ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Shichao Cai,Yurou Tan,Hongyi Li,Liwei Yang,Bo Chen,Feng He
Zero-valent iron (ZVI, Fe0) can effectively reduce a variety of chlorinated hydrocarbons. However, ZVI is incapable of dechlorinating 1,2-dichloroethane (1,2-DCA), a commonly found contaminant in groundwater, and the existing ZVI modification methods have little effect on this predicament. In this study, we prepared ZVI composites modified with Fe–N4 coordination structure (Fe0@FeNC), which exhibited outstanding dechlorination performance toward 1,2-DCA. Fe0@FeNC (1 g/L) can degrade 94% of 1,2-DCA (10 mg/L) within 37 days, with an ethene selectivity of nearly 100%, whereas nanoscale ZVI (nZVI) or even Pd-doped nZVI and sulfidated ZVI cannot degrade 1,2-DCA. The results from X-ray diffraction patterns and Mössbauer spectra confirmed the presence of Fe0 and Fe–N4 coordination structure in the Fe0@FeNC, which were proven to be the electron donor and dechlorination active center for 1,2-DCA dechlorination, respectively. Theoretical calculation reveals that the Fe–N4 coordination structure can reduce the free energy required for 1,2-DCA reduction, thus allowing 1,2-DCA to utilize electrons provided by Fe0 to achieve dechlorination. These findings can guide the design of ZVI-based materials to achieve in situ abiotic remediation of 1,2-DCA-contaminated groundwater.
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Youyou Feng,Jing Qin,Yu Zhou,Qin Yue,Jing Wei
Nanozyme has been regarded as an efficient antibiotic to kill bacteria using the reactive oxygen species (ROS) generated by Fenton-like reaction. However, its activity is still unsatisfied and requires large amount of hydrogen peroxide with side effects toward normal tissues. Herein, spherical mesoporous Fe-N-C single-atom nanozyme (SAzyme) is designed for antibacterial therapy via photothermal treatment enhanced Fenton-like catalysis process. Due to the large pore size (4.0 nm), high specific surface area (413.9 m 2 g −1 ) and uniform diameter (100 nm), the catalytic performance of Fe-N-C SAzyme is greatly improved. The Michaelis-Menten constant ( K m ) is 4.84 mmol L −1 , which is similar with that of horseradish peroxidase (3.7 mmol L −1 ). Moreover, mesoporous Fe-N-C SAzyme shows high photothermal conversion efficiency (23.3 %) owing to the carbon framework. The catalytic activity can be enhanced under light irradiation due to the elevated reaction temperature. The bacteria can also be killed via physical heat effect. Due to the synergistic effect of nanozyme catalysis and photothermal treatment, the antibacterial performance is much higher than that using single antibacterial method. This work provides an alternative for combined antibacterial treatment via photothermal treatment assisted catalytic process using spherical mesoporous single-atom nanozyme as an antibiotic.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
MIL-100(Fe) has been proven to have good hydrothermal stability and high vapor uptake and is considered as a promising dehumidification material. However, reduction of the production cost and assembly of the adsorbent and glass fiber paper substrate into the MIL-100(Fe) monolith are challenging. This work presented a dry gel conversion strategy for the rapid synthesis of the MIL-100(Fe) monolith at low temperatures. The porosity and crystalline phase of the products obtained under different crystallization temperatures and times were carefully studied. XRD and SEM characterization indicated that the MIL-100(Fe) crystal could be conveniently synthesized on the substrate at a low temperature of 50–70 °C and in a short time of 2–6 h. The spherical particles assembled from crystals dispersed evenly and tightly on the glass fiber paper. The synthesized MIL-100(Fe) monolith had a thickness of about 270 μm and a MIL-100(Fe) loading of 77.7%. Dynamic and static water vapor adsorption tests revealed that the monolithic adsorbent obtained at 50 °C for 6 h had the largest vapor saturation adsorption capacity (0.581 g/g) and the fastest adsorption rate. Moreover, the monolith owned a low regeneration temperature (below 80 °C) and a satisfactory cycle stability. Convenient equipment, mild synthetic conditions, low renewable energy consumption, and good performance will promote its application in the rotary dehumidification system.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 6
·9421-9432
·
IF 0
Che Mingda,Su Hongjian,Si Huimin,Guo Bin,Huang Renliang,Zhao Jing,Su Rongxin
As the representative volatile chlorinated hydrocarbons detected in wastewater, the removal of composite chlorinated ethenes is a major challenge in wastewater treatment. In the present study, an efficient removal system for composite chlorinated ethenes was reported, in which gallic acid was used to enhance the activation of persulfate by Fe/Ni nanoparticles. The influences of gallic acid-Fe/Ni and persulfate concentrations, initial pH value, reaction temperature, inorganic anions, and natural organic matters were evaluated in the composite chlorinated ethenes removal. Our results showed that the gallic acid-Fe/Ni-persulfate system with 9.0 mM of gallic acid-Fe/Ni and 30.0 mM of persulfate yielded about 100% trichloroethylene removal and 97.3%-98.6% perchloroethylene removal in the pH range of 3.0–12.0. Electron paramagnetic resonance analysis and radical quenching experiments indicated that SO 4 •− and • OH were the predominant radical species under acidic and alkaline conditions. Ultraviolet visible spectroscopy and inductively coupled plasma optical emission spectrometer tests revealed the Fe-gallic acid chelation could regulate the concentration of iron ions and improve the reactivity of gallic acid-Fe/Ni. These results demonstrated that the gallic acid-Fe/Ni-persulfate system was a promising strategy for treating composite chlorinated ethenes-containing wastewater.
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DOI
PubMed
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Hang Cui,Xiaogang Gu,Shuguang Lu,Xiaori Fu,Xiang Zhang,George Y. Fu,Zhaofu Qiu,Qian Sui
Ethylbenzene (EB) degradation performance in (S,S)-ethylenediamine-N,N-disuccinic acid (EDDS) chelated Fe(III) activated sodium percarbonate (SPC) system was investigated in this study. The effects of various factors, such as the dosages of SPC and Fe(III), molar ratio of EDDS/Fe(III), anions (Cl − , HCO 3 − , SO 4 2− , and NO 3 − ) concentration, natural organic matters (NOM), and initial solution pH were evaluated. The results showed that the addition of EDDS remarkably improved the EB removal in Fe(III)/SPC system. Both HCO 3 − anions and NOM had significantly inhibitive effect, while the influence of SO 4 2− , Cl − and NO 3 − could be negligible on EB degradation. The EB removal was inhibited at extremely low and high initial solution pH. Moreover, the results of free radical probe tests, scavenger tests and electron paramagnetic resonance (EPR) detection indicated that OH was the predominant species responsible for EB degradation even though both OH and O 2 − were generated in the SPC/EDDS–Fe(III) system. The oxidation products were analyzed and possible EB degradation pathways were proposed. In conclusion, this study provides an important insight into the application of SPC/EDDS–Fe(III) system in the removal of EB contaminant, especially for in situ remediation of BTEX-contaminated groundwater.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Hao Chen,Chaofang Li,Jing Yuan,Ding Bao,Fenghua Shen,Pingshan Wang,Xingzheng Dai,Zhanqing Lu,Kaisong Xiang,Hui Liu
The application of Fe-based ionic liquids (ILs) in elemental mercury (Hg 0 ) removal from flue gas is limited by the low oxidative activity of the Fe(III) center. Here, a strategy of engineering halogen ligand to enhance the oxidative activity of Fe-based ILs for mercury removal was proposed. We developed a series of ionic liquids [Bmim][FeCl 4-x Br x ] (x = 0–4) with varying ratios of Cl − and Br − ligand substitutions. Mercury removal performance evaluations demonstrated a positive correlation between the oxidative activity towards Hg 0 and the number of Br ligand substitutions in the ILs. [Bmim][FeBr 4 ] achieved ∼99 % removal efficiency in the temperature range of 50–150 °C, with a saturated adsorption capacity reaching 205.4 mg/g (at 150 °C). In-situ Raman spectroscopy, DFT calculations, Hg-TPD, and XPS collectively revealed that the introduction of Br significantly lowered the excitation energy of the ligand–metal p-d orbital electron transitions, which facilitates the generation of active bromine species with unfilled 4p orbital, consequently enhancing the oxidative removal performance of Fe-based ILs for Hg 0 . This work provides an application of metal-based ILs in the realm of mercury removal and broadens the scope of ligand–metal interaction for IL design.
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高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2020
·Vol. 647
·期 9
·1025-1030
·
IF 1.24
Yihan Wang,Hu Zhou,Jinghao Xiao,Aihua Yuan
Metal selenides as anode materials of lithium-ion batteries (LIBs) has received considerable attention recently. In order to boost the electronic conductivity and alleviate the volume change of electrode materials upon the cycles, a facile strategy is employed in this work, where Prussian blue analogue (PBA) nanocubes are encapsulated into three-dimensional (3D) network of graphene aerogel (GA), followed by a high-temperature selenization treatment to isolate the composite of FeCoSe 2 @GA. The composite can be directly employed as free-standing anode materials of LIBs. Studies reveal that the FeCoSe 2 @GA electrode demonstrates an intriguing cycle stability and rate capability with a specific capacity of ∼500 mAh g −1 at 100 mA g −1 after 100 cycles. The outstanding lithium-storage properties can be attributed to the 3D porous feature as well as the strong confinement effect of GA for FeCoSe 2 particles, which provides a large number of ion-exchange channels, and prevents the severe agglomeration and large volume expansion of active particles during the charge/discharge process.
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高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Hongyan Lu,Ying Li,Yan Zheng,Chenchen Dong,Yukun Li,Fanzhang Meng,Yong Wang,Chao Teng,Xiaoliang Wang,Dongshan Zhou,Gi Xue
Rechargeable aluminum-ion batteries (AIBs) are promising candidates for energy storage because of their low cost, high safety, and high-power density owing to the three-electron redox reaction . However, the applications of AIBs are hindered by their limited lifetime and practically achievable energy density . Herein, we present a novel Fe-doped Nickel selenide (Fe-NiSe) nanoflake cathode material , derived from a Ni–Fe layered double hydroxide , affording a long cycle life and high energy density . Synergism between the ultrafine nanostructure and Fe doping provided shorter ion diffusion pathways and created multiple active sites in the cathode. As a result, the prepared Fe–NiSe battery achieved an outstanding energy density of 402.5 W h kg −1 and an ultra-long lifespan of 13,500 cycles with a capacity decay of only 0.0026% per cycle. Furthermore, based on the mass of the entire pouch-type cell, the fabricated AIB delivered an energy density of 101.2 W h kg −1 . This work paves the way for serviceable high-energy density AIBs.
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高影响因子
ECS Journal of Solid State Science and Technology
·
2020
·Vol. 9
·期 12
·123007
·
IF 2.142
Guodong Zhang,Jiaqi Chen,Yao Liu
Iron-based soft magnetic composites (SMCs) were prepared by two-step ball milling with sodium silicate and ferroferric oxide. The presence of the precoated silicate layer has increased the resistivity of the powder surface, which also improved the agglomeration of ferroferric oxide. The addition of magnetic ferroferric oxide improves the dilution effect. Combining the advantages of both sodium silicate and ferroferric oxide, the prepared soft magnetic composite material has excellent performance. After annealing at 400 °C, the core loss is 214.5 W Kg−1 (1 T, 1000 Hz), and the saturation magnetic induction is 1.33 T.
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高影响因子
Water Supply
·
2022
·Vol. 22
·期 5
·5589-5602
·
IF 1.768
Lu Zhanpeng,Zeng Guilu,Zhou Zhengyuan,Liu Yulong,Wang Peng,Sheng Xianxian,Dong Jiaqi,Idress Ayesha,Sui Qian,Lyu Shuguang
As a kind of refractory chlorinated hydrocarbon, 1,2-dichloroethane (1,2-DCA) has been frequently detected in contaminated groundwater, and it is hard for common technology to degrade it due to its stability. Moreover, the existence of 1,2-DCA can do harm to human organs. Hence, it is urgent to develop an effective technology for the remediation of 1,2-DCA-contaminated groundwater. In this study, a calcium peroxide (CaO 2 ) system activated by Fe(III) was applied to the degradation of 1,2-DCA and 83.3% of 1,2-DCA could be effectively removed within 3 h when the molar ratio of CaO 2 /Fe(III)/1,2-DCA was 30/120/1. The results of probe experiments, electron paramagnetic resonance (EPR) detection, and scavenging tests demonstrated that both HO • and O 2 −• were the key factors for 1,2-DCA degradation. The released amount of Cl − (84.1%) revealed that most of the chlorine in 1,2-DCA could be dechlorinated. GC-MS was applied for the detection of intermediates during 1,2-DCA degradation and the possible degradation pathway was proposed that 1,2-DCA was first reduced to vinyl chloride (VC) and then oxidized to CO 2 and H 2 O. Finally, 73.4% removal of 1,2-DCA could be achieved in actual groundwater when the molar ratio of CaO 2 /Fe(III)/1,2-DCA was 100/400/1, demonstrating that the CaO 2 /Fe(III) system has a remarkable prospect in 1,2-DCA-contaminated groundwater remediation. Efficient degradation of 1,2-DCA in the CaO 2 /Fe(III) system was achieved. HO • and O 2 –• were the key factors for 1,2-DCA removal in the CaO 2 /Fe(III) system. The possible degradation pathway of 1,2-DCA was proposed. The effect of water matrices on 1,2-DCA degradation in the CaO 2 /Fe(III) system was investigated.
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高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Hui Huang,Bin Huang,Yichun Huang,Jinbei Yang,Yinnv Ye,Yucheng Chen
Attractive environmentally friendly magnetic metal-organic framework (MOF) nanocomposite GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) was synthesized by a solvothermal method and characterized by X-ray diffraction, Fourier transform infrared, scanning electron microscopy, Brunauer– Emmett–Teller, and vibrating sample magnetometer, and used as an effective adsorbent for the removal of orange G from aqueous solution. The various operating parameters that effect the adsorption process, such as adsorbent dosage (0.01–0.2 g), pH (1.0–10.0), initial concentration (50–400 mg L –1 ), and temperature (298.15–318.15 K) were studied. The percent removal of orange G increases with the increment of the adsorbent dosage and decrease of the initial concentration, and the optimum pH is 6.0. The Redlich–Peterson model can be favorably applied to describe the adsorption equilibrium data, indicating that the surfaces of GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) nanocomposite for the orange G adsorption are made up of homogeneous adsorption patches. The adsorption kinetics indicate that the adsorption process of GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) toward orange G obeys the pseudo-second-order model and the activation energy is 16.5 kJ mol –1 . Thermodynamic parameters, ΔH = 39.81 kJ mol –1 , ΔS = –46.80 J mol –1 K –1 , and ΔG < 0, exhibit that the adsorption is exothermic and spontaneous. The maximum adsorption capacity of orange G onto GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) nanocomposite is 128.8 mg g –1 . Therefore, magnetic GO@ Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) nanocomposite can be employed as an environmentally friendly and efficient adsorbent for the orange G removal from wastewater.
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高影响因子
NANOTECHNOLOGY
·
2019
·Vol. 30
·期 30
·305402
·
IF 3.399
Tong Wu,Yaying Li,Yuntong Li,Jing Hong,Haiyang Wu,Jie Mao,Yuzhe Wu,Qipeng Cai,Conghui Yuan,Lizong Dai
Simultaneous introduction of both transition metal and other inorganic elements into the carbon matrix has attracted great attention in the fabrication of carbon materials with high electrochemical properties. Herein, rational design of ligand-iron coordinative supramolecular precursors is achieved for the fabrication of Fe-N/C catalysts, which possess high oxygen reduction reaction (ORR) performance. A series of precursors are prepared by a simple coordination reaction between a three armed catechol monomer and iron ions. Particular interest is focused on tuning the doping species, surface area and morphology of the Fe-N/C catalysts through a simple selection of iron resources. We show that an Fe-N/C catalyst derived from Fe2(SO4)3 at a carbonization temperature of 800 °C, has the optimized ORR performance with an onset potential of 0.930 V and half-wave potential of 0.801 V. Detailed investigation indicates that the synergistic effect among doping elements of nitrogen and sulfur and the unique carbon structure determines the performance of the Fe-N/C catalysts. Our findings may be of significance for the fabrication of doped carbon materials using coordinative supramolecular polymers as precursors.
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高影响因子
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