ACS Applied Materials & Interfaces
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2018
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IF 8.097
Yanan Wei,Bingfeng Wang,Xinfang Cui,Yaseen Muhammad,Yanjuan Zhang,Zuqiang Huang,Xuesheng Li,Zhenxia Zhao,Zhongxing Zhao
MIL(Fe)/Fe-doped nanospongy porous biocarbon (Fe-SPC) composite was fabricated from MIL-100(Fe) via in situ growth on a unique Fe-doped nanospongy porous biocarbon (Fe-SPC) and was used as Fenton-like catalyst for advanced degradation of thiamethoxam (THIA). Fe was loaded on silkworm excrement and calcined to Fe-SPC with nanospongy and high sp2 C structure. The in situ growth strategy embedded the Fe-SPC into MIL-100(Fe) crystals and formed conductive heterojunctions with an intensified interface by Fe-bridging effect, which was confirmed by negative shift of Fe3+ binding energy in X-ray photoelectron spectroscopy. MIL(Fe)/Fe-SPC composites exhibited high degree of crystallinity and surface area (Brunauer–Emmett–Teller: 1730 m2/g). Liquid chromatography–mass spectrometry and density functional theory simulations demonstrated that THIA was converted to a relatively stable compound (C4H5N2SCl), which could be captured by MIL-100(Fe) with strong chemical bonding energy (Fe–N, −587 kJ/mol), followed by a significant geometric distortion, resulting in a thorough degradation. Efficient charge separation and synergistic chemisorption-catalysis strategy resulted in the high catalytic activity of MIL(Fe)/Fe-SPC. The composite catalyst concurrently exhibited high mineralization ratio with 95.4% total organic carbon removal (at 25 °C and 180 min) and good recycling ability under wider neutral/alkaline conditions. Endorsing to these intriguing properties, MIL(Fe)/Fe-SPC can be deemed an efficient contender for removal of hard-degradable pesticides and other environmental pollutants in practical applications.
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ACS Applied Materials & Interfaces
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2019
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IF 8.456
Zhongxi Xie,Shuang Liang,Xuechao Cai,Binbin Ding,Shanshan Huang,Zhiyao Hou,Ping’an Ma,Ziyong Cheng,Jun Lin
Hypoxia and overexpression of glutathione (GSH) are typical characteristics of the tumor microenvironment, which severely hinders cancer treatments. Here, we design a novel biodegradable therapeutic system, O2–Cu/ZIF-8@Ce6/ZIF-8@F127 (OCZCF), to simultaneously achieve GSH depletion and O2-enhanced combination therapy. Notably, the doped Cu2+ doubles the O2 storage capacity of the ZIF-8 matrix, which makes OCZCF an excellent pH-sensitive O2 reservoir for conquering tumor hypoxia, enhancing the photodynamic therapy (PDT) efficiency of chlorin e6 (Ce6) under 650 nm laser irradiation. Moreover, the released Cu2+ can act as a smart reactive oxygen species protector by consuming intracellular GSH. The byproduct Cu+ will undergo highly efficient Fenton-like reaction to achieve chemodynamic therapy (CDT) in the presence of abundant H2O2. The accompanying O2 will further alleviate hypoxia. The in vitro and in vivo experimental data indicate that OCZCF could cause remarkable tumor inhibition through enhanced synergetic PDT and CDT, which may open up a new path for cancer therapy.
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Journal of Environmental Sciences
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2019
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IF 3.556
Zhendong Li,Yanmei Sun,Wenli Huang,Cheng Xue,Yan Zhu,Qianwen Wang,Dongfang Liu
Magnetic CuO nanosheet (Mag-CuO), as a cheap, stable, efficient and easily separated peroxymonosulfate (PMS) activator, was prepared by a simple one-step precipitation method for the removal of organic compounds from salt-containing wastewater. The experiments showed that the removal efficiencies of various organic pollutants including Acid Orange 7, Methylene Blue , Rhodamine B and atrazine in a high-salinity system (0.2 mol/L Na 2 SO 4 ) with the Mag-CuO/PMS process were 95.81%, 74.57%, 100% and 100%, respectively. Meanwhile, Mag-CuO still maintained excellent catalytic activity in other salt systems including one or more salt components (NaCl, NaNO 3 , Na 2 HPO 4 , NaHCO 3 ). A radical-quenching study and electron paramagnetic resonance analysis confirmed that singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species for the oxidation of organic pollutants in high-salinity systems, which is less susceptible to hindrance by background constituents in wastewater than radicals ( • OH or SO 4 •− ). The surface hydroxylation of the catalyst and catalytic redox cycle including Cu and Fe are responsible for the generation of 1 O 2 . The developed Mag-CuO catalyst shows good application prospects for the removal of organic pollutants from saline wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Haichao Fu,Peng Zhao,Shengjun Xu,Gong Cheng,Zhuoqian Li,Yi Li,Kai Li,Shuanglong Ma
The novel Fe 3 O 4 and porous biochar originated from Myriophyllum aquaticum composites (Fe 3 O 4 /MC) with graphitized structure, hierarchical porous and strong magnetism were used as efficient catalysts for degradation of organic pollutants in the presence of peroxymonosulfate (PMS). Three types of catalysts pyrolyzed at 600, 700, 800 °C manifested quit different PMS activation effect with the much better p-hydroxybenzoic acid (HBA) degradation efficiency at 700 and 800 °C than that of 600 °C, which was assigned to the high graphitization degree and mesopores ration of catalysts pyrolyzed at higher temperature. Based on radicals quenching experiments and electron paramagnetic resonance (EPR) analyses, the radical pathway dominated by surface-bound SO 4 − was the prevailing way while the non-radical pathway performed as electro-transfer was the recessive way during the degradation process. The large amount of surface-bound SO 4 − radicals were produced through the reduction of PMS by Fe(II), which was regenerated by participation of O 2 − /O 2 . The non-radical pathway was achieved by the graphitized structure which acted as electron transfer bridges accepting electrons form organic pollutants and denoting electrons to PMS. Six HBA intermediates were detected and the possible HBA degradation pathway was proposed tentatively. Consequently, the conversion of Myriophyllum aquaticum to composite catalyst provides a brand-new idea for efficient utilization of waste biomass in a high value-added way and simultaneously achieving the contaminants elimination.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Lingshuai Kong,Guodong Fang,Yufeng Chen,Meng Xie,Feng Zhu,Long Ma,Dongmei Zhou,Jinhua Zhan
In this study, a flower-like Cu 2 FeSnS 4 (CFTS) nanomaterial was applied to the activation of persulfate (PS) for the degradation of bisphenol A (BPA) in model industrial wastewater. The efficiency of PS decomposition by CFTS, and the mechanism of contaminant degradation by SO 4 − were investigated. The results revealed that CFTS catalyzes PS decomposition more efficiently than the monometallic Cu/Fe/Sn sulfides and exhibits activity over a wide pH range. Electron spin resonance spectroscopy, X-ray photoelectron spectroscopy, and free radical quenching experiments revealed a tandem synergistic effect between Cu, Fe, and Sn in their quaternary chalcogenide systems upon PS activation. The intrinsic electron transfer between Cu, Fe and Sn, especially the Fe(II)* species formed upon the complexation of Fe(II) by S on the surface of the CFTS, overcomes the inhibition of the M (n+1)+ /M n+ redox cycle. CFTS shows promise as a catalyst for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yizhen Zhang,Lifen Liu,Bart Van der Bruggen,Michael K.H. Leung,Fenglin Yang
Berberine is a widely used antibiotic in China, its photocatalytic degradation is not well understood nor its efficient treatment reported. In this study, it is most quickly and efficiently degraded (97.9% under UV and 98.9% under visible light) using a free-standing 3D composite photo-electrode, with well dispersed Ag nanoparticles (Ag NPs) over well-aligned ZnO nanorods arrays (ZnO NAs) on Ni foam (NiF), compared to ZnO NAs/NiF, ZnO powder and P25. The composite photo-electrode was prepared by first directly growing ZnO NAs on NiF hydrothermally, followed by photo-deposition of Ag NPs, without any inactive binders or non-conductive substrates. It was characterized using scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), X-ray Diffraction (XRD), ultraviolet–visible spectrophotometry (UV–Vis) and electrochemical analysis (I-t, EIS). The highest activity of Ag NPs/ZnO NAs/NiF in degrading the target pollutant, is due to the synergy of easy pollutants diffusion and fast reaction on active sites, from suppressed electron-hole recombination by Ag NPs/ZnO NAs heterojunctions, extended light absorption by surface plasmon resonance (SPR) of Ag NPs and accelerated electron transport on the conductive macro-porous NiF. The reactive oxidizing species ( OH, O 2 − , h ± ), degradation intermediates and possible degradation pathways of berberine over Ag NPs/ZnO NAs/NiF were examined respectively. This free-standing whole piece photo-electrode with UV–visible light response, is easy to recycle and assemble, that not only degrades pollutant, but also generates electricity as photo-anode in a photo-catalytic fuel cell reactor using carbon fiber cloth as cathode.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Chao Liu,Liwei Chen,Dahu Ding,Tianming Cai
Conversion of agricultural biomass waste to value-added biochar based catalysts receives tremendous interests because it falls into the scope of resource recycle concept. In this work, a magnetic nitrogen doped biochar-supported CoFe 2 O 4 composite (MNBC) was synthesized by using rice straw, an abundant agricultural waste as the precursor. The prepared catalyst exhibited excellent performance in catalytic degradation of metolachlor (MET), a broad-spectrum chloroacetanilide herbicide, by coupling with peroxymonosulfate (PMS). The pyrolysis temperature played a significant role in the activity of the resultant catalysts. Among others, MNBC 800 catalyst performed the best stability and reusability. In-situ (EPR) analysis revealed that SO 4 •− , •OH and 1 O 2 participated into the degradation process and the SO 4 •− was the major contributor. The degradation was promoted at neutral and weak basic conditions, whilst significantly inhibited at strong basic condition (pH = 11). Eleven degradation intermediates were successfully identified through liquid chromatography – quadrupole time-of-flight – mass spectrometer (LC-Q-TOF-MS). The degradation mainly occurred via hydroxylation, dechlorination, and dealkylation reactions. Additionally, though the degradation was greatly inhibited in real wastewater , it was not remarkably influenced in river and groundwater, implying its applicability in river/groundwater remediation. Eventually, the easy separation and low toxicity make the catalyst promising for the degradation of MET from several aquatic systems. This study would pave the way to the catalytic degradations of organic pollutants by low-cost biochar based catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Ying Liu,Yong Feng,Yunfei Zhang,Shun Mao,Deli Wu,Huaqiang Chu
In this study, the presence of Cu(II) ions was found for the first time to severely inhibit +-dimethyl phthalate (DMP) degradation by ozone due to the formation of the stable complex Cu(II)-DMP. However, 100% DMP removal was rapidly reached when ethylenediamine tetraacetic acid (EDTA) was added with a Cu(II)/EDTA molar ratio of 3:1. Subsequent studies indicated that Cu(II)-DMP is sequestrated by EDTA, then DMP was degraded and Cu(II) was removed by precipitation. The freshly formed Cu-EDTA 2− and organic nitrogen intermediates further decomposed O 3 into OH, which induced to the rapid degradation of DMP. The k obs of Cu-EDTA/O 3 were 9–10 times greater than the k obs of DMP removed by ozonation alone within 10 min. The reaction mechanism involved a OH generation was proposed. The OH and O 2 - are generated from the rapid reaction between ozone and EDTA. Acting as a more strongly negative species, the specific Cu(II) in Cu-EDTA complexes is more inclined to react with O 2 - to give Cu(I), accelerating the forward reaction to produce more OH. The synergistic removal of DMP and Cu(II) can be achieved after reaction. Therefore, this study provides an effective method to dispose metal ion and organic pollutant wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Haichao Fu,Shuanglong Ma,Peng Zhao,Shengjun Xu,Sihui Zhan
Three novel graphitized hierarchical porous biochar (MX) and MnFe 2 O 4 magnetic composites (MnFe 2 O 4 /MX) have been prepared for degrading organic pollutants by peroxymonosulfate (PMS) activation. MX including MS, ML, MC synthesized using corn stems (S), leaves (L) and cores (C) as raw materials, respectively, possesses hierarchical porous structure, graphitization domains and tremendous surface area. The orange II removal effects of MX and MnFe 2 O 4 /MX outperform the corresponding carbonization products, despite that adsorption probably undertakes the major removal efficiency for MX and degradation contributes the most for MnFe 2 O 4 /MX. A structure-dependent degradation efficiency is discovered for MX and MnFe 2 O 4 /MX, among of which both MS and MnFe 2 O 4 /MS present the best removal effect, by electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS). The lowest EIS owning to its better balance between graphitization degree and specific surface area and micropore volume of MnFe 2 O 4 /MS among MnFe 2 O 4 /MX explains its best catalytic activity. The catalytic degradation occurs by the following three ways. First, the radical-induced oxidation is attained by surface-bound SO 4 − and OH on MnFe 2 O 4 nanoclusters and hierarchical porous carbon nanosheets generated by one-electron reduction of PMS under the participating and coupling of Mn(III)/Mn(II), Fe(III)/Fe(II), O 2 / O 2 − , and active sites on carbon surface. Second, non-radical pathway involves the contribution of 1 O 2 , which is produced in a large quantity by promoted self-decomposition of PMS in presence of MnFe 2 O 4 /MS. Third, non-radical pathway is achieved through electron transfer from organic compounds as electron donator to PMS as electron acceptor mediated by graphitization structures. Taking into consideration the excellent degradation performance, easy magnetic separation, and bulk availability of MnFe 2 O 4 /MS, this work is expected to pave a new way for precision utilization of corn biomass-based biochar for environmental application.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Guangyu Wu,Wenlei Qin,Lei Sun,Xiangjuan Yuan,Dongsheng Xia
The enhancement performance, mechanisms and kinetic study of peroxymonosulfate (PMS) towards ozonation via prometon (PMT) degradation have been comprehensively investigated via the semi-continuous experiments in the present study. The removal of PMT (>97.34%) and the pseudo-first-order rate constant ( k = 0.6095 min −1 ) were achieved after 7 min reaction with 7.5 mg min −1 O 3 and 100 mg L −1 PMS at pH 6.5. Meanwhile, the PMT degradation performance was systematically evaluated in terms of inlet O 3 concentration, PMS dose, solution pH, water matrix species and etc . It was notable that pH played a significant role on the PMT degradation efficiency in O 3 /PMS process, especially under the neutral and alkaline conditions. The mechanism of the synergistic effect was subsequently explored by the radical scavengers and electron paramagnetic resonance experiments, confirming that both OH and SO 4 − were the dominant reactive radicals in O 3 /PMS process. In addition, the second-order rate constants of PMT with OH and SO 4 − were determined to be 1.9 × 10 9 M −1 s −1 and 1.7 × 10 9 M −1 s −1 via competition kinetics for the first time. Moreover, the plausible degradation pathways of PMT were elucidated based on the seventeen transformation by-products detected. Furthermore, a modified kinetic model was put forward to quantify the relative contribution of OH and SO 4 − , in order to accurately predict the degradation rate of PMT in O 3 /PMS process. This investigation could provide a promising alternative in developing more efficient O 3 -based advanced oxidation process and supply a feasible approach for water decontamination.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Jinhong Fan,Hehe Qin,Simin Jiang
Peroxymonosulfate (PMS) is an alternative to hydrogen peroxide in advanced oxidation processes. Herein, we present a simple one-pot synthetic approach for the Mn-doped graphite phase carbon nitride (g-C 3 N 4 ) materials and make it as a catalyst to activate PMS for acetaminophen (ACT) degradation. Fabricated Mn-g-C 3 N 4 composites (MnCN) were characterized by SEM, EDS, XRD, XPS, and FTIR. Results showed that Mn was uniformly dispersed in the structure of g-C 3 N 4 mostly in the form of Mn-N coordination. The effects of pH, contents of doped Mn, catalyst dosage, and reusability of catalyst and corresponding kinetic study were conducted to determine the catalytic performance of MnCN. High reaction efficiency was obtained in a wide pH range of 3.2–9. 100% removal of ACT in 15 min under optimized conditions with initial pH 6.5, 0.8 g/L of PMS and 200 mg/L of catalyst of 0.5-MnCN. Additionally, the reaction mechanism of the PMS/MnCN system was investigated using the electron spin resonance technique, quenching studies as well as different organics with electron-donating or electron-withdrawing groups. No PMS decomposition was detected without substrates. No inhibition effect by ethanol or tert -Butyl alcohol and complete inhibition effect by benzoquinone and partly by furfuryl alcohol, as well as ESR spectrum of TEMP- 1 O 2 were observed, suggesting that the activation of PMS proceeded in a new way, which is different from traditional sulfate radical-based advanced oxidation processes. A possible mechanism was proposed for ACT removal. PMS was first bounded to Mn-N sites to generate the superoxide anion. Then singlet oxygen produced by superoxide anion would react with ACT by replacing the electron-donating group of acylamino.
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WATER RESEARCH
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2018
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IF 7.051
Yueping Bao,Wen-Da Oh,Teik-Thye Lim,Rong Wang,Richard David Webster,Xiao Hu
In this work, nano-bimetallic Co/Fe oxides with different stoichiometric Co/Fe ratios were prepared using a novel one-step solution combustion method. The nano-bimetallic Co/Fe oxides were used for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation. The stoichiometric efficiencies of the as-prepared nano-bimetallic catalysts were calculated and compared for the first time. The radical generation was identified by electron paramagnetic resonance (EPR) as well as chemical quenching experiments, in which different scavengers were used and compared. The catalytic PMS activation mechanism in the presence of catalyst was examined by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that besides SO 4 • - and •OH, •OOH was also detected in the PMS/CoFeO 2.5 system. Meanwhile, in addition to the previously proposed radical oxidation pathway, the results showed that SMX degradation also involved a non-radical oxidation, which could be verified by the degradation experiment without catalyst as well as the detection of 1 O 2 . In the PMS activation process, cobalt functioned as the active site on CoFeO 2.5 while Fe oxide functioned as the adsorption site. The electron transfer mechanism was proposed based on the XPS and metal leaching results. Additionally, via the detection of transformation products , different SMX transformation pathways involving nitration, hydroxylation and hydrolysis in the PMS/CoFeO 2.5 system were proposed.
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