CHEMOSPHERE
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2022
·
IF 8.943
Yangyang Bai,Xiaoqin Sun,Yuan Dang,Sha Yu,Jun-Jie Zhu,Yuanzhen Zhou
Electro-Fenton reaction was limited by the generation of H 2 O 2 and the circulation of Fe(Ⅱ)/Fe(Ⅲ). Herein, an efficient electro-Fenton-like process was constructed based on Fe 3 O 4 –CaO 2 cathode promoted by peroxymonosulfate (PMS). Levofloxacin (LEV) could be efficiently degraded (92.1%) and mineralized with the TOC removal of 74.5% in this self-circulating process. More importantly, the Fe 3 O 4 –CaO 2 exhibited good stability in the recycles due that CaO 2 was covered by Fe 3 O 4 , which inhibited the rapid release of H 2 O 2 . Mechanism analysis indicated that CaO 2 could not only replace H 2 O 2 to accelerate the oxidation of Fe(Ⅱ) to Fe(Ⅲ), but also could form complexes with Fe(Ⅲ) and PMS to transfer electrons from ligands to metals, thereby enhancing the reduction of Fe(Ⅲ) to Fe(Ⅱ). As a result, the electrical consumption was significantly reduced, which was only 5.0% of the Fe 3 O 4 in electro-Fenton reaction. Meanwhile, the hydrolyzed product of Ca(OH) 2 reacted with Fe(Ⅲ) in the presence of H 2 O 2 and converted into CaO 2 . Thus, the self-circulation of CaO 2 /Ca(OH) 2 and Fe(Ⅲ)/Fe(Ⅱ) was realized, which accelerated the generation of active species, such as, ·OH, O 2 · - and 1 O 2 . This work first proposed a self-circulating electro-Fenton-like system and demonstrated the potential application of Fe 3 O 4 –CaO 2 in the treatment of wastewater.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiahui Chen,Yue Meng,Zhiling Huang,Bo Xie,Zheming Ni,Shengjie Xia
Defect engineering advantages include regulating the band structure of photocatalytic materials, inhibiting the recombination of photoelectron-hole pairs, and promoting the conversion of photogenerated electrons into active radicals. In this paper, bismuth molybdate (Bi 2 MoO 6 ) photocatalysts with double vacancies (V Bi-O -BMO) were prepared by solvothermal and ionic eutectic solvent methods. EPR, TEM, and XPS results confirmed the successful construction of oxygen and bismuth vacancies on Bi 2 MoO 6 . The photocatalytic performance of the prepared catalysts was investigated by photodegradation of levofloxacin hydrochloride (LVF) under visible light. The double vacancies markedly enhanced the photocatalytic properties of Bi 2 MoO 6 , with the photodegradation rate of V Bi-O -BMO reaching 88.36 % for 40 mg/L LVF within 60 min. Kinetic studies have demonstrated that the reaction rate constant of V Bi-O -BMO can reach 0.0351 min −1 , which is 3.2 times higher than that of bulk-BMO. This can be attributed to the favorable synergistic effect of oxygen and bismuth double vacancies. V O not only captures oxygen and electrons, facilitating the generation of superoxide radicals ( O 2 − ), but also elevates the conduction band position and boosts the reduction capability of Bi 2 MoO 6 . V Bi not only captures photogenerated holes (h + ) to directly impact LVF degradation, but also promotes interfacial charge transfer and inhibits the recombination of electron-hole pairs. Furthermore, the intermediates and degradation pathways of LVF photodegradation were surmised based on the LC-MS analysis. The reaction mechanism of LVF photodegradation by V Bi-O -BMO was elucidated through the application of the free radical pathway. This study demonstrates a methodology for the creation of double vacancies in catalysts and the significant potential of V Bi-O -BMO for the remediation of antibiotic residues in water under visible light.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2025
·
IF 6
Sultan Akdağ Türkay,Alireza Khataee,Yasin Orooji
The V 4 AlC 3 MAX phase, as the precursor of MXene, was developed for levofloxacin degradation through sonocatalytic activation of peroxymonosulfate (PMS). The reactive sintering method was used to synthesize V 4 AlC 3 MAX phase. Vanadium, aluminium and graphite, with molar ratios 4:1.2:3, were mixed in ball milled (ball-to-material ratio of 3:1, 12 h, 350 rpm), compressed into a disc and placed in a tubular furnace (1600 ℃ for 2 h). The stacked layered morphology of the MAX phase was confirmed by SEM and TEM images. With an average crystal size of 48.5 nm and a narrow band gap (1.92 eV), the V 4 AlC 3 MAX phase exhibited remarkable sonocatalytic activity. Under optimum conditions, US/V 4 ALC 3 MAX phase/PMS process exhibited 88.4 % levofloxacin degradation efficiency in 60 min. First order rate constant (k app ) of the US/V 4 AlC 3 MAX phase/PMS process was 10.22, 7.43, and 4.78 times higher than that of US/V 4 AlC 3 MAX phase, US/PMS, and V 4 AlC 3 MAX phase/PMS processes, respectively. V 4 AlC 3 MAX phase showed remarkable reusability after 5 cycles. It was proved that superoxide radical was the main active substance in the degradation process. The possible intermediates were identified through LC-MS analysis, and four main degradation pathways were proposed. The mechanism of PMS-assisted sonocatalytic degradation of levofloxacin was described.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Fanqing Meng,Yingling Wang,Zhen Chen,Jinglu Hu,Guang Lu,Wei Ma
The occurrence of antibiotics in water environment has drawn great concerns in recent years. In this work, CQDs@FeOOH electro-catalyst with abundant active edges was synthesized and applied to the degradation of antibiotics. About 99.6 % levofloxacin (LEVO) and 53.7 % TOC could be efficiently removed by CQDs@FeOOH after 60 min degradation. The high LEVO degradation performance of CQDs@FeOOH was demonstrated to be attributed to the high mass transfer ability and the high OH generation ability of the special needles structure. The OH was found to be the main radical for LEVO degradation, and the highest OH generation ability of CQDs@FeOOH was found to be resulted from the moderate adsorption energy of the exposed (1 1 0) facets (needles) toward OH. A possible LEVO degradation pathway has been proposed and toxicity changes during LEVO degradation were detailed investigated. This study offers an efficient method to reduce the amount and toxicity of antibiotics in water.
研究领域:
环境科学
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电催化
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水处理技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Bo Li,Huan-Yan Xu,Yu-Long Liu,Yue Liu,Yan Xu,Si-Qun Zhang
As a fluoroquinolone antimicrobial agent, ofloxacin (OFX) has been widely used, consequently causing serious damage to the ecological environment. Advanced oxidation processes based on persulfate activation (SR-AOPs) are widely applied to degrade stubborn organic contaminants in wastewater treatment. Co 3 O 4 is being extensively investigated as a promising persulfate catalyst in SR-AOPs. In this work, four Co 3 O 4 polycrystals with specific morphologies were synthesized and used to activate peroxymonosulfate (PMS) for OFX degradation. The obtained samples and corresponding precursors were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and N 2 adsorption/desorption isotherms. Experimental results showed that 30 mg·L -1 OFX could be completely removed in the lamella-like Co 3 O 4 /PMS system within 30 min under ordinary conditions. The underlying degradation mechanism was elaborated by high-resolution TEM (HRTEM) combined with density functional theory (DFT) calculations. Based on quenching experiments and the electron paramagnetic resonance (EPR) technique, sulfate radicals were identified as the dominant reactive oxygen species (ROS) in the lamella-like Co 3 O 4 /PMS system, and superoxide radicals, hydroxyl radicals, and singlet oxygen made minor contributions to the degradation of OFX. Possible degradation pathways were proposed based on DFT calculations and Fukui theory and confirmed by ultrahigh-performance liquid chromatography-quadrupole-time of flight mass spectrometry (UHPLC-QTOF/MS). Furthermore, quantitative structure–activity relationship (QSAR) prediction was used to evaluate the developmental toxicity of the corresponding intermediates.
研究领域:
环境科学
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化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2018
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IF 3.779
Yunqing Pi,Peng Zhao,Lingjia Ma,Yangdan Cao,Huiqing Gao,Shuying Dong,Jianhui Sun
The Co(OH) 2 /reduced graphene oxide hybrids (Co(OH) 2 /rGO) was prepared and used as catalyst to enhanced heterogeneous activation of Oxone for the decomposition of Levofloxacin (LVF). The Co(OH) 2 /rGO composites with different Co(OH) 2 loading have been successfully synthesized, where the sample contain 20% Co(OH) 2 exhibited superior activation, attributing to the synergistic effect between Co(OH) 2 and rGO. Meanwhile, the effects of some important reaction parameters on the decomposition of LVF by Co(OH) 2 /rGO/Oxone process were investigated. The results indicated that the decomposition rate of LVF(>94.5%) was increased with the increasing of Oxone concentration, and 20% Co(OH) 2 /rGO dosage neutral pH. Moreover, the Co(OH) 2 /rGO catalyst showed high activity and stability during the repeated experiments.
研究领域:
环境科学
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材料科学
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药学
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DOI
高影响因子
DALTON TRANSACTIONS
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2023
·Vol. 53
·期 3
·917-931
·
IF 4
Shuyan Li,Mingxuan Sun,Xiangzhi Huang,Haohao Chen,Junjie Zhao,Ziyang Li
In this work, N-graphyne is in situ coupled with BiOCl0.5Br0.5via a facile one-step sonochemical method. To our knowledge, both the synthesis strategy for BiOCl0.5Br0.5 and the N-graphyne/BiOCl0.5Br0.5 photocatalytic system are new developments. A collection of characterization methods is adopted to detect the morphologies, structures, and electronic and optical properties. The results demonstrate that wrinkle-like N-graphyne nanosheets successfully enwind around or on flower-like BiOCl0.5Br0.5 microspheres, which are regularly assembled by BiOCl0.5Br0.5 nanosheets. Compared with pristine BiOCl0.5Br0.5, N-graphyne/BiOCl0.5Br0.5 composites exhibit superior adsorption capacity and visible-light-driven photocatalytic degradation of levofloxacin. In particular, the optimal N-graphyne amount for ameliorating the photocatalytic performance of BiOCl0.5Br0.5 is ascertained. In addition, the good stable performance for photocatalysis is confirmed by four cycling experiments. The dominant active species is confirmed to be O2˙− during photodegradation. The improved photocatalytic activity is attributed to the enhanced visible light response and the accelerated transfer/separation of photogenerated carriers by N-graphyne, which are verified using UV–vis absorption spectra, photocurrents, photopotentials, Nyquist plots, and Mott–Schottky curves. This study develops a new perspective for the synthesis and modification of BiOX solid solution, which can be used as an efficient photocatalyst.
研究领域:
材料科学
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环境科学
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光催化技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Manlu Cheng,Xingyu Long,Ping Song,Zenghui Diao,Gang Song,Diyun Chen,Lingjun Kong
Stabilization of Co was essential to address its pollution. In this work, geopolymerization was used to stabilize the Co 2+ in the presence of alumina-silicate under hydrothermal process, in which the Co 2+ is hypothesized to be a substitute of cation to balance the charge. Then the Co 2+ could be incorporated into the geopolymer stably being named as Al x Si y Co z -T. Interestingly, the Co 2+ stabilized Al x Si y Co z -T was recycled and reused for peroxymonosulfate (PMS) activation. The stability and catalytic activity of the Al x Si y Co z -T in PMS activation was evaluated. Results showed that the alumina and silicate geopolymerization played positive role in Co 2+ stabilization, what were determined by the molar ratio of alumina to silicate, hydrothermal process. Besides, the Al x Si y Co z -T performed favorable activity in PMS activation for LEV degradation with an efficiency of 98.84 % and rate constant of 0.1154 min −1 . In this case, the Co 2+ was the main catalyst in PMS activation, while the alumina-silicate geopolymerization not only contributed to Co 2+ stabilization, but also resulted in the formation of oxygen vacancy. Then the co-catalytic of alumina-silicate in PMS activation was understood by the synergy factor. The Co 2+ leaching efficiency of AlSi 2 Co 4 -200 is only 0.011 %, confirming the heterogeneous catalytic in PMS activation. The Al x Si y Co z -200 performed favorable stability that could be used for five cycles at least. 1 O 2 , SO 4 − • and •OH contributed to LEV degradation. Thus, the alumina and silicate geopolymerization could play important role in stabilization and co-catalytic for activating PMS, performing the dual effect on waste treatment and resource recycle.
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
ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Kexin Dong,Chuqi Shen,Ruyu Yan,Yanping Liu,Chunqiang Zhuang,Shijie Li
The escalating presence of pharmaceutical antibiotics in natural water poses an overwhelming threat to the sustainable development of society. Photocatalysis technology stands out as a promising and cutting-edge environmental purification alternative. C 3 N 5 , identified as a distinctive nonprecious nonmetal photocatalyst, holds potential for environmental protection. However, challenges persist originating from the sluggish photoreaction kinetics and severe photo-carrier reunion. Currently, the design of a special S-scheme photosystem proves to be a reliable strategy for obtaining outstanding photocatalysts. In this context, a plasmonic S-scheme photosystem involving Ag/Ag 3 PO 4 /C 3 N 5 was developed through a feasible route. The compactly connected 0D/0D/2D Ag/Ag 3 PO 4 /C 3 N 5 heterostructure, benefitting from the synergy between the plasmonic effect and the S-scheme junction, facilitates the efficient utilization of appreciably reinforced sunlight absorption, effective photo-carrier disassociation, and notable photoredox capacity. Consequently, this system generates •OH and
⋅ O 2 - effectively. Ag/Ag 3 PO 4 /C 3 N 5 demonstrates a superb photocatalytic levofloxacin eradication rate of 0.0362 min −1 , marking a substantial advancement of 24.8, 1.1, and 0.7 folds compared to C 3 N 5 , Ag 3 PO 4 , and Ag 3 PO 4 /C 3 N 5 , respectively. Impressively, Ag/Ag 3 PO 4 /C 3 N 5 delivers remarkable anti-interference performance and reusability. This achievement signifies a significant step toward developing potent C 3 N 5 -involved photosystems for environmental purification. Download: Download high-res image (106KB) Download: Download full-size image
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
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Gongduan Fan,Shangwu Yang,Banghao Du,Jing Luo,Xin Lin,Xia Li
A novel FeVO 4 /BiVO 4 heterojunction photocatalyst was synthesized by hydrothermal method. The FeVO 4 /BiVO 4 nanostructures were characterized by XRD, SEM, XPS, UV–vis, and photoluminescence spectroscopy. The effects of catalyst dosage, contaminant concentration, initial hydrogen peroxide (H 2 O 2 ) concentration, and pH value on the degradation of levofloxacin were investigated and several repeated experiments were conducted to evaluate the stability and reproducibility. The optimized process parameters were used for mineralization experiments. Reactive oxygen species , degradation intermediates, and possible catalytic mechanisms were also investigated. The results showed that the sonophotocatalytic performance of the FeVO 4 /BiVO 4 heterojunction catalyst was better than that of sonocatalysis and photocatalysis . In addition, the Type II heterojunction formed by the material still had good stability in the degradation of levofloxacin after 5 cycles. The possible degradation pathway and mechanism of levofloxacin by sonophotocatalysis were put forward. This work develops new sono-photo hybrid process for potential application in the field of wastewater treatment .
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Yichen Zhang,Shugui Hua,Xiaoqin Sun,Zhuoyue Liu,Yuan Dang,Liang Zhang,Yuanzhen Zhou
A sea urchin-like NiO/Co 3 O 4 composite cathode was synthesized by two-step hydrothermal in-situ growth method and a Fenton-like process inducing two-electron oxygen reduction reaction (ORR) was established to degrade levofloxacin (LEV) in this paper. NiO/Co 3 O 4 exhibited higher specific surface area and better electrical conductivity comparing with NiO or Co 3 O 4 , indicating an excellent synergistic effect between NiO and Co 3 O 4 . Moreover, NiO/Co 3 O 4 cathode could effectively degrade LEV wastewater, the removal efficiency could reach 77.8% after 120 min and the corresponding COD removal efficiency was 41.0%. Further studies showed that the effective conversion of Co(Ⅱ)/Co(Ⅲ) and Ni(Ⅱ)/Ni(Ⅲ) occurred on the electrode surface, which promoted the generation of •OH. Finally, a possible degradation pathway of LEV involved defluorination, deamination, demethylation and other processes was proposed. In short, the research could provide important reference for solving electrochemical problems related to electrocatalytic ORR and Fenton-like 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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DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Qinyue Wu,Yan Zhang,He Liu,Hongbo Liu,Jia Tao,Min-Hua Cui,Zhiyong Zheng,Donghui Wen,Xinmin Zhan
For preparing high performance biochar to be applicated in persulfate-based oxidation treatment of wastewater, the feasibility of deriving Fe-N biochar from pharmaceutical sludge by endogenous Fe and exogenous N doping was investigated. With exogenous urea doping, Fe x N contained biochar (PZBC800U) was successfully derived from endogenous Fe(OH) 3 contained pharmaceutical sludge . PZBC800U effectively activated peroxymonosulfate (PMS) to remove 80 mg·L −1 levofloxacin (LEV) within 90 min. The main mechanism of PMS activation by PZBC800U for LEV degradation was revealed as non-radical pathways dominated by 1 O 2 generation and direct electron transfer . The formation of Fe x N combined with the increase of pyridinic-N in the biochar changed the electronic structure, improved the electron transfer ability, and thus achieved the excellent PMS activation capacity of the biochar. The vital function of endogenous Fe(OH) 3 was verified by comparing PZBC800U to Fe leached and extra Fe added controls. A total of 18 intermediates in the degradation of LEV were identified, and degradation pathways were proposed. Combined with the average local ionization energy calculation, the priority of piperazine breakage during LEV degradation was experimentally proved and mechanistically elucidated. This study provides a new insight into Fe x N biochar preparation from pharmaceutical sludge and the mechanisms of its excellent PMS activation performance for LEV degradation.
研究领域:
环境科学
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制药工程
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废水处理
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）