本文選題：燃料電池　切入點(diǎn)：雙金屬　出處：《湖南大學(xué)》2011年碩士論文

【摘要】：直接甲醇燃料電池(DMFC)采用甲醇為燃料,解決了困擾人們的氫氣的儲(chǔ)存,運(yùn)輸?shù)葐?wèn)題。當(dāng)前DMFC商業(yè)化面臨的主要問(wèn)題是Pt價(jià)格高,電催化劑活性低,電催化劑長(zhǎng)期穩(wěn)定性有待進(jìn)一步提高。本文從開發(fā)新型電催化劑和提高電催化劑催化活性入手,開展了多壁碳納米管(MWCNT)負(fù)載地Pd基和Pt基雙金屬催化劑的化學(xué)法制備和對(duì)甲醇的電催化氧化研究。研究工作主要包括如下三個(gè)方面: 1.利用HAuCl4溶液與新制的Pd膠發(fā)生置換反應(yīng),制備了六種原子比的Pd-Au雙金屬納米顆粒再負(fù)載于MWCNT上,制得MWCNT/Pd-Au雙金屬催化劑,通過(guò)透射電子顯微鏡(TEM),能量色散X-射線光譜(EDS)和紫外可見(jiàn)分光光度計(jì)(UV-vis)對(duì)制備的MWCNT/Pd-Au催化劑進(jìn)行了形貌表征,并采用循環(huán)伏安法考察了不同Au: Pd原子比MWCNT/Pd-Au催化劑對(duì)甲醇的電催化氧化性能。結(jié)果表明,所制備的6種MWCNT/Pd-Au雙金屬催化劑對(duì)甲醇氧化的催化性能都明顯優(yōu)于單一金屬催化劑MWCNT/Pd或MWCNT/Au的催化性能。Au: Pd原子比不同導(dǎo)致MWCNT/Pd-Au雙金屬催化劑的催化效果也不相同,隨著Au: Pd原子比數(shù)值的上升,MWCNT/Pd-Au雙金屬催化劑對(duì)甲醇氧化的催化活性先升后降,當(dāng)Au:Pd原子比為0.06時(shí),MWCNT/ Pd-Au雙金屬催化劑的催化活性最大且抗中毒性能最好。 2.在無(wú)還原劑存在的情況下,用HAuCl4溶液與負(fù)載在MWCNT上的Pd納米顆粒發(fā)生置換反應(yīng),制備了Pd: Au原子比不同的五種MWCNT/Pd-Au雙金屬納米顆粒,并應(yīng)用于堿性條件下甲醇的電催化氧化。通過(guò)等離子體發(fā)射光譜(ICP),TEM和EDS對(duì)制備的MWCNT/Pd-Au催化劑進(jìn)行了原子比和形貌的表征,用循環(huán)伏安法考察了不同Pd: Au原子比的MWCNT/Pd-Au催化劑對(duì)甲醇的電催化氧化性能,并與單一金屬催化劑MWCNT/Pd和MWCNT/Au的催化性能進(jìn)行比較。結(jié)果表明,制備的5種MWCNT/Pd-Au雙金屬催化劑對(duì)甲醇氧化的催化性能均優(yōu)于單一金屬催化劑MWCNT/Pd或MWCNT/Au的催化性能,Pd: Au原子比不同導(dǎo)致MWCNT/Pd-Au雙金屬催化劑催化效果也不相同,隨著Pd: Au原子比數(shù)值的上升,MWCNT/Pd-Au雙金屬催化劑對(duì)甲醇氧化的催化活性先升后降,當(dāng)Pd: Au原子比為48時(shí)MWCNT/Pd-Au雙金屬催化劑的催化活性最好且具有較好的抗中毒性能。 3.采用KBH4還原的方法在水溶液中制備了負(fù)載在MWCNT上的原子比為3:1的MWCNT/Pt-Cu,MWCNT/Pt-Ni和MWCNT/Pt-Co雙金屬催化劑,再利用HNO3溶解賤金屬的方法制備了比雙金屬催化劑反應(yīng)表面積更大的MWCNT/Pt(Cu),MWCNT/Pt(Co),MWCNT/Pt(Ni)催化劑,將這六種不同催化劑應(yīng)用于酸性條件下甲醇的電催化氧化。采用TEM考察了MWCNT/Pt(Cu)催化劑的形貌并與MWCNT/Pt-Cu進(jìn)行比較,采用循環(huán)伏安曲線和i-t曲線比較了這六種催化劑對(duì)甲醇電催化氧化的性能和抗中毒性能。結(jié)果表明,這六種催化劑都具有良好的酸性條件下電化學(xué)催化甲醇氧化的功能,MWCNT/Pt(Cu)催化劑具有最好的催化活性和較好的抗中毒能力。
[Abstract]:Direct methanol fuel cell (DMFC) uses methanol as fuel to solve the problems of hydrogen storage and transportation.At present, the main problems facing the commercialization of DMFC are the high price of Pt, the low activity of electrocatalyst, and the long-term stability of electrocatalyst need to be further improved.In this paper, the preparation and electrocatalytic oxidation of methanol with multi-walled carbon nanotubes (MWCNT) supported PD and Pt-based bimetallic catalysts were studied by developing new electrocatalysts and improving their catalytic activity.The research includes the following three main areas:1.Six kinds of Pd-Au bimetallic nanoparticles with different atomic ratios were prepared by substitution reaction of HAuCl4 solution with new PD colloid on MWCNT to prepare MWCNT/Pd-Au bimetallic catalyst.The morphology of the prepared MWCNT/Pd-Au catalyst was characterized by TEM, energy dispersive X- ray spectroscopy (EDS) and UV-vis spectrophotometer.The electrocatalytic oxidation of methanol over MWCNT/Pd-Au catalysts with different au: PD atomic ratios was investigated by cyclic voltammetry.The results showed that the catalytic performance of the six MWCNT/Pd-Au bimetallic catalysts for methanol oxidation was obviously better than that of single metal catalyst MWCNT/Pd or MWCNT/Au. The catalytic activity of MWCNT/Pd-Au bimetallic catalyst was also different due to the difference of atomic ratio of au: PD.The catalytic activity of MWCNT / Pd-Au bimetallic catalyst for methanol oxidation increased first and then decreased with the increase of au: PD atomic ratio. When the Au:Pd atom ratio was 0.06, the catalytic activity of MWCNT / Pd-Au bimetallic catalyst was the highest and the resistance to poisoning was the best.2.In the absence of reductant, five kinds of MWCNT/Pd-Au bimetallic nanoparticles with different PD: au atomic ratios were prepared by displacement reaction between HAuCl4 solution and PD nanoparticles loaded on MWCNT. The results were applied to the electrocatalytic oxidation of methanol under alkaline conditions.The atomic ratio and morphology of the prepared MWCNT/Pd-Au catalysts were characterized by TEM and EDS. The electrocatalytic oxidation of methanol over MWCNT/Pd-Au catalysts with different PD: au atomic ratios was investigated by cyclic voltammetry.The catalytic performance of MWCNT/Pd and MWCNT/Au was compared with that of single metal catalyst.The results showed that the catalytic performance of the five MWCNT/Pd-Au bimetallic catalysts for methanol oxidation was better than that of single metal catalyst MWCNT/Pd or MWCNT/Au. The catalytic performance of MWCNT/Pd-Au bimetallic catalyst was also different due to the difference of PD: au atom ratio.With the increase of PD: au atom ratio, the catalytic activity of MWCNT / Pd-Au bimetallic catalyst for methanol oxidation first increased and then decreased. When PD: au atom ratio was 48, the catalytic activity of MWCNT/Pd-Au bimetallic catalyst was the best and had better antipoisoning performance.3.The MWCNT / Pt-Cu MWCNT / Pt-Ni and MWCNT/Pt-Co bimetallic catalysts supported on MWCNT with an atomic ratio of 3:1 on MWCNT were prepared by KBH4 reduction method. The MWCNT / PtCT-Cu / MWCNT / MWCNT/Pt-Co bimetallic catalysts with larger surface area than bimetallic catalysts were prepared by the method of HNO3 dissolution.These six catalysts were applied to the electrocatalytic oxidation of methanol under acidic conditions.The morphology of MWCNT / PttCuCu catalyst was investigated by TEM and compared with that of MWCNT/Pt-Cu. The performance and antipoisoning performance of MWCNT / PtCuCu catalyst for methanol electrooxidation were compared by cyclic voltammetry curve and i-t curve.The results show that all of the six catalysts have the best catalytic activity and the ability to resist poisoning.
【學(xué)位授予單位】：湖南大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2011
【分類號(hào)】：O643.32;TM911.4

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