發(fā)布時間：2018-11-12 20:07

【摘要】：質(zhì)子交換膜燃料電池(PEMFC)具有結(jié)構(gòu)簡單、比能量高、對環(huán)境友好等特點(diǎn),可用于小型電站及便攜式移動電源領(lǐng)域。然而,PEMFC陰陽極催化劑性能不佳,使其性能與商業(yè)化的要求仍有較大差距。因此,制備高性能陰陽極催化劑是PEMFC研究的一個重要課題。本文利用過渡金屬氰膠作為前驅(qū)體,制備了具有三維網(wǎng)狀結(jié)構(gòu)的多孔Pt基電催化劑,并研究了它們對甲醇氧化、氧氣還原的電催化性能。主要研究結(jié)果如下：1.雙貴金屬K2PdCl4/K2Pt(CN)4氰膠為具有三維骨架結(jié)構(gòu)的深黃色果凍狀,可以通過混合K2PdCl4和K2Pt(CN)4制備得到。利用K2PdCl4/K2Pt(CN)4氰膠作為反應(yīng)前驅(qū)體,三維珊瑚狀Pd-Pt合金納米結(jié)構(gòu)物可以通過簡單的NaBH4還原法反應(yīng)得到,而這種方法沒有表面活性劑和模板劑。Pd-Pt合金納米結(jié)構(gòu)物的尺寸,形貌和表面組成通過掃描電子顯微鏡(SEM),透射電子顯微鏡(TEM),選區(qū)電子衍射(SAED),能量散射光譜(EDX),EDX面掃,X射線衍射(XRD),X射線光電子能譜(XPS)等表征進(jìn)行研究。由于Pd-Pt合金納米結(jié)構(gòu)物獨(dú)特的三維互聯(lián)結(jié)構(gòu),電子效應(yīng)和協(xié)同效應(yīng),與商業(yè)化Pt和Pd黑相比,它對乙醇氧化有著優(yōu)異的電催化活性和穩(wěn)定性。2.三元K2PtCl4/K3Co(CN)6-K2PdCl4/K3Co(CN)6混合氰膠可以通過混合K2PtCl4、K2PdCl4、K3Co(CN)6制備得到。直接以NaBH4為還原劑可以制備出高合金化程度的三維Pt-Pd-Co三元合金納米網(wǎng)。三維Pt-Pd-Co三元合金納米網(wǎng)的大小,形貌和表面成分通過掃描電子顯微鏡(SEM),透射電子顯微鏡(TEM),選區(qū)電子衍射(SAED),能量散射能譜(EDX),X射線衍射(XRD)和X射線光電子能譜(XPS)等表征進(jìn)行研究。由于Pt-Pd-Co三元合金納米網(wǎng)獨(dú)特的三維結(jié)構(gòu),電子效應(yīng)和協(xié)同效應(yīng),與商業(yè)化Pt黑相比,三維Pt-Pd-Co三元合金納米網(wǎng)對氧還原反應(yīng)顯示出更高的電催化活性和穩(wěn)定性。3. K2PdCl4/K2Ni(CN)4首先通過混合K2PdCl4和K2Ni(CN)4制備得到。直接用NaBH4作為還原劑制備出PdNi合金納米網(wǎng),再通過Galvanic取代反應(yīng)合成富Pt的殼層以得到三維多孔PdNi@Pt核殼結(jié)構(gòu)物。PdNi@Pt核殼結(jié)構(gòu)物的尺寸,形貌和表面組成通過掃描電子顯微鏡(SEM),透射電子顯微鏡(TEM),選區(qū)電子衍射(SAED),能量散射光譜(EDX), EDX面掃,X射線衍射(XRD),X射線光電子能譜(XPS)等表征進(jìn)行研究。由于PdNi@Pt核殼結(jié)構(gòu)物獨(dú)特的三維結(jié)構(gòu),電子效應(yīng),與商業(yè)化Pt黑相比,PdNi@Pt核殼結(jié)構(gòu)物對甲醇氧化反應(yīng)有極高的質(zhì)量活性和穩(wěn)定性。
[Abstract]:Proton exchange membrane fuel cell (PEMFC) has the advantages of simple structure, high specific energy and environmental friendliness. It can be used in the field of small power plants and portable mobile power sources. However, the performance of PEMFC cathode catalyst is not good enough to meet the requirements of commercialization. Therefore, the preparation of high performance cathode and cathode catalysts is an important subject of PEMFC research. In this paper, porous Pt based electrocatalysts with three-dimensional reticular structure were prepared by using transition metal cyanide as precursors, and their electrocatalytic properties for methanol oxidation and oxygen reduction were studied. The main results are as follows: 1. Double precious metal K2PdCl4/K2Pt (CN) 4 cyanide gum is a dark yellow jelly with three dimensional skeleton structure, which can be prepared by mixing K2PdCl4 and K2Pt (CN) 4. Using K2PdCl4/K2Pt (CN) _ 4 cyanide as the precursor of the reaction, the three-dimensional coral-like Pd-Pt alloy nanostructures can be obtained by simple NaBH4 reduction method. The size, morphology and surface composition of the nanostructures of Pd-Pt alloys were characterized by scanning electron microscopy (SEM), (SEM), transmission electron microscope (TEM), selective electron diffraction (SAED),). The energy scattering spectra were characterized by (EDX), EDX surface scan and X ray diffraction (XRD), X ray photoelectron spectroscopy (XPS). Because of the unique three-dimensional interconnecting structure, electronic effect and synergistic effect of Pd-Pt alloy nanostructures, it has excellent electrocatalytic activity and stability for ethanol oxidation compared with commercial Pt and Pd black. 2. Ternary K2PtCl4/K3Co (CN) 6-K2PdCl4/K3Co (CN) 6 mixed cyanide gum can be prepared by mixing K2PtCl4K2PdCl4K3Co (CN) 6. Three dimensional Pt-Pd-Co ternary alloy nanowires with high alloying degree can be prepared by using NaBH4 as reducing agent. The size, Morphology and Surface composition of Three-Dimensional Pt-Pd-Co Ternary Alloy Nanonets by scanning Electron microscope, (SEM), Transmission Electron microscope, (TEM), selective Electron diffraction (SAED), Energy scattering Spectroscopy (EDX), X-ray diffraction (XRD) (XRD) and X-ray photoelectron spectroscopy (XPS) were studied. Due to the unique three-dimensional structure, electronic effect and synergistic effect of Pt-Pd-Co ternary alloy nanowires, compared with commercial Pt black, Three-dimensional Pt-Pd-Co alloy nanowires showed higher electrocatalytic activity and stability for oxygen reduction. K2PdCl4/K2Ni (CN) _ 4 was first prepared by mixing K2PdCl4 and K2Ni (CN) _ 4. The PdNi alloy nanowires were prepared by using NaBH4 as reductant, and then the shell layer rich in Pt was synthesized by Galvanic substitution reaction to obtain the three-dimensional porous PdNi@Pt core-shell structure. The size of PdNi@Pt core-shell structure was obtained. Morphology and surface composition by scanning electron microscope, (SEM), transmission electron microscope, (TEM), selective electron diffraction, (SAED), energy scattering spectrum, (EDX), EDX surface scanning, X ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) was studied. Because of the unique three-dimensional structure and electronic effect of PdNi@Pt core-shell structure, compared with commercial Pt black, PdNi@Pt core-shell structure has high mass activity and stability for methanol oxidation.
【學(xué)位授予單位】：南京師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：O643.36;TM911.4

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