Pt基及Pd基催化劑的制備及其對葡萄糖電催化氧化性能研究
本文選題:Pt基催化劑 切入點:Pd基催化劑 出處:《煙臺大學(xué)》2017年碩士論文 論文類型:學(xué)位論文
【摘要】:葡萄糖是自然界中最豐富的單糖,有較高的理論能量值,被完全氧化可釋放約2870k J/mol的能量,從中獲得有用的化學(xué)能轉(zhuǎn)化為電能是一種很好的選擇,故被廣泛的應(yīng)用于工業(yè)生產(chǎn)。貴金屬Pt、Pd是最為常見的直接燃料電池的陽極催化劑材料,然而Pt、Pd基催化劑存在易中毒、利用率低、成本高等缺點。本論文通過向貴金屬Pt、Pd中添加過渡金屬制備二元合金催化劑,然后對載體進行改性的方法,來提高催化劑的催化性能、增強其抗CO中毒性能,并降低其使用成本。我們系統(tǒng)的研究了所制備的催化劑在葡萄糖直接燃料電池(DGCE)中的應(yīng)用。通過XRD、TEM、XPS以及多種電化學(xué)測試手段對所制備的催化劑的結(jié)構(gòu)及活性穩(wěn)定性進行了表征和測試。其具體研究內(nèi)容概括如下:1.通過乙二醇浸漬還原方法向Pt催化劑中添加第二種金屬Sn制備一系列Pt-Sn/C催化劑。通過控制Pt量、溶液p H和Pt/Sn原子比等條件制備不同的催化劑探究它們對葡萄糖電催化氧化能力的大小。結(jié)果表明,在Pt的負(fù)載量為5%、溶液p H=9以及Pt/Sn原子比為3時催化劑的催化性能最好。2.在以上條件下,添加Ni、Co兩種過渡金屬,同樣采用乙二醇浸漬還原法制備Pt-M/C催化劑,對比不同金屬對催化劑催化性能的影響,對比發(fā)現(xiàn)Pt3Sn1/CPt3Ni1/CPt3Co1/CPt/C;本小節(jié)實驗在此基礎(chǔ)上又采用殼聚糖(CHI)對載體進行改性制備CHI不同負(fù)載量的Pt3Sn1/C-CHI。結(jié)果表明:殼聚糖修飾量為1%時,催化劑催化性能較好;繼續(xù)向Pt/C-CHI催化劑中添加第二金屬Ni、Co,得出Pt3Sn1/C-CHIPt3Co1/C-CHIPt3Ni1/C-CHIPt3Sn1/CPt/C-CHIPt/C。3.通過硼氫化鈉還原法制備Pd-Co/C二元金屬催化劑,通過改變Pd負(fù)載量、溶液p H及Pd/Co原子比,尋找催化劑催化葡萄糖氧化的規(guī)律。結(jié)果表明催化劑在Pd負(fù)載量為5%,溶液p H=9,Pd/Co原子比為3時表現(xiàn)出較好的催化性能;同時XRD、TEM、XPS及ESCA等結(jié)果表明:第二金屬Co的加入減小了Pd2+濃度,增加了Pd0百分含量,提高了Pd的分散度與電化學(xué)活性表面積,從而提高了Pd的利用率及其催化性能。
[Abstract]:Glucose is the most abundant monosaccharide in nature. It has a high theoretical energy value. Completely oxidized can release about 2870 k J / mol of energy, and it is a good choice to obtain useful chemical energy and convert it into electric energy. Therefore, it is widely used in industrial production. Precious metal PTO PD is the most common anode catalyst material for direct fuel cell. In this paper, binary alloy catalyst was prepared by adding transition metal to precious metal PtPd, and then modified the support to improve the catalytic performance of the catalyst and enhance its resistance to CO poisoning. We systematically studied the application of the prepared catalyst in glucose direct fuel cell (DGCE). The structure and activity of the prepared catalyst were stable by XRDX TEMX XPS and various electrochemical methods. The properties were characterized and tested. The specific research contents were summarized as follows: 1. A series of Pt-Sn/C catalysts were prepared by adding a second metal Sn to Pt catalyst by dipping reduction method of ethylene glycol. Preparation of different Catalysts for glucose Electrocatalytic Oxidation of glucose under different conditions such as pH and Pt/Sn Atomic ratio. The results show that, Under the conditions of Pt loading of 5, solution pH 9 and Pt/Sn atom ratio 3:00, the catalyst has the best catalytic performance. Under the above conditions, the Pt-M/C catalyst was prepared by glycol impregnation reduction with the addition of two transition metals. Comparing the effects of different metals on the catalytic performance of the catalyst, it was found that Pt3Sn1 / CPt3Ni1 / CPt3Co1 / CPt3Co1 / CPT / C; on the basis of this experiment, chitosan was used to modify the support to prepare Pt3Sn1 / C-CHI with different amounts of CHI. The results showed that when the amount of chitosan modified was 1%, The catalytic performance of the catalyst was better, and the second metal NiancoCo was added to the Pt/C-CHI catalyst, and it was obtained that Pt3Sn1 / C-CHIPt3Co1 / C-CHIPt3Ni1 / C-CHIPt3Sn1 / C-CHIPt1 / C.3.The binary Pd-Co/C catalyst was prepared by sodium borohydride reduction method, and the catalyst was prepared by changing the PD loading, solution pH and Pd/Co atomic ratio. The results showed that the catalyst exhibited good catalytic performance at PD loading of 5 and the atomic ratio of PD / Co in solution was 3:00. The results of XRD-Tem XPS and ESCA showed that the concentration of Pd2 decreased with the addition of the second metal Co. The percentage content of Pd0 was increased, the dispersion of PD and the surface area of electrochemical activity were increased, thus the utilization ratio of PD and its catalytic performance were improved.
【學(xué)位授予單位】:煙臺大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:O643.36;TM911.4
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