堿性介質中醇類電氧化Pd系催化劑的制備及性能研究
發(fā)布時間:2018-05-28 13:29
本文選題:堿性介質 + 直接醇類燃料電池。 參考:《沈陽理工大學》2015年碩士論文
【摘要】:直接醇類燃料電池(DAFC)因能量轉化效率高、燃料來源豐富、儲運方便、成本低廉等優(yōu)點而受到人們的廣泛關注。陽極催化劑的研制是直接醇類燃料電池的關鍵。為提高堿性介質中Pd系催化劑對醇類的催化活性和穩(wěn)定性,本文以炭材料為載體、乙二醇為還原劑,采用微波輔助合成法制備催化劑,通過引入其他金屬粒子、使用不同類型導電聚合物修飾載體以及使用混合載體提高催化劑的活性和穩(wěn)定性。采用透射電子顯微鏡(TEM)、X-射線光電子能譜(XPS)手段對催化劑的微觀形貌、組成及結構進行表征。以循環(huán)伏安法(CV)、線性掃描伏安法(LSV)、電化學阻抗譜(EIS)及計時電流法(CA)等電化學方法考察催化劑對堿性介質中醇類電氧化反應中的催化活性及穩(wěn)定性。主要研究結果如下:向Pd/CNTs催化劑中引入Ni、Fe、Cu金屬粒子,合金粒子較Pd粒子分散性得到改善、粒徑較小。Ni、Fe、Cu粒子能夠提高Pd/CNTs催化劑對醇的電催化性能。Ni、Fe、Cu與Pd粒子均顯示出雙功能效應。殼聚糖(Chit)和聚二烯二甲基氯化銨(PDDA)修飾載體后制備的催化劑中Pd粒子粒徑較小,幾乎無團聚現(xiàn)象,且Pd(0)含量較高。相比于基礎催化劑,Pd/C-Chit和Pd/CNTs-PDDA催化劑顯示出優(yōu)良的醇電催化氧化性能。聚吡咯修飾載體制備的催化劑中Pd粒子粒徑較小,粒徑分布范圍較小。聚吡咯提高了醇在Pd/C催化劑上電氧化的催化性能。相比于Pd/C催化劑,PANI@Pd/C催化劑的催化性能未能得到全面改善。使用石墨烯納米片-碳納米管和石墨烯納米片-炭黑改善Pd粒子的分散性,使粒徑減小。相比于單一載體催化劑,使用混合載體制備的催化劑提高了催化劑對醇的電催化氧化性能。
[Abstract]:Direct alcohol fuel cell (DAFC) has been widely concerned because of its high energy conversion efficiency, abundant fuel sources, convenient storage and transportation, low cost and so on. The development of anode catalyst is the key of direct alcohol fuel cell. In order to improve the catalytic activity and stability of PD catalyst for alcohols in alkaline medium, the catalyst was prepared by microwave assisted synthesis with carbon material as support and ethylene glycol as reducing agent. Other metal particles were introduced into the catalyst. The activity and stability of the catalyst were improved by using different types of conductive polymer modified support and mixed support. The microstructure, composition and structure of the catalyst were characterized by means of transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The catalytic activity and stability of the catalysts for the electrooxidation of alcohols in alkaline media were investigated by cyclic voltammetry, linear scanning voltammetry, electrochemical impedance spectroscopy (EIS) and chronoamperometric method (CAA). The main results are as follows: the Pd/CNTs catalyst was introduced into the Pd/CNTs catalyst, the dispersion of the alloy particles was improved than that of the PD particles, and the particle size was smaller than that of the PD particles. The electrocatalytic activity of the Pd/CNTs catalyst for alcohols was improved. Both NiFE-Fe Cu and PD particles showed a bifunctional effect. The particle size of PD particles was small, almost no agglomeration, and the content of PD _ 0) was higher in the catalysts modified with chitosan (Chitt) and polydiene dimethyl ammonium chloride (PDDA-PDDA). Compared with the basic catalysts, PD / C-Chit and Pd/CNTs-PDDA catalysts showed excellent catalytic oxidation of alcohols. The particle size and distribution range of PD particles in the catalyst prepared by polypyrrole modified support were smaller. Polypyrrole improved the catalytic performance of alcohol electrooxidation on Pd/C catalyst. Compared with Pd/C catalyst, the catalytic performance of Pani @ PD / C catalyst has not been completely improved. Graphene nanoparticles-carbon nanotubes and graphene nanoparticles-carbon black were used to improve the dispersion of PD particles and reduce the particle size. Compared with single support catalyst, the electrocatalytic oxidation of alcohol was improved by using mixed support catalyst.
【學位授予單位】:沈陽理工大學
【學位級別】:碩士
【學位授予年份】:2015
【分類號】:O643.36;TM911.4
【參考文獻】
相關期刊論文 前1條
1 衣寶廉;燃料電池的原理、技術狀態(tài)與展望[J];電池工業(yè);2003年01期
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