FUEL
·
2017
·
IF 4.601
Chuang Li,Guangyue Xu,Yongxiang Zhai,Xiaohao Liu,Yanfu Ma,Ying Zhang
Gamma-valerolactone (GVL) has been identified as a sustainable high-value platform molecular for the production of fuels and carbon-based chemicals. In this work, a series of activated carbon supported low-cost bimetallic Ni-Fe catalysts (Ni-Fe/AC) with different molar content of Fe species were prepared by using co-precipitation method for the liquid phase hydrogenation of ethyl levulinate (EL) to produce γ-valerolactone. The Ni-Fe 0.5 /AC exhibited the highest activity among the bimetallic or monometallic catalysts under mild reaction conditions (100 °C, 4 MPa H 2 , 6 h) and achieved 99.3% conversion of EL and 99.0% yield of GVL. Under more mild conditions (60 °C, 2 MPa H 2 ) and prolonging the reaction time to 24 h, EL could be converted completely and the obtained GVL yield was more than 98%. The catalysts were characterized by various techniques including XRD, TEM, HRTEM, EDX, XPS, H 2 -TPR and NH 3 -TPD. Based on the structure and activity relationship study, the formation of highly dispersed Ni-Fe alloy structure and the co-presented FeO x nanoparticles could be responsible for the high catalytic hydrogenation activity.
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DALTON TRANSACTIONS
·
2016
·Vol. 45
·期 19
·7952-7959
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IF 4.177
Qiao Sun,Min Liu,Keyan Li,Yitong Han,Yi Zuo,Junhu Wang,Chunshan Song,Guoliang Zhang,Xinwen Guo
A series of MIL-53(Fe)-type materials, Fe(BDC)(DMF,F), were prepared by using different ratios of n(FeCl3)/n(FeCl2), which have varied amounts of Fe2+ in their frameworks. From FeCl3 to FeCl2, the structures of the synthesized samples transform from MIL-53(Fe) to Fe(BDC)(DMF,F). Along with this structure transformation, the crystal morphology goes through a striking change from a small irregular shape to a big triangular prism. This phenomenon indicates that the addition of FeCl2 is beneficial for the formation of a Fe(BDC)(DMF,F) structure. The catalytic activity of these iron-containing MOFs was tested in phenol degradation with hydrogen peroxide as an oxidant at near neutral pH and 35 °C. The degradation efficiency of these samples increases gradually from MIL-53(Fe) to Fe(BDC)(DMF,F). 57Fe Mössbauer spectra reveal that Fe2+ and Fe3+ coexist in the Fe(BDC)(DMF,F) framework, and the highest amount of Fe2+ in the sample prepared with mixed FeCl3 and FeCl2 is 26.0%. The result illustrates that the amount of Fe2+ in the samples can be controlled using varied n(FeCl3)/n(FeCl2) in the feed. The diverse amount of Fe2+ in this series of FeMOF materials exactly explains the distinction of reaction efficiency. The iron leaching tests, structures of the fresh and used catalysts, and the data of the recycling runs show that the Fe-containing MOFs are stable in this liquid-phase reaction.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2017
·
IF 3.133
Li-Feng Zhu,Bo-Ping Zhang,Shun Li,Gao-Lei Zhao
The (1- x )Bi 1+ y (Fe 0.96 Mg 0.02 Ti 0.02 )O 3 - x BaTiO 3 (abbreviated as B 1+ y FMT- x BT) system was designed to explore the morphotropic phase boundary (MPB) separating rhombohedral ( R ) and tetragonal ( T ) phases, and the mechanism of performance enhancement. The phase structure of samples was discreetly investigated by X-ray diffraction, and Rietveld refinement results of the XRD data revealed that the B 1+ y FMT- x BT ceramics consist of an R phase at x = 0.24, two R and T phases at 0.26 ≤ x ≤ 0.32, and a single T phase at x = 0.34. Because of the MPB and the improvement of resistivity with adding excess Bi compensation, excellent piezoelectric properties of d 33 = 198 pC/N and k p = 30.9%, as well as high Curie temperature T C = 497 °C were achieved in the B 1+ y FMT- x BT system at x = 0.30 and y = 0.02. Here, the large d 33 = 198 pC/N which is the maximum value for the BF-BT-Bi(Mg,Ti)O 3 system so far, and high T C = 497 °C suggest that Bi(Fe,Mg,Ti)O 3 -BaTiO 3 ceramics have good prospects in high-temperature piezoelectric devices.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Jianqing Ma,Qunfeng Yang,Yuezhong Wen,Weiping Liu
Heterogeneous Fe-N complexes are a kind of promising catalysts for the Fenton-like reaction. The present study selected a stable and inexpensive g-C 3 N 4 as the chelating agent and combined with the graphitized mesoporous carbon (GMC). The fabricated Fe-g-C 3 N 4 /GMC composite was characterized by several techniques including FTIR, XRD, XPS, TEM and STXM. Results showed clear sheets of g-C 3 N 4 and graphite with Fe evenly distributed mostly in the Fe-N coordination form. The catalyst expressed high activity in the Fenton-like reaction in a wide pH range of 4–10. 99.2% removal of Acid Red 73 was obtained in 40 min, and the degradation data well fitted with the pseudo-first-order kinetics model. By correlating the constant of reaction rates calculated from the model and the Fe speciation contents of the samples prepared at different conditions, we deduced that Fe-N species are the most important active sites for the Fenton-like reaction. More importantly, hydroxyl radicals played a great role in the whole reaction yet their generation was independent of visible light. Cyclic voltammetry results confirmed that the GMC can accelerate the Fe(III)/Fe(II) redox cycle by enhancing electron transfer, and thus enable this Fenton-like catalyst to perform well in a wide pH range.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2014
·
IF 2.063
Zhigang Jia,Lulu Yang,Jianhong Liu,Qiuze Wang,Rongsun Zhu
Magnetic carbon spheres have been successfully prepared by the synchronous carbonation and activation of the 8-quinoliolato Fe(III) complexe with sphere morphology, which has been synthesized by solovthermal method. The obtained composite possesses relatively even pore diameter of 3.8 nm, high surface area of 335.59 m 2 /g with 52.67 wt.% Fe 3 O 4 coated, and a saturation magnetization (Ms) of 35.27 emu/g. Dye separation performance of the magnetic carbon spheres is investigated using methylene orange and methylene blue as modle. The resluts show that the maxium adsorption capacity for methylene orange and methylene blue is 128.70 mg g −1 and 151.29 mg g −1 , respectively, and the process can rapidly reach adsorption equilibrium within 5 min, which is important for the application of the as-prepared magnetic carbon spheres.
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JOURNAL OF POWER SOURCES
·
2014
·
IF 5.211
Guofu Ma,Jiajia Li,Kanjun Sun,Hui Peng,Jingjing Mu,Ziqiang Lei
A gel polymer PVA–KOH–K 3 [Fe(CN) 6 ] is prepared by potassium hydroxide and potassium ferricyanide doped polyvinyl alcohol, and a solid-state supercapacitor is assembled using the gel polymer as electrolyte and separator, activated carbons as electrode. The gel polymer exhibits flexible, high ionic conductivity and wide potential properties. The electrochemical properties of the supercapacitor are investigated using cyclic voltammetry , galvanostatic charge/discharge, and impedance spectroscopy techniques. The electrode specific capacitance of the supercapacitor can be as high as 430.95 F g −1 , and after 1000 cycles at a current density of 1 A g −1 it still remains higher than 380 F g −1 . The energy density and power density of the supercapacitor reach 57.94 Wh kg −1 and 59.84 kW kg −1 , respectively. These novel flexible gel polymers are desirable for applications in supercapacitor devices.
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Analytical Methods
·
2014
·Vol. 6
·期 19
·7973-7977
·
IF 1.938
Yingfeng Qin,Liangliang Zhang,Gaojie Ye,Shulin Zhao
A homogeneous label-free colorimetric sensing strategy for bleomycin (BLM) assay was developed on the basis of BLM enhanced Fe(II)–H2O2–ABTS reaction. Fe(II) exhibits a catalytic effect on H2O2-mediated oxidation of ABTS by Fenton chemistry. BLM·Fe(II) complex possessed a significantly higher catalytic ability than Fe(II) probably because of the further formation of more active “activated oxo-iron-bleomycin complex”. The present method was convenient without any complicated chemical synthesis, modification, or tedious experimental procedures. Analysis results can be seen with the naked eye and monitored by UV-vis spectra. The peak absorbance exhibits a linear relationship with BLM concentrations from 25 nM to 1 μM, and a detection limit of 16 nM can be achieved. The designed colorimetric strategy may provide a promising alternative for BLM detection in clinical samples.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2017
·
IF 6.198
Xiaolin Zhang,Mengfei Wu,Hao Dong,Hongchao Li,Bingcai Pan
Water decontamination from As(III) is an urgent but still challenging task. Herein, we fabricated a bifunctional nanocomposite HFO@PS-Cl for highly efficient removal of As(III), with active chlorine covalently binding spherical polystyrene host for in situ oxidation of As(III) to As(V), and Fe(III) hydroxide (HFO) nanoparticles (NPs) embedded inside for specific As(V) removal. HFO@PS-Cl could work effectively in a wide pH range (5–9), and other substances like sulfate, chloride, bicarbonate, silicate, and humic acid exert insignificant effect on As(III) removal. As(III) sequestration is realized via two pathways, that is, oxidation to As(V) by the active chlorine followed by specific As(V) adsorption onto HFO NPs, and As(III) adsorption onto HFO NPs followed by oxidation to As(V). The exhausted HFO@PS-Cl could be refreshed for cyclic runs with insignificant capacity loss by the combined regeneration strategy, that is, alkaline solution to rinse the adsorbed As(V) and NaClO solution to renew the host oxidation capability. In addition, fixed-bed experiments demonstrated that the HFO@PS-Cl column could generate >1760 bed volume (BV) effluent from a synthetic As(III)-containing groundwater to meet the drinking water standard (<10 μg As/L), whereas other two HFO nanocomposites, HFO@PS-N and HFO@D201 could only generate 450 and 600 BV effluents under otherwise identical conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Weirong Zhao,Yajun Li,Meng Zhang,Jinsheng Chen,Lihong Xie,Qiaomeng Shi,Xi Zhu
Fe-doped TiO 2 photocatalysts were synthesized rapidly and directly by the microwave–hydrothermal method and evaluated for hydrogen production by water splitting under UV–vis irradiation. The photocatalysts were characterized by X-ray diffraction, transmission electron microscopy, N 2 adsorption–desorption isotherms, inductively coupled plasma atomic emission spectroscopy, UV–vis spectroscopy, X-ray photoelectron spectra and photoelectrochemical experiments. The results showed that Fe-doped TiO 2 photocatalysts synthesized by the microwave–hydrothermal method exhibited a smaller crystallite size and higher specific surface area than TiO 2 photocatalysts. The microwave–hydrothermal method was a feasible way to increase the Fe doping concentration with enhanced electron–hole separation and electron transfer efficiency. It was also observed by first-principles density functional theory calculations that Fe can induce the formation of impurity levels near the valence band, leading to the reduction of the band gap and the improvement of photocatalytic activity. The highest photoactivity was achieved for TiO 2 doped with 0.5% Fe with a hydrogen production rate of 10.95 μmol h −1 .
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ChemCatChem
·
2017
·Vol. 9
·期 9
·1708-1715
·
IF 4.803
Jingtian Gao,Yun Wang,Shijian Zhou,Wei Lin,Yan Kong
Graphical Visibly better : A facile one-step pyrolysis process was developed to synthesize iron-doped graphitic carbon nitride nanosheets. The sample with 0.5 wt % FeCl 3 exhibited the best photocatalytic performance in the degradation of Methylene Blue and water splitting under visible light irradiation. A simple one-step pyrolysis process (compared with the routine method of liquid exfoliation and impregnation) was designed to synthesize Fe-doped graphitic carbon nitride (g-C 3 N 4 ) nanosheets with NH 4 Cl as dynamic gas template and FeCl 3 as the Fe source. Results of XPS and DRS indicated that the Fe species might exist at the state of Fe 3+ and form Fe−N bonds with N atoms, thereby expanding visible light absorption regions and reducing the band gap of g-C 3 N 4 nanosheets. Doping certain amounts of Fe could promote the exfoliation and further increase the specific surface area, while excessive Fe might break the sheet structure. The specific surface area of the optimized Fe-doped g-C 3 N 4 nanosheets reached 236.52 m 2 g −1 , which was 2.5 times higher than that of g-C 3 N 4 nanosheets. Among various photocatalysts prepared, the sample (0.5 wt % FeCl 3 ) exhibited maximum photocatalytic performance in degradation of Methylene Blue and water splitting under visible light irradiation. The degradation rate of MB was about 1.4 and 1.7 times higher than that of pure g-C 3 N 4 nanosheets and bulk g-C 3 N 4 , respectively. The H 2 production rate was 536 μmol h −1 g −1 , which was 1.8 and 6 times higher than that of pure g-C 3 N 4 nanosheets and bulk g-C 3 N 4 , separately.
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Small
·
2025
·
IF 12.1
Haiyang Shi,Lei Zhang,Xinhua Huang,Qingquan Kong,Abdukader Abdukayum,Yingtang Zhou,Guoyou Cheng,Sanshuang Gao,Guangzhi Hu
The design and fabrication of nanocatalysts with high accessibility and sintering resistance remain significant challenges in heterogeneous electrocatalysis. Herein, a novel catalyst is introduced that combines electronic pumping with alloy crystal facet engineering. At the nanoscale, the electronic pump leverages the chemical potential difference to drive electron migration from one region to another, separating and transferring electron-hole pairs. This mechanism accelerates the reaction kinetics and improves the reaction rate. The interface electronic structure optimization enables the CoFe/carbon nanotube (CNT) catalyst to exhibit outstanding oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performance. Specifically, this catalyst achieves an ORR half-wave potential (E₁/₂) of 0.895 V, outperforming standard Pt/C and RuO₂ electrocatalysts in terms of both specific activity and stability. It also demonstrates excellent electrochemical performance for OER, with an overpotential of only 287 mV at a current density of 10 mA cm⁻ 2 . Theoretical calculations reveal that the carefully designed crystal facets reduce the energy barrier of the rate-determining steps for both ORR and OER, optimizing O₂ adsorption and promoting the oxygen capture process. This study highlights the potential of developing cost-effective bifunctional ORR–OER electrocatalysts, offering a promising strategy for advancing Zn–air battery technology.
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Molecular Catalysis
·
2024
·
IF 3.9
Nan Zhou,Xiaoqing Jia,Siyuan Chen,Huafan Li,Feifei Li,Botao Qiao,Hailian Tang,Guoyi Bai
CO 2 methanation is an effective way for CO 2 recycling, and nickel-based catalysts have attracted much attention in this field due to their excellent CH 4 selectivity and cost-effectiveness; however, their applications are limited by their suboptimal catalytic activity. In this work, the catalytic activity of Ni-rutile-based catalysts was increased by almost an order of magnitude simply by doping the rutile with Fe. Series characterizations show that three factors that mainly contributed to the improved catalytic performance of the Ni/Fe-Rutile, which are the reduction of the Ni size, the increase of the basic sites, and the inhibition of the encapsulation of the Ni particles by the support. With Fe doping, the OH and oxygen vacancies on the rutile surface were reduced, which made the support difficult to reduce and thus suppressed the encapsulation of Ni by the support. As a result, the number of exposed active sites on the Ni/Fe-Rutile which with a smaller Ni size was further successfully increased, and the catalytic activity was significantly improved. This study provides new ideas for the design of activity-enhanced supported catalysts from the perspective of tuning the metal-support interaction and may be applicable to other reducible oxide-supported metal catalysts.
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