CHEMOSPHERE
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2019
·
IF 5.108
Hongbin Wang,Shixiang Wang,Yiqing Liu,Yongsheng Fu,Peng Wu,Gaofeng Zhou
As an emerging pollutant, Diclofenac (DCF) has potential threats to ecosystem and human health, and it can hardly be removed by conventional wastewater treatment processes . In this study, Fe(II)-activated bisulfite (BS), an advanced oxidation process , was used for rapid removal of DCF. The effect of initial pH, Fe(II) dosage, BS concentration, dissolved oxygen and reaction temperature on DCF removal and its degradation mechanism were investigated. Compared to Fe(II)/persulfate system, the removal efficiency of DCF was higher by Fe(II)/BS, and its degradation followed pseudo-first order kinetic model. Due to the morphology of Fe(II) and BS, the optimal pH for DCF degradation was 4.0. The increased initial Fe(II) or BS concentration promoted DCF degradation while excess Fe(II) or BS caused an inhibition effect as a SO 4 − scavenger. Dissolved oxygen was an essential factor inducing the conversion of SO 3 − to SO 4 − , while it had no effect on DCF removal in the range of 4.6–8.3 mg L −1 . The activation energy of this reaction was calculated to be 120.75 ± 3.43 kJ mol −1 based on the improved DCF degradation with increasing temperature. According to the radical scavenging experiments, the contribution of SO 4 − , HO and the other reactive species to DCF degradation in Fe(II)/BS system were 71.1%, 24.6% and 4.3%, respectively. Nine transformation products were detected using UPLC-Q-TOF-MS. The potential degradation mechanism of DCF was thus proposed showing five reaction pathways including hydroxylation, decarboxylation , dehydration, dechlorination and formylation.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Fuqin Zheng,Ziwei Zhang,Dong Xiang,Ping Li,Cheng Du,Zhihua Zhuang,Xiaokun Li,Wei Chen
Electrochemical water-splitting is an ideal strategy to produce the promising substitutable energy source, hydrogen (H 2 ). However, the sluggish kinetics of electrochemical oxygen evolution reaction (OER) and the prohibitive cost, low reserves and easy oxidation of noble metal-based electrocatalysts force researchers to explore efficient and low-cost electrocatalysts . Bimetal nanostructred materials are proved to have enhanced OER catalytic performances. In this study, a series of bimetallic metal-organic frameworks (Fe/Ni-MOFs) are prepared by a solvothermal method . The prepared MOFs present abundant unsaturated metal active sites for OER. The optimized Fe/Ni bimetal-MOF has low overpotentials of 236 mV at 10 mA cm −2 and 284 mV at 100 mA cm −2 for OER. In addition, in comparison with most of the previously reported OER electrocatalysts, the present MOF shows a lower Tafel slope of 49 mV dec −1 . Besides, the MOF catalyst exhibits high electrochemical stability and the OER activity shows a negligible change after stability test for 15 h and 10,000 voltammetric cycles. Meanwhile, the Fe-doped Ni-MOFs show faster catalytic kinetics and higher conductivity than the monometallic Ni-MOF. This work paves a way to exploit bi- or multi-metallic MOFs with high conductivities and electrocatalytic performances for electrochemical energy conversion .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Rong Chen,Hui Liu,Peng Zhang,Lei Zhao,Kang Ding,Songhu Yuan
Groundwater table fluctuation during natural and anthropogenic processes can facilitate the interaction between oxygen (O 2 ) from the unsaturated zone and ferrous iron (Fe 2+ ) from the saturated zone. In light of previous findings that Fe(III)-reducing bacteria can be killed by the reactive oxidants produced from Fe 2+ oxidation under static oxic conditions, we hypothesize that Fe(III)-reducing bacteria will be attenuated during groundwater table fluctuations. To test this hypothesis, this study explored the variations of cell numbers of Shewanella oneidensis strain MR-1 (MR-1), a typical strain of Fe(III)-reducing bacteria, together with dissolved oxygen (DO) and Fe 2+ , at different points during controlled groundwater table fluctuations in a sand column. The results showed that, during the rise of the water table, O 2 in the pore air was entrapped by the deoxygenated groundwater, and Fe 2+ in the groundwater was oxidized by the entrapped O 2 . In this process, 1.40–2.42 orders of magnitude of viable MR-1 cells were killed at different points in the column. Further investigation proposed that the death of MR-1 is caused by the production of intracellular reactive oxidants, such as O 2 • − and OH•, from the oxidation of adsorbed/absorbed Fe 2+ instead of by bulk reactive oxidants, such as OH• and Fe(IV), produced from the oxidation of aqueous Fe 2+ . The findings here provide new insights for Fe biogeochemical cycling in the redox-dynamic zone.
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Energy Storage Materials
·
2019
·
IF 0
Tao Dai,Lie Yang,Xiaohui Ning,Danli Zhang,R. Lakshmi Narayan,Ju Li,Zhiwei Shan
Due to their compactness, storage/supply flexibility, modularity and factory manufacturability, batteries are excellent candidates for large scale energy storage applications . However, the widespread application of most batteries hitherto developed is hindered by their high cost. Here, an intermediate temperature molten salt battery is developed that emphatically resolves this issue by using all earth-abundant and cheap elements. Operated at 170 °C, the cell comprises of an Fe metal anode, NaCl saturated NaAlCl 4 electrolyte and an AlCl 4 − intercalated graphite cathode in the fully charged state. It has a capacity retention of 85% after nearly 10,000 cycles. After characterizing the anode, it was determined that the high reversibility of the Fe to FeCl 2 solid state transformation are responsible for the absence of dendritic growth on such a metal anode. Different electrode capacity matching strategies are discussed in the context of ensuring safe operation during overcharging. Finally, the overall material cost of the Fe/Graphite cell is estimated to be 33.9 $ kWh −1 , which can potentially meet the demands of the commercial energy storage market.
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Advanced Materials Interfaces
·
2018
·Vol. 5
·期 8
·1701548
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IF 4.834
Lin Liu,Yang Yan,Zihe Cai,Shengxuan Lin,Xiaobin Hu
Metal–organic frameworks (MOFs) and graphene aerogels (GAs) are both considered as good candidates for high-performance supercapacitors. In this work, a growth-oriented Fe-based MOF synergized with GA composite for supercapacitor is prepared. MIL-88-Fe is in situ grown at (002) lattice plane on the surface of graphene via a one-step solvothermal method. Long periodic hexagonal structure and electrophilicity of MOF provide strong p–π interaction with graphene sheets. By utilizing the abundant interspace of GA, the existence of MOF could affect the electric double-layer characteristics of composites. The MOF/GA composites have the advantages of high capacitive volume, fast charge/discharge rate, and reliable cycling stability. The specific capacitance is as high as 353 F g −1 at the scan rate of 20 A g −1 , and the retention ratio is 74.4% after 10 000 cycles.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2018
·Vol. 29
·期 10
·8338-8346
·
IF 2.324
Song Kai,Ma Zizai,Yang Weiyou,Hou Huilin,Gao Fengmei
In the present work, we reported the fabrication of Fe-doped WO 3 nanofibers via a versatile electrospinning method towards efficient photoelectrochemical (PEC) water splitting. The resultant Fe-WO 3 nanofibers had a high purity in morphology, and the Fe doping levels within the WO 3 nanofibers were controlled in the range from 0.32 to 1.47 at.%, making the band gaps of WO 3 nanofibers tailored from 2.92 to 2.8 eV. The incorporated Fe dopants could not only increase the light absorption, but also improve the charge transport and charge transfer efficiencies, bringing an enhanced PEC activity of the WO 3 nanofiber photoanodes. The WO 3 nanofibers with the optimized 0.32 at.% Fe doping level exhibit the best PEC performance. The mechanism for the enhanced PEC behaviors was proposed.
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CATALYSIS TODAY
·
2018
·
IF 4.667
Yuexin Peng,Ling Zhang,Yiwen Jiang,Shichao Han,Qiuyan Zhu,Xiangju Meng,Feng-Shou Xiao
Catalytic combustion is considered as an efficient and economic technology to remove VOCs, and Al-ZSM-5 zeolite supported palladium catalysts (Pd/Al-ZSM-5) with good performances in this kind of reactions have been reported. In this work, it is found that Fe-ZSM-5 supported palladium catalyst (Pd/Fe-ZSM-5) exhibit higher catalytic activity in toluene combustion than the Pd/Al-ZSM-5, which is strongly related to more Pd 0 active species and higher concentration of absorbed oxygen species of Pd/Fe-ZSM-5 than those of Pd/Al-ZSM-5. More importantly, Pd/Fe-ZSM-5 has a good catalyst life and water-resistant ability, which should be potentially significant for practical applications in environment protection.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2018
·
IF 4.61
Xiaofei Li,Wenjing Zhang,Yunqi Qin,Tianyi Ma,Jingjing Zhou,Shanghai Du
To investigate the effect of different colloids on Fe migration in saturated porous media under different hydrochemical and hydrodynamic conditions, experiments were performed using colloidal silicon (inorganic) and colloidal humic acid (HA, organic), which are representative of the colloids in groundwater. Transport of Fe with and without colloid was investigated by column experiments using various porous media, colloid concentrations, ionic strengths (ISs), cation valences, and flow rates. The results show that colloidal silicon promotes and colloidal HA inhibits Fe transport, which is mainly because of their different bonding ratio, bonding modes with Fe and opposite surface charges between Fe–colloidal silicon and Fe–colloidal HA. Almost 100% of HA binds to Fe through the deprotonated functional groups, whereas only 13.3% of colloidal silicon binds to Fe, which is by electrostatic forces. Cotransport is also dependent on the hydrochemical and hydrodynamic conditions. For the Fe–colloidal silicon system, increasing the colloid concentration and flow rate, and decreasing the IS enhances Fe transport. Compared with colloidal silicon concentration = 10 mg/L, flow rate = 0.25 mL/min, and IS = 0.05 with CaCl 2 , a higher colloidal silicon concentration (20 mg/L), a higher flow rate (0.50 mL/min), and a lower IS (<0.0005 M) increase Fe recovery by 1.69%, 94.49% and 38.92%, respectively. Fe migration is also different in different porous media. For the Fe–colloidal HA system, Fe recovery decreases by 81.46% as the colloidal HA concentration increases from 0 to 20 mg/L. The type of porous medium and flow rate conditions have the same effects on Fe–colloidal HA transport as for colloidal silicon, although the electrical conditions have the opposite effect. With increasing IS, Fe–colloidal HA transport is enhanced because of competitive adsorption of the cations and Fe to colloidal HA and the porous medium.
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GEOCHIMICA ET COSMOCHIMICA ACTA
·
2018
·
IF 4.69
Tongxu Liu,Dandan Chen,Xiaobo Luo,Xiaomin Li,Fangbai Li
Redox reactions between iron and nitrogen drive the global biogeochemical cycles of these two elements and, concomitantly, change the fate of nutrients in and the mineralogy of the cycles. The microbially mediated NO 3 − -reducing Fe(II) oxidation process (NRFO) plays a key role in Fe/N interactions under neutral-anoxic conditions. Microbially mediated NRFO was considered a biological process, yet recently it has been documented that chemical mechanisms are also at play. However, the relative contributions of biological processes and chemical processes to Fe(II) oxidation remain largely unquantified owing to the co-occurrence of the reactions. Herein, the kinetics and secondary minerals of microbially mediated NRFO by Pseudogulbenkiania sp. strain 2002 and Acidovorax sp. strain BoFeN1 were investigated with acetate as electron donor unless otherwise stated. The results of Cells + NO 3 − suggested the two strains could biologically reduce NO 3 − to NO 3 − /NO x /N 2 O/N 2 and concomitantly oxidize acetate and result in cell growth. Fe(II) oxidation and NO 3 − reduction occurred simultaneously in the presence of Fe(II) (Cells + Fe(II) + NO 3 − ). For strain BoFeN1, the presence of Fe(II) slightly enhanced the NO 3 − reduction, acetate consumption, and cell growth, all of which were substantially retarded by Fe(II) for strain 2002. When compared with the microbial nitrite reduction, the relatively higher rate of chemical reaction between NO 2 − and dissolved Fe(II) confirmed the occurrence of chemodenitrification in the microbially mediated NRFO processes. After 5 days’ incubation, no green rust was observed, and lepidocrocite , goethite , and magnetite were observed with the Cells + Fe(II) + NO 3 − treatment, but only goethite was found with the Fe(II) + NO 2 − . The spectra for the EPSs + Fe(II) treatment suggested that the oxidized c -Cyts in the EPSs could oxidize Fe(II), which show the theoretical capability of taking electrons from Fe(II) into the cells via c -Cyts. A brief model was established by combining the verified reactions of (1) biological reduction of NO 3 − to NO 2 − /NO x /N 2 O/N 2 , (2) Fe(II) oxidation by NO 2 − , and (3) Fe(II) oxidation by c -Cyts in EPSs. Based on the model, the rate constant of Fe(II) oxidation by c -Cyts in EPSs was derived. For nitrite reduction, the relative contribution of biological processes to the nitrite reduction was higher than that of chemodenitrification. For Fe(II) oxidation, the relative contribution of the chemical process via nitrite to Fe(II) oxidation was higher than that of biological processes. These findings provide a quantitative interpretation of the chemodenitrification and biological reactions in the microbially mediated NRFO processes, which could assist the mechanistic understanding of the global biogeochemical cycles of iron and nitrogen in subsurface environments.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 32
·12186-12192
·
IF 4.052
Jiang-Yan Xue,Fei-Long Li,Zhong-Yin Zhao,Cong Li,Chun-Yan Ni,Hong-Wei Gu,Pierre Braunstein,Xiao-Qing Huang,Jian-Ping Lang
The development of bifunctional non-noble metal electrocatalysts demonstrating high activity and stability for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of great significance for renewable and clean energy. In this work, we report hierarchically structured integrated Fe–MoS2/Ni3S2/NF (NF = nickel foam) materials prepared by a facile in situ solvothermal method, and among them, the Fe-doped MoS2 was assembled into spine-like nanorods. The optimized electrocatalyst (denoted as Fe–MoS2/Ni3S2/NF-2) demonstrated excellent activity and durability for performing the HER and OER in an alkaline electrolyte (pH = 14) with low overpotentials of 130.6 mV and 256 mV (vs. RHE) at a current density of 10 mA cm−2, as well as no significant loss in catalytic performance even after 2000 cyclic voltammetry (CV) cycles. An outstanding durability of 180 h could be achieved for OER. The overall water splitting made up of the two-electrode system with Fe–MoS2/Ni3S2/NF-2 as both the anode and the cathode required a voltage of only 1.61 V to drive a current density of 10 mA cm−2 along with an outstanding long-term stability of 20 h, displaying its great potential for application in water splitting. The effective construction of multi-component synergistic structures shows a good pathway for high-performance electrocatalysis and energy storage.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Xiong Song,Suqing Wang,Guoping Chen,Tuo Gao,Yue Bao,Liang-Xin Ding,Haihui Wang
A novel lightweight, multi-functional layer comprised of 1D porous Fe-embedded nitrogen-doped carbon nanofibers (Fe-N-C) and 2D graphene sheets is introduced to modify a commercial polypropylene (PP) separator for use in lithium-sulfur batteries. Benefiting from the high electrical conductivity and strong lithium polysulfide (LiPS) chemical adsorption ability of Fe-N-C, the porous intercalation-structured modified layer exhibits excellent ability to suppress LiPS shuttling while maintaining high lithium-ion transport, and the modified layer functions as a highly conductive upper current collector to reutilize active sulfur species. The cell assembled with the modified multifunctional separator shows a high rate capability and excellent cycling stability, exhibiting a capacity of 847.9 mAh g −1 at 2 C and a low degradation rate of 0.053% per cycle over 500 cycles at 0.5 C.
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APPLIED CLAY SCIENCE
·
2012
·
IF 2.474
Zhujian Huang,Pingxiao Wu,Xing Zhang,Xiaorong Wang,Nengwu Zhu,Jinhua Wu,Ping Li
In this study, intercalation of Fe(III) complexes [Fe(Ox) 3 ] 3− and [Fe(Cit) 2 ] 3− in Mg 2 Al layered double hydroxides (LDHs) had been carried out by different routes: direct self-assembly, reconstruction and anion exchange. The result of XRD indicated that these two kinds of Fe(III) complexes intercalated LDHs (LDHs/Fe-complexes) could be successfully synthesized by anion exchange obtaining two well crystallized LDHs both with a large basal spacing. The chemical environment of iron ion in the intercalated Fe complexes was determined by FTIR , XPS and XAFS, the results of which concertedly proved that the intercalated Fe complexes were well preserved in the interlayer of LDHs. The arrangement of the Fe(III) complexes anions in the galleries of LDHs was studied by one-dimensional electron density projection. The results showed that the [Fe(Ox) 3 ] 3− anions were probably accommodated in the gallery of LDHs as an interdigitated bilayer arrangement, and the [Fe(Cit) 2 ] 3− were perpendicularly arranged against the LDHs sheets. Through the research, it is proved that the obtained LDHs/Fe-complexes markedly enhanced the UV–vis absorption ability of Fe complexes.
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