本文選題：燃料電池　切入點(diǎn)：氧還原反應(yīng)　出處：《聊城大學(xué)》2017年碩士論文

【摘要】：由于燃料電池具有能量轉(zhuǎn)換效率高、穩(wěn)定性高及無(wú)污染等特點(diǎn),使其成為替代使用常規(guī)化石燃料為能源的能量轉(zhuǎn)換裝置。但是,用于燃料電池的陰極氧還原催化劑資源短缺、價(jià)格昂貴阻礙了燃料電池的市場(chǎng)化。因此,制備新型、高效、價(jià)格便宜的氧還原催化劑是目前燃料電池研究的主要內(nèi)容�；趯�(duì)碳載體、含氮催化劑前體和金屬在催化劑催化活性中作用的研究,本文主要介紹了三種由碳(vulcan XC-72)負(fù)載的含氮非貴金屬聚合物(M-N_x/C)作為氧還原催化劑的研究。通過(guò)電子掃描電鏡(SEM)、X-射線光電子能譜(XPS)、紫外可見吸收光譜(UV)、紅外光譜(IR)、熱重分析(TGA)等手段對(duì)催化劑的物理特性進(jìn)行了分析。采用循環(huán)伏安法(CV)、線性掃描伏安法(LSV)、旋轉(zhuǎn)環(huán)盤電極測(cè)試法(RRDE)對(duì)催化劑的電催化特性進(jìn)行了測(cè)試。由數(shù)據(jù)計(jì)算得到H_2O_2的產(chǎn)量和電子轉(zhuǎn)移數(shù),了解各種催化劑的催化活性,進(jìn)一步通過(guò)動(dòng)力學(xué)分析明確在各種催化劑的作用下氧氣被還原時(shí)電子轉(zhuǎn)移途徑。(1)通過(guò)化學(xué)聚合法合成可溶性共軛聚合物標(biāo)記為PBBDP,并成功制備PBBDP/C和Cu-PBBDP/C催化劑。通過(guò)物理表征、電化學(xué)測(cè)試和動(dòng)力學(xué)分析表明:Cu-PBBDP/C的催化活性高于PBBDP/C。進(jìn)一步將Cu-PBBDP/C與商業(yè)Pt/C(20%)比較得出Cu-PBBDP/C在電子轉(zhuǎn)移數(shù)(ETN)和H_2O_2產(chǎn)量方面與Pt/C(20%)相近,并且催化活性高于文獻(xiàn)中相同類型的催化劑,是一種高效的催化劑。(2)通過(guò)化學(xué)聚合方法合成含1,10-菲咯啉單元的單體OCBP。通過(guò)引入銅離子形成超分子聚合物Cu-OCBP,并采用碳粉為載體制備Cu-OCBP/C催化劑。研究表明:Cu-OCBP/C的催化活性雖然低于Pt/C(20%),但是與文獻(xiàn)中同種類型的催化劑相比在電子轉(zhuǎn)移數(shù)及H_2O_2產(chǎn)量方面仍具有較大的優(yōu)勢(shì)。(3)采用聚酰胺-胺型樹枝狀高分子(G4-NH_2)與1,10-菲咯啉-5-羧酸反應(yīng)合成催化劑前體,標(biāo)記為PAMAMPhen。采用簡(jiǎn)單方法制備PAMAMPhen/C、PAMAMPhen-Cu/C催化劑。通過(guò)物理表征、電化學(xué)表征、動(dòng)力學(xué)分析表明PAMAMPhen-Cu/C的催化活性高于PAMAMPhen/C且與Pt/C相當(dāng)。
[Abstract]:Because the fuel cell has high energy conversion efficiency, high stability and no pollution, make it become an alternative to the use of conventional fossil fuel energy conversion device for energy. However, for the cathode oxygen reduction catalyst shortage, expensive market hindered the fuel cell. Therefore, the preparation of a new type, high price. Cheap oxygen reduction catalyst is the main content of the fuel cell research. Based on the study of effect of nitrogen containing carbon carrier, catalyst precursors and metal catalyst in catalytic activity, this paper mainly introduces three kinds of carbon (Vulcan XC-72) load of nitrogen containing non noble metal polymer (M-N_x/C) as catalyst for oxygen reduction research by scanning electron microscopy (SEM), X- ray photoelectron spectroscopy (XPS), ultraviolet visible absorption spectroscopy (UV), infrared spectroscopy (IR), thermogravimetric analysis (TGA) on the physical properties of catalyst and other means The analysis using cyclic voltammetry (CV), linear sweep voltammetry (LSV), a rotating ring disk electrode testing method (RRDE) on the electrocatalytic properties of the catalysts were tested. The number and yield of electron transfer by H_2O_2 data, understand the catalytic activity of various catalysts, further clear in all through the dynamic analysis the effect of catalyst under oxygen is reduced when the electron transfer pathway. (1) by chemical polymerization of soluble conjugated polymers labeled PBBDP, and successfully prepared PBBDP/C and Cu-PBBDP/C catalysts. The physical characterization, electrochemical testing and analysis of kinetics showed that the catalytic activity of Cu-PBBDP/C was higher than that of PBBDP/C. and Cu-PBBDP/C will be further compared with commercial Pt/C (20%) Cu-PBBDP/C in the number of electron transfer (ETN) and H_2O_2 yield and Pt/C (20%) are similar, and higher catalytic activity than that of the same type of catalyst in the literature, is a kind of high efficient The catalyst. (2) by chemical polymerization of OCBP. monomer containing 1,10- phenanthroline unit by introducing copper ions to form supramolecular polymer Cu-OCBP as the carrier, and Cu-OCBP/C catalysts were prepared by carbon powder. The study shows that the catalytic activity of Cu-OCBP/C was lower than Pt/C (20%), but compared with the literature in the same type of catalyst electron transfer number and the yield of H_2O_2 is still a big advantage. (3) using polyamidoamine dendrimer (G4-NH_2) and synthesis catalyst 1,10- phenanthroline -5- carboxylic acid precursors, labeled as PAMAMPhen. prepared to adopt PAMAMPhen/C, prepared by a simple method of PAMAMPhen-Cu/C catalyst. The physical characterization, electrochemical characterization, kinetic analysis showed that the catalytic activity of PAMAMPhen-Cu/C is higher than that of PAMAMPhen/C and Pt/C.

【學(xué)位授予單位】：聊城大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36

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