納米多孔Pd基燃料電池催化劑乙醇氧化反應(yīng)及氧氣還原反應(yīng)催化性能研究
發(fā)布時間:2018-05-31 04:17
本文選題:鈀 + 乙醇 ; 參考:《中國礦業(yè)大學(xué)》2017年碩士論文
【摘要】:直接醇類燃料電池(DEFC)因其具有高的功率密度,燃料存儲安全方便,以及環(huán)境友好等優(yōu)點(diǎn),受到了研究者的廣泛關(guān)注和研究。DEFC在投入到商業(yè)化生產(chǎn)中,仍面臨挑戰(zhàn),如電極動力學(xué)慢,有機(jī)小分子等材料能量密度低,容易引起催化劑中毒等。為降低燃料電池成本、提高催化劑利用效率,Pd基催化劑的研究受到重視。本文采用熔體快淬結(jié)合去合金化法制備了納米多孔PdM(NP-PdM)催化劑,其中M為Mn,Y,Ce,Ta,Nb,通過X射線粉末衍射(XRD),X射線光電子能譜分析(XPS),掃描電子顯微鏡(SEM),能量散射光譜(EDS),透射電子顯微鏡(TEM)對材料進(jìn)行表征,并研究了其在堿性條件下對乙醇氧化反應(yīng)(EOR)和氧還原(ORR)的電催化活性。主要研究內(nèi)容和結(jié)論如下:采用電弧熔煉和熔體快淬的方法制備了Pd_(15)Mn_5Al_(80)、Pd_(15)Y_5Al_(80)、Pd_(15)Ce_5Al_(80)、Pd_(15)Ta_5Al_(80)和Pd_(15)Nb_5Al_(80)合金條帶,用去合金化的方法制備出NP-PdMn、NP-PdY、NP-PdCe、NP-PdTa、NP-PdNb催化劑,并用XRD、XPS、SEM和TEM等測試方法對其結(jié)構(gòu)、形貌及組成進(jìn)行了分析。結(jié)果表明制備的催化劑具有納米多孔結(jié)構(gòu),孔徑約為5到10 nm左右。M金屬的加入使得催化劑的EOR催化活性得到了顯著提高,結(jié)果顯示:NP-PdMn(64.9 m2/g)、NP-PdY(34.8m2/g)、NP-PdCe(32.7 m2/g)、NP-PdTa(489.8 m2/g)、NP-PdNb(153.3 m2/g)催化劑的電化學(xué)活性面積分別約為商業(yè)Pd/C(11.7 m2/g)的5.5倍、3.0倍、2.9倍、41.8倍和13.1倍。加入乙醇后的峰值電流密度分別為760.0 mAmg-1、1420.0mAmg-1、1045.1 m Amg-1、1901.8 mAmg-1、587.9 mAmg-1,約為商業(yè)Pd/C(400.0mAmg-1)的1.9倍、3.6倍、2.6倍、4.8倍和1.5倍。起峰電位分別移動了230 mV、190 mV、120 mV、270 mV和170 mV。在EOR穩(wěn)定性測試結(jié)果顯示,NP-PdMn、NP-PdY、NP-PdCe、NP-PdTa、NP-PdNb催化劑的穩(wěn)定性優(yōu)于商業(yè)Pd/C催化劑。在對NP-PdCe、NP-PdTa、NP-PdNb催化劑的ORR催化性能測試結(jié)果顯示:三種催化劑與商業(yè)Pd/C催化劑的半波電位分別移動了53 m V、44 mV和44 mV,同時在電位為0.875 V時的質(zhì)量活性分別約為商業(yè)Pd/C催化劑的3.5倍、3.5倍和3.1倍。通過NP-PdCe、NP-PdTa、NP-PdNb催化劑循環(huán)5000圈測試后,半波電位分別移動了10 mV、1 mV和19 mV,表現(xiàn)出良好的穩(wěn)定性。這使得NP-PdMn、NP-PdY、NP-PdCe、NP-PdTa、NP-PdNb催化劑成為優(yōu)于商業(yè)Pd/C的直接醇類燃料電池陽極和陰極催化劑。
[Abstract]:Because of its advantages of high power density, convenient fuel storage, and environmental friendliness, direct alcohol fuel cell (DEFC) has been widely concerned and studied by researchers. DEFC is still facing challenges in commercial production, because of its advantages such as high power density, convenient fuel storage, and environmental friendliness. For example, the electrode dynamics is slow and the energy density of organic small molecules is low, which can easily lead to catalyst poisoning and so on. In order to reduce the cost of fuel cell and improve the utilization efficiency of catalyst, the research of PD based catalyst has been paid more attention. In this paper, nano-porous PdMN NP-PdM) catalysts were prepared by melt rapid quenching and dealloying. Among them, M is Mn-YYC CeTaNb. The materials were characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), energy scattering spectroscopy (EDS), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The electrocatalytic activities of EOR and ORR for ethanol oxidation under alkaline conditions were studied. 涓昏鐮旂┒鍐呭鍜岀粨璁哄涓,
本文編號:1958255
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