Journal of Water Process Engineering
·
2024
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IF 6.3
Huijiao Wang,Siyuan Xue,Weiyi Wang,Fan Gao,Shizuo Yi,Jiayin Li,Yuxin Yang,Erzhuo Zhao,Jianchao Wang,Jianbing Wang
In this study, an efficient Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 electrode was fabricated for triclosan electro-oxidation by co-doping the transition metal Ce and carbon nanotubes (CNTs) into the PbO 2 active layer . Characterization results show that the co-doped Ce and CNTs present a synergistic effect on covering the obvious cracks on the Ti/SnO 2 -Sb 2 O 3 surface, decreasing the PbO 2 crystal size, increasing the electrode oxygen evolution potential from 1.60 to 2.17 V vs SCE, and reducing the charge transfer resistance by 66 %. Consequently, Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 was the most effective and energy-efficient electrode for hydroxyl radical (•OH) generation and triclosan electro-oxidation in this study. Compared with other two electrodes (Ti/SnO 2 -Sb 2 O 3 and Ti/SnO 2 -Sb 2 O 3 /Ce-PbO 2 ), triclosan removal by Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 was accelerated by 1.8–2.6 times, with the energy demand for abating 90 % triclosan (E EO ) decreased by 49 % – 67 %. Furthermore, triclosan degradation pathways were proposed based on density functional theory (DFT) calculation and transformation product (TP) identification, with •OH addition at C14 and C11 sites being the most favorable pathway. In addition, the estimated acute and chronic toxicities of TPs were generally decreased than their mother compound. Therefore, the results of this study suggest the feasibility and effectiveness of the Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 electrode for triclosan electro-oxidation.
研究领域:
环境科学
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材料科学
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电化学工程
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2023
·Vol. 170
·期 9
·092505
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IF 3.9
Shuna Liu,Ben Yang,Anran Zuo,Yongming Tang
Ti/SnO2-Sb/PbO2 anodes were electrodeposited from methanesulfonate-based baths, and the effect of dopants such as PVP and Fe on the surface morphology, phase composition, electrocatalytic activity and stability was investigated. It is revealed that the inclusion of Fe effectively enhances the stability of PbO2 anode, while PVP can significantly improve its electrocatalytic activity. The Fe,PVP-codoped anode, Ti/SnO2-Sb/Fe-PVP-PbO2, exhibits the higher stability and electrocatalytic activity compared to the respective inclusion of Fe and PVP. The gradation efficiency of methyl orange (MO) on the Ti/SnO2-Sb/Fe-PVP-PbO2 anode is affected by the applied current density and the initial MO concentration. During degradation, the azo structure of MO is firstly cleaved, resulting in the rapid decolorization of solution. Demethylated MO and the anion of sulfanilic acid are detected as intermediates, and thus a plausible pathway of MO degradation is proposed.
研究领域:
环境科学
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材料科学
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电化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
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2023
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IF 8.8
Xiangjuan Ma,Cong He,Yan Yan,Jianming Chen,Huajun Feng,Jinfei Hu,Hang Zhu,Yijing Xia
Reducing energy comsuption is crucial to commercialize electrochemical oxidation technologies . In this study, a novel PbO 2 composite electrode (Ti-foam/PbO 2 -GN) was successfully fabricated based on a porous titanium (Ti) foam substrate and a β-PbO 2 active layer embedded with multiple graphene (GN) interlayers, and applied as an anode for energy-efficient pulse electrochemical oxidation of ciprofloxacin (CIP). In contrast to PbO 2 and Ti-foam/PbO 2 electrodes, the Ti-foam/PbO 2 -GN electrode surface exhibited a more compact structure, smaller crystal grain size, and greater electrochemical active surface area. CIP removal of 89.7% was obtained with a low energy consumption (EE/O) of 6.17 kWh m −3 under pulse electrolysis conditions with a current density of 25.00 mA cm −2 , pulse frequency of 5000 Hz, and pulse duty cycle of 50.0%. Up to 70.7% of the energy was saved in the pulse current mode compared to the direct current mode. Narrowing the electrode spacing to 2 cm facilitated the mass transfer process and enhanced oxidation efficiency. According to the intermediates identified, the pulse electrolysis of CIP primarily involved hydroxylation of the quinolone ring, breaking of the piperazine ring, defluorination , and decarboxylation processes, and a possible degradation mechanism of CIP was proposed. The continuous oxidation performance of CIP and the relatively low leaching of Pb 2+ suggested that the Ti-foam/PbO 2 -GN electrode exhibited excellent stability, repeatability, and safety. The degradation results of CIP in real water also exhibits the great potential of environmental application. As a result, pulse electrochemical oxidation using a Ti-foam/PbO 2 -GN electrode has proven to be an energy-efficient and promising alternative for antibiotic wastewater treatment .
研究领域:
环境科学
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电化学工程
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水处理技术
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DOI
PubMed
高影响因子
Journal of Hazardous Materials Advances
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2023
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IF 0
Yonghao Zhang,Wen Li,Lulu Huang,Zhaoyi Zhang,Liu Liu,Jie Zhang,Qian Li,Jing Yang,Kajia Wei
In this work, a novel Ti/TiO 2 -NTA/meso-flower PbO 2 electrode (TMF-PbO 2 ) was developed by anodic oxidation and modified oxygen bubble-template electrodeposition. Characterization of the electrode confirmed that the meso-flower layer exhibited a unique 3D and hierarchical structure with a rough morphology. N 2 adsorption-desorption isotherms and cyclic voltammetry suggested that TMF-PbO 2 possessed a 2.18 times larger specific surface area and at least a 1.46 times larger electroactive area than the electrode with a porous PbO 2 layer. The investigation of the effect of the operation parameters indicated that the optimal conditions were a pH value of 3, supporting electrolyte concentration of 10.0 g L −1 and current density of 25 mA cm −2 . The electrochemical degradation of 1H-1,2,4-triazole (Tz) by TMF-PbO 2 was studied by HPLC and LC‒MS with the assistance of quantum chemical calculations. The TMF-PbO 2 achieved 100% removal of Tz and 70.4% removal of COD on the advanced treatment of actual pesticide tailwater with an energy consumption of 29.40 kWh kg −1 COD. The EC 50, 48 h value and BOD 5 /COD ratio of the treated wastewater were 70.6±5.9% and 0.64, respectively, indicating significantly low toxicity and high biodegradability. Cyclic testing also suggested that TMF-PbO 2 was stable during application. The excellent performance of TMF-PbO 2 in this study indicated that this kind of electrode is highly applicable for the treatment of pesticide tailwater.
研究领域:
环境科学
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电化学工程
✓ 已验证
DOI
Environmental Science-Nano
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2024
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IF 5.8
Yaxuan Wang,Peitong Cen,Hongyu Wang,Chenxi Li,Ziyin Xia,Guoqing Wu,Meng Li,Lei Huang,Jia Yan,Shaoqi Zhou,Ce-Hui Mo,Hongguo Zhang
Electrochemical oxidation (EO) for the removal of antibiotics is a promising technique because of the green and sustainable electrical-to-chemical energy conversion. However, the interaction mechanism between different electrolyte molecules and organic pollutants along with the generation pathway of reactive oxygen species remains unclear. Here, a β-PbO2 electrode was successfully prepared and employed as an effective tool for organic pollutant removal. The EO process with the β-PbO2 electrode and Na2SO4 electrolyte could completely remove tetracycline (TC) and achieve an impressive kinetic rate constant of 0.239 min−1. Quantum chemical calculations confirmed that hydrogen bonding was the primary binding force between TC and Na2SO4. Density functional theory calculations emphasized the key roles of radical and non-radical pathways in TC removal via the key reaction site (O atom in PbO2). Consequently, this study provided a novel insight into the intrinsic electrochemical behavior changes with various electrolytes, paving the way for a novel electrochemical process in water treatment applications.
研究领域:
环境科学
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电化学工程
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理论化学
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产品关联
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
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2023
·Vol. 40
·期 12
·3059-3067
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IF 2.7
Yin Zihang,He Ruibo,Nie Fei,Wei Zhen,Jia Bo,Feng Qing,Fu Xiaolong,Zhang Wenyan
The oxygen evolution kinetics of industrial copper electrodeposition is slow, resulting in low electrocatalytic activity and high energy consumption. In this work, a quaternary composite of carbon coated active particles containing Mn, Co and Ce were prepared (Mn-Co 3 O 4 /CeO 2 @C), and Ti/Sb-SnO 2 /PbO 2 electrode doped with these active particles was prepared by co-electrodeposition. The microstructure and chemical composition of the electrode was characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and X-ray diffractometry (XRD). Linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS) and Tafel polarization curve (Tafel) were used to study the electrochemical properties of anode materials. The results showed that the doping of Mn-Co 3 O 4 /CeO 2 @C active particles promoted the crystal transition of PbO 2 , decreased the average grain size, and the doping of Ce increases the average valence state of Co. The modified titanium electrode showed excellent catalytic activity of the oxygen evolution reaction (OER) characteristics. The overpotential of the doped Ti/Sb-SnO 2 /PbO 2 anode was only 453 mV when the current density was 20 mA cm −2 in 0.5 M H 2 SO 4 solution, which is 508 mV lower than that of the undoped Ti/Sb-SnO 2 /PbO 2 anode. In simulated copper electro-deposition experiments, the cell voltage was reduced by about 400 mV, compared to the undoped Ti/Sb-SnO 2 /PbO 2 electrode.
研究领域:
材料科学
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电化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2015
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IF 3.091
Yapeng He,Weimin Huang,Rongling Chen,Wenli Zhang,Haibo Lin,Hongdong Li
The electrochemical abatement of aspirin, a representative anti-inflammatory drug, is carried out through anodic oxidation by employing PbO 2 , boron-doped diamond (BDD) and porous Ti/BDD as anodes. The effect of nature characteristic and structure of the electrode material on the electrochemical oxidation is systematic investigated. The redox behavior of aspirin on different electrodes is studied by linear sweep voltammetry. Completely mineralization of aspirin could be achieved on BDD electrodes. The results show that the electrochemical incineration of aspirin on three electrodes follows a pseudo first-order kinetics behavior with apparent rate constant of 0.051, 0.185 and 0.367 h −1 for PbO 2 , flat BDD and porous BDD electrode. Electrochemical degradation mechanism on BDD electrodes involves the direct and indirect electrochemical oxidation while there is only indirect oxidation for aspirin on PbO 2 electrode. Porous Ti/BDD presents the best excellent electrochemical oxidation ability for aspirin compared with flat BDD and PbO 2 electrode. The discrepancy of electrochemical oxidation could be explained in terms of in situ generation and utilization rate of hydroxyl radicals on the surface of electrode materials.
研究领域:
环境科学
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电化学
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药物降解
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Jieqi Feng,Hao Lan,Qibin Tao,Wenqing Chen,Qizhou Dai
In this study, a novel NCNS-Ce-PbO 2 electrode was prepared by electrodeposition method using the rare earth metal Ce and synthesized nitrogen-doped carbon nanosheets (NCNSs). Various characterization and electrochemical performance tests showed that the NCNS-Ce-PbO 2 electrode possessed a denser surface and smaller grains than other NCNS-PbO 2 and Ce-PbO 2 electrodes, with more active surface sites and thus could generate more hydroxyl radicals. N , N -diethyl-m-toluamide (DEET) was selected as the model contaminant to evaluate the electrochemical performance of the novel NCNS-Ce-PbO 2 electrode. The effects of initial pollutant concentration, current density, electrolyte concentration, and initial pH on the removal rates of DEET and chemical oxygen demand (COD) were investigated. Under optimal conditions, after degradation of 150 min, the removal rate of DEET and COD reached 100% and 80.52%, respectively. GC–MS was used to identify intermediate products in the degradation process. The degradation mechanism and possible degradation pathways of DEET with NCNS-Ce-PbO 2 electrode were discussed. The good stability of the NCNS-Ce-PbO 2 anode was confirmed by accelerated lifetime experiments.
研究领域:
环境科学
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电化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Miao Lu,Siyuan Zhang,Zhongmei Song,Liang Ma,Haining Liu,Ming Fang,Huifang Zhang,Xiushen Ye,Zhijian Wu
Increased levels of octadecylamine (ODA) and 4-dodecylmorpholine (DMP) in the aqueous, primarily utilized as flotation agents in the worldwide production of potash fertilizer, imperil the stability of ecosystems and the downstream production of high-end chemicals. Nevertheless, there is a dearth of exhaustive studies pertaining to the elimination of ODA and DMP. Herein, the Ti/SnO 2 -Sb/β-PbO 2 anode was fabricated by a thermal decomposition-electrodeposition technique for the electrocatalytic degradation of ODA and DMP. The degradation efficiency of ODA and DMP can achieve complete degradation, reaching 100%, after treatment periods of 10 min and 120 min, respectively. Meanwhile, the TOC removal efficiency of ODA and DMP is up to 85% and 61% at 30 min and 120 min, respectively. In particular, sulphate exhibits inhibitory degradation activity of ODA and DMP in comparison to chloride salt. The recycling and accelerated lifetime tests indicate excellent stability and recyclability of the Ti/SnO 2 -Sb/β-PbO 2 electrode. The mechanism of electrocatalytic degradation involves indirect electrochemical oxidation mediated by free radicals. The primary reactive species responsible for the degradation of DMP and ODA, as determined through scavenger quenching experiments and ESR, are ·OH and Cl·. The degradation of the ODA and DMP commences with the elimination of N element, leading to the formation of the N O 3 - . The carbon chain subsequently undergoes the breakdown. The degradation pathways of ODA and DMP were also proposed based on the GC–MS and H-NMR analyses, respectively. Moreover, the Ti/SnO 2 -Sb/β-PbO 2 anode performed excellently in the removal of ODA and DMP in real samples, TOC removal from ODA and DMP in natural samples was 56% and 52%, respectively, within 180 min. This study provides the first exploration of electrocatalytic degradation mechanisms and pathways of ODA and DMP based on the Ti/SnO 2 -Sb/β-PbO 2 anode.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Yuanzhen He,Dengjie Zhong,Yunlan Xu,Ran Jiang,Pengfei Liao,Jiayou Zhang
In this work, Ti/SnO 2 -Sb 2 O 4 -La/β-PbO 2 electrode was successfully prepared by electrodeposition method. The surface morphology, crystal structure, elemental states and electrochemical characteristics of the electrode were examined by SEM, XRD, XPS, CV, and LSV. The results demonstrated that the conductivity, specific surface area, electrochemical oxidation performance and stability of the β-PbO 2 coated electrode with SnO 2 -Sb 2 O 4 -La as the intermediate layer were greatly improved. Under the conditions of initial rhodamine B (RhB) concentration of 20 mg/L, initial pH of 3.0, electrolyte concentration of 0.1 M, and current density of 30 mA cm −2 , the removal rates of color and TOC reached 100 % and 83.64 % after 20 mins and 30 mins, respectively. The electrode can also completely degrade methylene blue and methyl orange wastewater after 30 mins under the same conditions. The accelerated lifetime of the electrode reached 175 mins (1000 mA cm −2 , 1 M H 2 SO 4 ), and the actual lifetime was up to 3208 hrs. Based on the results of free radical quenching experiment and GC–MS detection, RhB degradation pathway was proposed: the aniline-based conjugated system of RhB molecule was attacked by the combined action of free radicals (indirect oxidation) and electrocatalysis (direct oxidation), which decomposed macromolecules into small molecules and ultimately mineralized them into CO 2 and H 2 O. This work is expected to provide a fresh research concept for preparing DSA electrodes with excellent catalytic performance and high stability.
研究领域:
环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Ruirui Zhang,Shugui Hua,Yuan Dang,Bing Zhang,Xiaoqin Sun,Sha Yu,Yingying He,Shuangli Chen,Yuanzhen Zhou
In this paper, the electrocatalytic performance of Ti/β-PbO 2 anode was improved by doping Cs into SnO 2 intermediate layer (Ti/Cs-SnO 2 /β-PbO 2 ) for the efficient degradation of fluoroquinolone wastewater. Compared with the conventional Ti/Sb-SnO 2 /β-PbO 2 anode, Cs-SnO 2 with the rougher surface increased the deposition amount and the thickness of β-PbO 2 active layer, thus forming the denser PbO 2 coating with smaller particle size and exposing more active sites. The partial replacement of Sn by Cs with the smaller ion radius induced the deformation of crystal lattice of SnO 2 , which further led the outer β-PbO 2 active layer grew along the advantageous (200) crystal plane and formed more point defects in the crystal lattice of β-PbO 2 . Thereby, the electron transfer rate at the anode interface was accelerated and the electrocatalytic performance of Ti/β-PbO 2 was significantly improved. To verify the practical application of the improved Ti/Cs-SnO 2 /β-PbO 2 electrode, levofloxacin (LFX) and ciprofloxacin (CIP) were selected as the typical target fluoroquinolones to evaluate the degradation efficiency of Ti/Cs-SnO 2 /β-PbO 2 anode. The removal rate exceeded more than 90% for the single and mixed fluoroquinolones wastewater. Moreover, after 5 times’ recycle, the degradation efficiency of LFX on Ti/Cs-SnO 2 /β-PbO 2 anode still remained over 90%. The potential mechanism of the enhanced electrocatalytic performance of Ti/Cs-SnO 2 /β-PbO 2 and the degradation pathways of fluoroquinolones were also inferred. It’s the first time to enhance the electrocatalytic performance of the Ti/β-PbO 2 anode by introducing monovalent alkali metal (C S ) into the SnO 2 intermediate layer and the proposed Ti/Cs-SnO 2 /β-PbO 2 anode would be a promising candidate to realize the efficient removal of the practical fluoroquinolones antibiotic wastewater.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Liping Zhang,Hexia Yuan,Yiyun An,Huitong Li,Yiqing Gao,Huaran Sun
Coking reverse osmosis concentrated water contains refractory organic pollutants . If not treated, it will generate hazardous solid waste that cannot be utilized in the subsequent evaporation and crystallization process . In order to effectively remove organic substances from coking reverse osmosis concentrated water, Ti/PbO 2 electrode, Ti/Ce,Nd-PbO 2 electrode, and Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode were prepared. The electrodes were characterized by scanning electron microscopy, X-ray diffraction spectroscopy, and X-ray photoelectron spectroscopy, revealing that the average crystal grain size of lead dioxide on the surface of the Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode is 29.58 nm. The electrochemical performance of the electrodes was tested using cyclic voltammetry and electrochemical impedance spectroscopy , which showed oxidation peaks at 1.37 V, 1.81 V, and 2.1 V for the Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode, with a charge transfer resistance of 56.34 Ω. Accelerated life test indicated that the Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode has an accelerated lifespan of 1050 min. The effects of interelectrode distance, pH value, current density , and other factors on the electrocatalytic oxidation of 3,5-di-tert-butylphenol by the Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode were investigated, achieving a removal efficiency of 98.67 % under optimal conditions. Performance analysis of the Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode demonstrated good stability. Treatment of actual coking reverse osmosis concentrated water using the Ti/P(ANI-co-Py)/Ce,Nd-PbO 2 electrode resulted in removal efficiencies of 87.76 %, 47.92 %, and 77.42 % for COD , TOC, and UV 254 , respectively. The current efficiency and energy consumption of electrocatalytic degradation of coking reverse osmosis concentrated water were 9.38 % and 0.15 kWh/g COD. This study provides a better treatment solution for the degradation of organic matter in coking reverse osmosis concentrated water.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）