本文選題：直接甲醇燃料電池 + Pt基催化劑�。� 參考：《內(nèi)蒙古大學》2017年碩士論文

【摘要】：近年來,隨著經(jīng)濟的不斷發(fā)展,化石能源的使用日益增長。雖然改善了我們的生活質(zhì)量,但是同時也帶來了嚴重的環(huán)境污染。目前,我國出現(xiàn)大面積的霧霾天氣,給公民的身體健康帶來了嚴重的威脅。因此,開發(fā)一種綠色環(huán)保的能源迫在眉睫。直接甲醇燃料電池(DMFC)作為一種新型能源利用方式,反應過程中不排放污染物,是理想的化石能源的替代品。雖然鉑是目前DMFC的首選催化劑材料,但是它的催化性能低、持續(xù)性不長久以及價格高,嚴重阻礙了燃料電池的商業(yè)化。針對上面的問題,我們提出了一步法合成氧功能化碳復合的鉑及其合金催化劑催化甲醇氧化以及氧還原,具體內(nèi)容如下:1.在溶劑熱條件下,通過氯化甲烷和丙三醇兩相界面,成功合成了氧功能化的鉑碳復合結(jié)構(gòu)Pt@C-O,并且通過改變氯甲烷的種類,合成了三種不同形貌且含氧量不同的Pt@C-O催化劑。乙酰丙酮鉑、苯甲酸和氯仿丙三醇兩相是形成Pt@C-O結(jié)構(gòu)的關鍵因素。進一步測試,我們發(fā)現(xiàn)合成的催化劑,同商用Pt/C相比,表面有很多的C-O基團和Pt-0基團。最后,通過甲醇氧化電化學性能的測試,我們發(fā)現(xiàn)含氧量最高的催化劑Pt@C-O具有最好的電催化穩(wěn)定性以及抗一氧化碳中毒能力。2.在油浴中,二乙二醇二甲醚作為溶劑,150℃C回流,用NaBH4還原Pt(acac)2,Co(acac)2以及Ni(acac)2,合成了氧功能化碳復合PtNi@C-O二元合金以及PtNiCo@C-O三元合金。其中,利用NaCl來調(diào)控晶粒的尺寸以及溶劑碳化形成核殼結(jié)構(gòu)是很新穎的合成方法。最后,通過甲醇氧化和氧還原電化學性能的測試,我們發(fā)現(xiàn)氧功能化碳復合的合金比20%wt.商用Pt/C具有更好的電催化性能以及抗一氧化碳中毒能力,并且三元合金的催化效率最高。3.為了進一步增加催化劑中功能化碳的含量,在油浴中,我們使用聚乙二醇為溶劑,160℃回流,用NaBH4還原Pt(acac)2,Co(acac)2以及Ni(acac)2,合成了具有更高含量的類石墨烯層狀氧功能化碳負載的PtNi/C-O二元合金以及PtNiCo/C-O三元合金。通過甲醇氧化以及氧還原電化學性能的測試,我們發(fā)現(xiàn)氧功能化碳復合的PtNi/C-O二元合金比20 wt.%的商用Pt/C以及前面所得的所有催化劑具有更好的電催化性能。說明更高的C-O含量以及類石墨烯結(jié)構(gòu)都有助于電化學性能的提高。但是當C-O含量繼續(xù)升高,如PtNiCo/C-O三元合金,其在電催化過程出現(xiàn)強烈的產(chǎn)氫現(xiàn)象,說明甲醇氧化對C-O基團的含量具有極限值要求。
[Abstract]:In recent years, with the development of economy, the use of fossil energy is increasing day by day. Although it has improved our quality of life, it has also brought serious environmental pollution. At present, there is a large area of haze weather in China, which brings a serious threat to the health of citizens. Therefore, it is urgent to develop a green energy source. Direct methanol fuel cell (DMFC), as a new energy utilization mode, is an ideal alternative to fossil energy because it does not emit pollutants during the reaction. Although platinum is the preferred catalyst material for DMFC at present, its low catalytic performance, short duration and high price seriously hinder the commercialization of fuel cells. In order to solve the above problems, we proposed a one-step method for the synthesis of oxygen functionalized carbon composite platinum and its alloy catalysts for methanol oxidation and oxygen reduction. The specific contents are as follows: 1. Under solvothermal conditions, a platinum-carbon composite structure PtC-O with oxygen functionalization was successfully synthesized through the two-phase interface between methane chloride and glycerol. Three kinds of Pt@C-O catalysts with different morphology and different oxygen content were synthesized by changing the kinds of chloromethane. Acetylacetone platinum, benzoic acid and chloroform glycerol are the key factors for the formation of Pt@C-O structure. Further tests show that there are many C-O and Pt-0 groups on the surface of the synthesized catalyst compared with commercial Pt/C. Finally, through the electrochemical performance test of methanol oxidation, we found that the catalyst Pt@C-O with the highest oxygen content has the best electrocatalytic stability and the ability of resisting carbon monoxide poisoning. In the oil bath, diethylene glycol dimethyl ether (DME) was refluxed at 150 鈩，

本文編號：1880463