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
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废水处理
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产品关联
DOI
PubMed
高影响因子
Nano Research
·
2023
·Vol. 16
·期 8
·11042-11047
·
IF 9.9
Wang Lei,Zhang Yuehan,Sun Xiaoxuan,Li Yunhui,Zhai Junfeng,Dong Shaojun
Eco-friendly chemical oxygen demand (COD) sensors are highly desired with respect to the importance of COD determination in environmental protection. In this work, a new FTO/TiO 2 /PbO 2 (FTO = fluorine-doped tin oxide) electrode was fabricated with a two-step method and used as an eco-friendly electrochemical COD sensor. The interlayer TiO 2 was employed to strengthen the adhesion of PbO 2 on the FTO substrates by providing a large TiO 2 /PbO 2 interface area. The effects of the factors including applied potential, supporting electrolyte concentration and stirring speed on the sensing performance were investigated. Under the optimized conditions, linear responses to the COD of water with different COD sources were achieved, and a linear range from 5 to 120 mg/L was obtained in the case of sucrose as the COD source. The relative standard deviations (RSD) were determined to be less than 9% for the glucose solutions with the COD of 7.5, 12.5 and 17.5 mg/L. For real sample analysis, the obtained results were comparable with those measured with the conventional dichromate method, with a relative error less than 11%.
研究领域:
环境科学
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分析化学
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产品关联
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
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
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材料科学
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2025
·Vol. 172
·期 4
·043505
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IF 3.3
Xuefei Zhang,Bing Wu,Siwei Zhuang,Jianglin Cao
Electrocatalytic oxidation using PbO2 electrodes is a prospective strategy for treatment of bio-refractory dye wastewater. However, it is hindered by high energy consumption, poor degradation efficiency, and low anode stability. Here, PbO2 electrodes were reconstructed by intercalating and surface-intervening with graphene oxide (GO) to enhance the stability of the composite electrodes and achieve high-efficiency oxidation of cationic red GTL. Compared with that on PbO2, reactive oxygen species (e.g., ·OH and ·O) on GO-PbO2 were less consumed by the oxygen evolution reaction due to their larger spacing on GO-PbO2. In addition, GO-PbO2 showed lower cell voltage than PbO2, indicating a higher electron transfer rate and lower energy consumption. The coupled free radical behavior and electron transfer enhanced the decolorization (1.7 times that of PbO2) and mineralization (1.4 times that of PbO2) rate of cationic red GTL on GO-PbO2. Furthermore, doping of GO with multilayer structure improved the stability of PbO2 anode and its performance improvement mechanism was revealed. The prepared GO-PbO2 electrode prolonged service-life (162 h) under accelerated electrolysis, about 2.7 times that of the PbO2 electrode (60 h). This work provides a novel GO-PbO2 electrode for efficient electrocatalytic degradation of GTL, and can be easily extended to electro-degradation of non-biodegradable wastewater.
研究领域:
环境科学
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电化学工程
✓ 已验证
产品关联
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
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材料科学
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电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
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
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
·
电化学
·
污染控制
✓ 已验证
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
Journal of Hazardous Materials Advances
·
2023
·
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
·
电化学工程
✓ 已验证
DOI
Environmental Science-Nano
·
2024
·
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
·
电化学工程
·
理论化学
✓ 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）