本文選題：直接甲醇燃料電池　切入點：Pd　出處：《齊齊哈爾大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：在直接甲醇燃料電池(direct methanol fuel cellDMFC)中,催化劑對其催化性能起到了關(guān)鍵性作用,目前最常用的催化材料是鉑(Pt)基催化劑,由于Pt的資源匱乏,價格昂貴且會在甲醇電氧化過程中生成中間產(chǎn)物CO等物質(zhì)而中毒導(dǎo)致活性下降,且DMFC的成本較高,限制了其大規(guī)模的應(yīng)用。本文以Pd為基礎(chǔ)材料,復(fù)合了幾種物質(zhì)作催化劑材料,研究其對甲醇的電催化性能及電化學(xué)穩(wěn)定性。本文制備了鈀/石墨烯(Pd/RGO)、鈀/聚二甲基二烯丙基氯化銨-石墨烯(Pd/PDDA-RGO)、鈀/氧化鎂-石墨烯(Pd/MgO-RGO)和鈀/氧化鎂-聚二甲基二烯丙基氯化銨-石墨烯(Pd/MgO-PDDA-RGO)四種催化劑,并利用透射電子顯微鏡(TEM)和X-射線衍射(XRD)對其進行表征,利用循環(huán)伏安法(CV)和計時電流法(CA)研究其對甲醇的電化學(xué)行為。正向陽極峰電流密度(If)/反向陽極峰電流密度(Ib)的值可反映甲醇的氧化率以及中間含碳物質(zhì)的中毒耐受性。Pd/RGO、Pd/PDDA-RGO、Pd/MgO-RGO和Pd/MgO-PDDA-RGO的If/Ib值分別為1.57、1.68、2.87和3.23且If/Ib值依次增大,結(jié)果表明,Pd/MgO-PDDA-RGO表現(xiàn)出更高的電催化活性和更好的CO中毒耐受性。第n次循環(huán)正向陽極峰電流密度(In)/第一次循環(huán)正向陽極峰電流密度(I0)的值可評價催化劑的長期穩(wěn)定性,在1000次循環(huán)之后,Pd/MgO-PDDA-RGO、Pd/MgO-RGO、Pd/PDDA-RGO和Pd/RGOIn/I0值分別為83%、78%、71%和69%且依次減小,結(jié)果表明,Pd/MgO-PDDA-RGO表現(xiàn)出更高的電催化性能以及更好的穩(wěn)定性。本文制備了鈀/石墨烯(Pd/RGO)和鈀/乙二銨四乙酸-石墨烯(Pd/EDTA-RGO)兩種催化劑,利用循環(huán)伏安法(CV)和計時電流(CA)研究其對甲醇的電化學(xué)行為。Pd/EDTA-RGOIf/Ib值是Pd/RGOIf/Ib值的1.08倍,表明Pd/EDTA-RGO表現(xiàn)出更高的電催化活性和更好的CO中毒耐受性。在1000次循環(huán)之后Pd/EDTA-RGOIn/I0值是79%高于Pd/RGO In/I0值的69%,結(jié)果表明,Pd/EDTA-RGO表現(xiàn)出更高的電催化性能以及更好的穩(wěn)定性。比較Pd/MgO-PDDA-RGO和Pd/EDTA-RGO對甲醇的電催化性及穩(wěn)定性,Pd/MgO-PDDA-RGO的If/Ib值是EDTA/Pd-RGO的If/Ib值的2.56倍,在1000次循環(huán)之后Pd/MgO-PDDA-RGO In/I0值為83%高于EDTA/Pd-RGO In/I0值的79%,表明Pd/MgO--PDDA-RGO對甲醇的電催化性更高且有更好的長期循環(huán)穩(wěn)定性。
[Abstract]:In direct methanol fuel cell DMFCs, the catalyst plays a key role in its catalytic performance. At present, the most commonly used catalyst is platinum-based catalyst, due to the lack of Pt resources. Due to the high cost and poisoning of intermediate products such as CO in the process of methanol electrooxidation, the activity of DMFC is decreased, and the cost of DMFC is high, which limits its application on a large scale. In this paper, PD is used as the basic material. Several substances were used as catalyst materials, The electrocatalytic properties and electrochemical stability of palladium / graphene (PD / graphene), palladium / poly (dimethyldiallylammonium chloride) graphene (PD / PDDA-RGOO), palladium / magnesium oxide-graphene (PD / MgO-RGOO) and palladium / magnesium oxide (PD / MgO-RGOO) were prepared. Diallyl ammonium chloride-graphene (PD / MgO-PDDA-RGO) four kinds of catalysts, It was characterized by transmission electron microscopy (TEM) and X-ray diffraction (XRD). The electrochemical behavior of methanol was studied by cyclic voltammetry (CV) and chronoamperometric method (CACA). The values of forward anodic peak current density / reverse anodic peak current density can reflect the oxidation rate of methanol and the poisoning of middle carbonaceous substance. The If/Ib values of PD / PDDA-RGON PD / RGOO / PD / MgO-RGO and Pd/MgO-PDDA-RGO were 1.57 / 1.682.87 and 3.23, respectively, and the If/Ib values increased in turn. The results show that PD / MgO-PDDA-RGO exhibits higher electrocatalytic activity and better tolerance to CO poisoning. The value of the nth cycle forward anode peak current density / the first cycle forward anode peak current density (I _ 0) can be used to evaluate the long-term stability of the catalyst. After 1, 000 cycles, the PD / MgO-PDDA-RGON / PD / MgO-RGOG / PD / PDDA-RGO and Pd/RGOIn/I0 values were 83% and 69%, respectively, and decreased in turn. The results show that PD / MgO-PDDA-RGO has higher electrocatalytic performance and better stability. In this paper, palladium / graphene (PD / RGO) and palladium / diammonium tetraacetic acid-graphene (PD / EDTA-RGO) catalysts were prepared. Cyclic voltammetry (CV) and chronoelectric current (CAA) were used to study the electrochemical behavior of methanol. The value of PD / EDTA-RGOIf / Ib was 1.08 times that of Pd/RGOIf/Ib. The results showed that Pd/EDTA-RGO showed higher electrocatalytic activity and better tolerance to CO poisoning. After 1 000 cycles, the Pd/EDTA-RGOIn/I0 value was 79% higher than that of Pd/RGO In/I0. The results showed that PD / EDTA-RGO showed higher electrocatalytic activity and better stability. The electrocatalytic activity and stability of Pd/MgO-PDDA-RGO and Pd/EDTA-RGO to methanol were 2.56 times of the If/Ib value of EDTA/Pd-RGO, and the If/Ib value of PD / MgO-PDDA-RGO was 2.56 times higher than that of EDTA/Pd-RGO. After 1 000 cycles, the Pd/MgO-PDDA-RGO In/I0 value of 83% is higher than that of EDTA/Pd-RGO In/I0, which indicates that Pd/MgO--PDDA-RGO has higher electrocatalysis and better long-term cycle stability for methanol.
【學(xué)位授予單位】：齊齊哈爾大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TQ426;TM911.4

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