Preparation of functionalized graphene multilayer films supported Au catalyst and its electro-oxidation for hydrazine
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摘要: 以聚二甲基二烯丙基氯化铵功能化石墨烯(PDDA-GNs)和磷钼酸功能化石墨烯(PMo12-GNs)为原料,利用层层自组装法制备了功能化石墨烯多层膜({PDDA-GNs/PMo12-GNs}),以此多层膜为载体,通过恒电位电沉积法制备功能化石墨烯多层膜载金催化剂(Au/{PDDA-GNs/PMo12-GNs}n)。采用XRD、XPS和SEM等表征Au/{PDDA-GNs/PMo12-GNs}n催化剂的组成、结构和形貌。结果表明:实验成功制备了Au/{PDDA-GNs/PMo12-GNs}n催化剂,且多层膜载体改善了Au粒子的分散性。利用循环伏安(CV)、计时电流(It)和交流阻抗(EIS)等评价催化剂对肼氧化的电催化性能。结果表明,Au/{PDDA-GNs/PMo12-GNs}n催化剂使肼氧化的电催化活性和稳定性得到很大提高。与Au/玻碳电极(GCE)相比,Au/{PDDA-GNs/PMo12-GNs}n催化肼氧化反应的峰电流密度从0.46 mA/cm2提高到0.87 mA/cm2,600 s时的稳态电流密度是Au/GCE的2.5倍。Abstract: The multilayer films consisting of polydimethyldiallyl ammonium chloride functionalized graphene (PDDA-GNs) and phosphomolybdate functionalized graphene (PMo12-GNs) ({PDDA-GNs/PMo12-GNs}) were fabricated on the substrate by layer-by-layer self-assembly technique. The {PDDA-GNs/PMo12-GNs} multilayer films were used as catalyst carrier for electrodeposition of Au nanoparticles (Au/{PDDA-GNs/PMo12-GNs}n). The Au/{PDDA-GNs/PMo12-GNs}n fabricated catalyst was characterized by XRD, XPS and SEM. The results indicate that Au nanoparticles are uniformly-dispersed on the {PDDA-GNs/PMo12-GNs}n multilayer films. Cyclic voltammetry (CV), chronoamperometry (It) and electrochemical impedance spectra (EIS) analyses show that the Au/{PDDA-GNs/PMo12-GNs}n has high electrocatalytic activity and stability regarding hydrazine oxidation. Compared with Au/glassy carbon electrode (GCE), the hydrazine oxidation current density of Au/{PDDA-GNs/PMo12-GNs}n increases from 0.46 mA/cm2 to 0.87 mA/cm2. And the steady current density of the Au/{PDDA-GNs/PMo12-GNs}n catalyst is 2.5 times as high as the Au/GCE catalyst.
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图 1 功能化石墨烯多层膜载金(Au/{PDDA-GNs/PMo12-GNs}n)催化剂的制备示意图
Figure 1. Schematic illustration of preparation of functionalized graphene multilayer films supported Au(Au/{PDDA-GNs/PMo12-GNs}n) catalyst (PDDA-GNs—Polydimethyldiallyl ammonium chloride functionalized graphene;PMo12-GNs—Phosphomolybdate functionalized graphene)
图 8 {Au/PDDA-GNs/PMo12-GNs}n/GCE(a)和Au/GCE(b)在5 mmol/L [Fe(CN)6]3−/4−和0.1 mol/L KCl溶液中的交流阻抗图谱
Figure 8. Electrochemical impedance spectra of{Au/PDDA-GNs/PMo12-GNs}n/GCE(a) and Au/GCE(b) in 5 mmol/L [Fe(CN)6]3−/4− and 0.1 mol/L KCl solution(RΩ—Solution resistance; Rct—Charge transfer resistance; Cd—Electrical doule layer capacitor)
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