本文選題：燃料電池 + 陽(yáng)極　； 參考：《大連理工大學(xué)》2017年博士論文

【摘要】：直接甲醇燃料電池(DMFC)具有理論能量密度高、液體燃料攜帶方便和系統(tǒng)結(jié)構(gòu)簡(jiǎn)單等優(yōu)勢(shì),在移動(dòng)電源和備用電源方面具有廣闊的應(yīng)用前景。但是,甲醇氧化過(guò)程(MOR)涉及六電子轉(zhuǎn)移,反應(yīng)過(guò)程復(fù)雜、過(guò)電位高、動(dòng)力學(xué)速率緩慢,因此研究和開(kāi)發(fā)高活性、高穩(wěn)定性的MOR電催化劑一直是DMFC研究的熱點(diǎn)和難點(diǎn)。PtRu催化劑是目前研究最為廣泛的MOR電催化劑,但其催化活性和穩(wěn)定性仍亟待進(jìn)一步提高。本論文采用改性傳統(tǒng)碳載體、制備新型碳載體和引入第三組元活性金屬組分等途徑提高了 PtRu基電催化劑的MOR活性和穩(wěn)定性,系統(tǒng)、深入地研究了催化劑微觀形貌、組成和結(jié)構(gòu)與其MOR性能之間的關(guān)系。通過(guò)間歇微波法合成了 WO_3-C和SnO_2-C兩種復(fù)合材料,并以該復(fù)合材料為載體制備了 PtRu/WO_3-C和PtRu/SnO_2-C催化劑,研究了 WO_3的摻雜量以及熱處理對(duì)催化劑活性和穩(wěn)定性的影響。與PtRu/C催化劑相比,PtRu/WO_3-C和PtRu/SnO_2-C催化劑均表現(xiàn)出較高的MOR活性,而且PtRu/WO_3-C的穩(wěn)定性明顯高于PtRu/SnO_2-C催化劑。PtRu/WO_3-C催化劑中WO_3的優(yōu)化含量為5 wt%。通過(guò)固相席夫堿反應(yīng)體系高溫?zé)峤夂桶睔飧邷靥幚砗铣闪藘煞N氮摻雜碳材料,并作為載體制備了 PtRu催化劑。研究了含氮前驅(qū)體熱解溫度、載體孔結(jié)構(gòu)、載體氮含量以及氮的類(lèi)型對(duì)PtRu催化劑活性和穩(wěn)定性的影響。其中,含氮前驅(qū)體在700℃熱解得到的氮摻雜碳具有較大的比表面積和氮含量(10.6 wt%),以此為載體的PtRu/C催化劑具有最高的MOR活性和穩(wěn)定性。利用軟模板法制備出三種不同孔徑的蠕蟲(chóng)孔狀介孔碳(WMCs),并作為載體制備了 PtRu催化劑。研究了 WMCs的孔徑對(duì)催化劑顆粒尺寸及催化性能的影響。研究發(fā)現(xiàn)WMCs載體的孔徑很大程度上影響了PtRu催化劑的MOR性能。WMCs載體孔徑大于PtRu顆粒直徑2倍時(shí),PtRu催化劑的電化學(xué)面積明顯增加,MOR性能高于商品化XC-72R負(fù)載的PtRu催化劑。以RuCu/C為硬模板,利用K_2PtCl_4與Cu之間的置換反應(yīng)并通過(guò)調(diào)節(jié)RuC13溶液的用量,制備出7種不同鉑釕比的PtxRuyCu/C三元空心催化劑。研究了不同PtRu原子比對(duì)甲醇氧化反應(yīng)的催化活性和穩(wěn)定性的影響規(guī)律。其中,Pt10Ru1Cu/C表現(xiàn)出最優(yōu)的MOR催化活性,Pt1Ru1Cu/C表現(xiàn)出最優(yōu)的抗毒化能力。
[Abstract]:Direct methanol fuel cell (DMFC) has many advantages, such as high theoretical energy density, convenient liquid fuel carrying and simple system structure, so it has a broad application prospect in mobile power supply and backup power supply. However, methanol oxidation process involves six-electron transfer, complex reaction process, high overpotential, slow kinetic rate, so the research and development of high activity, High stability MOR electrocatalyst has been a hot and difficult point in DMFC research. PtRu catalyst is the most widely studied MOR electrocatalyst, but its catalytic activity and stability still need to be improved. In this paper, the MOR activity and stability of PtRu based electrocatalysts were improved by using the modified traditional carbon carrier, the new carbon support and the introduction of the third component active metal component. The microcosmic morphology of the catalyst was studied in detail. The relationship between composition and structure and MOR performance. Two kinds of composite materials WO_3-C and SnO_2-C were synthesized by intermittent microwave method. PtRu/WO_3-C and PtRu/SnO_2-C catalysts were prepared on the basis of the composite materials. The effects of the doping amount of WO_3 and the heat treatment on the activity and stability of the catalysts were studied. Compared with the PtRu/C catalyst, the MOR activity of PtRuS / WO _ 3-C and PtRu/SnO_2-C catalysts were higher, and the stability of PtRu/WO_3-C was obviously higher than that of PtRu/SnO_2-C catalyst .PtRuWO3-C catalyst. The optimized content of WO_3 in the catalyst was 5 wt. Two kinds of nitrogen-doped carbon materials were synthesized by high temperature pyrolysis of solid Schiff base reaction system and high temperature treatment of ammonia, and PtRu catalysts were prepared as support. The effects of pyrolysis temperature, pore structure, nitrogen content and type of nitrogen on the activity and stability of PtRu catalyst were studied. The nitrogen-doped carbon obtained from the pyrolysis of nitrogen-containing precursors at 700 鈩，

本文編號(hào)：1836842