicals (·OH) was identified as the main active species. In addition, the possible degradation pathways of TC were proposed, according to the results of high-performance liquid chromatography-mass spectrometry (HPLC-MS). The Fe 3 O 4 /Fe 0 /Fe 3 C-2-600 cathode presented a promising strategy for developing an efficient and straightforward method to construct internal electric fields that could accelerate electron transfer in Fenton reactions. Moreover, the integration with the double-cathode electro-Fenton system, realizes the concept of reagent-free and sustainable catalysis, enhancing its practical application value.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Zhicheng Wang,Chen Wang,Xiaohui Wu,Wen-Da Oh,Mingjie Huang,Tao Zhou
Electrochemical advanced oxidation processes (EAOPs) based on natural air diffusion electrode (NADE) promise efficient and affordable advanced oxidation water purification , but the sustainable operation of such reaction systems remains challenging due to severe cathode electrowetting. Herein, a novel floating cathode (FC) composed of a stable hydrophobic three-phase interface was established by designing a flexible catalytic layer of FC. This innovative electrode configuration could effectively prolong the service life of the cathode by mitigating the interference of H 2 bubbles from the hydrogen evolution reaction (HER), and the H 2 O 2 production rate reached 37.59 mg h −1 ·cm −2 and realize a long-term stable operation for 10 h. Additionally, an FC/carbon felt (CF) dual-cathode electro-Fenton system was constructed for in situ sulfamethoxazole (SMX) degradation. Efficient H 2 O 2 production on FC and Fe(III) reduction on CF were synchronously achieved, attaining excellent degradation efficiency for both SMX (ca. 100%) with 2.5 mg L −1 of Fe(Ⅱ) injection. For real wastewater , the COD removal of the FC/CF dual-cathode electro-Fenton system was stabilized at exceeding 75%. The practical application potential of the FC/CF dual-cathode electro-Fenton system was also demonstrated for the treatment of actual landfill leachate in continuous flow mode. This work provides a valuable path for constructing a sustainable dual-cathode electro-Fenton system for actual wastewater treatment .
研究领域:
环境科学
·
电化学工程
·
水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Cheng Shu,Ziqi Cai,Zhenghua Zhang
The current peroxymonosulfate-electrochemical advanced oxidation process (PMS-EAOP) systems face the challenges of poor stability and efficiency, limiting the application in industry and practical scenarios. Herein, a dual-cathode sandwich (DCS) PMS-EAOP system was established for efficient degradation of aqueous emerging contaminants with long-term stability. A titanium-based antimony/iridium-doped tin oxide (Ti/AITO) anode was enclosed symmetrically by dual stainless-steel cathodes, achieving reliable water purification through a synergistic mechanism of reactive oxygen species generation and direct electron transfer (DET)-based non-radical pathways. Comprehensive investigations were conducted on the degradation performance of diverse pharmaceutical and personal care products and endocrine-disrupting chemical. Operational parameters were systematically optimized to maximize pollutant removal efficiency. Mechanistic insights were gained through degradation pathway analysis, toxicity assessment, and radical species identification. The removal of the model ranitidine contaminant with a pseudo-first-order rate constant of 0.198 min −1 was attributed to the synergistic action of •OH, SO 4 • − and 1 O 2 , and the DET-based non-radical pathway. The DCS-PMS system demonstrated robust operational stability in complex water matrices, including natural and urban water bodies, and maintained exhilarating performance under long-term continuous operation for over 60 h. Notably, the system achieved a ∼67% total organic carbon removal within 120 min when applied to high-concentration real antibiotic wastewater. This work offers insights for advancing the development of EAOPs with scalable design, simple assembly, and high durability in wastewater treatment.
研究领域:
环境科学
·
电化学
·
水处理技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Dongliang Wang,Jingping Hu,Bingchuan Liu,Huijie Hou,Jiakuan Yang,Yuxiao Li,Yi Zhu,Sha liang,Keke Xiao
The electrogeneration of H 2 O 2 and electro-regeneration of ferrous are conflicting matters in electro-Fenton system. In this research, the degradation of Rhodamine B, methyl orange (MO) and 4-chlorophenol (4-CP) was investigated using a novel dual-cathode microbial fuel cell (MFC) electro-Fenton (EF) hybrid system. An air-cathode of an EF system was used for H 2 O 2 electrogeneration and a carbon felt cathode of a MFC was used to accelerate Fe 2+ regeneration. Synergistic improvement of MFC power generation and the degradation of the above refractory organics through EF reaction was achieved. The EF air-cathode was fabricated by adopting activated carbon/graphite powder mixture and PVDF binder, which showed higher H 2 O 2 generation but slower Fe 3+ reduction rate than MFC carbon felt cathode. The Rhodamine B removal rate constant and mineralization current efficiency of the MFC coupled EF were 64% and 42% higher than that of uncoupled EF, respectively. The MFC-EF coupled system also exhibited significantly higher removal efficiency for MO and 4-CP than that of un-coupled EF system. Moreover, the power density of MFC was greatly enhanced by coupling EF due to higher Fe 3+ /Fe 2+ redox potential than oxygen reduction.
研究领域:
环境科学
·
电化学工程
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）