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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Energy-efficient pulse electrochemical oxidation of Acid Blue 9 using a Ti/SnO2-Sb/α,β-Polytetrafluoroethylene-Fe-PbO2 electrode: Kinetics, mass transfer and mechanism

Xiangjuan Ma,Yan Yan,Qizhou Dai,Jianxian Gao,Shengjue Liu,Yijing Xia

This study focused on the electrochemical oxidation of Acid Blue 9 (AB 9) under direct and pulse current modes using a Ti/SnO 2 -Sb/α,β-Polytetrafluoroethylene-Fe-PbO 2 (PTFE-Fe-PbO 2 ) anode. The results showed that 99.0% of AB 9 and 68.9% of COD could be eliminated at initial pH of 5, initial AB 9 concentration of 100 mg L -1 , pulse frequency of 4000 Hz, current density of 20 mA cm −2 and pulse duty cycle of 50% after 120 min of electrolysis. The pulse electrochemical oxidation of AB 9 at the investigated conditions followed pseudo-first-order kinetics. Compared with the direct current mode, 76.0% of energy consumption could be saved at pulse current mode. The effect of mass transfer and electrode distance on the pulse electrochemical oxidation of AB 9 was also investigated in terms of mass transfer coefficient and effectiveness factor, the results showed that the reduced electrode distance was beneficial to improve the mass transfer and oxidation efficiency, as well as the energy efficiency. LC-MS analysis revealed that benzenesulfonate group, C-N and C-S bonds in AB 9 molecule were initially cleaved under the attack of ⋅OH, then some carboxylic acids were formed and eventually mineralized to CO 2 and H 2 O. Therefore, pulse electrochemical oxidation with a PTFE-Fe-PbO 2 electrode might be a promising alternative to enhance the practicability of electrochemical treatment for dye wastewater.

研究领域: 环境工程 · 电化学 · 废水处理
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BIOELECTROCHEMISTRY · 2023 · IF 5

A sandwich-type electrochemical immunosensor for sensitive detection of HER2 based on dual signal amplification of La-MOF-PbO2 and PEI-MoS2NFs composites

Qin Xia,Zhaode Mu,Min Qing,Jing Zhou,Lijuan Bai

In recent decades, the incidence of breast cancer has increased year by year, posing a serious threat to human health and quality of life, and about 30% of breast cancer patients have human epidermal growth factor receptor 2 (HER2) overexpression. Therefore, HER2 has become an important biomarker and indicator for the clinical evaluation of breast cancer in diagnosis, prognosis and recurrence. In this work, polyethyleneimine functionalized MoS 2 nanoflowers (PEI-MoS 2 NFs) with good electrical conductivity and abundant active binding sites were designed and employed as a sensing platform for immobilizing the primary antibody of HER2 (Ab 1 ). In addition, a La-MOF-PbO 2 composite with a large specific surface area and good conductivity was used to load lots of electroactive toluidine blue (TB) and the secondary antibody of HER2 (Ab 2 ) via gold nanoparticles (AuNPs) as the linker. Thus, the constructed sandwich-type electrochemical immunosensor was applied for sensitive detection of HER2, which showed a wide linear range from 100 fg mL −1 to 10 μg mL −1 with a lower limit of detection of 15.64 fg mL −1 . Therefore, the resulting immunosensor in this study would have a potential application in clinical bioanalysis.

研究领域: 生物医学工程 · 分析化学 · 癌症研究 · 电化学
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RSC Advances · 2015 ·Vol. 5 ·期 103 ·84856-84864 · IF 3.84

Electrochemical degradation of perfluorooctanoic acid (PFOA) by Yb-doped Ti/SnO2–Sb/PbO2 anodes and determination of the optimal conditions

Qianchi Ma,Lei Liu,Wei Cui,Ruifeng Li,Tingting Song,Zhaojie Cui

Model aqueous solutions of perfluorooctanoic acid (PFOA, 100 mg L−1) were electro-oxidized in a homemade container. The electrocatalytic behavior and anodic performance of Ti/SnO2–Sb/Yb–PbO2, Ti/SnO2–Sb–PbO2 and Ti/SnO2–Sb–Yb anodes in sodium electrolytes were compared. The SnO2–Sb/Yb–PbO2 anode demonstrated better electrocatalytic performance compared with the SnO2–Sb–PbO2 and SnO2–Sb–Yb electrodes in terms of both degradation and defluorination. Then a systematic experimental study was designed as follows to analyze the influencing factors: initial concentration of PFOA (10 mg L−1 to 200 mg L−1), current density (1 mA cm−2 to 40 mA cm−2), initial pH value (3 to 11) and electrode distance (5 mm to 20 mm). After a 150 min electrolysis, the optimum reaction conditions were obtained and the degradation and defluorination ratios reached 95.11 ± 3.9% and 75.7 ± 2.8%, respectively. Under the optimum conditions, the degradation of PFOA followed pseudo-first-order kinetics (0.0193 min−1) and the degradation half-life was 35.9 min. The produced F− was measured using a fluoride ion selective electrode, whereas the intermediate PFCAs with short-chain lengths were measured using HPLC-MS. A detailed degradation pathway was proposed in this study by analyzing the intermediates and the recovery of fluoride.

CAS / MDL: 422-64-0
研究领域: 环境科学 · 化学工程 · 分析化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Hydrophobic Ce-doped β-PbO2-SDS anode achieving synergistic effects for enhanced electrocatalytic oxidation of As(III)

Wenlan Ji,Yuan Wang,Yuanjie Xiong,Tian C. Zhang,Shaojun Yuan

To strengthen the utilization of free radicals and effectively enhance electrocatalytic performance and service lifetime of the β -PbO 2 electrode, herein, a novel hydrophobic TNAs/SnO 2 /PPy/ β -PbO 2 -Ce-SDS (abbreviated as β -PbO 2 -Ce-SDS) anode was synthesized by doping Ce 3+ and anionic surfactant (SDS) to TNAs/SnO 2 /PPy/ β -PbO 2 (abbreviated as β -PbO 2 ), which was constructed by growing SnO 2 /PPy/ β -PbO 2 multilayers on TiO 2 nanotube arrays (TNAs) via combination of electrodeposition and electro-polymerization processes. Notably, co-modification with Ce 3+ and SDS remarkably enhanced the surface hydrophobicity, electrochemical performance and catalytic ability of β -PbO 2 anode. Such β -PbO 2 -Ce-SDS anode not only substantially enhanced the As(III) conversion (96.96%) in the electrocatalytic oxidation process, but also prominently strengthened its service lifetime. Furthermore, the as-prepared β -PbO 2 -Ce-SDS anode possessed an excellent stability as its kinetic constant was only reduced from 0.18 to 0.14 min −1 even underwent 10 cycles of the electrocatalytic process, while that of the unmodified β -PbO 2 electrode decreased markedly by about 49%, owing to its appropriate surface hydrophobicity, smaller grains and denser β -PbO 2 layer. The reaction mechanism of electrocatalytic oxidation was associated with synergistic effects of hydroxyl radical ( OH), superoxide radicals ( O 2 − ), and sulfuric acid root radicals ( SO 4 − ). The β -PbO 2 -Ce-SDS anode provides a novel and feasible approach to development of various electrodes by doping metal ions and/or regulating with surfactants.

研究领域: 电化学 · 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Electrochemical study of a novel high-efficiency PbO2 anode based on a cerium-graphene oxide co-doping strategy: Electrodeposition mechanism, parameter optimization, and degradation pathways

Xiaolu Fu,Yanhe Han,Han Xu,Zhimin Su,Lina Liu

A novel and efficient Ti/SnO 2 -Sb/PbO 2 -GO-Ce electrode was successfully fabricated based on the co-deposition of Ce ions and graphene oxide (GO) into β-PbO 2 crystals and used as an anode for electrocatalytic oxidation of phenol . The electrodeposition mechanism, parameter optimization, mechanism analysis, and potential degradation pathways were discussed in depth. The co-doping of GO and Ce resulted in the high directional specificity of β(301), orderly and dense grain arrangement of PbO 2 crystals. At the same time, the oxygen evolution potential, •OH generation capacity and lifetime were also improved. The effects of experimental parameters on phenol removal efficiency were evaluated, including the applied current density, electrode gap, supporting electrolyte, initial NaCl concentration, initial pH, and initial phenol concentration. Under the optimal conditions, the removal efficiency of phenol can reach 375.6 g m -2 h -1 for 20 min electrolysis, which is about 1.2 times that of the pure PbO 2 electrode. The active oxygen species (•OH, ClO - and HClO) were important attributes to the degradation of phenol. Additionally, a potential degradation pathway for phenol was proposed. After 10 successive recycles, there was no significant difference of the electro-generated •OH, cell voltage and phenol removal rate, which confirms the stability and admirable reusability of Ti/SnO 2 -Sb/PbO 2 -GO-Ce electrode.

研究领域: 电化学 · 材料科学 · 环境工程 · 催化
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Constructing a multilayered film βPbO2ZrO2 electrode for energy-efficient zinc electrowinning

Jianqiang Ye,Buming Chen,Shixing Wang

The zinc electrowinning process demands considerable energy, prompting the quest for energy-efficient solutions to curtail costs. Hence, the development of energy-saving anode materials for zinc hydrometallurgy is an important issue. Herein, multilayered PbO 2 film materials were prepared through thermal decomposition and composite electrodeposition, yielding a new PbO 2 –ZrO 2 electrode featuring ZrO 2 particles as the second phase for energy-saving zinc electrowinning. The introduction of ZrO 2 leads to reduced PbO 2 crystal size, heightened the specific surface area of the electrode, and preferential growth of crystal planes. Electrochemical tests underscore that the PbO 2 –ZrO 2 electrode manifests a reduced charge-transfer resistance ( R ct ) and overpotential alongside a 46.15 % extension in service life compared to the pure PbO 2 electrode. Simulated zinc electrowinning experiment affirms PbO 2 –ZrO 2 electrode has a 3.63 % surge in the current efficiency and a substantial 244.61 kWh/t reduction in energy consumption relative to the traditional Pb–0.6wt%Ag anode. This study provides a strategic framework for designing and developing cost-efficient, cost-effective anode materials, promoting advancements in energy conservation and consumption reduction within zinc electrowinning processes.

CAS / MDL: 1314-23-4
研究领域: 材料科学 · 电化学工程
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International Journal of Electrochemical Science · 2023 ·Vol. 13 ·期 12 ·11720-11729 · IF 1.5

Electrochemical Oxidation of Tetracaine Hydrochloride using a Transition Metal Doped PbO2 Electrode

Mili Weng,Miaoquan Huang

Pharmaceutical wastewater is a kind of biorefractory organic wastewater and could not be treated efficiently by the traditional biological wastewater process with the ever-increasing discharge standard. This work prepared Al/Zn doped PbO 2 anodes and used them to treat tetracaine hydrochloride by electrochemical oxidation process. The effects of operational factors, such as current density, initial concentration of tetracaine hydrochloride and the initial value of pH, were explored and discussed. The results showed that the electrochemical oxidation using Al/Zn doped PbO 2 electrode is an effective solution to treat this kind of wastewater. And the removal efficiency of tetracaine hydrochloride and COD were above 97.35% and 59.56% after 120 min at typical condition. The degradation mechanism was analyzed and the reaction mechanism was discussed by the free radical reaction mechanism of direct oxidation and indirect oxidation. This paper could provide basic data of electrochemical oxidation for the tetracaine hydrochloride and other pharmaceutical wastewater pollution control.

研究领域: 环境工程 · 电化学 · 水处理 · 高级氧化技术
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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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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Eu/GO/PbO2 composite based anode for highly efficient electrochemical oxidation of hydroquinone

Zhengting Zhang,Guiyun Yi,Peng Li,Xikui Wang,Xiaodong Wang,Chuanxiang Zhang,Yulong Zhang,Qi Sun

Herein, a novel europium/graphene oxide/lead oxide (Eu/GO/PbO 2 ) composite based anode with excellent electrocatalytic performance towards degradation of hydroquinone was prepared by a facile co-electrodeposition method. The composition and micromorphology of the anode was investigated by scanning electron microscopy (SEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) and the results confirmed that europium (Eu) and graphene oxide (GO) were successfully composited with PbO 2 and a more compact structure was obtained, which was conductive to enhancing the corrosion resistance of the electrode. Besides, electrochemical measurements indicated that Eu/GO/PbO 2 electrode possessed longer service lifetime (87 h), higher oxygen evolution potential (2.64 V), and lower charge transfer resistance (41.08 Ω) than GO/PbO 2 and pure PbO 2 electrode. The promoted electrocatalytic activity of Eu/GO/PbO 2 electrode was ascribed to its stronger hydroxyl radical generation ability, more active sites and lower electron transfer resistance. Additionally, effects of initial hydroquinone concentration, applied current density and initial pH value on the degradation performance of Eu/GO/PbO 2 anode were systematically investigated. The behind degradation mechanism of hydroquinone by Eu/GO/PbO 2 anode was speculated on the basis of the major intermediates identified by high performance liquid chromatography-mass spectrometer (HPLC-MS). Under the continuous attack of free hydroxyl radicals, hydroquinone was finally decontaminated into CO 2 and H 2 O. The present work demonstrated that Eu/GO/PbO 2 composite anode exhibited excellent degradation performance towards hydroquinone.

研究领域: 环境科学 · 材料科学 · 电化学
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ChemCatChem · 2026 ·Vol. 18 ·期 17 ·e71045 · IF 4.1

Ni-Mediated Pb-O Bond Activation in β-PbO2 for Efficient Ozone Electrosynthesis

Sheng Huang,Lianwei Deng,Gao-Feng Chen,Liang-Xin Ding,Haihui Wang

Electrocatalytic ozone production (EOP) provides a sustainable route for advanced oxidation processes. Among various candidates, β-PbO 2 stands out as a proven ozone catalyst; however, its widespread implementation is severely hindered by sluggish kinetics and poor selectivity. Herein, we report a Ni-mediated electrocrystallization strategy that perturbs the local Pb–O environment within the β-PbO 2 framework without appreciable Ni incorporation into the final catalyst. Synchrotron x-ray absorption spectroscopy (XAS), combined with x-ray diffraction (XRD) and x-ray photoelectron spectroscopy (XPS), suggests the presence of lattice strain, electronic-state redistribution, and enhanced local structural disorder. These coupled geometric and electronic changes are consistent with enhanced lattice-oxygen participation during EOP. Consequently, the lattice oxygen-activated PbO 2 (O act -PbO 2 ) exhibits an O 3 yield of 425.6 mg h −1 g cat −1 (a 4.21-fold enhancement over pristine PbO 2 ) and a Faradaic efficiency of 14.73% at 2.5 V versus Ag/AgCl. Notably, an O 3 concentration of 12.30 mg L −1 is achieved within 5 min, and the electrode maintains stable operation for 300 h at 100 mA cm −2 . Furthermore, we establish a rapid and reliable analytical protocol for the quantification of electrogenerated O 3 . This work provides atomic-level insights into lattice oxygen activation and offers an effective strategy for the design of high-efficiency ozone electrosynthesis catalysts. Graphical A Ni-mediated electrocrystallization strategy is employed to regulate the local Pb–O framework without appreciable Ni incorporation. The resulting geometric and electronic modulations favor lattice-oxygen participation during ozone electrosynthesis, enabling an O 3 concentration of 12.30 mg L −1 and stable operation for 300 h.

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ChemElectroChem · 2022 ·Vol. 9 ·期 22 ·e202200919 · IF 4.782

Phase/Size-Controlled Synthesis of Nanostructured PbO2 Microspheres for Efficient Electrochemical Ozone Generation

Qiuyang Yu,Xiaohong Hu

Graphical O 3 generation : By adjusting the concentration of sodium hydroxide during hydrothermal preparation process, the phase and size-controlled synthesis of PbO 2 was achieved. Later, a phase/size effect in electrochemical ozone generation reaction was found and an optimal PbO 2 microsphere catalyst was successfully screened out. This achieved a 61 % higher O 3 current efficiency at 2 A cm −2 than electrochemically prepared PbO 2 -based catalyst. Traditional electrochemically prepared lead dioxide (e-PbO 2 ) is one of the most used electrode materials for electrochemical ozone production (EOP), because of its high catalytic activity, excellent electrical conductivity, relative stability and low cost. But the electrochemically prepared conditions are complicated and harsh. Bulk PbO 2 electrodes have the very limited surface area and are inconvenient to process into the fine film electrodes for a PEM electrolyser. In contrast, chemical synthesis is easy to prepare uniform PbO 2 catalysts with high surface area and catalytic activity. Here, a facile one-pot approach to prepare a highly active PbO 2 microsphere catalyst was established and used for the EOP reaction in a PEM ozone generator. Sodium hydroxide could be used to regulate the relative content of α/β allotropic phase and crystallite size of PbO 2 microspheres. Experiment results revealed that high β phase content and large β-PbO 2 crystallite size were beneficial to the high EOP activity. By optimizing the composition and crystal structure, chemically prepared PbO 2 could have much better EOP performance than e-PbO 2 .

CAS / MDL: 9002-84-0
研究领域: 材料科学 · 环境科学
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International Journal of Electrochemical Science · 2023 · IF 1.5

Coating Electrode for Oxygen Evolution Reaction

Shiwei He,Ruidong Xu,Bohao Yu,Yuqing Guo,Zhongsheng Hua,Fuyuan Zhang,Huihong Lv

In this study, β-PbO2-WC composite coatings were synthesized on a substrate using the electrodeposition method in an electrolyte containing Pb 2+ and WC particles. The preparation process study shows that the β-PbO2 bath containing WC particles becomes more stable for an ultrasonic dispersion time within 30 minutes. WC particles in the β-PbO2 bath are positively charged, with anions being adsorbed onto the particles. Compared to the β-PbO2 composite electrode, the oxygen evolution overpotentials for the P-PbO2-WC electrode are decreased, which demonstrates an energy-saving effect. The nucleation behavior study shows that the co-deposition of WC particles into the layer has little effect on the crystal growth of P-PbO2. The main process during the deposition time of 0~5 min were the nucleation of the β-PbO2 grains, the adsorption of WC particles, growth of β-PbO2 grains, and WC particles coated.

研究领域: 材料科学 · 电化学
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