本文關(guān)鍵詞：直接甲酸燃料電池陽極電催化劑中碳載體材料的研究　出處：《燕山大學》2014年碩士論文　論文類型：學位論文

  更多相關(guān)文章： 直接甲酸燃料電池 電氧化 鈀納米粒子 催化劑 碳載體材料

【摘要】：直接甲酸燃料電池作為一種清潔高效的能量轉(zhuǎn)換裝置，由于其相對于直接甲醇燃料電池的快速氧化動力學、低毒性、低Nafion膜透過率而受到越來越多的關(guān)注。然而，陽極催化劑的低催化活性、低穩(wěn)定性、易失活和載體易腐蝕仍然限制著直接甲酸燃料電池的實際應用。 本文主要研究了幾種常用碳材料作為催化劑載體時對鈀基催化劑催化甲酸電氧化的性能影響，發(fā)現(xiàn)了多壁碳納米管作為載體材料時具有較高的催化活性和穩(wěn)定性。由于鈀和碳材料之間的強相互作用，碳材料的添加對于鈀催化劑的新型活性位點的形成起著至關(guān)重要的作用。結(jié)果表明碳材料在催化劑中不僅僅起著載體的作用，而且參與了甲酸電氧化過程中鈀基催化劑的新型活性位點的形成，該發(fā)現(xiàn)對于研究Pd/C催化劑催化甲酸電氧化的反應機理、尋找合適的載體材料起著至關(guān)重要的作用。 同時，本文也系統(tǒng)研究了氮摻雜乙炔碳黑對甲酸電氧化反應的影響。通過在氮氣流中不同溫度下熱解乙炔碳黑和三聚氰胺得到氮摻雜的乙炔碳黑，并將該材料負載鈀納米粒子用作甲酸電氧化的催化劑。發(fā)現(xiàn)當熱處理溫度為900℃時，所對應的催化劑Pd/N-C-900具有最大的催化活性、穩(wěn)定性和耐一氧化碳中毒性能。在0.5mol·L-1H2SO4和0.5mol·L-1HCOOH的混合溶液中，Pd/N-C-900催化劑的催化活性是普通Pd/C催化劑和商業(yè)Pd/C催化劑的2.84倍和0.96倍。同時研究了甲酸濃度和溫度效應對Pd/N-C催化劑的影響，結(jié)果表明氮摻雜的確可以提高甲酸電氧化的性能。發(fā)現(xiàn)氮摻雜提高甲酸電氧化性能的原因是改善的鈀納米粒子的分散和修飾的電子效應，，結(jié)果表明Pd/N-C催化劑在直接甲酸燃料電池中作為一種高性能催化劑具有廣闊的應用前景。
[Abstract]:As a clean and efficient energy conversion device, direct formic acid fuel cell (DFC) is less toxic than direct methanol fuel cell (DMFC) because of its rapid oxidation kinetics. Low Nafion membrane transmittance has attracted more and more attention. However, the anode catalyst has low catalytic activity and low stability. Deactivation and carrier corrosion still limit the practical application of direct formic acid fuel cells. In this paper, the effect of several common carbon materials on the electrooxidation of formic acid over palladium based catalysts was studied. It was found that multi-walled carbon nanotubes had high catalytic activity and stability when they were used as carrier materials because of the strong interaction between palladium and carbon materials. The addition of carbon materials plays an important role in the formation of new active sites of palladium catalysts. The results show that carbon materials not only act as carriers in the catalysts. It is also involved in the formation of new active sites of palladium based catalysts in the process of formic acid electrooxidation. This discovery is useful for the study of the reaction mechanism of Pd/C catalysts for formic acid electrooxidation. Finding suitable carrier materials plays an important role. At the same time, the effect of nitrogen-doped acetylene black on the electrooxidation of formic acid was studied systematically. The nitrogen-doped acetylene black was obtained by pyrolysis of acetylene carbon black and melamine at different temperatures in nitrogen flow. The palladium nanoparticles were used as catalysts for the electrooxidation of formic acid. It was found that the corresponding catalyst Pd/N-C-900 had the highest catalytic activity when the heat treatment temperature was 900 鈩

本文編號：1395195