CHEMOSPHERE
·
2021
·
IF 7.086
Jieqi Feng,Qibin Tao,Hao Lan,Yi Xia,Qizhou Dai
In this study, nitrogen-doped carbon nanosheets (NCNSs) were prepared and successfully combined into the PbO 2 electrode by the composite electrodeposition technology , thereby NCNS–PbO 2 electrode was obtained. The electrochemical degradation of sulfamethoxazole (SMX) in aqueous solution by NCNS–PbO 2 electrode was studied. The main influence factors on the degradation of SMX, such as the initial concentration of SMX, current density, electrolyte concentration and initial pH value, were analyzed in detail. Under the optimal process conditions, after 120 min of treatment, the removal ratio of SMX and chemical oxygen demand (COD) reached 99.8 % and 60.7 %, respectively. The results showed that the electrochemical degradation of SMX fitted pseudo-first-order reaction kinetics. The electrochemical performance of NCNS–PbO 2 electrode was better than that of PbO 2 electrode by scanning electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy, as well as the use of cyclic voltammetry and electrochemical impedance spectroscopy for electrochemical performance testing. This was because the doping of nitrogen atoms improved the properties of carbon nanosheets. After the composite, the active sites on the surface of PbO 2 were improved, the particle size of PbO 2 was reduced, and the electrical conductivity and electrocatalytic activity of the electrode were improved. In addition, the intermediate products were determined by GC-MS method, and the possible degradation pathways of SMX were proposed.
研究领域:
环境科学
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电化学
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污染控制
✓ 已验证
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
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 .
研究领域:
环境科学
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电化学工程
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污染控制
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产品关联
DOI
PubMed
高影响因子
ECS Journal of Solid State Science and Technology
·
2020
·Vol. 9
·期 12
·123012
·
IF 2.142
Junze Zhang,Hongning Wang,Ruoyu Chen
During the electrochemical preparation process, the electron transport rate in the PbO2 active layer could be greatly increased resulting from reduction in the oxidation of the Ti substrate, which effectively improved the service life and catalytic degradation efficiency of the PbO2 Dimension Stable Anode (PbO2 DSA) electrode. Through adding nano-acetylene black (ACET) and polyvinyl pyrrolidone (PVP) into the plating solution, an ACET doped Ti/PbO2 electrode was successfully prepared via an anodic oxidation method. Results of field emission scanning electron microscope (FESEM), diffraction of X-rays (XRD), transmission Electron Microscope(TEM) and X-ray photoelectron spectroscopy (XPS) characterization indicated that 2.10 ∼ 2.75 wt% of ACET doping amount hardly changed the morphology and lattice constant of the PbO2 electrode. With electrochemical alternating current impedance spectroscopy (EIS) and cyclic voltammetry (CV), it confirmed that ACET reduced the charge transfer impedance (Rct) of the PbO2 electrode up to 95%, and restrained the potential of oxygen evolution reaction(OER). With the increase of electron transport rate, the generation rate of hydroxyl radicals (·OH) on the electrode surface was enhanced significantly. Compared with the Ti/PbO2 electrode, the ACET-doped Ti/PbO2 electrode exhibited higher electrocatalytic efficiency to phenol degradation. During the degradation process, the consumption of time and energy could be reduced by 33% and 34%, respectively. At the same current density, the required voltage for preparing the ACET-modified Ti/PbO2 electrode was much lower. In the assistant of lower deposition voltage, the ACET-doped Ti/PbO2 electrode possessed a stronger binding force to Ti substrate, and meanwhile obtained a longer lifespan.
研究领域:
电化学
·
材料科学
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DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Yi Xia,Jieqi Feng,Siqi Fan,Wan Zhou,Qizhou Dai
In this study, the CNTs were successfully compounded in PbO 2 electrode through composite electrodeposition technology to obtain multi-layer CNT-PbO 2 electrode. Scanning electron microscope , X-ray diffraction and X-ray Photoelectron Spectroscopy were comprehensively used to characterize the lead dioxide electrode and the electrochemical performance were also tested by cyclic voltammetry, and electrochemical impedance spectroscopy. Results showed that CNT-PbO 2 significantly improved the electrochemical performance, which was attributed to that the compound of CNTs in PbO 2 improved the active sites on the surface, with higher oxidation peaks, smaller particle size, larger specific surface area, and lower charge transfer resistance. In the degradation experiment, the chemical oxygen demand removal efficiency of isoniazid by CNT-PbO 2 electrode were 1.37 times of that by pure PbO 2 electrode. The main influence factors on the degradation of ISN, such as initial ISN concentration, Na 2 SO 4 concentration, current density and initial pH value was analyzed in detail. Considered comprehensively the effects of ISN removal efficiency, COD and average current efficiency, the degradation of ISN and COD reached 99.4% and 86.8%, respectively, after the electrode was degraded by electrochemical oxidation for 120 min under the best conditions. In addition, the degradation mechanism of ISN in electrochemical oxidation was studied. According to the intermediate products detected by GC-MS, the possible degradation pathway of ISN in electrochemical oxidation system were proposed.
研究领域:
环境科学
·
材料科学
·
电化学工程
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yan Yan,Xiangjuan Ma,Yijing Xia,Huajun Feng,Shengjue Liu,Cong He,Yangcheng Ding
A PbO 2 electrode integrating electrocatalytic and adsorptive functions was successfully fabricated by embedding layer-by-layer graphene nanoplatelets (GNPs) into β-PbO 2 active layer (GNPs/PbO 2 ) and employed as anode for high-efficient removal of sulfadiazine (SDZ). In electrochemical degradation experiments, SDZ was quickly enriched on the surface of GNPs/PbO 2 film via adsorption and then oxidized by ⋅OH in-site. In terms of the electrocatalytic performance and adsorption of electrode, the optimal electrodeposition time for each β-PbO 2 outer layer was 4 min (GNPs/PbO 2 -4). Compared with conventional PbO 2 electrode, the layer-by-layer GNPs resulted in the smaller crystal size and denser surface of PbO 2 electrode, thus facilitating the generation of active oxygen species. At the same time, the specific surface area, oxygen evolution potential (OEP) of the anode were enhanced and the charge-transfer resistance was reduced. For GNPs/PbO 2 -4 anode, the optimal conditions of electrochemical oxidation of SDZ were identified as initial pH 9, 50 mg/L of SDZ and 20 mA/cm 2 of current density using response surface methodology (RSM), 98.15% of SDZ could be removed in this case. The contribution of radical oxidation and non-radical oxidation to SDZ removal was about 79% and 21%, respectively. Moreover, the reaction pathways of SDZ on the GNPs/PbO 2 -4 electrode involving hydroxylation, radical reaction and ring cleavage were speculated. Finally, the continuous SDZ degradation and accelerated service lifetime test suggested that the GNPs/PbO 2 -4 electrode was shown to be stable and repeatable, and the Pb 2+ concentration was measured to ensure the safety of the treated solution. Consequently, the above findings provide an innovative way to design and prepare an effective and stable PbO 2 electrode for electrochemical degradation of antibiotic wastewater.
研究领域:
环境科学
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电化学工程
·
废水处理
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Yifei Peng,Yan Yan,Xiangjuan Ma,Bowen Jiang,Ruya Chen,Huajun Feng,Yijing Xia
This paper aims to develop a flow-through electrochemical system with a series of graphene nanoparticles loaded PbO 2 reactive electrochemical membrane electrodes (GNPs-PbO 2 REMs) on porous Ti substrates with pore sizes of 100, 150, 300 and 600 μm, and apply them to treat antibiotic wastewater. Among them, the GNPs-PbO 2 with Ti substrate of 150 μm (Ti-150/GNPs-PbO 2 ) had superior electrochemical degradation performance over the REMs with other pore sizes due to its smaller crystal size, larger electrochemical active specific area, lower charge-transfer impedance and larger oxygen evolution potential. Under the relatively optimized conditions of initial pH of 5, current density of 15 mA cm −2 , and membrane flux of 4.20 m 3 (m 2 ·h) −1 , the Ti-150/GNPs-PbO 2 REM realized 99.34% of benzylpenicillin sodium (PNG) removal with an EE/O of 6.52 kWh m −3 . Its excellent performance could be explained as the increased mass transfer. Then three plausible PNG degradation pathways in the flow-through electrochemical system were proposed, and great stability and safety of Ti-150/GNPs-PbO 2 REM were demonstrated. Moreover, a single-pass Ti-150/GNPs-PbO 2 REM system with five-modules in series was designed, which could consistently treat real antibiotic wastewater in compliance with disposal requirements of China. Thus, this study evidenced that the flow-through electrochemical system with the Ti-150/GNPs-PbO 2 REM is an efficient alternative for treating antibiotic wastewater.
研究领域:
环境科学
·
材料科学
·
污水处理
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 12
·123502
·
IF 4.386
Qibin Tao,Hao Lan,Lanlan Wei,Lu Chen,Mili Weng,Qizhou Dai
An innovative CMS-PbO2 electrode was fabricated by combining hydrothermally synthesized carbon microspheres (CMS) on a PbO2 electrode by electrodeposition. Using the CMS-PbO2 electrode, the main factors affecting Isopropylantipyrine (PRP) degradation were studied. Under optimum process conditions, the concentration of PRP was 50 mg l−1, the applied current density was 30 mA cm−2, the electrolyte (Na2SO4) concentration was 0.1 mol l−1, and pH was 7. The PRP degradation rate reached 100%, and chemical oxygen demand (COD) removal rate reached 43.42% after 120 min of electrochemical oxidation. Using field-emission scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, cyclic voltammetry, linear sweep voltammetry, and electrochemical impedance spectroscopy, the electrochemical performance of the two electrodes was discussed. The composite of carbon microspheres successfully improved the electrochemical activity of the electrode and its conductivity. Furthermore, the ability of the two electrodes to generate hydroxyl radicals was compared and the possible degradation pathway of PRP was considered. In addition, electrode stability and safety were evaluated by accelerated lifetime experiments and detection of lead ions in solution after electrochemical oxidation. The CMS-electrode was more stable and safer than the PbO2 electrode. The CMS-PbO2 electrode provides a new strategy for the treatment of pharmaceutical wastewater.
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
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jianqiang Ye,Buming Chen,Jun Guo,Hui Huang,Yapeng He,Shixing Wang
High oxygen evolution overpotential and low corrosion resistance are regarded as the main drawbacks of anode materials in zinc electrowinning . To improve the electrocatalytic activity of oxygen evolution reactions (OER) and reduce energy consumption in zinc electrowinning, a Co 3 O 4 nanoparticle-modified PbO 2 anode was prepared on a Ti substrate with Sn-SbO X as an interlayer through pulse electrodeposition . The surface morphology, phase composition, and electrochemical properties of the as-prepared anode were systematically investigated. The introduction of Co 3 O 4 nanoparticles refined the crystal size of PbO 2 and increased the surface roughness of the anode. Electrochemical tests suggested the excellent electrocatalytic activity of the Co 3 O 4 nanoparticle-modified PbO 2 anode. Density functional theory (DFT) calculations revealed that Co 3 O 4 nanoparticles reduced the OER free energy (1.58 eV) and that pulse electrodeposition reduced the PbO 2 crystal size and increased the active surface area of the anode. In the simulated zinc electrowinning test, an improved current efficiency (90.6 %) was achieved, and the low energy consumption (2,508.29 kW·h) for zinc production per ton was significantly reduced as compared with that for the conventional Pb-0.75 %Ag anode. The lifetime of the modified electrode is increased by approximately 36.8 %. This provides a reference for the design and development of anode materials with high oxygen evolution activity and strong corrosion resistance in zinc electrowinning systems.
研究领域:
材料科学
·
电化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
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
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 12
·123504
·
IF 4.316
Yuan Du,Liu Hao,Wang Zixuan,Wang Xi,Miao Guirong,Wu Xu
β-PbO2 is an important high oxygen overpotential anode coating material. Further study on nanoscale β-PbO2 with higher performance and lower cost is a critical issue in order to develop the electrochemical ozone generator. Herein, an improved β-PbO2 nanoparticles synthesizing strategy based on the traditional Pb(OAc)4 hydrolysis method is proposed in this work, which is more scalable for industrial-scale production compared with existed nano β-PbO2 synthesizing methods. The possible mechanism of synthesizing β-PbO2 nanoparticles via Pb(OAc)4 hydrolysis was discussed for the first time. Based on the proposed mechanism, the size and morphology of the β-PbO2 nanoparticles were effectively controlled, and alternative raw material that can significantly reduce costs was developed. SEM, TEM, XRD, and XPS results indicate that pure phase β-PbO2 nanoparticles range from 10–30 nm were obtained. In addition, the use of alternative raw materials reduces the cost by 90%–95% compared to the traditional Pb(OAc)4 hydrolysis method. The β-PbO2 nanoparticles showed good ozone generation performances. The energy consumption per unit ozone of the β-PbO2 nanoparticles is reduced by 51.9% at the optimized operation condition than the reference PbO2 particles used for comparison.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yijing Xia,Jingsong Dai,Yan Yan,Xiangjuan Ma,Huajun Feng,Yangcheng Ding
The purpose of this research is to study the pulse electrochemical oxidation of paracetamol (PCT) using a novel PbO 2 anode based on pulse electrodeposition strategy (PbO 2 -PE). The pulse electrodeposition strategy used to prepare a PbO 2 anode resulted in rougher surface, higher directional specificity of β(101) and more redox couples of Pb 4+ /Pb 2+ . Additionally, the oxygen evolution potential (OEP) and charge transfer resistance were also improved. When compared to direct current electrochemical oxidation process, pulse electrolysis in had a slightly higher PCT removal efficiency and active species (·OH and active chlorine) production, while 72.04% of energy consumption was saved. The effects of operating parameters on PCT degradation efficiency and specific energy consumption were studied. The findings suggested that the pulse electrochemical oxidation of PCT followed a pseudo-first-order kinetic model, with PCT removal reaching 98.63% after 60 min of electrolysis under optimal conditions. Possible mechanisms describing reaction pathways for PCT were also proposed. Finally, combinating with the economic feasibility and safety evaluation, we could conclude that pulse electrolysis with a PbO 2 -PE electrode was a promising option for improving the practicability of electrochemical treatment for refractory organic wastewater.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Yonghao Zhang,Liankai Gu,Ying Zhang,Jing Yang,Qian Li,Shuyan Yu,Congju Li,Kajia Wei
In this work, a novel porous-structure electrochemical PbO 2 filter (PEF-PbO 2 ) was developed to achieve the reuse of bio-treated textile wastewater. The characterization of PEF-PbO 2 confirmed that its coating has a variable pore size that increases with depth from the substrate, and the pores with a size of 5 μm account for the largest proportion. The study on the role of this unique structure illustrated that PEF-PbO 2 possesses a larger electroactive area (4.09 times) than the conventional electrochemical PbO 2 filter (EF-PbO 2 ) and enhanced mass transfer (1.39 times) in flow mode. The investigation of operating parameters with a special discussion of electric energy consumption suggested that the optimal conditions were a current density of 3 mA cm −2 , Na 2 SO 4 concentration of 10 g L −1 and pH value of 3, which resulted in 99.07% and 53.3% removal of Rhodamine B and TOC, respectively, together with an MCE TOC of 24.6%. A stable removal of 65.9% COD and 99.5% Rhodamine B with a low electric energy consumption of 5.19 kWh kg −1 COD under long-term reuse of bio-treated textile wastewater indicated that PEF-PbO 2 was durable and energy-efficient in practical applications. Mechanism study by simulation calculation illustrated that the part of the pore of the PEF-PbO 2 's coating with small size (5 μm) plays an important role in this excellent performance which provides the advantage of rich ·OH concentration, short pollutant diffusion distance and high contact possibility.
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
PubMed
高影响因子
危险品化学品经营许可证（带存储）