有机酸掺杂Pd-PANI纳米复合材料的制备及对甲醇的电催化氧化
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摘要
以PdCl_2为金属前驱体,苯胺为单体,避光条件下液相合成了有机酸掺杂的Pd-聚苯胺(PANI)-十二烷基苯磺酸(DBSA)和Pd-PANI-磺基水杨酸(SSA)纳米复合材料。用XRD、FESEM、FT-IR和UV-vis等技术对样品进行了表征,并采用四探针法对其导电性能进行了测试。采用循环伏安法和计时电流法研究了有机酸掺杂Pd-PANI纳米复合材料修饰玻碳电极对甲醇的电催化氧化。结果表明,2种有机酸均成功掺杂到纳米复合材料中。Pd-PANI-DBSA纳米复合材料在15.3°和23.1°出现2个衍射峰,形貌呈类球状,电导率是Pd-PANI-SSA纳米复合材料的3.24倍,修饰电极对甲醇展示了良好的电催化活性和抗中毒性。
Palladium(Pd)-polyaniline(PANI)nanocomposites doped with dodecylbenzene sulfonic acid(DBSA)and sulphosalicylic acid(SSA),respectively,were synthesized in the liquid phase under the dark conditions using aniline as monomer and palladium chloride(PdCl_2)as the palladium precursor.The samples were characterized by X-ray powder diffraction(XRD),field emission scanning electron microscope(FESEM),Fourier-transform infrared spectroscopy(FT-IR)and ultraviolet-visible spectroscopy(UV-vis).The conductivity of nanocomposites was measured with the four-probe method.Electrochemical performance of methanol oxidation was also investigated at a glassy carbon electrode modified using nanocomposites by cyclic voltammetry(CV)and chronoamperometry.The results showed that Pd-PANI-DBSA and Pd-PANI-SSA nanocomposites have been obtained respectively.Two diffraction peaks at 15.3° and 23.1° were observed in the Pd-PANI-DBSA nanocomposites and Pd-PANI-DBSA nanocomposites was sphere-like nanostructures.The conductivity of Pd-PANIDBSA was 3.24 times that of Pd-PANI-SSA.Compared with the Pd-PANI-SSA,Pd-PANI-DBSA exhibited the more outstanding electrocatalytic activity and anti-poisoning property for methanol oxidation.
Palladium(Pd)-polyaniline(PANI)nanocomposites doped with dodecylbenzene sulfonic acid(DBSA)and sulphosalicylic acid(SSA),respectively,were synthesized in the liquid phase under the dark conditions using aniline as monomer and palladium chloride(PdCl_2)as the palladium precursor.The samples were characterized by X-ray powder diffraction(XRD),field emission scanning electron microscope(FESEM),Fourier-transform infrared spectroscopy(FT-IR)and ultraviolet-visible spectroscopy(UV-vis).The conductivity of nanocomposites was measured with the four-probe method.Electrochemical performance of methanol oxidation was also investigated at a glassy carbon electrode modified using nanocomposites by cyclic voltammetry(CV)and chronoamperometry.The results showed that Pd-PANI-DBSA and Pd-PANI-SSA nanocomposites have been obtained respectively.Two diffraction peaks at 15.3° and 23.1° were observed in the Pd-PANI-DBSA nanocomposites and Pd-PANI-DBSA nanocomposites was sphere-like nanostructures.The conductivity of Pd-PANIDBSA was 3.24 times that of Pd-PANI-SSA.Compared with the Pd-PANI-SSA,Pd-PANI-DBSA exhibited the more outstanding electrocatalytic activity and anti-poisoning property for methanol oxidation.
引文
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[4]Dasa A K,Kimb N H,Pradhana D,et al.Electrochemical synthesis of palladium(Pd)nanorods:An efficient electrocatalyst for methanol and hydrazine electro-oxidation[J].Composites Part B:Engineering,2018,144:11-18.
[5]Pagliaro M V,Bellini M,Filippi J,et al.Hydrogen production from the electrooxidation of methanol and potassium formate in alkaline media on carbon supported Rh and Pd nanoparticles[J].Inorganica Chimica Acta,2018,470:263-269.
[6]Zheng W,Man H W,Ye L,et al.Electroreduction of carbon dioxide to formic acid and methanol over a palladiumpolyaniline catalyst in acidic solution:a study of the palladium Size effect[J].Energy Technology,2017,5(6):937-944.
[7]Soleimani-Lashkenari M,Rezaei S,Fallah J,et al.Electrocatalytic performance of Pd-PANI-TiO2nanocomposites for methanol electrooxidation in alkaline media[J].Synthetic Metals,2018,235:71-79.
[8]Zheng W,Nayak S,Yuan W,et al.A tunable metal-polyaniline interface for efficient carbon dioxide electro-reduction to formic acid and methanol in aqueous solution[J].Chemical Communications,2016,52(96):13901-13904.
[9]Abdolahi A,Hamzah E,Ibrahim Z,et al.Synthesis of uniform polyaniline nanofibers through interfacial polymerization[J].Materials,2012,5(8),1487-1494.
[10]Wang Y L,Bian L,Tan D X,et al.Sonochemical synthesis of“sea-island”structure silver-polyaniline nanocomposites for the detection of L-tyrosine[J].Journal of Thermoplastic Composite Materials,2017,30(8):1033-1044.
[11]谭德新,王艳丽,卞玲,等.钯-聚苯胺复合团簇的可见光辅助溶致液晶模板合成及对乙醇的电催化[J].高分子材料科学与工程,2017,33(2):11-15.
[12]Mirzaagha B.Aqueous dispersions of DBSA-doped polyaniline:One-pot preparation,characterization,and properties study[J].Journal of Applied Polymer Science,2009,113(6):3980-3984.
[13]Deep A,Saraf M,Bharadwaj SK,et al.Styrene sulphonic acid doped polyaniline based immunosensor for highly sensitive impedimetric sensing of atrazine[J].Electrochimica Acta,2014,146:301-306.
[14]Xia Y,Wiesinger J M,MacDiarmid A G,et al.Camphorsulphonic acid fully doped polyaniline emeraldine salt:conformations in different solvents studied by an ultraviolet-visible-near-infrared spectroscopic method[J].Chemistry of Materials,1995,7(3):443-445.
[15]周兆懿,赵亚萍,蔡再生,等.纤维表面不同无机酸掺杂聚苯胺的制备及表征[J].化工进展,2010,29(5):909-913.
[16]Qiu Y,Xin L,Chadderdon D J,et al.Integrated electrocatalytic processing of levulinic acid and formic acid to produce biofuel intermediate valeric acid[J].Green Chemistry,2014,16(3):1305-1315.
[17]Kibsgaard J,Gorlin Y,Chen Z,et al.Meso-structured platinum thin films:active and stable electrocatalysts for the oxygen reduction reaction[J].Journal of The American Chemical Society,2012,134(18):7758-7765.
[18]Peng C,Hu Y,Liu M,et al.Hollow raspberry-like PdAg alloy nanospheres:high electrocatalytic activity for ethanol oxidation in alkaline media[J].Journal of Power Sources,2015,278:69-75.