CHEMICAL ENGINEERING JOURNAL
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2021
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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
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电化学工程
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Ruirui Zhang,Shugui Hua,Yuan Dang,Bing Zhang,Xiaoqin Sun,Sha Yu,Yingying He,Shuangli Chen,Yuanzhen Zhou
In this paper, the electrocatalytic performance of Ti/β-PbO 2 anode was improved by doping Cs into SnO 2 intermediate layer (Ti/Cs-SnO 2 /β-PbO 2 ) for the efficient degradation of fluoroquinolone wastewater. Compared with the conventional Ti/Sb-SnO 2 /β-PbO 2 anode, Cs-SnO 2 with the rougher surface increased the deposition amount and the thickness of β-PbO 2 active layer, thus forming the denser PbO 2 coating with smaller particle size and exposing more active sites. The partial replacement of Sn by Cs with the smaller ion radius induced the deformation of crystal lattice of SnO 2 , which further led the outer β-PbO 2 active layer grew along the advantageous (200) crystal plane and formed more point defects in the crystal lattice of β-PbO 2 . Thereby, the electron transfer rate at the anode interface was accelerated and the electrocatalytic performance of Ti/β-PbO 2 was significantly improved. To verify the practical application of the improved Ti/Cs-SnO 2 /β-PbO 2 electrode, levofloxacin (LFX) and ciprofloxacin (CIP) were selected as the typical target fluoroquinolones to evaluate the degradation efficiency of Ti/Cs-SnO 2 /β-PbO 2 anode. The removal rate exceeded more than 90% for the single and mixed fluoroquinolones wastewater. Moreover, after 5 times’ recycle, the degradation efficiency of LFX on Ti/Cs-SnO 2 /β-PbO 2 anode still remained over 90%. The potential mechanism of the enhanced electrocatalytic performance of Ti/Cs-SnO 2 /β-PbO 2 and the degradation pathways of fluoroquinolones were also inferred. It’s the first time to enhance the electrocatalytic performance of the Ti/β-PbO 2 anode by introducing monovalent alkali metal (C S ) into the SnO 2 intermediate layer and the proposed Ti/Cs-SnO 2 /β-PbO 2 anode would be a promising candidate to realize the efficient removal of the practical fluoroquinolones antibiotic wastewater.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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
Environmental Science-Nano
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2024
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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
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电化学工程
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Yuanzhen He,Dengjie Zhong,Yunlan Xu,Ran Jiang,Pengfei Liao,Jiayou Zhang
In this work, Ti/SnO 2 -Sb 2 O 4 -La/β-PbO 2 electrode was successfully prepared by electrodeposition method. The surface morphology, crystal structure, elemental states and electrochemical characteristics of the electrode were examined by SEM, XRD, XPS, CV, and LSV. The results demonstrated that the conductivity, specific surface area, electrochemical oxidation performance and stability of the β-PbO 2 coated electrode with SnO 2 -Sb 2 O 4 -La as the intermediate layer were greatly improved. Under the conditions of initial rhodamine B (RhB) concentration of 20 mg/L, initial pH of 3.0, electrolyte concentration of 0.1 M, and current density of 30 mA cm −2 , the removal rates of color and TOC reached 100 % and 83.64 % after 20 mins and 30 mins, respectively. The electrode can also completely degrade methylene blue and methyl orange wastewater after 30 mins under the same conditions. The accelerated lifetime of the electrode reached 175 mins (1000 mA cm −2 , 1 M H 2 SO 4 ), and the actual lifetime was up to 3208 hrs. Based on the results of free radical quenching experiment and GC–MS detection, RhB degradation pathway was proposed: the aniline-based conjugated system of RhB molecule was attacked by the combined action of free radicals (indirect oxidation) and electrocatalysis (direct oxidation), which decomposed macromolecules into small molecules and ultimately mineralized them into CO 2 and H 2 O. This work is expected to provide a fresh research concept for preparing DSA electrodes with excellent catalytic performance and high stability.
研究领域:
环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Huachang Jin,Xuejiao Zhang,Yang Yu,Xueming Chen
The extensive evaporation-induced aggregation of scale inhibitors in the wastewater of recirculating cooling systems causes severe environmental pollution . In this study, Amino Trimethylene Phosphonic Acid (ATMP), an ordinary scale inhibitor, was degraded via electrochemical oxidation using a multi-layered Ti/IrO 2 -RhO x -TiO 2 /α-PbO 2 /β-PbO 2 electrode. The electrochemical oxidation experimental results verified the superior electro-catalytic properties of the β-PbO 2 electrode. Accelerated lifetime tests suggested that Ti/IrO 2 -RhO x -TiO 2 /α-PbO 2 /β-PbO 2 possesses a service lifetime of 201 h under a current density of 40000 A/m 2 , which is 3.4–100.5 times as long as other β-PbO 2 electrodes reported by other researchers. Four major operational parameters, namely electrolyte, current density, initial ATMP concentration, and pH, were discovered to significantly affect the ATMP degradation rate and electrical efficiency. The direct oxidation mechanism predominated in the degradation process of ATMP, achieving a 55.11% and 38.82% removal efficiency in Na 2 SO 4 and NaCl solutions, respectively. In addition, two possible degradation pathways of ATMP were proposed: induced by the breaking of either C-P or C-N bonds.
研究领域:
环境工程
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电化学
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废水处理
✓ 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）