JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Jialin Jia,Dongmei Liu,Qiao Wang,Huarui Li,Jiaxin Ni,Fuyi Cui,Jiayu Tian
In this work, degradation of bisphenol F (BPF), bisphenol AF (BPAF) and bisphenol S (BPS) by peroxymonosulfate (PMS) with TiO 2 nano-tubes arrays (TiO 2 NTAs) under simulated sunlight irradiation was investigated and compared for the first time. All three bisphenols exhibited appreciable degradation following the order of BPS < BPAF < BPF, and acidic conditions were more conducive to their degradation. The SO 4 •- , · OH, h + and • O 2 - were all identified in three bisphenols degradation processes. Among these, SO 4 •- and • O 2 - were proven to play a dominant role in BPF oxidation process , but SO 4 •- and h + were confirmed as the main reactive species for BPAF and BPS removal. Owing to the different reactive species worked in different bisphenols degradation processes, the influences of inorganic anions on three bisphenols degradation were also different. By analyzing the oxidation intermediates of the three bisphenols, it was found that there were some common degradation pathways including bond-cleavage and hydroxylation of the benzene ring shared by three bisphenols. Besides, some specific degradation pathways were also identified, for example, the self-coupling was found in BPF and BPS degradation process, while the benzene ring splitting was occurred only in BPAF transformation process
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Hang Li,Yan-Ling Yang,Xing Li,Xiao-Yan Fan,Nan Wang
Vacuum ultraviolet/ persulfate (VUV/PS) has been a prospective method for antibiotics removal, however, the enhanced degradation mechanism is still unclear. This study compared the sulfamethazine (SMT) degradation by VUV/PS and ultraviolet/persulfate (UV/PS) processes using a photoreaction system. Results showed that the SMT degradation rate and PS activation rate by VUV/PS was 1.36 times and 1.39 times those of the conventional UV/PS process under the same dosage of PS, respectively. VUV/PS also achieved a high SMT mineralization. SO 4 • − and HO• played important roles in the degradation of SMT by both processes, while the role of •O 2 − was little. SMT concentration changed the distributions of 185 nm and 254 nm photons absorbed by solution components and altered the initiated photolysis reaction. Both processes had faster degradation rates at low initial SMT concentrations and the optimum reaction condition was at solution pH of 5. The inhibited level of the SMT degradation in both processes by four anions was in the following order: NO 3 − > Cl − > HCO 3 − >SO 4 2 . VUV/PS process was also more efficient than UV/PS for degrading environmental (200 μg/L) and high (5 mg/L) concentration of SMT from three kinds of typical water matrices (tap, river and lake water). Finally, ten photoproducts of SMT degradation by VUV (or UV) were identified, which were mainly the oxidized products of C-N, -NH 2 and S-C on SMT molecules, and four degradation pathways were proposed. Overall, these findings could provide useful insights into the application of VUV/PS in efficient antibiotics removal from water.
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JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Naiku Xu,Jiao Han,Yan Feng,Changfa Xiao
Membrane process is used to decontaminate dye wastewater. In the process of separation, the adsorbed and/or rejected dyes can greatly foul the membrane and negatively affect separation efficiency. Fenton oxidation can non-selectively mineralize dyes to prevent fouling the membrane. Therefore, this work focused on synthesizing the membrane coupled with Fenton catalyst for dye wastewater treatment . Polyacrylonitrile (PAN)/poly (acrylic acid) (PAA) composite nanofiber membrane was first prepared by layer-by-layer sequential electrospinning and then served as the substrate to load iron ions by the coordination of carboxyl groups of PAA with iron ions , after which a catalytic membrane was successfully prepared. During the application process, water would inevitably elute some iron ions from the catalytic membrane. In order to minimize the loss of iron ions, another PAA/PAN composite nanofiber membrane with the function of rejecting iron ions was then designed and superimposed onto the catalytic membrane using the adhesiveness of upper PAA layer. In this sense, the obtained composite membrane can stably catalyze H 2 O 2 to effectively oxidize methylene blue (MB) due to low leaching-out of iron ions. The results showed that the iron ion loading ratio of PAN/PAA composite nanofiber membrane was increased by 167% compared to that of PAN nanofiber membrane, and the total iron ion elution ratios of PAN nanofiber membrane and PAN/PAA composite nanofiber membrane were 27 times and 6 times higher than that of superimposed composite membrane , respectively. As a result of high loading and low elution of iron ions, the superimposed composite membrane exhibited considerably stable efficiency for MB removal within 30 operation cycles, which reached up to 97.0%. Additionally, the superimposed composite membrane presented better mechanical property and more adjustable permeation flux than the control membranes, so that it would show a great potential for the application in the field of dye wastewater treatment .
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International Journal of Nanomedicine
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2021
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IF 6.4
Xiaodi Gong,Xin Pu,Jing Wang,Linlin Yang,Yunxia Cui,Lijuan Li,Xiao Sun,Jichang Liu,Jingfeng Bai,Yudong Wang
Purpose Iron-based nanomaterials have recently been developed as excellent and potent Fenton reagents to reactive oxygen species (ROS) during chemodynamic therapy (CDT). The performance of the materials, however, can be impaired by the intrinsic antioxidant defense mechanism in organisms, such as autophagy. Methods The nanoscale metal-organic frameworks (nMOFs), nMIL-100 (Fe), were exploited and characterized. Also, the Fenton-like catalytic characteristics, anti-endometrial cancer (EC) effects and potential mechanisms of nMIL-100 (Fe) nanoparticles were investigated in vitro. Results The synthesized nMIL-100 (Fe) nanocatalyst catalyzed hydroxyl radicals (·OH) production in the presence of hydrogen peroxide (H 2 O 2 ) and simultaneously depleted intracellular glutathione (GSH). Combining with H 2 O 2 , nMIL-100 (Fe) nanoparticles exhibited enhanced cytotoxicity for EC cells, especially for progesterone treatment-insensitive KLE cells, probably due to relatively lower expression of the catalase gene. The accumulated ·OH initiated PTEN induced putative kinase 1 (PINK1)/E3 ubiquitin-protein ligase Parkin-mediated cytoprotective mitophagy in turn to partially rescue ·OH-induced cell apoptosis. Furthermore, both pretreatments of EC cells with siRNA-mediated Parkin knockdown and Mdivi-1 (a mitophagy inhibitor) addition were sufficient to ensure nMIL-100 (Fe) synergizing with H 2 O 2 -induced oxidative damages. Conclusion These results suggest that the degree of mitophagy should be taken into consideration to optimize therapeutic efficiency when developing ROS based-CDT for EC cancer therapies. Therefore, a nMIL-100 (Fe)-guided, elevated ROS and overwhelmed mitophagy-mediated therapeutic strategy may have greater promise for EC therapy compared with current treatment modalities.
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CHEMOSPHERE
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2021
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IF 7.086
Fuyou Du,Zhan Lai,Huiyang Tang,Haiyan Wang,Chenxi Zhao
In this work, a novel BiOCl/Cu-doped Bi 2 S 3 photocatalyst was designed to efficiently remove ciprofloxacin (CIP) with high photocatalytical activity and good stability over a wide pH range. Compared with Cu-doped Bi 2 S 3 , Bi 2 S 3 , BiOCl, BiOCl/Bi 2 S 3 , and Cu-doped BiOCl, the photocatalytical degradation rate of CIP (97.1% at 20 mg/L) over BiOCl/Cu-doped Bi 2 S 3 was enhanced by about 84.77, 44.23, 2.95, 2.27, and 1.96 times within 20 min, respectively. Notably, the BiOCl/Cu-doped Bi 2 S 3 photocatalyst also displayed high photocatalytical performance in the degradation of other antibiotics including norfloxacin, ofloxacin, and tetracycline (40 mL, 20 mg/L; 88.3%, 100%, and 95.2% of degradation rate within 30 min, respectively) under visible light irradiation. Radical trapping experiments and electron spin resonance technique indicated that superoxide radicals (•O 2 − ) and photogenerated holes (h + ) played crucial roles in the photocatalytic degradation of CIP. Finally, the possible CIP degradation pathways was proposed by detecting the CIP intermediates in photocatalytical reaction process.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Huihui Wu,Jingjing Yan,Xin Xu,Qianhui Yuan,Jinhang Wang,Jun Cui,Aijun Lin
Advanced oxidation processes (AOPs) are promising ways for oxidative degradation of organic pollutants. Atom-dispersed transition metal–nitrogen–carbon (M–N–C) materials exhibit excellent efficiency in activating peroxide bonds and have been extensively pursued for environmental remediation. However, M–N–C with single atoms suffer from intrinsic performance limit of complicated catalytic reactions due to structural simplicity and lack of synergistic active sites. Herein, derived from Fe/Cu–coordinated zeolitic imidazolate frameworks with molecular-scale cages, a well–designed catalyst featuring Fe–Cu dual–metal sites coordinated with N–doped carbon (Fe/Cu–N–C) was fabricated. Compared to the single-atom iron catalyst (Fe–N–C), Fe/Cu–N–C significantly enhanced the chloramphenicol removal rate from 0.073 to 0.093 min −1 due to the synergistic effects of Fe–Cu dual active site. Furthermore, Fe/Cu–N–C exhibits fantastic reactivity for peroxydisulfate (PDS) activation in a wide pH range (3.1 – 10.3). Density functional theory calculations revealed that Fe/Cu–N is the major active site, where electrons transfer from Cu to Fe ensure the low-valence state of Fe for catalytic oxidation. Besides, the optimization of adjacent Cu–N sites improves the bonding orbital distribution of Fe 3d orbitals and promotes the adsorption and cracking of PDS. These findings reveal the cooperative mechanism of Fe–Cu dual–atom site on PDS activation and develop a promising platform toward environmental purification.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 41
·19432-19438
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IF 3.591
Fangyuan He,Heyi Zhang,Xiaonan Li,Jie Yang,Wenqing Ma,Hong Zhang
In this study, for the first time, we selected a size-matched polyoxometalate α-Mo8O26, and successfully prepared Mo8-UiO-66(Zr) as a catalyst with double active sites for extractive and catalytic oxidative desulfurization systems (ECODS). UiO-66(Zr) can encapsulate Mo8O26 in the cage and avoid its leaching, while the sulfur compounds can also enter the cage to approach the sites. As a result, in the presence of H2O2 as an oxidant, the catalyst exhibited extraordinary oxidative desulfurization performance towards benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT). It only takes 10 min for the desulfurization efficiency to reach 100%. The catalyst can be reused for at least 4 times without significant loss in the desulfurization activity. Also, the possible reaction mechanisms of the catalytic oxidation process have also been proposed.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xiaona Dong,Xiaoxue Yang,Sheng Hua,Ziqian Wang,Tianming Cai,Canlan Jiang
The continuous accumulation of triphenyl phosphate (TPHP) in soil poses a potential threat to human health. Persulfate-based advanced oxidation processes (SR-AOPs) are promising soil remediation technologies. Naturally occurring soil constituents could interact with persulfate (PS) during soil remediation by SR-AOPs. However, the production and transformation of reactive oxygen species (ROS) by synthetic reactions between PS and different soil constituents, as well as their roles in the pollutants degradation, are still largely unknown. This study systematically investigated the generation of ROS and their roles in degradation of TPHP in soil constituents activated PS process and in soil constituents-heat (50 °C) co-activated PS process. Comprehensive studies including ROS identification, electron paramagnetic resonance analysis, and ROS-generated model systems were carried out. An appreciable degradation rate of TPHP (~21.9%) in soil-PS system and the significant discrepancy in degradation rate (69.0–97.0%) in heat-soil-PS systems with three different soils suggested that soil constituents exhibited complex effects on the activation of PS. The Fe/Mn-minerals in soil effectively activated PS and facilitated TPHP degradation. Specially, the iron redox cycle (Fe(II) ↔ Fe(III)) plays a key role in ROS generation. Small molecular soil organic matter (SOM) rapidly consumed the produced ROS which led to their mineralization, while the remaining macromolecular SOM became more hydrophilic by interaction with ROS. SO 4 •− , •OH, and 1 O 2 played major roles directly in TPHP degradation, while O 2 •− could not degrade TPHP directly but might promote TPHP degradation by reducing Fe(III)- to Fe(II)-minerals or converting to other ROS. This study provides new and deeper insights into the interaction between PS and soil constituents and their roles in organic pollutant degradation in contaminated soil using SR-AOPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yang You,Zekai Shi,Yunhe Li,Zhuanjun Zhao,Bo He,Xiuwen Cheng
In this work, cost-effective peroxymonosulfate (PMS) was used as oxidants and magnetic cobalt ferrite biochar composite was used as catalyst to remove lomefloxacin hydrochloride (LFH), a new pollutant in water. PMS activation by CoFe 2 O 4 was promoted by compositing with biochar. The MBC/CoFe 2 O 4 /PMS system degraded 86.9% of LFH in 20 min. MBC/CoFe 2 O 4 measured by vibrating sample magnetometer (VSM) had good magnetic properties and was convenient for separation and recovery. Furthermore, the main active oxide species were determined by EPR measurement. The catalytic mechanism of MBC/CoFe 2 O 4 /PMS system was attributed to the generation of sulfate radicals (SO 4 ∙- ), hydroxyl radicals (∙OH), singlet oxygen ( 1 O 2 ) and superoxide radicals (∙O 2 – ) additionally, of which SO 4 ∙- played the leading role. Moreover, a possible degradation pathway of LFH was proposed. MBC/CoFe 2 O 4 /PMS system still had 85.7% LFH removal efficiency after five times of reuse. Thence, the MBC/CoFe 2 O 4 composite material might be a candidate for removing difficult pollutants in environmental remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Congyu Wang,Zepeng Rao,Asad Mahmood,Xiao Wang,Yan Wang,Xiaofeng Xie,Jing Sun
In the process of photocatalytic oxidation (PCO), titanium dioxide (TiO 2 ) shows excellent capabilities. However, when TiO 2 is used to remove volatile organic compounds (VOCs), there are some drawbacks including weak adsorption of gaseous contaminants, insufficient utilization of sunlight, and rapid recombination of photogenerated carriers. Herein, a TiO 2 -based ternary heterogeneous photocatalyst, g-C 3 N 4 /Ag-TiO 2 , was successfully fabricated to photodegrade gaseous acetaldehyde (one of the representatives of oxygenated VOCs) under visible light. Among the various samples, the g-C 3 N 4 /50 wt% Ag-TiO 2 exhibited an excellent photocatalytic activity , which was 5.8 times of bare TiO 2 . The mineralization efficiency of acetaldehyde was also increased by 3.7 times compared to bare TiO 2 . The substantial improvement in the PCO performance of the ternary system can be associated with the good adsorption to acetaldehyde gas and light-harvesting capability, as well as improved charge separation process. The application of Langmuir-Hinshelwood kinetic model suggested that relative humidity played a significant role in the VOCs degradation. Also, the photodegradation of gaseous acetaldehyde primarily occurred on the catalysts surface. Based on several characterizations, i.e., UV–vis spectroscopy, photoluminescence spectrum, photocurrent spectroscopy and electron spin-resonance test, a suitable degradation mechanism is proposed. This study provides a novel ternary photocatalyst with improved photocatalytic performance and stability, which can be used for the low-concentration VOCs abatement in the indoor environment.
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Environmental Science-Nano
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2021
·Vol. 8
·期 7
·2049-2058
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IF 8.131
Yuqi Zhang,Xiang Yu,Huan Liu,Xinyi Lian,Bin Shang,Yue Zhan,Tingting Fan,Zhou Chen,Xiaodong Yi
Transition metal oxides (TMOs) are emerging as a promising class of photocatalysts for pollutants' treatment. In this report, by integrating anti-solvent crystallization and thermal treatments, we have developed a facile and environmental approach for the synthesis of MoO3−x nanosheets in the presence of hexadecyl-trimethyl ammonium bromide (CTAB). The thickness of MoO3−x nanosheets varies from 20 nm to 40 nm. CTAB promotes the formation of nanosheet morphology and Mo5+ defects. Combining experimental results and density functional theory (DFT) calculations, we demonstrate that the Mo5+ defect state in MoO3−x nanosheets can enhance visible light harvest and promote the separation of photo-generated electron–hole pairs. Hence, MoO3−x-8, the optimal photocatalyst, shows the highest concentration of surface Mo5+ defect (18.7%) and the best photocatalytic activity toward rhodamine B (RhB) photodegradation. About 95.9% RhB is degraded within 15 min under visible-light irradiation (λ > 420 nm). The kinetic rate of MoO3−x-8 reaches 117 times that of commercial MoO3. It was proved by the total organic carbon (TOC) measurements that about 43.3% of RhB molecules were degraded to CO2 and H2O. Overall, this work provides an effective pathway for the nanomaterial design and potential applications in the photocatalytic oxidation of organic pollutants.
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CHEMOSPHERE
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2021
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IF 7.086
Likun Chen,Kewen Xing,Qikai Shentu,Yifei Huang,Weiyang Lv,Yuyuan Yao
Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C 3 N 4 catalyst (HFeNC-g-C 3 N 4 ) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C 3 N 4 could not only effectively anchor Fe atom to create the well-dispersed Fe-N x active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C 3 N 4 catalyst with single-atom Fe-N x active sites, verified by XRD , XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe 2+ catalyst. The mechanism of O 2 •- dominated radical combined with nonradical 1 O 2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C 3 N 4 /PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.
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