ELECTROCHIMICA ACTA
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2021
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IF 6.901
Jianyu Zhang,Chunli Zheng,Yujie Dai,Chi He,Hongxia Liu,Shouning Chai
In this work, a scaled-up electro-Fenton (EF) system was performed on the treatment of amoxicillin (AMX) wastewater. The effects of operational parameters on AMX degradation efficiency were investigated, such as Fe 2+ concentration, pH, applied current (mA) and initial AMX concentration. Kinetic analysis exhibited the degradation process followed the First-order kinetic model. Box-Behnken design (BBD) was applied here to determine and analyze the optimum operating condition. Up to17.68 mg•L −1 of H 2 O 2 could be in situ generated in 120 min without external O 2 supply and reusability of the electrodes were analyzed. Moreover, a degradation mechanism with hydroxyl radicals (•OH) as dominant oxidant was proposed. UPLC-MS analysis was performed to identify oxidation intermediates and thus a reasonable degradation pathway of AMX was speculated. Acute toxicity assessment showed a 50% decrease in bio-toxicity of the treated effluent. The EF system provided a new insight into the effective pretreatment of antibiotic wastewater.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Xingyu Fang,Lu Gan,Linjie Wang,Han Gong,Lijie Xu,Ying Wu,Haiqin Lu,Shuguang Han,Juqing Cui,Changlei Xia
In this study, mixed metal cobalt zinc oxide embedded nitrogen enriched porous carbon composites (CoZnO-PC) were prepared via pyrolyzing polyvinylpyrrolidone (PVP) encapsulated Co, Zn-bimetal centered zeolitic imidazolate frameworks (ZIF). The prepared composites were then used to activate peroxymonosulfate (PMS) for bisphenol A (BPA) removal in water. When mole ratio of Co/Zn was 2/1, the resulted Co 2 Zn 1 O-PC possessed spinel structure with prominent degradation capability, in which the introduction of Zn accelerated the PMS activation performance of Co through establishing bimetal synergistic interactions. Both radical and non-radical activation pathways were existed in the Co 2 Zn 1 O-PC/PMS system, in which Co 2 Zn 1 O dominated the radical pathway whereas PC dominated the non-radical way. Since PVP contained abundant nitrogen atoms and could form strong coordination interactions with the ZIF precursor, the introduction of PVP in the ZIF precursor prevented pore collapsing during pyrolysis process , as well as enhancing the nitrogen content in the pyrolzed composites, which significantly promoted the generation of singlet oxygen. With combined pathways, the Co 2 Zn 1 O-PC/PMS system showed a wide pH application range with promising mineralization rate. Meanwhile, the spinel-structured Co 2 Zn 1 O-PC was magnetically separable with desirable recyclability . This study presents a novel composite with remarkable performance for the removal of refractory organic pollutants in municipal wastewater .
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Wei Wu,Shishu Zhu,Xiaochen Huang,Wei Wei,Chao Jin,Bing-Jie Ni
Persulfate (PS) activation on biochar (BC) is a promising technology for degrading the aqueous organic contaminants. However, the complexity of activation mechanisms and components in biomass that used to produce BC makes it difficult to predict the performance of PS activation. In this study, we employed eight sludges as the representative biomass that contained absolutely different organic or inorganic components. Results showed that the elemental composition, surface properties, and structures of the sludge-derived BCs (SBCs) clearly depended on the inherent components in the sludges. The intensities of persistent free radicals (PFRs) in the electron paramagnetic resonance (EPR) correlated positively with N-containing content of sludges as electron shuttle, but negatively with the metal content as electron acceptor. Linking with PFRs as crucial sites of triggering a radical reaction, a poly-parameter relationship of predicting PS activation for organic degradation using the sludge components was established (kobs,PN = 0.004 × Cprotein + 0.16 × CM–0.895 −0.118). However, for the PS activation on those SBCs without PFRs, this redox process only relied on the sorption or conductivity-related characteristics, not correlating with the content of intrinsic components in biomass but with pyrolysis temperatures. This study provided insightful information of predicting the remediation efficiency of PS activation on BCs and further understanding the fate of contaminants and stoichiometric efficiency of oxidants in a field application.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Haocheng Song,Qiang Li,Yuxuan Ye,Fei Pan,Dajie Zhang,Dongsheng Xia
Antibiotic contamination has become a serious environmental problem and much attention has been paid to its purification. The sulfate radical (SO 4 − ) based advanced oxidation processes (AOPs) exhibited significant potential in the treatment of antibiotics. In this study, the magnetic biochar (Fe 2 O 3 @LBC) derived from loofah was prepared to activate persulfate (PS) for cephalexin (CEX) degradation. Under the optimal conditions, 73.9% of CEX was removed in the Fe 2 O 3 @LBC/PS system. Free radicals quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that HO and SO 4 − were responsible for the degradation of CEX. The C-OH of the catalyst played a crucial role in the degradation process. In addition, the conversion between Fe 3+ and Fe 2+ enhanced the degradation of CEX by producing SO 4 − . The degradation performance of other antibiotics and CEX in different water matrices indicated the broad adaptability and applications of Fe 2 O 3 @LBC. The main intermediates and the possible transformation pathways were proposed. These results provided a potential insight into biochar based catalysts for the degradation of antibiotics by activation of persulfate.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jun Cao,Qing Sun,Ai-Guo Shen,Bing Fan,Ji-Ming Hu
Killing harmful bacteria in biofilms is a major challenge for current root canal therapy. Although traditional chemical disinfectants have a good bactericidal effect on plankton, they have little efficiency for the removal and sterilization of bacterial biofilms, and even lead to the emergence of bacterial resistance and high toxic side effects. Herein, we propose for the first time biosafe nanocomposites that integrate photothermal and peroxidase-like catalytic activity for efficient removal and killing of bacterial biofilms in root canals. The integration of gold (core) and copper (Ⅰ, Ⅱ) sulfide (shell) shows excellent catalytic effect, which can catalyze the decomposition of hydrogen peroxide at biosafe concentrations to hydroxyl radicals for efficient removal of biofilms. Moreover, studies on the mechanism of antibiofilm showed that the nanocomposites ( [email protected] 2-x S) have significant degradation effects on proteins and polysaccharides-the main components of biofilm. The in vitro results indicated that the synergism of free radical and heat shows higher sterilization rate against both gram-positive Enterococcus faecalis and gram-negative Fusobacterium nucleus , compared with free radical and heat treatment alone. More importantly, the bactericidal results on isolated dental slices and in root canal models and beagle dog demonstrated the [email protected] 2-x S is highly effective in inactivating the bacteria in biofilms. Hence this safe and synergistic antimicrobial system has great potential in antibiofilm-oriented root canal therapy.
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CERAMICS INTERNATIONAL
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2021
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IF 4.527
Qingming Meng,Wenna Liu,Juan Jiang,Xinle Zhang
CuO/ZnO p-n heterojunction nanofibers were fabricated by coupling p-type CuO with n-type ZnO nanofibers for efficacious elimination of pyridine in fuel oil. The structural and photoelectric characteristics of the as-synthesized nanofibers were systematically studied. The photodegradation system was appropriate for the oxidation of pyridine from fuel oil utilizing the ambient air without mixing with other oxidants. Under visible light illumination, more than 90% of the pyridine (100 mL, 100 μg/g) could be degraded within 60 min by 17.5 mg of MCuZn-0.5 (the photocatalyst with a Cu/Zn molar ratio of 0.5 at%). The visible-light-induced photocatalytic denitrification efficiency of the MCuZn-0.5 nanofibers was nearly 1.5 times as high as that of ZnO alone. The superior denitrification activity of p-CuO/n-ZnO heterojunction nanofibers could be attributed to the enhanced optical absorption capacity and efficacious separation of photoexcited charge pairs. In addition, five-cycle experiments confirmed that MCuZn-0.5 nanofibers also displayed satisfactory photocatalytic denitrification properties. Mechanistic investigations proposed that the photoexcited holes played a dominant role in the formation of reactant intermediates, while superoxide radicals promoted the ultimate mineralization process of pyridine.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Yijing Luo,Yubin Su,Yao Lin,Liangbo He,Li Wu,Xiandeng Hou,Chengbin Zheng
Despite the increased interest and great progress obtained on arsenic test, it is still a challenge to accomplish the on-site determination of arsenic in rice due to the expensive instrumentation and harsh digestion process. In this work, MnFe 2 O 4 micromotors were found to retain high catalytic activity to simultaneously produce large amounts of hydroxyl radicals and O 2 bubbles in the presence of H 2 O 2 . Interestingly, the generated bubbles autonomously propel the micromotors and prevent them from depositing, thus keeping their high catalytic activity. As a result, a MnFe 2 O 4 micromotors enhanced digestion method was developed for the field digestion of rice samples within 100 min only using H 2 O 2 , which was further utilized to realize the on-site detection of arsenic in rice by coupling with the Gutzeit method followed headspace solid phase extraction . A quantification limit of 40 μg kg −1 was obtained for the determination of arsenic in rice. Owing to their capabilities of the efficient and rapid adsorption of arsenic and continuous movement, a MnFe 2 O 4 micromotors enhanced solid phase extraction was also established for the sensitive determination of arsenic in water with a 1 μg L −1 of quantification limit. The accuracy of the developed method was validated via analysis of a Certified Reference Material of rice (GBW10043) and a series of rice and water samples with satisfactory results, showing promising potential in the sensitive on-site detection of arsenic in rice and water samples.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Mengfei He,Peng Zhao,Ran Duan,Shengjun Xu,Gong Cheng,Mengjia Li,Shuanglong Ma
In this study, chitosan, a low-price and easily obtainable natural polymerized sugar containing abundant nitrogen element, was employed as a precursor for preparing hierarchically porous carbon (PC) to activate peroxymonosulfate (PMS). The PC fabricated at 800 °C obtained the optimum catalytic performance with complete removal of p-hydroxybenzoic acid (HBA) in 30 min. The selective degradation toward phenolic pollutants with different substituent groups and the resistance over the interference of typical anions and natural organic matter implied a non-radical pathway contributed most for HBA degradation. The investigation of structure-activity relationship suggested a positive linear correlation between graphitic N content and HBA removal. The chemical quenching experiment and electron paramagnetic resonance (EPR) excluded the crucial role of radicals and 1 O 2 . Solid evidence based on electrochemical techniques demonstrated the essential contribution of electron transfer pathway achieved by three successive processes including the first close adsorption of PMS by PC800 to form metastable intermediates, then an internal electron transfer from active graphitic N to PMS within metastable intermediates and finally external electron transfer from HBA to metastable intermediates. This study provided insightful mechanism understanding of a promising organics elimination strategy by PMS activation through N-doped carbonaceous materials utilizing chitosan as a simultaneous carbon and nitrogen precursor.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Rui Zhou,Haoran Song,Daoyuan Zu,Shiting Pan,Yuwei Wang,Fangxian Wang,Zhuo Li,Yongming Shen,Changping Li
The self-floating Ti 3 C 2 MXene-coated polyurethane sponge (MXene@PU module) was prepared via the simple coating operation for thermal activation of peroxydisulfate (PDS) and production of clean water. Coating MXene on the surface of PU significantly improved the degradation of model pollutant carbamazepine (CBZ) compared with PU alone under simulated solar radiation. Because of the excellent photothermal conversion performance of Ti 3 C 2 MXene and the unique double-deck structure of MXene@PU module, the interfacial temperature of MXene@PU module reached about 140 °C, far higher than that of PU (about 82 °C). Radical identification experiments demonstrated that both hydroxyl radical and sulfate radical contributed to the degradation of organic pollutant. Addition of Cl − , HPO 4 2− , HCO 3 − and natural organic matter in solution generated inhibitory effect on CBZ degradation. The prepared MXene@PU module exhibited excellent stability after long-time experiment. Importantly, the interfacial evaporation process produced abundant recycled water and no pollutant was detected in recycled water. This study provides a feasible way to utilize the renewable solar energy for removal of organic pollutants and production of clean water.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Dongdong He,Ke Zhu,Jin Huang,Yaqian Shen,Lele Lei,Hongmei He,Wenjin Chen
Heteroatoms doped carbon materials are widely used in the advanced oxidation process (AOPs) to remove organic pollutants in water due to the synergies effect between different heteroatoms. In this study, a novel kind of N, S co-doped magnetic mesoporous carbon nanosheets (Fe@NS-C) was prepared by simple one-step pyrolysis . Further, the influence of doping amount of S ( L -methionine) and N (melamine) on catalytic activity was studied, the optimized sample Fe@NS-C-2-12/PMS showed a satisfying degradation ( 91.07%) for high concentrations of tetracycline (80 mg/L TC) in 10 min, which was attributed to the proper ratio of S content to N content (S(at.%)/ N(at.%) = 0.2097) in the sample could better play its synergistic effect by XPS analysis. The Fe@NS-C-2-12/ PMS system also exhibited satisfactory degradation effects in a wide pH range (3−10) and the existence of inorganic ions and humic acid . Then, the degradation mechanisms were mainly through the non-radical pathway ( 1 O 2 and electron transfer) and the major active sites were pyridinic N compared to thiophene S, C O, and Fe-N x . This study could inspire the design of high-performance active and low-cost heteroatomic doping nano-magnetic catalysts for PMS-based waste treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Li Chen,Tahir Maqbool,Congyu Hou,Wanyi Fu,Xihui Zhang
In recent years, activation of persulfate via Mn-based composites has gained interest due to extraordinary kinetics and performance for the degradation of organic contaminants. However, the potential of pristine manganese oxides (Mn 3 O 4 ) in removing organic compounds and its mechanism has not been comprehensively explored yet. This study systemically investigated the Mn 3 O 4 based peroxymonsulfate (PMS) activation to effectively mitigate bisphenol A (BPA) in different real water matrixes. Substantial mineralization (75.9%) with efficient removal of BPA (96.7%) has been achieved at optimum conditions in 60 min. A long-term performance, eight cycles of reusability, has shown merely an 11% reduction in BPA removal, highlighted the higher stability of Mn 3 O 4 . The oxidizing contributions of reactive oxygen species (ROS) were in the order of 1 O 2 > O 2 •- > SO 4 •- > • OH. The different water matrixes have influenced BPA degradation by<10%. Linear changes in BPA aromatic contents were recorded using log-transformed ultraviolet (UV) spectra and fluorescence excitation-emission matrix (EEM). Total 17 transformation products (TPs) were detected in Mn 3 O 4 /PMS/BPA system, with 13 decreasing concentrations and 4 TPs in increasing concentration with the β-scission reaction as the main pathway for the degradation of BPA. The toxicity of BPA after degradation was also significantly suppressed measured by the activated sludge inhibition method.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Jinling Xie,Liu Chen,Xuan Luo,Li Huang,Siyu Li,Xiaobo Gong
Peroxymonosulfate (PMS) based advanced oxidation process has been proved to be an efficient method for Antibiotic treatment. B, N co-doped carbon porous material was derived from metal-organic frameworks. B-NC catalysts showed excellent efficiency for removal of tetracycline hydrochloride. Nitrogen doping essentially changed the degradation pathway of tetracycline hydrochloride, while boron doping provided more active sites. through more defect sites, which is closely related to the adsorption and catalytic performance of the catalyst. The major active species of B-NC/PMS system was singlet oxygen ( 1 O 2 ) through quenching experiments and electron paramagnetic resonance (EPR) studies. Electron transfer was another non-radical oxidation pathway of B-NC/PMS system. This provides a new idea for the selective oxidation of antibiotics by metal-free activated PMS.
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