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PbO2电极
JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2022 · IF 4.598

Enhanced electrochemical removal of dye wastewater by PbO2 anodes using halloysite nanotubes with different surface charge properties

Jiali Yuan,Zhen Chen,Qiang Yu,Wei Zhu,Shuting Li,Lei Han,Xia Lu,Shutong Li,Yize Wu,Ze Lv,Hongjun You,Bangyao Chen

Electrode materials are the core of electrocatalytic oxidation technology. Herein, chitosan (CTS)-modified halloysite nanotubes (HNTs) were used for the first time in the doping modification of PbO 2 electrodes by electrodeposition technique, and novel HNTs-CTS-PbO 2 anodes were prepared and used for the electrochemical removal of the thiazine dye methylene blue (MB). The surface structure information, electrochemical properties and oxidation activity of the materials were systematically investigated, and possible degradation pathways of methylene blue were proposed. The results showed that after doping modification, the coating became flatter and denser, and the crystalline shape and crystalline phase of the PbO 2 electrode did not change, but the grain size was significantly reduced; moreover, the modified electrode had higher oxygen precipitation overpotential, larger reactive surface area and lower charge transfer resistance. Additionally, the decolorization degradation of MB by HNTs-CTS-PbO 2 electrode mainly adopts an indirect degradation mechanism and follows the pseudo-first-order kinetic model, which exhibits higher decolorization degradation rate. Analyzing the mechanism of the electrochemical removal of MB from the modified anode, which mainly involves the breakage of C N bonds under the action of ·OH, followed by demethylation and aromatic ring cleavage to obtain monoaromatic amines, sulfonic acids and phenolic compounds, and finally mineralized into inorganic small molecules such as CO 2 and H 2 O. The above results show that HNTs-CTS-PbO 2 anode is a promising candidate in the field of dye wastewater degradation and provide new insights for the application of HNTs .

研究领域: 环境科学 · 材料科学 · 电化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Application of response surface methodology in electrochemical degradation of amoxicillin with Cu-PbO2 electrode: Optimization and mechanism

Jun Hu,Xinze Bian,Yi Xia,Mili Weng,Wan Zhou,Qizhou Dai

In this study, Cu doped PbO 2 electrode was prepared by electrodeposition and used for electrochemical oxidation degradation of amoxicillin (AMX), which showed that the effect of Cu doped PbO 2 electrode was better than that of undoped PbO 2 electrode in degrading amoxicillin. An optimized model was setup with the help of response surface method (RSM). The optimal values of experimental parameters and the interactions between the parameters were explored, including current density, pH and initial AMX concentration. The combustion efficiency was calculated in the electrochemical oxidation of amoxicillin in aqueous solution and the enhancement was found with Cu doped PbO 2 electrode. The enhanced mechanism with Cu doped PbO 2 electrode was discussed based on the analysis of hydroxyl radicals and the combustion efficiency. The mechanism of amoxicillin degradation was discussed. This paper can provide basic data and technique reference for amoxicillin pollution control.

CAS / MDL: 61336-70-7
研究领域: 环境科学 · 化学工程
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CHEMOSPHERE · 2019 · IF 5.108

Electrochemical removal of amoxicillin using a Cu doped PbO2 electrode: Electrode characterization, operational parameters optimization and degradation mechanism

Xinze Bian,Yi Xia,Tingting Zhan,Lin Wang,Wan Zhou,Qizhou Dai,Jianmeng Chen

This work investigated the electrochemical degradation of amoxicillin (AMX) in aqueous solution with Cu-PbO 2 electrode. The main influence factors on the degradation of AMX, such as Na 2 SO 4 concentration, initial AMX concentration, current density and initial pH value, were analyzed in detail. Under the optimal conditions, the removal rates of AMX and chemical oxygen demand (COD) reached 99.4% and 46.3% after 150 min treatment. The results indicated that the electrochemical degradation of AMX fitted pseudo-first-order reaction kinetics. Compared with undoped PbO 2 electrode, Cu-PbO 2 electrode had a smaller crystal size, more proportion of hydroxyl oxygen species, greater AMX and chemical oxygen demand (COD) removal efficiency, higher average current efficiency (ACE) and lower electrical efficiency per log order (EE/O). Electrochemical oxidation using Cu-PbO 2 electrodes was an effective way to eliminate amoxicillin in aqueous solution. Moreover, a possible degradation pathway including ring open and mineralization was proposed by intermediate products determined by GC-MS method. This paper could provide basic data and technique reference for the amoxicillin wastewater pollution control .

CAS / MDL: 61336-70-7
研究领域: 环境科学 · 电化学工程 · 污染控制
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2022 · IF 4.598

Crystal facet controlled stable PbO2 electrode for efficient degradation of tetracycline

Chongjie Zou,Chenglong Ma,Fang Chen,Xiang Shao,Limei Cao,Ji Yang

Achieving the robust PbO 2 electrode with the high onset potential is of considerable importance for applying electrochemical pollutants degradation. Herein, the crystal plane strategy was adopted to modify the PbO 2 surface structure through the surfactant induction during synthesis in the electrodeposition process. PbO 2 (β(3   0   1)) and PbO 2 (α(2   0   0), β(3   0   1)) electrodes were obtained by the controlling conditions of surfactants sodium dodecyl sulfate (SDS) and hexadecyl trimethyl ammonium bromide (CTAB). Compared with conventional PbO 2 , the PbO 2 (CTAB) electrode exhibits outstanding performance in electrochemical stability and higher onset potential versus the PbO 2 (SDS). Accelerated life of the PbO 2 (CTAB) electrode is 147 h longer than that of the pure PbO 2 under a high current density of 1A·cm −2 , and the amount of lead ion dissolution is only 45% of that observed in pure PbO 2 . In this work, tetracycline (TC) was taken as an example to evaluate the degradation effect of electrodes. Due to its unique crystal texture, the PbO 2 (CTAB) electrode exhibits higher COD removal rate and TOC removal rate, 35% and 20% respectively beyond that of the conventional lead dioxide electrode. Therefore, it is of great value for its industrial electrode degradation of pollutants.

研究领域: 环境科学 · 材料科学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2019 ·Vol. 166 ·期 13 ·D638 · IF 3.12

Fabrication of Ti/SnO2-Sb/Ce-PbO2 Anode from Methanesulfonate Bath and Its Electrocatalytic Activity

Pengfei Xu,Xiaohong He,Junwei Mao,Yongming Tang

In this paper, Ti/SnO2-Sb/Ce-PbO2 anode is electrodeposited from MSA bath, and the effect of Ce3+ concentration in bath on the phase composition and morphology of lead dioxide electrode is elucidated. It is found that with the addition of 2 mM Ce3+ ion to the bath the Ce-PbO2 anode exhibits highest stability in 0.5 M H2SO4, and cerium exists as Ce (IV) in the PbO2 film. The electrocatalytic activity of lead dioxide anode for phenol removal is slightly enhanced by the inclusion of Ce. The significant improvement in electrocatalytic activity can be achieved by the addition of small amount of Bi3+ ion to the bath containing Ce3+ ion. In this study, electrocatalytic activities of various anodes follow the order: Ce,Bi-PbO2 > Ce-PbO2 > undoped PbO2 > Bi-PbO2.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Electrochemical decomposition of PPCPs on hydrophobic Ti/SnO2-Sb/La-PbO2 anodes: Relationship between surface hydrophobicity and decomposition performance

Xubin Qian,Kefu Peng,Lei Xu,Shaoyu Tang,Weilai Wang,Min Zhang,Junfeng Niu

The global detection and potential harm of pharmaceuticals and personal care products (PPCPs) call for the effective decomposition technology. In this study, the modified β-PbO 2 anodes with different hydrophobicity (Ti/SnO 2 -Sb/La-PbO 2 , Ti/SnO 2 -Sb/La-PbO 2 -PTFE and Ti/SnO 2 -Sb/La-PbO 2 -PVDF) were prepared to decompose aqueous PPCPs, i.e. isoniazid, methotrexate, carbamazepine, sulfamethoxazole and ibuprofen. PTFE and PVDF modification improved the physical property, electrochemical property, stability and safety of β-PbO 2 electrode. Moreover, Ti/SnO 2 -Sb/La-PbO 2 -PVDF had the highest oxygen evolution potential (1.95 V vs. SCE), the largest electroactive area (88.85 cm 2 ), the highest HO • production rate (10.44 mM min −1 m −2 ) and the best degradation performance for all the five PPCPs. The hydrophobic surface increased the proportion of free HO • , resulting in higher radical utilization rate and better degradation performance. The excessive hydrophobicity could decrease the degradation performance of PPCPs with high log K ow due to the relatively large hydrophobic force zone. Furthermore, the hydrophobicity enhanced the mineralization (current) efficiency of isoniazid, and its electrochemical degradation mechanism on Ti/SnO 2 -Sb/La-PbO 2 -PVDF was thoroughly proposed. These results demonstrated that Ti/SnO 2 -Sb/La-PbO 2 -PVDF anode exhibited a good application prospect in treating wastewater containing PPCPs.

研究领域: 环境科学 · 电化学工程
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

Electrochemical degradation of chloramphenicol with a novel Al doped PbO2 electrode: Performance, kinetics and degradation mechanism

Jianmeng Chen,Yijing Xia,Qizhou Dai

This study presents an electrochemical method for the degradation of chloramphenicol (CAP) in aqueous solution with a novel Al doped PbO 2 electrode. The Al-doped PbO 2 electrode showed high electrochemical activity, oxygen evolution potential, radical utilization rate, reusability and safety. The influence factors on CAP degradation with the Al-doped PbO 2 electrode were investigated in detail, and under the optimal conditions the removal rates of CAP and TOC reached 87.30% and 52.06% in acid conditions after 2.5   h electrolysis with a 0.2   mol   dm −3 Na 2 SO 4 at a current density of 30   mA   cm −2 , respectively. The electrochemical degradation of CAP at Al-doped PbO 2 electrode electrode followed pseudo-first-order kinetics. The degradation mechanism was proposed by cyclic voltammograms tests and it was deduced that hydroxyl radicals generated in the electrochemical process played a key role in oxidizing CAP. Finally, based on the reaction products identified, a possible degradation pathway including radical reaction, ring open and mineralization was proposed.

研究领域: 环境科学 · 电化学工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Strategy for enhancing the electrocatalytic performance of Ti/β-PbO2 anode: Optimizing SnO2 intermediate layer by Cs doping and application for the efficient removal of mixed fluoroquinolones

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 · 材料科学 · 化学工程
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Journal of Water Process Engineering · 2024 · IF 6.3

CNTs/Ce co-doped PbO2 anode for electro-oxidation of triclosan: Fabrication, kinetics, and degradation mechanism based on DFT calculations

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.

CAS / MDL: 3380-34-5
研究领域: 环境科学 · 材料科学 · 电化学工程
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2025 · IF 3.3

Degradation of Sulfamethazine by Ni-Doped Lead Dioxide Electrode in Electrocatalytic Ozonation Process

Zhouwei Li,Lianzhong Shen,Yu Ye,Qizhou Dai

An Ni-doped PbO2 electrode (Ti/TNAs/Ni-PbO2) with titanium dioxide nanotube arrays (TNAs) self-growth on the titanium metal surface as an intermediate layer was prepared by electrodeposition. Characterization and electrochemical testing of the Ti/TNAs/Ni-PbO2 showed a denser surface structure, a larger surface active area (0.50 m2 g-1), and smaller crystallite size (38.61 nm), which provided more surface active sites and promoted the generation of hydroxyl radicals (•OH). The electrocatalytic ozonation process was established using the electrode. The sulfamethazine (SMT) was selected as the target contaminant. The performance on SMT removal in electrocatalytic ozonation was systematically evaluated. The effects of initial SMT concentration, current density, electrolyte concentration, initial pH, and ozone dosage on the degradation rate of SMT and chemical oxygen demand (COD) removal were also investigated. Under optimal conditions, after 60 min of degradation, the removal rates of SMT and COD reached 100% and 46.13%, respectively. Intermediates in the degradation process were identified by ultra-performance liquid chromatography-quadrupole time-of-flight tandem mass spectrometry, and the degradation mechanism and degradation pathways of the Ti/TNAs/Ni-PbO2 anode in the electrocatalytic ozonation process were explored. The excellent efficacy and stability of this anode in this process were verified and showed a potential for widespread application in highly concentrated organic wastewater treatment

研究领域: 环境科学 · 化学工程 · 废水处理
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 11 ·116503 · IF 4.316

Enhanced Activity and Stability of PbO2 Electrodes by Modification with Octadecyl Phosphonic Acid

Jiajie Zhou,Senhui Huang,Zhiqiao He,Shuang Song

A novel Ti/Sn-SbOx/PbO2-ODP electrode was constructed using a β-PbO2 layer modified with octadecyl phosphonic acid (ODP) through a co-electrodeposition method. Scanning electron microscopy with an energy dispersive spectrometer, X-ray diffraction and contact angle goniometry confirmed that ODP was successfully embedded into the β-PbO2 layer of Ti/Sn-SbOx/PbO2-ODP, increasing the water contact angle at the electrode surface from 75.9° to 133.9°. The Ti/Sn-SbOx/PbO2-ODP electrode exhibited excellent electrocatalytic oxidation of ciprofloxacin (CIP). The pseudo first-order rate constant for CIP removal was 3.92 h−1 at an electrolytic potential of 10 V, 2.6 times greater than that when using the unmodified electrode. Moreover, electrode stability was greatly improved after ODP modification. The Ti/Sn-SbOx/PbO2-ODP electrode had longer accelerated life (324 h) than the Ti/Sn-SbOx/PbO2 electrode (91 h). The enhanced electrocatalytic performance of Ti/Sn-SbOx/PbO2-ODP was attributed to improved utilization of hydroxyl radicals (•OH) resulting from higher oxygen evolution potential. Furthermore, the hydrophobic surface of Ti/Sn-SbOx/PbO2-ODP was beneficial for stronger adsorption of CIP, as evidenced by the initial surface concentration test.

研究领域: 材料科学 · 环境工程 · 电化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2018 ·Vol. 165 ·期 11 ·H717 · IF 3.662

Enhancement of the Activity and Stability of PbO2 Electrodes by Modifying with Polydimethylsiloxane

Zhiqiao He,Jiajie Zhou,Xinwen Huang,Shihan Zhang,Shuang Song

The β-PbO2 of a Ti/Sn-SbOx/PbO2 electrode was modified with polydimethylsiloxane (PDMS) (Ti/Sn-SbOx/PbO2-PDMS) through a facile electrodeposition method. The results from scanning electron microscopy, energy-dispersive spectrometry and X-ray diffraction demonstrated that the PDMS was irreversibly adsorbed on the β-PbO2 of Ti/Sn-SbOx/PbO2-PDMS, leading to a decrease in the crystal size, surface cracks and preferential growth trend of β-PbO2. Compared with its PDMS-unmodified counterparts, the Ti/Sn-SbOx/PbO2-PDMS electrode exhibited relatively higher activity, selectivity and stability in the anodic oxidation of p-chlorophenol. Moreover, the Ti/Sn-SbOx/PbO2-PDMS electrode was more stable than the Ti/Sn-SbOx/PbO2 electrode, as evidenced by the accelerated life test. Based on the quantitative measurements of contact angle, hydroxyl radicals (HO•) and the initial surface concentration of various p-substituted phenols, including p-cresol, p-methoxyphenol, phenol, and p-chlorophenol, and with the help of electrochemical characterization of linear sweep voltammetry, it could be concluded that the improved electrochemical activity and stability of Ti/Sn-SbOx/PbO2-PDMS originated from the enhanced hydrophobicity of the electrode surface. Different from a traditional Ti/Sn-SbOx/PbO2 electrode with adsorbed HO• as the dominant active species, the Ti/Sn-SbOx/PbO2-PDMS with a hydrophobic surface favors the generation of more free HO•.

CAS / MDL: 98-54-4 70131-67-8
研究领域: 材料科学 · 环境科学 · 电化学
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