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Facile Synthesis of 3D Fe/N Codoped Mesoporous Graphene as Efficient Bifunctional Oxygen Electrocatalysts for Rechargeable Zn-Air Batteries

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ACS SUSTAINABLE CHEMISTRY & ENGINEERING 2019年第16期7卷 13873-13885页

作者： wang, Chen Li, Zhongfang wang, Likai Niu, Xueliang wang, suwen Shandong Univ Technol Sch Chem & Chem Engn Zibo 255049 Peoples R China

Exploring the oxygen electrocatalysts with both high oxygen reduction reaction (ORB.) and oxygen evolution reaction (OER) performance is crucial to developing the rechargeable Zn-air batteries (ZABs). Herein, we prepared a bifunctional three-dimensional graphene-like iron-nitrogen doped oxygen electrocatalyst (3D Fe/N-G#4, polyacrylamide (PAM):-NaCl = 1:4, mass ratio) by a facile synthesis with PAM and iron as precursors and NaCl as template. The NaCl template melted during the pyrolysis process, which could fabricate a stable 3D network structure in the precursors to form more mesopores, higher specific surface area, and more exposed active sites and prevent the loss of precursors. The low-cost and water-soluble PAM as the N precursor provided abundant N and dissolved adequately with NaCl solution. The Fe precursor coordinated with the N to form Fe-N-x active sites that were investigated by HR-TEM, XRD, XPS, and RDE techniques. The 3D Fe/N-G#4 exhibited excellent electrochemical activity with a high half-wave potential (0.852 V vs RHE) for ORR and a low overpotential (393 mV at 10 mA cm(-2)) for OER in the alkaline conditions. In addition, the homemade rechargeable ZAB based on the prepared 3D Fe/N-G#4 exhibits high power density (168.2 mW cm(-2)) and excellent discharge-charge cycling stability (over 60 h) at 20 mA cm(-2). This work provides a cost-efficient, simple, and eco-friendly method to synthesize excellent bifunctional non noble electrocatalysts for commercialization of ZABs.

关键词： Oxygen reduction reaction Oxygen evolution reaction 3D Fe/N codoped graphene Freeze-drying NaCl template

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Cerium sulfophenyl phosphate, a novel inorgano-organic solid proton-conducting material

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MATERIALS LETTERS 2011年第9期65卷 1431-1433页

作者： Dong, Feilong Li, Zhongfang wang, suwen wang, Zhenhai Shandong Univ Sci & Technol Sch Chem Engn Zibo 255049 Peoples R China

Cerium sulfophenyl phosphate (CeSPP), a novel inorgano-organic solid proton conductor, was synthesized from the reaction of m-sulfophenyl phosphonic acid and hydrated cerous nitrate. The synthesized CeSPP was characterized by Fourier-transform infrared spectroscopy, X-ray diffraction, thermogravimetric analysis (TGA), scanning electron microscopy, and energy-dispersive X-ray spectroscopy. The TGA results reveal that CeSPP has good thermal stability. The synthesized CeSPP exhibited considerable high-proton conductivity. The proton conductivity was about 0.13 S/cm at 150 degrees C under 100% relative humidity. The proton conductivity at 105 degrees C at different RH was also measured. (C) 2011 Elsevier B.V. All rights reserved.

关键词： Composite materials Functional Proton conductor m-sulfophenyl phosphonic acid Cerium sulfophenyl phosphate

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Inhibition of the Corrosion of Copper in a Sodium Chloride Solution Using 4-((4-dodecylphenylimino)methyl)phenol

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INTERNATIONAL JOURNAL OF ELECTROCHEMICAL SCIENCE 2013年第5期8卷 6513-6523页

作者： Li, Zhongfang Jin, Lei wang, Weiyun wang, suwen Shandong Univ Technol Sch Chem Engn Zibo 255049 Peoples R China

A new kind of Schiff base, 4-((4-dodecylphenylimino)methyl)phenol (DPMP), is synthesized. Its structure is characterized by Fourier-transform infrared (FT-IR) and H-1 nuclear magnetic resonance. Self-assembled films of DPMP are prepared on a copper surface. Electrochemical impedance spectroscopy (EIS) and polarization curve analyses are performed to measure the protection ability against copper corrosion in a 0.5 mol/L NaCl solution. FT-IR spectroscopy and scanning electron microscopy are used for the surface topography measurements. The results indicate that DPMP could self-assemble on the copper surface. The inhibition efficiency (IE) increases with increasing DPMP solution concentration. The maximum IE in 0.01 mol/L DPMP-ethanol solution after 2 h of self-assembly is 99.87%.

关键词： Schiff base Copper corrosion Electrochemical Impedance spectroscopy Polarization curve Inhibition efficiency

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Preparation and properties of sulfonated poly(phthalazinone ether sulfone ketone)/tungsten oxide composite membranes

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ASIA-PACIFIC JOURNAL OF CHEMICAL ENGINEERING 2012年第4期7卷 528-533页

作者： wang, suwen Dong, Feilong Li, Zhongfang Jin, Lei Shandong Univ Technol Sch Chem Engn Zibo 255049 Peoples R China

Sulfonated poly(phthalazinone ether sulfone ketone) (SPPESK)-based composite membranes doped with hydrated tungsten oxide were prepared and studied for proton-exchange membrane applications. Hydrated tungsten oxide (WO3 center dot 2H2O) was synthesized from acidic hydrolysis of sodium tungstate. The SPPESK/WO3 composite membranes were prepared by mixing proper amounts of SPPESK and hydrated WO3 in dimethylacetamide as casting solvent. The composite membranes were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), thermal gravimetric analysis (TGA), and atomic force microscope (AFM). Infrared results indicated that the adding of WO3 center dot 2H2O did not destroy the structure of polymer. In particular, SEM as well as AFM measurements showed a dense structure of the membranes, and the homogenous dispersion of WO3 center dot 2H2O TGA results revealed thermal stability of the composite membranes at below 200 degrees C. The conductivity of the SPPESK/WO3 (30 wt%) composite membrane was about 0.033 S/cm at 140 degrees C under 100% relative humidity. The methanol permeabilities of the SPPESK/WO3 composite membranes were in the range of 1.715 x 10-7 to 0.496 x 10-7 cm2/s, much lower than that of Nafion (R) 117 (2.4 x 10-6 cm2/s). The presence of the oxide not only enhanced the proton conductivity of the SPPESK membranes but also improved their heat resistance and therefore decreased the methanol permeabilities. Copyright (c) 2011 Curtin University of Technology and John Wiley & Sons, Ltd.

关键词： direct methanol fuel cells composite membrane sulfonated poly(phthalazinone ether sulfone ketone) hydrated tungsten oxide proton conductivity

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Non-precious cathode electrocatalyst for magnesium air fuel cells: Activity and durability of iron-polyphthalocyanine absorbed on carbon black

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JOURNAL OF POWER SOURCES 2013年 242卷 157-165页

作者： Li, Zhongfang Yang, Jianwei Xu, Guofeng wang, suwen Shandong Univ Technol Sch Chem Engn Zibo 255049 Shandong Peoples R China

A planar iron-polyphthalocyanine (PPcFe) oxygen reduction reaction (ORR) catalyst for magnesium air fuel cells (MAFC) is prepared by dispersing PPcFe on carbon black (C) and heating under argon. Thermogravimetric analysis shows PPcFe is stable below 600 degrees C. The X-ray diffraction and X-ray photoelectron spectroscopy results show the active site of PPcFe/C is the FeN4 in the phthalocyanine ring. The rotating disk electrode measurements in 0.5 M L-1 H2SO4, solution show the initial potential for ORR is 0.82 V vs. RHE at 20 degrees C and that it mainly occurs via a four-electron process. Almost no performance degradation is observed over continuous cyclic voltammetry at 10,000 cycles, linear sweep voltammetry at 200 cycles, and 60 h of the chronoamperometry test. The infrared spectrum of PPcFe, after all the durability tests, shows no changes from the initial characteristics. The polarization curves of the air electrodes with PPcFe/C, iron-phthalocyanine/C and Pt/C catalysts exhibit excellent polarization performances. The discharge performance of a MAFC single cell with PPcFe/C cathode catalyst shows an open circuit potential of 1.74 V, with a peak power density of 50.5 mW cm(-2) at 20 degrees C. The cell voltage decreases less than 0.01 V during continuing discharge @ 20 mA cm(-2) for more than 11 h. (C) 2013 Elsevier B.V. All rights reserved.

关键词： Magnesium air fuel cells Air electrode Catalyst Oxygen reduction reaction Iron polyphthalocyanine Durability

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Spinel CoFe2O4 supported by three dimensional graphene as high-performance bi-functional electrocatalysts for oxygen reduction and evolution reaction

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 2019年第3期44卷 1610-1619页

作者： Zhang, Tingwei Li, Zhongfang wang, Likai Zhang, Zhixu wang, suwen Shandong Univ Technol Sch Chem & Chem Engn Zibo 255049 Peoples R China Anshan Normal Univ Sch Chem & Life Sci Anshan 114007 Peoples R China

Spinel CoFe2O4 supported on three dimensional graphene (3DG) is prepared by hydrothermal reaction, which is denoted as CoFe2O4/3DG. The 3DG is prepared by the templated method, where coal tar pitch (CTP) and MgO are used as the carbon source and the template, respectively. The microstructure and composition of the resultant have been investigated by X-ray diffraction as well as X-ray photoelectron spectroscopy indicating the formation of spinel CoFe2O4 and composite of CoFe2O4/3DG. The multilayer structure of 3DG and CoFe2O4/3DG is also examined by the Raman spectra. Electrochemically, CoFe2O4/3DG shows high-performance half-wave potential is 0.80 V vs. RHE in O-2-saturated 0.1 M KOH, which is compared to 20 wt% Pt/C. When evaluated for OER activity, CoFe2O4/3DG obtains a low overpotential 1.63 V vs. RHE (at j = 10 mA cm(-2)), which is 180 mV better than 20 wt% Pt/C. Moreover, it possesses excellent durability superior to 20 wt% Pt/C. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

关键词： Bi-functional electrocatalysts Oxygen reduction reaction Oxygen evolution reaction Spinel CoFe2O4 Three dimensional graphene

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Performance enhancement of polybenzimidazole based high temperature proton exchange membranes with multifunctional crosslinker and highly sulfonated polyaniline

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JOURNAL OF MEMBRANE SCIENCE 2018年 549卷 660-669页

作者： Sun, Peng Li, Zhongfang wang, suwen Yin, Xiaoyan Shandong Univ Technol Sch Chem & Chem Engn 266 Xincun West Rd Zibo 255049 Shandong Peoples R China

Polybenzimidazole (PBI) based high temperature proton exchange membranes were prepared by covalent crosslinking with triglycidylisocyanurate (TGIC) and doping with highly sulfonated polyaniline (SPAN). Insoluble SPAN with high degree of sulfonation was synthesized as the proton conductor. SPAN was homogeneously dispersed in the PBI-TGIC matrix. The composite membranes presented good thermal, dimensional, mechanical and oxidative stability for fuel cell applications. Since TGIC was a tri-functional cross-linker, with a relatively low cross-linking degree (CLD), the mechanical strength, dimensional stability and oxidative resistance of the composite membranes were improved. The low CLD also allowed high doping level of SPAN and consequently high proton conductivity. The proton conductivity of PBI-TGIC(5%)/SPAN(50%) and PBI-TGIC(10%)/SPAN (50%) at 180 degrees C and 100% RH was 0.13 and 0.12 S cm(-1), respectively. At 180 degrees C and 50% RH, the proton conductivity of these two PEMs was 0.064 and 0.058 S cm(-1), respectively. At 180 degrees C and 0% RH, the proton conductivity of them was 0.018 and 0.016 S cm(-1), respectively. The methanol resistance and membrane selectivity of PBI-TGIC/SPAN were also good and thus the membranes could be well applied in direct methanol fuel cells.

关键词： High temperature proton exchange membrane Polybenzimidazole Sulfonated polyaniline Covalent cross-linking Proton conductivity

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α-MnO2 nanorods supported on three dimensional graphene as high activity and durability cathode electrocatalysts for magnesium-air fuel cells

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CATALYSIS TODAY 2020年 355卷 304-310页

作者： Zhang, Tingwei Li, Zhongfang Sun, Peng wang, Likai Niu, Xueliang wang, suwen Shandong Univ Technol Sch Chem & Chem Engn Zibo 255049 Peoples R China Anshan Normal Univ Sch Chem & Life Sci Anshan 114007 Peoples R China

Magnesium-air fuel cells are considered as a potential energy conversion device owing to a high theoretical specific capability, economic viability and environmental friendliness. In this work, alpha-MnO2 nanorods are supported on three-dimensional graphene (3D-G) which is fabricated with coal tar pitch as the carbon precursor and MgO as the template via hydrothermal reaction. The synergistic interactions between alpha-MnO2 nanorods and 3D-G improve the activity and durability performance for oxygen reduction reaction in 0.1 mol L-1 KOH solution. alpha-MnO2/3D-G exhibits a high half-wave potential (0.81 V) and superior to alpha-MnO2/C (0.72 V) and alpha-MnO2/rGO (0.76 V), and close to 20 wt% PVC (0.83 V). alpha-MnO2/3D-G also possesses higher durability than commercial PVC. Furthermore, the magnesium-air fuel cells based on alpha-MnO2/3D-G, air-cathode display the peak power density (106.2 mW cm(-2)), and continuously durability (discharge for 16 h at 50 mA cm(-2) with the mere decay of cell voltage by 7.6%). These results prove that alpha-MnO2 /3D-G catalyst with high activity and durability can be a promising electrocatalyst in magnesium-air fuel cells.

关键词： Magnesium-air fuel cells Oxygen reduction reaction alpha-MnO2 nanorods Three-dimensional graphene Electrocatalyst

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Planar polyphthalocyanine cobalt absorbed on carbon black as stable electrocatalysts for direct methanol fuel cell

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JOURNAL OF POWER SOURCES 2010年第15期195卷 4731-4735页

作者： Xu, Guofeng Li, Zhongfang wang, suwen Yu, Xianjin Shandong Univ Technol Sch Chem Engn Zibo 255049 Shandong Peoples R China

In this work, a novel catalyst is prepared by dispersing planar polyphthalocyanine cobalt (PPcCo) synthesized by polymerizing cobalt (II)-4, 4',4",4''' phthalocyanine tetracarboxylic acid (TcPcCo) using a high surface area carbon powder (Vulcan XC 72), and then heat-treated in argon (Ar) atmosphere. The polymer and PPcCo/C catalysts are characterized systematically by a variety of methods, such as ultraviolet-visible (UV-vis) spectrophotometer, Fourier transform infrared spectrometer (FT-IR), thermogravimetric analysis (TGA), X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscope (TEM). Results show that the PPcCo obtained is stable below 600 degrees C. The active site of PPcCo/C is CoN4 in phthalocyanine ring, and the PPcCo is dispersed homogeneously on the surface of XC 72. Electrocatalytic properties and electrochemical stability of the catalysts in 0.5 mol L-1 H2SO4 are evaluated by RDE measurements. The initial potential for O-2 reduction in O-2-saturated H2SO4 is 0.81 V and it catalyzed O-2 reduction mainly through a four-electron process. Almost no performance degradation is observed over continuous cyclic voltammetry (CV) at 10,000 cycles (4 days). Polarization curves obtained by linear sweep voltammetry (LSV) at 200 cycles also show no change. PPcCo/C catalysts display significant electrocatalytic performance for O-2 reduction, tolerance towards methanol, and long-term stability. (C) 2010 Elsevier B.V. All rights reserved.

关键词： Direct methanol fuel cell Electrocatalyst Oxygen reduction reaction Polyphthalocyanine cobalt Stability

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Simple synthesis of iron^III sulfophenyl phosphate nanosheets as a high temperature inorganic-organic proton conductor

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IONICS 2014年第10期20卷 1399-1406页

作者： Liu, Guohong Li, Zhongfang Jin, Lei wang, suwen Shandong Univ Technol Sch Chem Engn Zibo 255049 Shandong Peoples R China

Iron(III) sulfophenyl phosphate (FeSPP) is successfully synthesized by an optimized process from the reaction of iron(III) chloride and m-sulfophenyl phosphonic acid (msPPA) by a simple and environmentally friendly method. Experimental results show FeSPP has a kind of layered structure, and multilayer sheet is about 2 nm thick. FeSPP exhibits good thermal stability and does not decompose under 200 A degrees C. Protons transfer through vehicle and Grotthuss mechanisms at different relative humidities (RH). The conductivity of FeSPP can reach to 0.115 S/cm at 180 A degrees C and RH = 100 %. Under this condition, vehicle mechanism plays the leading role, and the Grotthuss mechanism plays the minor role. At low RH, Grotthuss plays the leading role, and vehicle plays the minor role. In a drying oven at 180 A degrees C, the proton conductivity remains 2.15 x 10(-3) S/cm. Good conductivities at different RH and thermal stabilities clearly demonstrate that FeSPP is a highly effective conductor. It can be used as catalysts, chemical sensors, and in the preparation of composite membrane.

关键词： Proton conductor Iron(III)sulfophenyl phosphate Nanostructure powder Proton conductivity Relative humidity

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