JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2020
·Vol. 31
·期 6
·4797-4807
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IF 2.22
Lyu Cong,Ju Lunan,Yang Xuejiao,Song Lan,Liu Ning
Iron-based catalysts as peroxymonosulfate (PMS) activator are commonly used to oxidize and degrade azo dye. However, there are still some issues such as low catalytic performance, relatively less reactive oxygen species and high metal iron dissolution. As such, a novel iron oxyhydroxide (FeOOHs) with four crystal form was synthesized and employed as efficient PMS activator for AO7 degradation in this study. It was found that the crystal form of catalyst had significant influence on its catalytic performance. β -FeOOH exhibited the best catalytic performance, owing to its smallest lattice size, maximum specific surface area and highest surface hydroxyl density. β -FeOOH/PMS system possessed a great high apparent reaction rate constant (1.3919 h −1 ), which was about 17, 3, 31, 20, 14, 49 and 23 times higher than that in β -FeOOH/persulfate(PS), Fe 0 /PMS, Fe 0 /PS, Fe 2 O 3 /PMS, Fe 2 O 3 /PS, Fe 3 O 4 /PMS and Fe 3 O 4 /PS system, respectively. More importantly, radical quenching tests and Electron spin resonance (ESR) analysis revealed that OH . , SO 4 .− , O 2 .− and 1 O 2 were involved in the reaction process. The catalytic mechanism proposed that β -FeOOH had the effective electron transfer rate performance, and Fe 3+ underwent a reduction to Fe 2+ during the β -FeOOH/PMS catalytic oxidation process. Then, the regeneration of Fe 2+ on the hydroxylated surface of FeOOH promoted the formation of FeOH + , which was crucial for PMS activation and reactive oxygen species (ROS) generation. The recyclability tests proved good stability and reusability of β -FeOOH. This study provides a kind of new understanding of peroxymonosulfate activation for environmental remediation and advances the study of iron-based oxyhydroxide in heterogeneous catalysis.
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ACS Biomaterials Science & Engineering
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2020
·
IF 4.152
Guangchao Xie,Liang Zhang,Jinbin Pan,Xuejun Zhang,Shao-Kai Sun
Photothermal agents with good biocompatibility, high tumor accumulation efficiency, large-scale production ability, and low cost are crucial for potential photothermal treatment in clinic. Herein, we proposed a green and highly efficient strategy to fabricate a kilogram-scale alginate-Ca2+-Fe powder hydrogel (ALG-Ca2+-Fe) by turning commercial Fe powder into hydrogel for enhanced photothermal therapy. The ALG-Ca2+-Fe was formed by simply dispersing commercial Fe powder into the preformed alginate-Ca2+ hydrogel in a green and energy-/time-saving way. The hydrogel exhibited the advantages of ultrahigh loading capacity of Fe powder (>100 mg mL–1), excellent large-scale production capacity (>1 kg in lab synthesis), low cost (<1.7 $/kg), and good injectability. More importantly, large size and hydrophobicity endowed Fe powder with excellent tumor retention effect and minimal diffusion to surrounding tissues, greatly benefiting improving treatment efficiency and reducing side effects. In vivo and in vitro studies both proved that the large-scale produced ALG-Ca2+-Fe can be used for highly efficient and biosafe tumor treatment in vivo by simple noninvasive injection. The developed ALG-Ca2+-Fe with multiple superiors opens up a novel green way to develop efficient and safe photothermal therapeutic agents with great clinic transformation potential.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Wei Li,Yongli Zhang,Pingju Zhao,Peng Zhou,Yang Liu,Xin Cheng,Jingquan Wang,Bo Yang,Hongguang Guo
Advanced oxidation processes (AOPs) based on the bimetallic system has been demonstrated as a promising way to enhance the degradation of pollutants in the water. In this study, the degradation of Rhodamine B (RhB) in a zero-valent iron (ZVI)/ peroxymonosulfate system with Cu 2+ was thoroughly investigated. RhB could be efficiently removed (99.3 %) in the optimal ZVI/PMS/Cu 2+ system, while only 58.2 % of RhB could be degraded in the ZVI/PMS system. The influence of reaction parameters on the degradation of RhB was further investigated. Quenching experiments and electron paramagnetic resonance (EPR) tests revealed that various reactive oxygen species could be generated in the ternary system, of which, 1 O 2 and O 2 − were identified for the first time. The effect of various anions, NOM and different water matrix were also considered at different concentrations. A variety of byproducts and degradation pathways were identified using HPLC/MS/MS. Finally, the Quantitative Structure Activity Relationship (QSAR) method of Toxicity Estimation Software Tool (TEST) was applied to estimate the toxicity of the byproducts and the results indicated that the overall toxicity of the target was relatively reduced. This study demonstrated the potential for the removal of environmental reluctant pollutants in water via the combined radical and non-radical pathways.
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ENVIRONMENTAL POLLUTION
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2020
·
IF 6.793
Shanshan Deng,Yixiang Bao,Giovanni Cagnetta,Jun Huang,Gang Yu
Perfluorohexane sulfonate (PFHxS) has been newly recommended to be added into the Stockholm Convention on persistent organic pollutants (POPs). As one of the major perfluoroalkyl pollutants, its long half-time in human serum and neurotoxicity are cause for significant concern. Although mechanochemical degradation has been evaluated as a promising ecofriendly technology to treat pollutants, the extraordinary stability of poly- and perfluoroalkyl substances (PFASs) raises harsh requirements for co-milling reagents. In the present study, zero-valent iron (ZVI) and ferrate(VI) were for the first time used as the co-milling reagents to degrade PFHxS. When ZVI and ferrate(VI) were used alone, both the degradation and defluorination efficiencies were low. However, after milling at the optimum ratio (ferrate(VI):ZVI = 1:2) for 4 h, the synergistic effect of ZVI and ferrate(VI) resulted in almost complete degradation (100%) and defluorination (95%). Two points can account for this excellent performance: (1) the mechanochemical energy input in the system initiates and prominently promotes related reactions; and (2) the active species generated from the reactions among ZVI, ferrate(VI) and other high-valent iron species will accelerate the process of electron transfer . The sulfonate group comprises the favorable attack sites, as corroborated by both the identified intermediates and quantum chemical calculations. The homolysis of the C–S bond is not only the triggering step, but also the rate-limiting step. In summary, the present work confirms the feasibility and underlying mechanism of the ZVI–ferrate(VI) co-milling system to defluorinate PFHxS, which might be a promising technology to treat PFASs in solid wastes.
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JOURNAL OF MOLECULAR LIQUIDS
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2020
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IF 5.065
Xiaojie Liu,Chunying Zhu,Taotao Fu,Youguang Ma
The densities and viscosities of ternary solution of piperazine (PZ) + 2-Amino-2-methyl-1-propanol (AMP) + H 2 O were measured at P = 101 kPa and T = (303.15–343.15) K. The effects of temperature and concentration on the density and viscosity of ternary solution were investigated. The apparent molar volume ( V φ ), the limiting partial molar volume ( V φ 0 ), viscosity B -coefficient, Helper's constant and the free energies of activation per mole of solvent ( Δμ 1 0≠ ) and solute ( Δμ 2 0≠ ) were calculated from the density and viscosity, respectively. The solute-solute and solvent-solute interactions were analyzed from the volumetric and viscometric properties. The results show that the PZ has a destructive effect on the structure of mixed solvent.
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RSC Advances
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2020
·Vol. 10
·期 7
·4148-4155
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IF 3.119
Hong Huang,Guoshuai Liu,Xiuheng Wang
Bromate (BrO3−) is a carcinogenic and genotoxic by-product of the ozone disinfection process. In this study, a new zero-valent metal, bismuth, was used to reduce bromate. Bismuth samples were prepared by a solvothermal method and characterized by powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The morphology of the bismuth powder was microspheres assembled with dense nanosheets. The kinetics of the direct bromate reduction by bismuth accorded with the pseudo-first-order kinetics model. The rate coefficients of the initial bromate concentration of 1.00 mg L−1, 2.50 mg L−1, 5.00 mg L−1 were identically close to 0.08 min−1. For 0.20 mg L−1, a reaction rate coefficient near 0.10 min−1 was obtained. The reducing products of bromate included bromide ions (Br−) and bismuth oxybromides. The bromate removal efficiency was enhanced remarkably in the presence of ultraviolet (UV) light, and the corresponding kinetic coefficient was 4 times higher than that of direct reduction. The mechanism of ultraviolet enhancement was analyzed by diffuse reflectance spectroscopy (DRS), the density functional theory (DFT) calculation, open circuit potential (OCP) analysis, photocurrent measurement and linear sweep voltammetry (LSV). Besides, the influence of dissolved oxygen (DO) on bromate reduction efficiency and the sustainability of the as-prepared sample were investigated. DO inhibited the reduction rate obviously, but showed a slight effect on the formation of bromide ions. In the long-term periodic experiments, the kinetic coefficient decay occurred in both direct (without UV irradiation) and ultraviolet assisted bromate reduction. However, the kinetic coefficient of UV-assisted reduction (0.115 min−1) was about 2 times higher than that of the direct reduction in the last cycle of periodic experiments. In conclusion, the novel bromate reduction strategy based on the zero-valent bismuth metal material has been proved efficient and sustainable, which contributes to the development of drinking water treatment technologies.
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TRIBOLOGY INTERNATIONAL
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2021
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IF 4.872
Jian Wu,Yanlong Luo,Yifeng Chen,Xiaohua Lu,Xin Feng,Ningzhong Bao,Yijun Shi
Ionic liquids (ILs) are very potential lubricant additives for their strong adsorption and tribochemical reactions at the interface. In this work, poly(ionic liquid) of PImC 6 NTf 2 is used as lubricant additive in base oil of PEG, which can reduce the wear volume by around 65 times under 2.5 GPa. The lubricity is much more advantageous than the geminal dicationic IL of BIm 5 -(NTf 2 ) 2 . The adsorption strength of lubricants is studied by employing the microcalorimeter to evaluate the adsorption heat, AFM to test the adhesion force, and molecular dynamics simulation to calculate the interfacial binding energy. As a result, the adsorption strength of PImC 6 NTf 2 is obviously higher than BIm 5 -(NTf 2 ) 2 , and the lubricity is strongly dependent on the adsorption strength of ILs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Xiaoming Wang,Qianqian Peng,Xilin Zhang,Xucheng Lv,Xin Wang,Yongzhu Fu
Refractory high-entropy alloy nanocomposites (HEA-NPs) are important class of materials with unique structure and potential applications. Although several synthetic methods have been reported, developing novel routes to prepare nanoscale HEA-based catalysts facilely is still urgently desired. This work takes advantage of confinement assisted arc and plasma shock (APS) to prepare a series of HEA-NPs by regulating the type and proportion of metal precursors. The phase constitutes and morphology of the HEA-NPs are fully characterized. The prepared refractory HEA-NPs possesses five highly dispersed metal components, including titanium (Ti), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo) and simultaneously exhibits an uniform hexagonal morphology of nanocrystals . By taking advantage of its unique corrosion resistance , TiNbTaCrMo HEA-NPs can function as a promising candidate for electrocatalytic hydrogen evolution reaction (HER) in natural seawater . And its catalytic performance after alloying is significantly enhanced compared with the elemental metal. Theoretically, the promoted HER activity can be attributed to the strong adsorption for the various metal components in HEA-NPs caused by the upshifting d -band center close to the Fermi level . Furthermore, this confinement strategy can be further extended to synthesize other HEA-NPs. Our strategy provides a novel method to synthesize various HEA-NPs for further catalytic application.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Gaihong Wang,Lina Qian,Xiaoyu Yong,Yajun Wang,Wei An,Honghua Jia,Jun Zhou
Oil refineries produce a variety of relatively intricate and biodegradable wastewater streams. A ternary micro-electrolysis filler (iron (Fe)-biochar (BC)-copper (Cu)) was synthesized using BC produced from waste Lycium barbarum L. branches by high-temperature anaerobic calcination, and was then used to treat oil refinery water. To evaluate the applicability of Fe-BC-Cu, the effects of various reaction parameters, including the initial pH of wastewater, Fe-BC ratio, and Fe-BC-Cu ratio, were investigated. A comparative study was conducted using three different kinds of fillers (BC, Fe-BC, and Fe-BC-Cu) to determine the reaction behavior, which was characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) surface area analysis, scanning electron microscopy (SEM), energy dispersive spectrometry (EDS), and EDS mapping. The results of batch studies revealed that the maximum chemical oxygen demand (COD) and total organic carbon (TOC) removal efficiency was 77.11% and 68.71%, respectively, under the optimal conditions of an initial wastewater pH of 4.0, Fe-BC ratio of 1:1, and Fe-BC-Cu ratio of 1:1:1. The reusability of the Fe-BC-Cu filler was measured to ensure that the COD removal efficiency was maintained at around 80% during 10 cycles. The results of a heavy metal analysis of the effluent indicated that the application of the Fe-BC-Cu filler in wastewater treatment presented no risk of heavy metal release. The microscopic ball-shaped structure revealed by SEM facilitated a suitable micro-electrolysis reaction rate. The removal mechanism of organic pollutants in the wastewater by the Fe-BC-Cu micro-electrolysis filler could be due to the synergistic effects of electrochemical oxidation, adsorption, and coprecipitation of iron hydroxides. The extraordinary performance of the Fe-BC-Cu micro-electrolysis filler for organic pollutant removal indicated its practical potential for industrial applications.
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RENEWABLE ENERGY
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2021
·
IF 8.001
Wenjing Tian,Jianhao Li,Lirong Zhu,Wen Li,Linyan He,Li Gu,Rui Deng,Dezhi Shi,Hongxiang Chai,Meng Gao
Recent investigations verified CaO 2 accelerated hydrolysis of lignocellulose, but its residue caused a harmful oxidizing environment. This study therefore proposed the combined CaO 2 pretreatment and zero-valent iron (ZVI) addition to enhance high-solid anaerobic digestion of wheat straw, trying to eliminate negative effect of residual oxides . Effects of CaO 2 pretreatment without/with ZVI addition on digestion performance were investigated. Results showed that in non-ZVI added digesters, as CaO 2 dosage increased, total production of SCOD and VFAs increased linearly, while activities of coenzyme F 420 and electron transport system were negatively correlated. Pretreatment using appropriate CaO 2 dosage indirectly increased biogas production by promoting hydrolysis and acidification. Comparably, initial ORP in ZVI-added digesters sharply declined below −350 mV, which was suitable for methanogen growth. ZVI significantly improved activities of cellulase , hemicellulase , acetic kinase and coenzyme F 420 , with the highest improvement percentages of 138%, 48%, 35% and 58%, respectively. Since ZVI could provide electrons for conversion of CO 2 to CH 4 , compared with non-ZVI added digesters (R0-R4), methane content in ZVI-added digesters (RZ0-RZ4) increased by 8.1%, 9.0%, 11.2%, 17.0% and 18.0% successively. Consequently, 0.6 g/g VS CaO 2 pretreatment combined with 0.4 g/g VS ZVI addition achieved the maximum methane production, increasing by 35.6% compared to control digester.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yang Zong,Hua Zhang,Yufei Shao,Wenjie Ji,Yunqiao Zeng,Longqian Xu,Deli Wu
Periodate (PI)-based advanced oxidation processes have recently received increasing attentions. Herein, PI was readily activated by nano zero-valent iron (nZVI) and subsequently led to the enhanced oxidation of organic contaminants , with the removal performance of sulfadiazine (SDZ) in the nZVI/PI process even higher than that in the nZVI/peroxydisulfate process under identical conditions. Kinetic experiments indicated that the decay of SDZ was susceptible to the dosage of nZVI and PI, but was barely affected by pH values (4.0–7.0) under buffered conditions, suggesting the promising performance of the nZVI/PI process in a relatively wide pH range. Selective degradation of contaminants and 18 O-isotope labeling assays collectively demonstrated that iodate radical ( • IO 3 ), high-valent iron-oxo species (Fe(IV)) and hydroxyl radical ( • OH) were responsible for the abatement of organic contaminants . More importantly, due to the relatively weak steric hindrance effect of PI, PI easily adsorbed on the surface of nZVI and no iron leaching was detected throughout the reaction, implying that PI activation induced by nZVI was a surface-mediated process. Besides, PI was not transformed into harmful reactive iodine species. This study proposed an environmental-friendly approach for PI activation and shed new lights on the PI-based processes.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Shuang Zhang,Yuanyuan Ren,Xinxin Ma,Weijie Guan,Ming Gao,Yu-You Li,Qunhui Wang,Chuanfu Wu
To solve the problem of acidification during high-load anaerobic digestion of food waste, the effects of adding Fe 0 on acidified fermentation system were investigated. Four adding Fe 0 groups and four control groups were set under different inoculum-to-substrate ratios (ISRs) of 1.00, 0.80, 0.65, and 0.50. Results showed that adding Fe 0 significantly increased methane production, except for the over-acidification group under ISR= 0.5. As for the control groups, the pH of system decreased to below 5.8 with the decrease of ISR, which led to the instability of the system and the stop of gas production. Compared with the control groups, pH recovered faster and the concentration of volatile fatty acids was lower with Fe 0 addition under the same ISR. Moreover, in the Fe 0 group under ISR= 0.65, the pH recovery effect was the most obvious and microbial-community analysis showed that the relative abundance of Clostridium increased by 14.9%. As a result, the best recovery effect was obtained by adding Fe 0 under ISR= 0.65, and the cumulative CH 4 yield increased by 77.3% compared with the control group. Therefore, adding Fe 0 to the acidified fermentation system can effectively alleviate acidification and thus increase methane production when ISR > 0.5.
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