SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Chuankun Yin,Aimal Khan,Qiaohui Gao,Quan Li,Xiaoyun Zhou,Xiuying Liu,Aihua Xu,Xiaoxia Li
Recently, the development of efficient mixed metal oxide catalysts for organic pollutants degradation via peroxymonosulfate (PMS) activation is a hot topic in the area of wastewater treatment . In this work, the silver-copper mixed-oxide, Ag 2 Cu 2 O 3 (ACO) was reported for the first time as a highly active catalyst for removing organic pollutants in the presence of PMS. ACO was successfully synthesized from Ag + and Cu 2+ ions at 60 °C, and its structure was strongly influenced by the temperature. The catalyst could almost completely remove p -nitrophenol and other pollutants with 0.65 mM PMS after 20 min, and also exhibited satisfactory stability and recyclability. The system efficiency was shown to vary with the concentration of PMS and catalyst, as well as solution pH. Scavenger experiment and EPR analysis indicated that radicals produced by the oxidation of Ag(I) and Cu(I) with PMS could promote degradation reaction. The synergistic effect between Cu and Ag in the bimetallic catalyst was demonstrated to contribute to the high performance: Cu(II)-O-Ag(I) bonds promote the conversion of Cu(II) species to Cu(I) through reaction with PMS, and facilitate the oxidation of Cu(I) and Ag(I) by PMS to generate active radicals. The study provides a feasible strategy to design efficient and stable bimetal oxide catalysts for PMS activation.
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Journal of Water Process Engineering
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2022
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IF 7.34
Wenchao Liao,Shuyi Liao,Su Xu,Qingsong Li,Linbo Han
A chemical-less microwave enhanced photolysis process (named MW/UV) was established for sulfamethoxazole (SMX) degradation and the mechanisms were specifically studied. 96.7% of SMX could be removed in an extremely short reaction time of 140 s under 400 W of microwave and 23.0 mW/cm 2 of UV light at 254 nm. The half-live of SMX was greatly shortened to 5 s in MW/UV process, compared with 67 s in UV process and 1386 s in MW process. MW/UV process was also effective when applied to complex real water matrices, such as river water, seawater, and synthetic waste water. Non-thermal effects of microwave were found to play an essential role in elevating photolysis degradation efficiency. The ROS formation detected by quenching experiments and EPR test showed that SMX degradation by MW/UV followed non-radicals dominated method, although 1 O 2 and OH co-existed in this system. 16 intermediates in total were detected by HPLC-Q-TOF and three degradation pathways based on 1 O 2 and OH oxidation were proposed according to the structural characteristics of the intermediates. Besides, toxicity evaluation of SMX and its intermediates revealed that MW/UV process could effectively reduce the toxicity of SMX. This study provides an efficient and promising scheme for practical SMX degradation.
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MICROCHIMICA ACTA
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2022
·Vol. 189
·期 6
·1-11
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IF 6.408
Guo Jingjing,Liu Yangyang,Mu Zhao,Wu Shu,Wang Jueyu,Yang Yue,Zhao Min,Wang Yan
A bifunctional Ni-MOF nanosheet was synthesized and developed for label-free fluorescent detection of H 2 O 2 and glucose. The Ni-MOF exhibited intrinsic peroxidase-like activity and its catalytic activity was demonstrated to be originated from the hydroxyl radicals (•OH) produced in catalytic process. Since the generated •OH enabled terephthalic acid, the non-fluorescent organic ligand of Ni-MOF, to form a strongly fluorescent 2-hydroxy terephthalic acid, the Ni-MOF nanozyme was endowed with dual-function properties of mimicking peroxidase and emitting fluorescence. Based on this bifunctional Ni-MOF nanozyme, the proposed label-free fluorescence sensing strategy was applied to detecting H 2 O 2 and glucose with wide linear ranges of 0.1–20 mM and 8–30 μM, and low detection limits of 4.0 × 10 −5 M and 4.0 × 10 −6 M, respectively. Furthermore, the bifunctional Ni-MOF-based label-free sensing platform was successfully used for the glucose detection in human serum samples, showing good reproducibility and high accuracy. This strategy provides a green and sensitive method for the determination of small biomolecules in practical applications by the combination of enzyme cascade reaction. Graphical abstract
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Jingdong Yang,Yu Li,Zequn Yang,Kaimin Shih,Guang-Guo Ying,Yong Feng
The presence of 1,4-dioxane in various water streams poses a threat to the health of human beings. In this study, the oxidative combination of ozone with peroxymonosulfate (PMS) was for the first time used to remove 1,4-dioxane from water. Near complete abatement of 1,4-dioxane was achieved by ozone-PMS after reaction of only 15 min and the degradation kinetics was found to be positively correlated with doses of PMS and ozone. Ozone-PMS oxidation had the optimum performance at slight base pH values. Both sulfate radicals and hydroxyl radicals were generated in ozone-PMS oxidation and these radicals resulted in the degradation of 1,4-dioxane. The effects of common water constituents and real water matrices were investigated. It was found that bicarbonate ions with a concentration up to 10 mM had a slight promoting effect, while either chloride ions or natural organic matter inhibited only slightly the degradation. Meanwhile, no obvious difference in the degradation of 1,4-dioxane was found among the real water matrices and deionized water , which demonstrates that ozone-PMS oxidation has high tolerance and stability. The results from this study demonstrate that ozone-PMS may be a promising technology for the removal of 1,4-dioxane from various water matrices.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Jiahuan Li,Shaojie Ren,Xiao Qiu,Shan Zhao,Rui Wang,Yunkun Wang
To combat the spread of antibiotic resistance into the environment, we should adequately manage wastewater effluent treatment to achieve simultaneous removal of antibiotics, antibiotic resistant bacteria (ARB), and antibiotic resistance genes (ARGs). Herein, we fabricate a multifunctional electroactive poly(vinylidene fluoride) ultrafiltration membrane (C/PVDF) by phase inversion on conductive carbon cloth. The membrane possesses not only excellent retention toward ARB and ARGs but also exhibits high oxidation capacity as an electrode. Notably, sulfamethoxazole degradation involving hydroxylation and hydrolysis by the anode membrane is predominant, and the degradation efficiency is up to 81.5% at +4 V. Both electro-filtration processes exhibit significant ARB inactivation, anode filtration is superior to cathode filtration. Moreover, the degradation of intracellular ARGs (iARGs) located in the genome is more efficient than those located in the plasmid, and these degradation efficiencies at −2 V are higher than +2 V. The degradation efficiencies of extracellular ARGs (eARGs) are opposite and are lower than iARGs. Compared with regular filtration, the normalized flux of electroactive ultrafiltration membrane is improved by 18.0% at −2 V, 15.9% at +2 V, and 30.4% at +4 V during treating wastewater effluent, confirming its antifouling properties and feasibility for practical application.
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ACS Applied Nano Materials
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2022
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IF 6.14
Zhenying Jiang,Xianjun Tan,Jingyi Xu,Yuxiong Huang
The internal electric field induced by a piezoelectric effect is a promising method to suppress rapid electron–hole recombination of photocatalysis for environmental remediation. Herein, we fully utilized both piezoelectric and photocatalytic properties of Bi2WO6 nanoplates for the removal of organic pollutants. The degradation rate constant of piezo-photocatalysis is dramatically boosted to 0.077 min–1 by the Bi2WO6 nanoplates, which is 4.2-fold of the photocatalysis alone. The superior catalytic activity of Bi2WO6 nanoplates was attributed to the accelerated electron–hole pair separation efficiency associated with the enhancement of the piezoelectric effect-induced internal electric field. Based on the theoretical calculation, the bandgap of Bi2WO6 nanoplates would decrease from 1.99 to 1.67 eV under mechanical strains, indicating that broader light harvesting and faster charge transfer can be achieved with the assistance of the piezoelectric field. Accordingly, multiple reactive oxygen species (·O2– and ·OH) are dominant for the degradation activity based on the quenching experiments and EPR analysis, outperforming piezocatalysis and photocatalysis. We have provided a new strategy to improve the catalytic decontamination performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Tao Wang,Qiuyue Men,Xiqing Liu,Hongquan Zhan,Yongqing Wang
0D/2D interface heterostructure of 0D CuInS 2 and 2D NiAl-LDH were obtained via strong interfacial contact. Mott-Schottky analysis confirmed both materials were n-type feature. Thus, a staggered n-n heterojunction was formed via the balance of Fermi level. This 0D/2D composite exhibited enchantable activity for photocatalytic degradation 2,4-Dichlorophenol under visible-light illumination, far superior than pure CuInS 2 and NiAl-LDH. The improvement of photocatalytic performance mainly attributed to the large BET surface area and interfacial contact, which resulted in more active sites, effective charge separation and transfer. Moreover, the optimal CuInS 2 /NiAl-LDH composite showed higher photostability for cycle experiments. At the same, the possible photocatalytic reaction process was proposed based on the trapping experiments, ESR technique and band position. This work provided a theory and foundation for designing and preparing of 0D/2D heterostructure system for photocatalytic application.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Jun Wang,Ying Zhao,Chunting Li,Zijun Yu,Yang Zhang,Yuan Li,Xiaoyao Tan,Shaomin Liu,Shaobin Wang,Xiaoguang Duan
Hierarchically porous iron/nitrogen-doped carbons (Fe-N-PC) were developed for the oxidation of ibuprofen (IBP) with peroxymonosulfate (PMS). The incorporation of trace-level iron and nitrogen dopants promoted the catalytic performance remarkably, leading to 4.8, 16.4 and 22.9-fold enhancement over N-doped carbon (N-PC), porous carbon (PC), and Fe-doped carbon (Fe-PC), respectively. Fe(III) was anchored in nitrogen-coordinated pots (Fe-N x ) in the sp 2 -hybridized carbon network, and graphitic-N could synergistically boost the catalysis. Notably, methyl phenyl sulfoxide (PMSO) transformation, quenching tests, in situ electrochemical analysis and Raman spectroscopy verified high-valent iron-oxo species and direct electron transfer pathway accounted for pollutant oxidation. The relationship between the kinetic constants (ln k obs ) and the oxidation peak potential ( E op ) of pollutants was established with good correlation, manifesting particular selectivity toward oxidizing electron-rich pollutants and great immunity to background inorganic ions and natural organic matters (NOMs) for real wastewater treatment . The deactivation mechanisms of Fe-N-PC were revealed via surface oxidation and dopant refabrication. This work delicates to deepen the understanding of the nonradical mechanisms and structure-oriented PMS activation by engineered carbonaceous materials .
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ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Tianyao Shen,Xiaojing Wang,Peng Xu,Chunyan Yang,Jiaqin Li,Peng Wang,Guangshan Zhang
Dielectric barrier discharge plasma (DBDP) is an emerging and promising advanced oxidation process (AOP) for wastewater treatment . After investigating the effect of input voltage, O 3 (generated by dielectric barrier discharge), and peroxydisulfate (PDS) dosage, the DBDP O3 /PDS system was established. With the assistance of PDS, the atrazine (ATZ) removal efficiency increased from 69.67% to 82.46% within 25 min. Synergistic effect calculation suggests that there were markedly synergies between DBDP, O 3 , and PDS. Under the effect of SO 4 −• , the total organic carbon (TOC) removal and dechlorination efficiency were significantly improved. In addition, the DBDP O3 /PDS system maintained the ATZ removal efficiency at a high level over a wide range of initial pH values. According to quenching experiments and electron paramagnetic resonance (EPR) detection, the dominant radical for ATZ degradation in the DBDP O3 /PDS system was HO • . A possible degradation pathway of ATZ was proposed based on density functional theory (DFT) analysis, quadrupole-time of flight-liquid chromatography/mass spectrometry (Q-TOF-LC/MS) results, and related literature. The acute toxicity to aquatic minnows and the developmental toxicity of intermediate products prediction confirmed that the DBDP O3 /PDS system could effectively reduce ATZ toxicity. The electrical energy per order ( E EO ) was 7.10 kWh m −3 order −1 illustrating that the DBDP O3 /PDS was a more energy-economic system than other energy-intensive processing technologies .
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Minghui Xiong,Juntao Yan,Guozhi Fan,Yanyu Liu,Bo Chai,Chunlei Wang,Guangsen Song
The strong electronic interaction between heterogeneous composite catalysts facilitates the charge separation and transfer, which is favorable for the enhancement of catalytic performance. Herein, the rape straw derived biochar (BC) supported ultrafine Co 3 O 4 composites were synthesized for tetracycline hydrochloride (TC) degradation via activating peroxymonosulfate (PMS), and the built-in electric field (BIEF) driven catalytic degradation mechanism was proposed. The results indicated that 20 wt% Co 3 O 4 /BC catalyst could achieve 90% degradation efficiency of TC within 20 min, and demonstrated that BC not only served as a support to significantly inhibit the agglomeration of Co 3 O 4 nanoparticles and improve the stability of catalyst, but also behaved as an activator of PMS to participate in the catalytic degradation reaction. Both radical pathway ( SO 4 · - , · OH and O 2 · - ) and non-radical process ( 1 O 2 and direct electron transfer) were involved in the Co 3 O 4 /BC/PMS system, and the role of the latter is more prominent, in which Co 2+ /Co 3+ redox cycle and C = O groups on the BC were the possible active sites. Furthermore, the density functional theory (DFT) calculations revealed that a BIEF pointing from BC to Co 3 O 4 at the interface was formed, which could act as the internal driving force for electron transfer to accelerate the redox cycle of Co 2+ /Co 3+ and induce the direct electron transfer, and thus resulting in the better degradation of TC. This work not only offered a mechanistic insight into synergistic effects of composite catalyst in PMS activation, but also provided a win–win strategy of realizing the resource utilization of agricultural waste and environmental remediation simultaneously.
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FOOD RESEARCH INTERNATIONAL
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2022
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IF 7.425
Jianmei Yang,Likang Qin,Yong Zhu,Chongyun He
In this study, the radicals formed in camellia oil upon a heating process were identified and quantified using Electron Spin Resonance (ESR) spectroscopy coupled with spin-trapping technique. PBN and DMPO were served as spin traps. The total amounts of free radicals of heated camellia oil showed an increasing trend with the extension of heating time at 140 °C, 150 °C and 160 °C. In accordance with hyperfine splitting constants (aN, aH) ─ the crucial parameter for identifying free radical species ─ of free radical, it was definitely confirmed that alkyl, alkoxyl, oxygen-centered and DMPO oxidate free radicals were present in heated camellia oil. A free radical transition pathway was proposed that alkyl free radical is initially generated, then, alkyl peroxy free radical is subsequently generated in the presence of oxygen which eventually shifts into alkoxyl free radical by means of an intermediate formed from H-capture reaction of alkyl peroxy free radical.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xiurong Zhu,Lei Ge,Wei Yan,Shengjiong Yang,Gen Wang,Delu Miao,Pengkang Jin
Heterogeneous activation of peroxymonosulfate (PMS) has been frequently proposed for the degradation of organic pollutants via the generation of reactive oxygen species (ROS). Spinel ferrite such as CoFe 2 O 4 shows great advantage for PMS activation but suffers from aggregation problem and lack of microstructure. Herein, network-like CoFe 2 O 4 immobilized on volcanic rock was synthesized for PMS activation for degrading sulfamethoxazole (SMX). The immobilized CoFe 2 O 4 network exhibited good catalytic performance for SMX removal. Systematic investigations, including in situ ATR-FTIR and Raman spectroscopy analysis, chemical quenching experiments and electron paramagnetic resonance (EPR) tests, revealed that a redox cycle of Co 2+ /Co 3+ induced the generation of ROS (SO 4 •− , OH • and 1 O 2 ) that participated in the degradation of SMX. Background constituents (e.g., inorganic ions and natural organic matters) exhibited limited influence on SMX removal. A continuous flow-through reaction in a fixed-bed column revealed the immobilized CoFe 2 O 4 network could efficient degrade SMX with long-term durability, which therefore can be a promising catalyst for PMS activation for the degradation of SMX.
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