ENVIRONMENT INTERNATIONAL
·
2019
·
IF 7.943
Chengzhi Zhou,Yanping Wang,Jie Chen,Junfeng Niu
Electrochemical degradation of trace antiretroviral drug stavudine was investigated by using a reactive electrochemical membrane (REM) with Ti/SnO 2 -Sb anode. From the results it was evident that the stavudine degradation followed pseudo-first-order kinetics, with the values of the degradation rate constant and half-life being 0.24 min −1 and 2.9 min, respectively, at a current density of 8 mA cm −2 . The degradation rate was obviously decreased under alkaline condition (pH = 11.0) and the degradation was also inhibited in the presence of NO 3 − and Cl − . Five intermediates were identified in the electrochemical degradation of stavudine, and the degradation pathways were proposed. Density functional theory calculation revealed that the double bond carbon atom nearby hydroxymethyl group was the site attacked by OH and the cleavage of C N bond was the rate-determining step in the electrochemical degradation of stavudine. The nitrogen in stavudine was mainly converted to nitrate and ammonium. Quantitative structure-activity relationship model indicated that the toxicity of some intermediates was higher than the parent compound stavudine. The electric energy consumption for 90% stavudine degradation ranged from 0.87 to 2.29 Wh L −1 at the experimental conditions, indicating that stavudine can be degraded efficiently by the REM with Ti/SnO 2 -Sb anode.
研究领域:
环境科学
·
电化学工程
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Chuang Li,Dan Wang,Norihiro Suzuki,Chiaki Terashima,Yichun Liu,Akira Fujishima,Xintong Zhang
Oxygen evolution over semiconductor photoanodes plays a decisive role in water splitting via photoelectrochemical (PEC) process. While the hematite photoanode with a photocurrent threshold of 600 nm is promising for practical PEC water oxidation, it still suffers from the small minority carrier diffusion length, which makes it difficult to realize adequate light absorption and efficient charge separation concurrently. To address this issue, hematite nanorods were grown on macroporous SnO 2 :Sb substrates, forming a coral-like hematite (ATO-Fe 2 O 3 ) photoanode. The ATO-Fe 2 O 3 photoanode exhibited a 150 mV cathodic shift of onset relative to Fe 2 O 3 nanorods directly on planar SnO 2 :F (FTO-Fe 2 O 3 ). The photocurrent density reached 1.32 mA cm −2 at 1.23 V vs. RHE, approximately 8.8 times higher than FTO-Fe 2 O 3 , and it was further increased to 1.81 mA cm −2 after passivation with a thin TiO 2 overlayer. The improved photocurrent was attributed to the increased light harvesting, reduced charge transfer resistance (R ct ), and smaller contact area of oxygen bubble to hematite photoanode. Our research confirmed the effectiveness of macroporous ATO templated coral-like morphology on balancing the adequate light absorption and efficient charge separation issues of hematite photoanodes. This research may also be applicable to other semiconductor photoanodes for high-efficiency PEC water splitting.
研究领域:
材料科学
·
能源转换
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 4
·E69
·
IF 3.12
Li Xu,Ye Wang,Qiutong Xu,Huiying Duan
Ti/SnO2-Sb-Fe electrodes have been prepared by a novel precipitation printing method, the traditional sol-gel method, and the direct current deposition method. The microstructure of the electrodes was systematically characterized through X-ray diffraction (XRD) observation and high-resolution transmission electron microscopy (HRTEM) verification. In addition, the morphology was characterized by scanning electron microscopy (SEM), while the electrochemical properties and the stability were further investigated by cyclic voltammetry (CV), linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS), and accelerated life testing. The results indicate that the Ti/SnO2-Sb-Fe electrode prepared by precipitation printing has the smallest nanoparticle structure (< 10 nm), a higher electrochemical porosity (49.6%), and a higher oxygen evolution potential (2.20 V). As a comparison, the Ti/SnO2-Sb-Fe electrode prepared by the sol-gel method has the longest service life. To further evaluate the electrocatalytic activity of the Ti/SnO2-Sb-Fe electrodes, Acid Red 73 was employed as simulated sewage for electrochemical degradation. After 180 min, the removal efficiency of AR 73 reached 86.8%, 63.4%, and 74%, respectively, for Ti/SnO2-Sb-Fe electrodes prepared by precipitation printing method, traditional sol-gel method, and direct current deposition method. Furthermore, the degradation of AR 73 followed pseudo-first-order kinetics.
研究领域:
材料科学
·
电化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 60
·37806-37814
·
IF 3.108
Anlin Xu,Xiang Dai,Kajia Wei,Weiqing Han,Jiansheng Li,Xiuyun Sun,Jinyou Shen,Lianjun Wang
The broad application of highly electrocatalytic SnO2–Sb electrodes for wastewater treatment is limited by their short service lifetime. Herein, a novel substrate structure, tubular porous titanium, was applied to prepare a TiO2-NT/SnO2–Sb electrode, which could greatly improve the stability of the electrode for electrochemical oxidation process. Based on the analysis conducted using a field emission scanning electron microscope (FE-SEM), linked with an energy dispersive spectrometer (EDS), it was demonstrated that a solid solution between Sn and Sb presented a smooth surface of the tubular porous electrode. The crystalline structure and chemical composition of the electrode coating are determined by X-ray diffraction (XRD). Accelerated service life test reveals that under the 0.2 A cm−2 current density in a 0.5 M H2SO4 solution, the TiO2-NT/SnO2–Sb tubular porous electrode has the longest accelerated service lifetime of 68.9 h, which is 10.9 times that of the TiO2-NT/SnO2–Sb plate electrode. Cyclic voltammetry curves (CVs) and linear sweep voltammetry curves (LSVs) reveal the enhanced electroactive surface area and higher oxygen evolution potential (OEP = 1.85 V vs. Ag/AgCl) of the electrode. Moreover, the TiO2-NT/SnO2–Sb tubular porous electrode has the larger outer voltammetric charge q*. During the electrochemical oxidation of pyrimidine, the tubular system constructed using the TiO2-NT/SnO2–Sb tubular porous electrode as the anode also exhibited best electrocatalytic performance, and 97.9% pyridimine removal efficiency and 79.4% COD removal efficiency at 6 h were achieved.
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 THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 9
·092505
·
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
·
材料科学
·
电化学
✓ 已验证
DOI
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
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENT INTERNATIONAL
·
2021
·
IF 9.621
Chao Yang,Yiang Fan,Shanshan Shang,Pu Li,Xiao-yan Li
Electrochemical oxidation (ECO) is an appealing technology for treating emerging organic pollutants in wastewater. However, the conventional flow-by ECO process is expensive with a low energy efficiency owing to the limitations of mass transport of contaminants to the limited surface area of the anode. In this study, a novel freestanding porous and permeable SnO 2 -Sb anode was fabricated by one-step sintering using micrometer-sized (NH 4 ) 2 CO 3 grains as the pore-forming agents. This permeable SnO 2 -Sb anode without Ti substrate functioned as a reactive anodic filter (RAF) in an ECO cell to treat wastewater containing ciprofloxacin (CIP). Forcing the wastewater through the porous RAF depth-wise improved the mass transport and vastly enlarged the electroactive surface area. Compared with the conventional flow-by configuration, the flow-through RAF exhibited a 12-fold increase in the mass transfer rate constant (60.7 × 10 −6 m s −1 ) and a 5-fold increase in the CIP degradation rate constant (0.077 min −1 ). At a cell potential of 4.0 V, more than 92% of the CIP was degraded in a single-pass operation at a filtration flux of 54 L m −2 h −1 and a short retention time of 1.7 min through the RAF. The robustness and stability of the RAF were demonstrated by its remarkable CIP degradation efficacy of 99% during 200 h of operation. The mechanism of CIP degradation was examined using probe molecules and density functional theory calculations and found to be a combined effect of direct electron transfer and oxidation by generated radicals ( OH and SO 4 − ). The great potential of RAF in flow-through ECO was further validated by its effective removal (>92%) of various organic pollutants in actual municipal wastewater at a low energy consumption of 0.33 kWh m −3 . The RAF-based ECO process thus provides an advanced environmental technology for the oxidation of toxic and recalcitrant organic pollutants in wastewater treatment.
研究领域:
环境工程
·
化学工程
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Yunlei Cen,Yuanyuan Zhou,Mingshi Zhu,Ke Zheng,Shaoqi Zhou
In this work, Ti/TiO2-RNTs/SnO2–Sb–Ni-La electrodes were developed in three deposition stages. TiO2-RNTs improved the bonding of the bottom layer, and Ni–La codoping resulted in higher film stability. Compared with other electrodes, this electrode exhibits excellent performance with a denser structure, higher OEP (2.17 V), lower Rct (5.36 Ω), longer electrode strengthening life, and larger active specific surface area. The degradation of oily wastewater revealed an oil removal rate equal to 97.88% under optimal conditions. In comparison to the Ti/TiO2-RNTs/SnO2–Sb obtained via the one-step hydrothermal technique, the service life improved by 8.60 times, and the degradation rate (RD) of the current electrode (k = 0.0254 min–1) was enhanced by 2.67 times, whereas the removal rate remained stable after 10 cycles. Under the continuous attack of free radicals such as •OH, 48 types of organic matter in wash oil were decomposed, and most of the alkanes and polycyclic aromatic hydrocarbons were mineralized. Compared with direct current, pulse current electrolysis of the oil-washing wastewater can save 47.95% electrical energy, and the energy consumption of chemical oxygen demand removal per unit mass can be reduced by 72.02%. Therefore, the Ti/TiO2-RNTs/SnO2–Sb–Ni-La pulse electrochemical oxidation method is expected to reduce energy loss and improve the electrochemical treatment of oily 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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Yongyang Chen,Fulin Li,Xiaochun Dong,Dan Guo,Yixuan Huang,Shanping Li
Efficient and stable rGO@Ti/SnO 2 –Sb composite electrodes were prepared by the sol-gel method. The microscopic morphology , crystal structure, and electrochemical properties of the rGO@Ti/SnO 2 -Sb composite electrodes were characterized by a range of characterization techniques. The electrocatalytic oxidation activity of the electrodes was evaluated by the degradation efficiency of the fluoroquinolone antibiotic norfloxacin (NOR). Simultaneously, the effects of different experimental conditions on the degradation efficiency of NOR were also investigated, such as calcination temperatures, brushing times, initial pH, initial electrolyte concentration , etc. The enhanced electrocatalytic oxidation activity can be attributed to the excellent electron transfer efficiency, higher electrode specific surface area, and stronger adhesion of the electrode coating to the substrate. Additionally, the possible NOR degradation pathway was deduced through the main intermediates, and the mechanism of NOR degradation was discussed based on experimental and characterization results. This work provides a simple and effective method to prepare highly active composite electrodes for electrocatalytic oxidation to remove organic pollutants from water.
研究领域:
环境科学
·
电化学工程
·
材料科学
·
水处理技术
·
污染控制化学
·
纳米复合材料
·
环境功能材料
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Hoang Nguyen Tien,Fredrick M. Mwazighe
In this work, a novel La-doped βPbO 2 (Ti/SnO 2 –Sb/La-βPbO 2 ) was prepared using electrodeposition method and applied to the degradation of prednisolone (PRD), 8-Hydroxyquinoline (8-HQ), and other typical organic pollutants. Compared with the conventional electrode Ti/SnO 2 –Sb/βPbO 2 , La 2 O 3 doping enhanced oxygen evolution potential (OEP), reactive surface area, stability and repeatability of the electrode. The 10 g L −1 of La 2 O 3 doping exhibited the highest electrochemical oxidation capability of the electrode with [•OH]ss being determined at 5.6 × 10 −13 M. The quenching experiments were conducted to confirm the main oxidizing species (here: •OH) in the electrochemical process. The study showed that the pollutants were removed in the electrochemical (EC) process with different degradation rates and indicated that the second-order rate constant of organic pollutants towards •OH ( k OP,•OH ) has a linear relationship with the degradation rate of organic pollutants ( k OP ) in the electrochemical process. Another new finding in this work is that a regression line of k OP,•OH and k OP can be used to estimate k OP,•OH of an organic chemical, which cannot be determined using the competition method. k PRD,•OH and k 8-HQ,•OH were determined to be 7.4 × 10 9 M −1 s −1 and (4.6–5.5) × 10 9 M −1 s −1 , respectively. Compared with conventional supporting electrolyte (like SO 4 2− ), H 2 PO 4 − and HPO 4 2− improved k PRD and k 8-HQ by 1.3–1.6-fold, while SO 3 2− and HCO 3 − inhibited k PRD and k 8-HQ significantly, down to 80%. Additionally, the degradation pathway of 8-HQ was proposed based on the detection of intermediates from GC-MS.
研究领域:
环境科学
·
电化学工程
·
污染控制
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Hao Wu,Jun Yu,Zhongzhou Li,Guanyu Yao,Rui Cao,Xiaogan Li,Huichao Zhu,Aixiang He,Zhenan Tang
High-performance, low-power microhotplate (MHP) gas sensors loaded with 3D hierarchical structured PdO/PdO 2 -SnO 2 :Sb materials on a pair of Al gas sensing electrodes were fabricated through advanced high-accuracy electrohydrodynamic printing method. The PdO/PdO 2 -SnO 2 :Sb materials with various PdO/PdO 2 concentrations were initially synthesized via a mild and simple hydrothermal reaction. Their micromorphology and chemical composition were characterized by SEM, XRD, TEM, and XPS, which proved the successful synthesis. The gas sensing performance of the sensors to benzene, ethanol, acetone, formaldehyde, and ethanol-acetone mixed gas (volume ratio 1:1) was tested. The sensing property of the materials is regulated with different content of PdO/PdO 2 . The identification of the VOCs is realized by two-step principal component analysis (PCA). Simulation calculations on the I–V characteristic of the MHP gas sensors reveal that carriers have to get through Al 2 O 3 barriers by Poole-Frenkel emission, which significantly affects the carrier conduction as well as the gas sensing properties. The gas sensing mechanism is analyzed from the aspects of gas sensing material and electrodes.
研究领域:
材料科学
·
传感器技术
·
化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Jiawei Lei,Pingzhou Duan,Weijun Liu,Zhirong Sun,Xiang Hu
Due to the potential threatening of antibiotics in aqueous environment, a novel electro-oxidation (EO) — electro-Fenton (EF) —persulfate (PS) system with the addition of peroxydisulfate and Fe 2+ was installed for the degradation of cefotaxime. Ti/CNT/SnO 2 –Sb–Er with an ultra-high oxygen evolution potential (2.15 V) and enhanced electrocatalytic surface area was adopted as anode. The OH production and electrode stability test demonstrated great improvement in the electrochemical performances. Ni@NCNT cathode was tested with higher H 2 O 2 generation by the presence of nitrogen functionalities due to the acceleration of electron transfer of O 2 reduction. Experiment results indicated CNT and ErO 2 modification increased the molecular and TOC removal of cefotaxime. Coupling processes of EO-EF and EO-PS both resulted in shorter electrolysis time for complete cefotaxime removal, however, the mineralization ability of EO-PS process was lower than EO-EF, which might result from the immediate vanishing of PS. Thus, a further improved treatment EO-EF-PS system achieved an 81.6% TOC removal towards 50 mg L −1 cefotaxime after 4 h electrolysis, under the optimal working condition Fe 2+ = PS = 1 mM. The influence of current density and initial concentration on the performance of all processes was assessed. Methanol and tert-butanol were added in the system as OH and SO 4 − scavengers, which illustrating the mechanism of EO-EF-PS oxidizing process was the result of the two free radicals. Major intermediates were deduced and the degradation pathway of cefotaxime was analyzed. This research provides a potential coupling process with high antibiotic removal efficiency and effective materials for practical uses.
研究领域:
环境科学
·
生物医学工程
✓ 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）