APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Zhuang Wang,Jinhu Wang,Lin Zhu,Yi He,Tao Duan
The effective removal of toxic and radioactive uranium (VI) (UO 2 2+ ) is very important for environmental protection and human health. Nevertheless, there is a lack of scalable adsorption materials for high-efficient and cost-effective removal of UO 2 2+ from water. In the present work, Fe@FeO core-shell nanoparticle (NP)-embedded wood is utilized for adsorption of UO 2 2+ from stimulated wastewater. The effect of various experimental conditions such as pH, reaction time, reaction temperature, and UO 2 2+ are investigated. The maximum adsorption capacity of UO 2 2+ is obtained at pH 4 (2.08 g UO 2 2+ of g Fe@FeO NPs), which is comparable to that of the reported FeNP and much higher than other Fe-containing nanoparticles for UO 2 2+ adsorption. The adsorption mechanism is ascribed to the redox reaction between Fe@FeO nanoparticles and UO 2 2+ , which reduce UO 2 2+ to UO 2 that is immobilized at the center of nanoparticles, while the wood matrix provides a support and does not adsorb UO 2 2+ . Meanwhile, the Fe@FeO NP-embedded wood is able to float on the surface of wastewater, which is easily separated and reused. More importantly, the low-cost Fe@FeO NP-embedded wood allows for scalable preparation, further improving the adsorption performance toward UO 2 2+ using the large-scale wood for future practical applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Guoru Li,Xiaobo He,Fengxiang Yin,Biaohua Chen,Huaqiang Yin
The development of highly efficient electrocatalysts with low cost for oxygen reduction reaction (ORR) is urgently required for metal-air batteries and fuel cells. In this work, Fe Co/MIL-101(Cr) with various molar ratios of Fe/Co as hybrid catalysts was prepared by a facile and mild impregnation method. MIL-101(Cr) increased the specific surface areas of the hybrid catalysts, thus improving the dispersion of Fe and Co species at their surfaces. The effects of Fe and Co species on ORR activity of the hybrid catalysts were investigated. It is found that the synergistic effects between the well-dispersed Fe and Co species contribute mainly to ORR activity. More specifically, Fe species exert a partial-charge-transfer-activation effect on Co ones, which reduces the charge transfer resistance and thus improves the catalytic activity . As a result, Fe Co/MIL-101(Cr) showed the excellent ORR activity, in which Co 50 Fe 50 /MIL-101(Cr) exhibited the superior ORR activity to the other prepared hybrid catalysts.
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JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2019
·Vol. 66
·期 12
·1610-1618
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IF 1.188
Tao Wang,Aiyun Hu,Haijun Wang,Yongmei Xia
Layered double hydroxides (LDHs) and their derivatives have been reported to be widely used as heterogeneous catalysts in various reactions. Herein, Ni-Fe LDHs with the controlled Ni/Fe molar ratios (2:1, 3:1, 4:1) were synthesized via an easy hydrothermal method, which were used to catalyze the selective reduction of biomass-derived furfural into furfuryl alcohol using 2-propanol as a H-donor under autogenous pressure and characterized using FT-IR, XRD, TGA, BET, SEM, NH 3 -TPD, and CO 2 -TPD. It was found that the LDH with a Ni/Fe molar ratio of 3:1 demonstrated the best catalytic activity among the LDHs with different Ni/Fe molar ratios, which showed 97.0% conversion of furfural and 90.2% yield of furfuryl alcohol at 140°C for 5 hr. This was attributable to the synergistic effect of acidic sites and basic sites of the catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Zhefu Li,Binling Chen,Xianfeng Wang,Jun Nie,Guiping Ma
In this work, a novel catalyst of oxygen reduction reaction (ORR) was designed and fabricated by electrospinning, photo-curing and carbonization, based on polymer poly(dimethylsilylene ethynylenephenyleneethynylene) (PMSEPE) and metal organic frameworks (MOFs)—Materiaux de l'Institute Lavosier-101(Fe) (MIL-101(Fe)). The optimal catalyst PMSEPE/MIL-101(Fe)-800, which was carbonized at 800 °C, presented a bamboo-like nanofiber structure with a high degree of graphitization, a high specific surface area (302.3 m 2 /g) and a high yield (64.17%). Fe 3 C particles were found to be encapsulated into the Fe-Si-N co-doped carbon nanofibers. In the electrochemical tests, PMSEPE/MIL-101(Fe)-800 showed an onset potential of 0.935 V ( vs . RHE) and a diffusion limit current of 6.01 mA/cm 2 ( vs . RHE) in 0.1 M KOH aqueous solution, of which performances are competitive to commercial 20 wt% Pt/C. PMSEPE/MIL-101(Fe)-800 also exhibited a higher methanol tolerance and duration stability. Further Zn-air battery test used by PMSEPE/MIL-101(Fe)-800 suggested its potential for the application of fuel cell.
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高影响因子
Energy Technology
·
2019
·Vol. 7
·期 10
·1900649
·
IF 3.163
Yiqun Du,Shimeng Zhao,Cheng Xu,Wenyang Zhang,Pan Li,Huixin Jin,Youjian Zhang,Zihan Wang,Jianxin Zhang
Rechargeable aluminum batteries (RABs) have been intensively studied recently in virtue of high volumetric energy density and cheapness. However, limited options for suitable cathode materials is the major obstacle to their large-scale application. Herein, nickel-iron layered double hydroxide (NiFe–LDH) microspheres with reduced graphene oxide (rGO) are reported as cathode for RABs. It is demonstrated that NiFe–LDH can provide large interlayer spacing for aluminum ions to interact, and the introduction of rGO endows NiFe–LDH with excellent structure stability, electronic conduction, and electrochemical reaction kinetics. The aluminum battery with a NiFe–LDH/rGO cathode delivers a high reversible capacity of 131 mA h g −1 at 1 A g −1 with nearly 100% coulombic efficiency after 100 cycles. The characterization results reveal that the reversible Al 3+ insertion/extraction along with the multielectron redox reactions occurs in the NiFe–LDH/rGO during the cycling process. The aforementioned strategies shed new light on the selection of compatible cathodes for RABs.
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Energy Technology
·
2019
·Vol. 7
·期 7
·1801128
·
IF 3.163
Weicheng Cui,Hongye Bai,Konggang Qu,Fagen Wang,Peng Guan,Dongbo Xu,Weiqiang Fan,Weidong Shi
Kinetics play a critical role in the photoelectrochemical (PEC) system, whereas co-catalysis is mainly responsible for reducing the reaction barrier and facilitates water splitting. Here, the unsaturated Fe sites through the metal-organic framework (MOFs) structure promote the kinetics of water oxidation over TiO 2 are successfully in situ decorated. This heterostructure further helps us to better understand the PEC behaviors of organic–inorganic hybrid systems. MIL-100(Fe), as the typical MOFs model, is facilely achieved by an FeOOH sacrificial template method, a strategy which could anchor the compact and ultrathin MIL-100(Fe) films on the surface of TiO 2 to obtain abundant unsaturated Fe sites. The photocurrent density of MIL-100(Fe)/TiO 2 reaches about 2.4 times at 1.23 V vs reversible hydrogen electrode (RHE) compared with bare TiO 2 , and the incident photon to current conversion efficiency value increases up to 47% (at 390 nm). Furthermore, the photocurrent density of MIL-100(Fe)/TiO 2 is maintained at 84% after 3 h, showing that the organic component of MIL-100(Fe) takes a nature of favorable stability. The configuration of MIL-100(Fe)/TiO 2 will bring a new insight for learning the basic function of unsaturated metal sites in the PEC system.
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INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Wei Wang,Mehran Amiri,Tao Huang,Lev N. Zakharov,Yining Zhang,May Nyman
Isolating Fe(III) clusters from water without stabilizing ligands is significantly challenged by the high acidity of Fe3+-bound water, leading to uncontrolled precipitation of iron oxyhydroxides. Here we demonstrate a freeze-drying solvent-exchange method that enabled the isolation of a metastable Fe(III) sulfate decameric cluster formulated [Fe10O2(SO4)12(OCH3)2]·14CH3OH (Fe10). Without stabilization by solvent-exchange, the aqueous species undergoes rapid conversion to the iron sulfate mineral schwertmannite. Monitoring the hydrolysis process from cluster intermediates to schertmannite by small-angle X-ray scattering, we observe the progression from Fe10 to 37 Å soluble nanoparticles prior to the precipitation process. This condensation behavior of Fe10 is further exploited to develop a simple laboratory synthesis of schwetmannite. In addition, we demonstrate the versatility of the freeze-drying solvent-exchange method by isolating Al(III), Zn(II), and Cd(II) substituted Fe(III) sulfate clusters. The freeze-drying solvent-exchange method provides a unique opportunity to isolate cluster intermediates and models to aid in our understanding of metal-ion hydrolysis processes in environmental, material science, and geological studies.
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JOURNAL OF POWER SOURCES
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2019
·
IF 7.467
Xuelong Zhou,Liyu Lin,Yunhui Lv,Xiangyang Zhang,Liangdong Fan,Qixing Wu
Component materials and flow fields are key design parameters that influence the advection-diffusion-reaction process and thereby the performance of a Sn–Fe hybrid flow battery . In this work, various electrode configurations (empty chamber and porous carbon-based electrodes), membranes (cation and anion conducting) and flow fields (serpentine and interdigitated) are systematically investigated to elucidate their effects on the unique charge/discharge behaviors of the Sn–Fe flow battery with tin metal plating/striping. It is found that the battery capacity roughly increases linearly with the porosity of the porous electrode especially at low current densities , and a highly porous electrode (graphite felt) is more desirable than an empty chamber configuration in terms of capacity and power density. In addition, as compared to cation exchange membrane (Nafion 212), the anion exchange membrane (Fumasep FAP-450) exhibits improved capacities and columbic efficiencies in sulfuric acid-based electrolytes at low current densities due to the reduction of cation crossover. Interestingly, it is showed that although a serpentine flow field and a low flow rate generally lead to poor battery performance, they tend to ameliorate the maldistribution of plated tin at the negative electrode owing to the restricted mass transfer of reactants.
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Nanoscale
·
2019
·Vol. 12
·期 3
·2126-2132
·
IF 6.97
Hui Xu,Hongyuan Shang,Cheng Wang,Liujun Jin,Chunyan Chen,Yukou Du
Although great successes have been accomplished on the controlled synthesis of 2D and 3D Pd-containing nanomaterials, tapping into the novel Pd-containing electrocatalysts that combined the advantages of both 2D and 3D structures remains a significant challenge. Here, an approach to systematically produce porous Fe-doped Pd nanosheet assemblies (NSAs) with a geometry tuning from PdFe hollow nanospheres (HNSs), PdFe nanocages (NCs), to PdFe nanoplates (NPs) is reported. The inherent ultrathin and porous features endow these PdFe catalysts with excellent electrocatalytic performance. As a result, the optimized 3D PdFe NCs show a much-improved methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR) activities in comparison with PdFe HNSs, Pd NPs, and commercial Pd/C catalysts. Moreover, these PdFe nanocatalysts also display greatly enhanced electrocatalytic stability, which can endure 500 cycles with negligible activity loss and structural changes. The mechanism investigations reveal that the introduced Fe atom efficiently modulates the electronic structure of Pd, leading to the downshift of the d-band center of Pd, which is beneficial for the adsorption of reactants. Moreover, the porous nanosheet assembly structure can provide rich mass and electron transfer channels, further boosting the improvement of electrocatalytic performance.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Yunwen Wu,Xiaotong Chen,Yu Han,Dongting Yue,Xinde Cao,Yixin Zhao,Xufang Qian
Nanoscale zerovalent iron (nZVI) particles have received much attention in environmental science and technology due to their unique electronic and chemical properties. However, the aggregation and oxidation of nZVI brings much difficulty in practical application of environmental remediation. In this study, we reported a composite nano-Fe(0)/mesoporous carbon by a chelation-assisted coassembly and carbothermal reduction strategy. Nano-Fe(0) particles with surface iron oxide (Fe2O3·FeO) were wrapped with graphitic layers which were uniformly dispersed in mesoporous carbon frameworks. The unique structure made the nano-Fe(0) particles stable in air for more than 20 days. It was used as a peroxydisulfate (PDS) activator for the oxidation treatment of 2,4,6-trichlorophenol (TCP). The TOF value of MCFe for TCP degradation is nearly 3 times higher than those of FeSO4 and Fe2O3·FeO and nearly 2 times than that of commercial nZVI. The reactive oxygen species (ROS) including •SO4–, HO•, and •O2–, 1O2 are efficiently generated by PDS activation with MCFe. The PDS activation process by nano-Fe(0) particles was intrinsically induced by the ferrous ions (Fe(II)) continuously generated at the solid/aqueous interface. Namely, the nano-Fe(0) particles were highly efficiently utilized in sulfate radical-based advanced oxidation processes (SR-AOP). The porous structure also assists the absorption and transfer of TCP during the degradation process.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2019
·
IF 3.261
Shengchao Miao,Zhenxing Zha,Ying Li,Xinxiang Geng,Jiahui Yang,Shihai Cui,Jing Yang
The novel semiconductor heterojunction of MIL-53(Fe)/BiOCl composite was first prepared through the solvothermal reaction. The prepared materials were characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Brunner-Emmet-Teller (BET) and ultraviolet-visible diffuse reflectance spectroscopy (DRS). MIL-53(Fe)/BiOCl heterojunction is a kind of photoexcited materials and it accelerates the photoreactivity of BiOCl under the visible light irradiation. It was used to remove Rhodamine B (RhB) with the existence of persulfate (PS). The UV–vis spectrophotometer and the TOC detector show that the degradation rate and TOC removal efficiency of RhB (20 mg/L) are 99.5% and 69.4%within 30 min visible-light irradiation, respectively. Due to the proper band gap of material and the presence of electron acceptor, PS, the survival time of active radicals are increased. The active species h + , ·SO 4 − and ·OH are found to play the important roles during the reaction system. The possible mechanism for the RhB degradation of MIL-53(Fe)/BiOCl/PS is also proposed. Furthermore, the results of the material reusability for the degradation of RhB indicate that the MIL-53(Fe)/BiOCl has a good stability and can be used in the environmental water sample treatment.
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ANALYST
·
2018
·Vol. 144
·期 2
·656-662
·
IF 3.864
Shujuan Zhuo,Yuanyuan Guan,Hui Li,Jing Fang,Ping Zhang,Jinyan Du,Changqing Zhu
In this paper, we have presented a novel strategy to fabricate Fe-doped carbon quantum dots (Fe-CQDs) for dopamine sensing applications. The Fe-CQDs are obtained by one step hydrothermal carbonization, using ethylenediamine tetraacetic acid salts and ferric nitrate as the carbon and iron source, which simultaneously incorporates Fe (dopamine-bonding site) and luminescent carbon quantum dots (fluorophores). The added dopamine containing catechol groups might form complexes with Fe ions (doped in CQDs) due to coordination. Subsequently, dopamine was oxidized to generate dopamine-quinone (a known potent electron acceptor) species by ambient O2. Thus, the coordination induced dopamine in proximity to the CQDs, which provided favourable electron acceptors in close proximity to the CQDs and produced high quenching efficiencies. Such fluorescence responses can be used for well quantifying dopamine in the range of 0.01–50 μM with a detection limit of 5 nM (S/N = 3). The proposed sensing system has been successfully used for the assay of dopamine in human urine samples. Preliminary cell image study indicates that the obtained Fe-CQDs possess high photostability and low cytotoxicity, which make them promising for biological applications.
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