RSC Advances
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2022
·Vol. 12
·期 17
·10634-10645
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IF 4.036
Wenhao Jiang,Junli Wang,Xuanbing Wang,Jiang Liao,Jinlong Wei,Ruidong Xu,Linjing Yang
The conventional Pb–Ag alloy possesses a high oxygen evolution reaction overpotential, poor stability, and short service life in acidic solutions, making it an unsuitable sort of anode material for the zinc electrowinning process. Therefore, a layered carbon-covered cobalt tetroxide (Co3O4@C)-reinforced PbO2-coated electrode is fabricated via a facile two-step pyrolysis-oxidation and subsequent electrodeposition process. As a result, the reinforced PbO2-coated electrode exhibits a low OER overpotential of 517 mV at 500 A m−2 and a Tafel slope of 0.152 V per decade in a zinc electrowinning simulation solution (0.3 M ZnSO4 and 1.53 M H2SO4). The reduced overpotential of 431 mV at 500 A m−2 compared to traditional Pb–0.76%Ag alloy leads to improved energy savings, which is attributable to the presence of Co3O4@C to refine the grain size and thus increase the effective contact area. Moreover, the reinforced PbO2-coated electrode has a prolonged service life of 93 h at 20 000 A m−2 in 1.53 M H2SO4. Therefore, an accessible and efficient strategy for preparing a coated electrode to improve OER performance for zinc electrowinning is presented in this research.
研究领域:
材料科学
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电化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Dongyue Feng,Zhijie Shang,Pan Xu,Haoyu Yue,Xinxue Li
The anode materials play a key role in the electrochemical oxidation process. In this work, a new type of Ti/Sn-SbO x /α-PbO 2 /La-In-β-PbO 2 electrode has been prepared through electrodeposition and applied to the degradation of high concentration aqueous solution of hydrolyzed polyacrylamide (HPAM). Scanning electron microscopy (SEM), X-ray diffraction (XRD), and Energy-dispersive spectroscopy (EDS) were employed to characterize the surface morphological and structural properties of the electrodes, which indicated that the La-In-PbO 2 electrode had smaller grain size, denser surface and larger active surface area compared with undoped and single-doped PbO 2 electrode. Cyclic voltammetry (CV), linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) were also utilized to investigate the electrochemical performance of electrodes. The results showed that the La-In-PbO 2 electrode exhibited higher oxidation peak current, oxygen evolution potential (2.22 V) and lower charge transfer resistance. The La-In-PbO 2 electrodes were used as anode to degrade HPAM solution under different conditions. The results revealed that the viscosity reduction rate of HPAM reached to 97.63 % after 60 min under the condition of electrolyte concentration, initial concentration of HPAM, initial pH and current density were 0.05 M, 3 g·L −1 , 7 and 20 mA·cm −2 , respectively. The kinetic behavior of HPAM degradation was analyzed by the viscosity reduction experiment. The intermediates in the electrochemical oxidation process were identified by GC–MS and the possible degradation mechanism of HPAM was explored by UV–visible absorption spectra and the Fourier Transform Infrared (FT-IR) spectra.
研究领域:
环境工程
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材料科学
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电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yingcai Wang,Min Chen,Can Wang,Xiaoyang Meng,Weiqiu Zhang,Zefang Chen,John Crittenden
Methylisothiazolinone (2-methyl-4-isothiazolin-3-one) (MIT) is a commonly used biocide in wastewater treatment processes. Residual MIT in wastewater leads to high environmental risks and toxicity. The degradation of MIT via electrochemical oxidation, including kinetics, energy efficiency, oxidation mechanism and degradation pathway, was investigated in this study. Findings from energy and cost evaluation by using electrochemical technology were compared with those of other technologies. Experimental results indicate that electrolyte, current density and initial concentration can significantly affect MIT degradation. The lowest electrical energy per order was less than 3.85 kWh m −3 when NaCl was used as the electrolyte. Electrochemical degradation is advantageous because it can be easily applied without adding chemicals into wastewater and has relative low costs. The oxygen evolution, production of recalcitrant byproducts, and the mass transfer limitation resulted in the decrease of instantaneous current efficiency and mineralization current efficiency. Electron efficiency analysis demonstrated that 68.8% of the electrons used for MIT oxidation were effectively utilized to mineralize MIT into CO 2 . The proportion of direct and indirect oxidation of MIT during electrochemical degradation was quantitatively determined as 37.7% and 62.3%, respectively. HO was the most effective species for MIT degradation. MIT degradation pathway was proposed, in which the C C bond in MIT was broken down. C 3 H 7 NOS and C 3 H 7 NO 4 were detected, indicating the occurrence of ring opening reaction. Sulfur was oxidized into SO 4 2− and cleaved from C 3 H 7 NOS.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
HYDROMETALLURGY
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2020
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IF 3.338
Xuanbing Wang,Ruidong Xu,Suyang Feng,Chen Chen,Buming Chen
In this paper, a Co 3 O 4 - and CNT-doped 3D PbO 2 electrode was fabricated through galvanostatic electrodeposition in a Pb(Ac) 2 -NH 2 SO 3 H solution, and the electrochemical properties were systematically investigated in a zinc electrolyte. The XRD results show that the deposit is a mixture of an α + β phase (a dominant β-PbO 2 phase with a minor α-PbO 2 phase present), and the SEM images show that Co 3 O 4 and CNT have been simultaneously deposited with PbO 2 . The 3D-Ti/PbO 2 -(4 g·L −1 ) Co 3 O 4 -(0.4 g·L −1 ) CNT electrode exhibits a voltammetric charge 5 times larger than that of the 3D-Ti/PbO 2 electrode, which indicates outstanding electrocatalytic activity. The oxygen evolution reaction overpotential and cell voltage are only 394 mV and 3.74 V at 500 A∙m −2 , respectively. In addition, the obtained electrode showed a high current efficiency of 95.3% and a service life of 26 h under a current density of 20,000 A∙m −2 . Hence, this study offers a facial synthesis route to prepare composite electrodes for zinc electrowinning and provides deep insight into the relationship among doping substances, microstructures and electrocatalytic activity.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2018
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IF 3.235
Xiezhen Zhou,Siqi Liu,Hongxia Yu,Anlin Xu,Jiansheng Li,Xiuyun Sun,Jinyou Shen,Weqing Han,Lianjun Wang
A highly ordered three-dimensional macro-porous PbO 2 (3D porous PbO 2 ) electrode has been prepared for electrochemical oxidation of nitrogen-heterocyclic compounds. The 3D porous PbO 2 electrode was fabricated by templated electrochemical deposition method with TiO 2 nanotube arrays as substrate and SnO 2 -Sb as intermediate layer. The morphology and composition characterization of the 3D porous PbO 2 electrode was performed by field emission scanning electron microscopy and X-ray diffraction, which revealed a uniform distribution of highly ordered macro-porous β-PbO 2 structure. The Brunner−Emmet−Teller analysis suggested the electrode possessed large specific surface area of 37.39 m 2 ·g −1 . Electrochemical measurements indicated the electrode had a favourable oxygen evolution potential of 1.89 V and inner voltammetric charge of 14.48 mC·cm −2 , which were higher than that of conventional PbO 2 electrode. Furthermore, the electrochemical oxidation and TOC removal percentage of pyrrole , pyrazole and tetrazole obtained by 3D porous PbO 2 electrode were 93.4%, 72.7%, 61.2% and 66.7%, 57.3%, 38.6% respectively, which were also superior to conventional PbO 2 electrode. The intermediates were detected and analyzed by high-performance liquid chromatography, gas chromatography-mass spectrometer, and ion chromatography to propose a degradation pathway of pyrrole, pyrazole and tetrazole. Finally, quantum chemical calculation was introduced in this study by density function theory method, which is consistent with the experimental detection.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMOSPHERE
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2023
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IF 8.8
Zeyi Wang,Rong Su,Maojie Zhao,Luyao Zhang,Lu Yang,Feng Xiao,Weishan Tang,Lichuan Chen,Ping He,Dingming Yang
The application of PbO 2 for electrochemical oxidation technology is limited by its low electrocatalytic activity and short service life. Herein, based on the facile one-step electrodeposition , we prepared a boron carbide (B 4 C) and cerium (Ce) co-modified Ti/PbO 2 (Ti/PbO 2 –B 4 C–Ce) electrode to overcome these shortcomings. Compared with Ti/PbO 2 electrode, the denser surface is displayed by Ti/PbO 2 –B 4 C–Ce electrode. Meanwhile, electrochemical characterization indicates that the introduction of B 4 C and Ce significantly enhance the electrochemical performance of PbO 2 electrode. In degradation experiments, under optimized conditions (current density 20 mA cm −2 , pH 9, 0.15 M Na 2 SO 4 and 30 °C), the fully degradation of tetracycline (TC) can be completed within 30 min. Furthermore, the trapping experiment demonstrates that ∙OH and SO 4 ·- radicals have a synergistic effect in the degradation process of TC. Based on results of liquid chromatography-mass spectrometer, the generated ·OH preferentially attacks amides, phenols and conjugated double bond groups in TC. Importantly, Ti/PbO 2 –B 4 C–Ce electrode maintains a constant degradation efficiency even after 10 recycling tests, and its service life is 2.4 times of traditional Ti/PbO 2 electrode. Hence, Ti/PbO 2 –B 4 C–Ce electrode is a promising electrode for degradation of organic wastewater containing amides, phenols, and conjugated double bond groups.
研究领域:
环境科学
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电化学工程
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产品关联
DOI
PubMed
高影响因子
Engineering
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2025
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IF 11.6
Bin Zhao,Jialin Yang,Ruiping Liu,Jiuhui Qu,Meng Sun
The contamination of wastewater with organic pollutants and nitrogen compounds poses significant environmental challenges. The primary objective of wastewater treatment is the simultaneous denitrification and decarbonization of ammonia nitrogen into harmless by-products. This study presents a novel method for the directional generation of chlorine radical species like ·ClO and ·Cl using electro-reactive membranes (EMs), which were fabricated using an electro-deposition coupled template approach known as RuO 2 @PbO 2 -M. This method facilitates the rapid and efficient conversion of ammonia to nitrogen and concurrently reduces the chemical oxygen demand in the effluent. Our system achieved ultra-efficient simultaneous denitrification and decarbonization with minimal energy consumption in single-filtration mode, thereby eliminating the need for chemical precursors. We elucidate the formation pathway of ·ClO and ·Cl during the electrochemical oxidation process involving RuO 2 @PbO 2 -M, where ·Cl generated from RuO 2 reacts with ·OH from PbO 2 under hypochlorous acid conditions, thereby enhancing nitrogen and carbon removal. These findings highlight a novel filtration model that utilizes single-channel electro-filtration and an innovative reactive membrane design for ·ClO synthesis, which provides a new research framework for the concurrent removal of nitrogen and carbon, and offers a promising solution to enhance wastewater treatment efficiency.
研究领域:
环境科学
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水处理技术
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电化学
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膜科学
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化学工程
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可持续废水管理
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Guoquan Zhang,Shaowei Hu,Xiaoyu Zhu,Xiaoxin Hu,Fenglin Yang
An interlocking “ T -shape” structure was built by uniform filling β-PbO 2 crystalline inside the trace Ti 3+ self-doping TiO 2 nanotube arrays (TNAs) channels and depositing the cauliflower-like β-PbO 2 clusters on its upper surface through a facile current pulse deposition method. We elaborated the interfacial engineering strategy for generating compact oxide layers at TNAs bottoms and growing β-PbO 2 crystalline from the selectively conductive TNAs bottoms. Different characterization techniques and electrochemical analyses were conducted to characterize the morphology, structure, and electrochemical property of the β-PbO 2 partial filling/covering TNAs (β-PbO 2 /TNAs/Ti) materials. We also systematically investigated and elucidated the performance and mechanism of β-PbO 2 /TNAs/Ti anode activated peroxymonosulfate (PMS) system via berberine removal/mineralization, reactive oxygen species (ROS) identification/contribution, intermediates analysis, energy consumption and practical applicability estimation. Results illustrated that filling β-PbO 2 inside TNAs can efficiently improve the directional electron-transfer efficiency, oxygen evolution over-potential, tolerance to the varied water matrices and service lifetime of β-PbO 2 /TNAs/Ti anode activated PMS system. The ROS including • OH, S O 4 ∙ - and 1 O 2 that generated from PMS electro-activation are responsible for efficient berberine degradation through two pathways. This study will provide a general approach to construct the versatile tube-filled TNAs-based materials for wide applications in water/wastewater treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Weishan Qin,Ting Su,Guodong Chai,Xinhong Wang,Weichao Qin,Hongbin Yu
Photoelectrocatalysis is a promising method for removing biorefractory organic pollutants. However, the inefficient utilization of light and electricity by photoanodes and the failure to effectively execute cathode functions typically lead to poor degradation performance. Therefore, in this study, a photoelectrocatalytic (PEC) system coupled with electro-activated persulfate (E-PS) was constructed using a 3D nanostructured PbO 2 /Sb-SnO 2 //blue-TiO 2 //WO 3 bifacial anode and a Mo-CuFeO 2 -modified carbon felt cathode. The results indicate that the bifacial anode could effectively implement electro-assisted photocatalysis on the irradiating side and electrocatalysis on the back side. This significantly accelerated acetaminophen degradation with a synergy index of 48.98 %. Additionally, the PEC/E-PS system was established by combining a bifacial anode with a persulfate-activated cathode, which promoted the efficient utilization of photogenerated electrons and increased the number of active species in the coupled system. Density functional theory calculations confirmed that Mo tended to dope the Fe sites and promote the adsorption of PS on Mo-CuFeO 2 , facilitating the continuous activation of persulfate. In the coupled system, the contribution order of different active species to acetaminophen degradation was h + > OH > SO 4 − > 1 O 2 > O 2 − . Their mutual conversion enabled the PEC/E-PS system to efficiently remove acetaminophen with a relatively high current efficiency (22.69 %) and low energy consumption (0.06 kWh⋅gCOD −1 ). The proposed PEC/E-PS system is an efficient and sustainable method for treating organic contaminants in wastewater.
研究领域:
环境科学
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电化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
·
IF 8
Zeyi Wang,Luyao Zhang,Rong Su,Lu Yang,Feng Xiao,Lichuan Chen,Ping He,Dingming Yang,Yali Zeng,Yun Zhou,Ying Wan,Bin Tang
The abuse and uncontrolled discharge of antibiotics present a severe threat to environment and human health, necessitating the development of efficient and sustainable treatment technology. In this work, we employ a facile one-step electrodeposition method to prepare polyaniline/graphite oxide (PANI/GO) and samarium (Sm) co-modified Ti/PbO 2 (Ti/PbO 2 -PANI/GO-Sm) electrode for the degradation of amoxicillin (AMX). Compared with traditional Ti/PbO 2 electrode, Ti/PbO 2 -PANI/GO-Sm electrode exhibits more excellent oxygen evolution potential (2.63 V) and longer service life (56 h). In degradation experiment, under optimized conditions (50 mg L −1 AMX, 20 mA cm −2 , pH 3, 0.050 M Na 2 SO 4 , 25 °C), Ti/PbO 2 -PANI/GO-Sm electrode achieves remarkable removal efficiencies of 88.76% for AMX and 79.92% for chemical oxygen demand at 90 min. In addition, trapping experiment confirms that ·OH plays a major role in the degradation process. Based on theoretical calculation and liquid chromatography-mass spectrometer results, the heterocyclic portion of AMX molecule is more susceptible to ·OH attacks. Thus, this novel electrode offers a sustainable and efficient solution to address environmental challenges posed by antibiotic-contaminated wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Huijiao Wang,Zhongyi Li,Fengyuan Zhang,Yuxiang Wang,Xian Zhang,Jianbing Wang,Xuwen He
Three types of Magnéli phase anodes (Ti/Ti 4 O 7 , Ti/Ti 4 O 7 -PbO 2 -Ce, and Ti/Ti 4 O 7 nanotube arrays (NTA)) were fabricated, characterized, and compared with other typical active and non-active anodes (i.e., BDD, Ti/Pt, Ti/RuO 2 -IrO 2 , and Ti/IrO 2 -Ta 2 O 5 ) for electro-oxidation treatment of p -nitrophenol (PNP) solution and a real coal chemical concentrated brine in this study. Characterization results indicate a nanotube array structure of Ti/Ti 4 O 7 NTA, and a compact coating of Ti 4 O 7 microparticles and PbO 2 -Ce nanocrystals on the Ti substrate for Ti/Ti 4 O 7 and Ti/Ti 4 O 7 -PbO 2 -Ce, respectively. The three anodes present relatively high oxygen evolution potentials (2.16–2.44 V vs SCE), showing good capacity of electro-generating reactive oxidative species for pollutant degradation. After 30 min of EO treatment, Ti/Ti 4 O 7 NTA and Ti/Ti 4 O 7 removed 89–92% of PNP, which were 10–60% higher than Ti/Pt, Ti/RuO 2 -IrO 2 , and Ti/IrO 2 -Ta 2 O 5 , and were almost comparable with BDD (95%). Furthermore, Ti/Ti 4 O 7 NTA and Ti/Ti 4 O 7 kept very efficient for mineralization of PNP solution and real coal chemical concentrated brine. For Ti/Ti 4 O 7 -PbO 2 -Ce, its degradation efficiency was lower than other two Magnéli phase anodes, but still competitive compared with other active anodes. Thanks to their high removal efficiencies, the three Magnéli phase anodes required relatively low energy demand for pollutant mineralization. Besides, operational parameters such as electrolyte and current density were also very significant for efficient pollutant removal. The results of this study suggest Magnéli phase electrodes as promising and cost-effective anode materials for industrial wastewater treatment, with Ti/Ti 4 O 7 NTA and Ti/Ti 4 O 7 being more efficient options.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Yilong Yan,Yijing Gao,Haiyang Zheng,Bowen Yuan,Qiaoqiao Zhang,Yu Gu,Guilin Zhuang,Zhongzhe Wei,Zihao Yao,Xing Zhong,Xiaonian Li,Jianguo Wang
OH radicals produced via an eco-friendly O 3 decomposition reaction in water are employed in a wide range of applications. In this work, three-dimensional (3D) β-PbO 2 /Ta 2 O 5 and Pt/Ta 3 N 5 samples with a rod-like morphology were successfully fabricated and coupled to carry out electrochemical ozone production (EOP) and hydrogen evolution reaction (HER), respectively. Moreover, the results on the in-situ electrodegradation of dimethoate also indicate that the β-PbO 2 /Ta 2 O 5 NRs show a great potential to be used in advanced oxidation processes (AOPs) applications. Experimental results and theoretical calculations reveal that the excellent EOP performance of the β-PbO 2 /Ta 2 O 5 NRs can be attributed to the adsorption energy of the O species, which can be modulated via the synergic effect between β-PbO 2 and Ta 2 O 5 . This work provides a reference for the development of stable electrocatalysts with high efficiency for the simultaneous production of O 3 and H 2 in environmental applications and energy conversion.
研究领域:
电化学
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环境科学
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材料科学
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能源转换
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）