本文選題：鈀 + 醇類燃料電池��； 參考：《上海師范大學》2017年碩士論文

【摘要】：直接醇類燃料電池作為一種綠色高效的新型能源有望成為傳統(tǒng)化石燃料的理想替代物。貴金屬鉑(Pt)基催化劑是目前直接醇類燃料電池(DAFCs)領域最有效的催化劑,但其所面臨的成本較高、儲量有限、易中毒等問題嚴重制約了DAFCs的商業(yè)化進程。發(fā)展低成本、高性能的催化劑以減少鉑的用量、提高使用效率是解決鉑資源短缺、降低燃料電池成本、從而實現(xiàn)DAFCs商業(yè)化的關鍵。因此關于低含量鉑或無鉑催化劑方面的研究有著重要的實際意義。由于鈀(Pd)與Pt為同主族元素,電子差異僅為0.77%,大量的工作已經(jīng)研究了合成新穎、高效的鈀基燃料電池催化劑。其中需解決的問題是進一步探究提高鈀基催化劑的活性和利用率的實驗方案。本論文從制備技術、載體材料、材料形貌與結構的角度,系統(tǒng)探討了三種不同鈀基復合催化劑的設計與制備方法,針對其對于堿性介質(zhì)中的甲醇電催化性能進行了詳細的考察,并進行了相關機理的解釋。具體研究工作包括以下內(nèi)容:(一)利用多巴胺分子氧化自聚所形成的尺寸均一的聚多巴胺納米球為模板,制備了有序多孔的鈀/聚多巴胺納米花狀材料。聚多巴胺作為一種多功能材料包含羥基等官能基團,它的引入有利于在電催化反應中有效氧化除去一氧化碳等碳中間產(chǎn)物,進而顯著改善了催化劑的抗毒化能力。(二)采用溴化十六烷基吡啶作為形貌導向劑,通過優(yōu)化導向劑用量,反應溫度,前軀體配比等條件,利用一步水熱法成功合成了金鈀異質(zhì)結構。ICP測試結果顯示,最優(yōu)條件下制備的催化劑中Pd與Au的原子比為1/2,Au的引入大大提高了鈀的利用率,同時改善了催化性能,該催化劑相比商用催化劑催化活性提高了約7倍。(三)在植酸鈉(IP6)的保護下,首先利用水熱法合成氧化銅納米棒,其外圍的植酸鈉層可與PdCl42-充分結合,再通過還原反應制備了獨特的氧化亞銅修飾的鈀納米網(wǎng)狀材料。該納米網(wǎng)由尺寸10 nm左右的納米粒子融合而成。植酸鈉不僅起到橋聯(lián)劑作用,同時使該材料分散性良好,具有電化學表面積大,穩(wěn)定性好等特點。氧化亞銅與鈀之間的協(xié)同作用有利于催化性能的改善。該材料的催化活性分別是商用鈀碳以及鈀黑催化劑的2.73、3.03倍,并表現(xiàn)出了顯著增加的電化學穩(wěn)定性以及催化電流密度。
[Abstract]:As a new green and efficient energy, direct alcohol fuel cell is expected to be an ideal substitute for traditional fossil fuels. Precious metal Pt / Pt-based catalyst is the most effective catalyst in the field of direct alcohol fuel cell (DAFCs) at present, but its problems such as high cost, limited reserves and easy poisoning seriously restrict the commercialization process of DAFCs. Developing low cost and high performance catalysts to reduce the amount of platinum and improve the efficiency is the key to solve the shortage of platinum resources reduce the cost of fuel cells and realize the commercialization of DAFCs. Therefore, the research on low-content platinum or non-platinum catalysts has important practical significance. Since palladium (PD) and Pt are the same group elements, the electron difference is only 0.77. A lot of work has been done to study the synthesis of novel and efficient palladium based fuel cell catalysts. The problem to be solved is to further explore the experimental scheme to improve the activity and utilization of palladium-based catalysts. In this paper, three kinds of palladium based composite catalysts were designed and prepared from the angles of preparation technology, carrier materials, morphology and structure of materials, and the electrocatalytic properties of methanol in alkaline media were investigated in detail. The related mechanism is explained. The specific research work includes the following contents: (1) the ordered porous Palladium / Polydopamine nano-flower material was prepared by using the uniform size polydopamine nanospheres formed by the oxidation self-polymerization of dopamine molecule as template. Poly (dopamine), as a multifunctional material, contains functional groups such as hydroxyl groups. The introduction of polydopamine is beneficial to the removal of carbon monoxide and other carbon intermediates in electrocatalytic reactions, thus significantly improving the antipoisoning ability of the catalysts. (2) using hexadecylpyridine bromide as the morphometric guide, the heterogeneity of au and PD was successfully synthesized by one step hydrothermal method. The results of ICP test showed that, by optimizing the dosage of guidance agent, reaction temperature and the ratio of precursor to body, the heterostructure of au and PD was synthesized successfully by one step hydrothermal method. Under the optimum conditions, the PD / au atom ratio of 1 / 2 au in the catalyst greatly improved the utilization of palladium and the catalytic performance. The catalytic activity of the catalyst was about 7 times higher than that of the commercial catalyst. (3) under the protection of sodium phytate (IP _ 6), copper oxide nanorods were synthesized by hydrothermal method. The sodium phytate layer around the nanorods could be fully combined with PdCl _ 42-, and then a unique cuprous oxide modified palladium nano-network material was prepared by reduction reaction. The nanowet is composed of nanoparticles about 10 nm in size. Sodium phytate not only acts as a bridging agent, but also has good dispersion, large electrochemical surface area and good stability. The synergism between cuprous oxide and palladium is beneficial to the improvement of catalytic performance. The catalytic activity of this material is 2.73 times higher than that of commercial palladium carbon and palladium black catalyst respectively, and the electrochemical stability and catalytic current density of the catalyst are obviously increased.
【學位授予單位】：上海師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O643.36;TM911.4

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