透過您的圖書館登入
IP:3.16.48.181
  • 學位論文

高活性與分散性電化學觸媒Pt/MWNTs 與Pt-Ru/MWNTs之製備

Preparation of active and highly dispersive Pt and PtRu nanoparticles on functionalized MWNTs for electrocatalysts

指導教授 : 江右君

摘要


儘管有很大的潛力可作為新能源,燃料電池仍然有幾個問題阻礙其廣泛的商業化。其中一人是發展的廉價,高性能的電催化劑。高度分散的電催化劑上的裝飾需要的支持。本研究的目的是調查的特點和性能高度分散的Pt納米粒子電催化劑裝飾碳納米管(MWNTs)編寫的微波合成。 作為接收的多壁碳納米管進行了修改,通過幾個步驟的表面功能。酸性氧化進行超聲或回流碳納米管在H2SO4/HNO3解決方案。硫醇使用NH2C6H4SH進行了介紹 SH組的碳納米管。鉑納米粒子的製備碳納米管的裝飾採用微波輔助加熱法多元醇。此外,PtRu納米粒子的裝飾碳納米管還編寫了類似的過程。 所有樣本均經 X射線衍射儀(XRD),傅立葉變換紅外光譜(FTIR),X射線光電子能譜(XPS),高分辨透射電子顯微鏡(HRTEM),能量色散X射線光譜儀(能譜),電感耦合等離子體質譜(ICP)和熱重分析(TGA)。對電催化劑的性能進行了檢查,循環伏安法(CV)和甲醇氧化反應(鐵道部)。 高溫高壓負荷(≈40重量。%)可實現對多壁碳納米管的表面功能化。酸性氧化有很大的影響不改變粒子的大小。不過,硫醇具有很大的影響來改變粒子的大小。粒度小到納米 3.77上可觀察到thiolized樣本。在場的S2P程式的峰值由XPS證實,表面巰基化過程是成功的。在CV測試,Pt載量低的樣品具有較高的歐空局的比Pt載量高的樣本。在鐵道部的測試,PtRu樣品具有很高的正向掃描峰電流(IF)。如果能找到最高的PtRu/r3s2MWNTs樣本已如果三百三十七毫安。這些結果表明,多壁碳納米管的表面功能化和微波輔助加熱的多元醇合成可能是一個很有前途的方法製備的鉑電催化劑的燃料電池中的應用。

關鍵字

官能基 觸媒 奈米碳管

並列摘要


Despite of great potential to be used as new energy sources, fuel cell still has several problems that hinder its wide commercialization. One of them is development of cheap and high performance electrocatalysts. Highly dispersed electrocatalysts decorated on a support are needed. The purpose of this study is to investigate characteristic and performance of highly dispersed Pt nanoparticles electrocatalyst decorated on carbon nanotubes (MWNTs) prepared by microwave synthesis. The as-received MWNTs were modified by several steps of surface functionalization. Acid oxidation was conducted by sonicate or reflux MWNTs in H2SO4/HNO3 solution. Thiolation by using NH2C6H4SH was conducted to introduce SH group on MWNTs. The Pt nanoparticles decoration on MWNTs was prepared by microwave-assisted polyol heating method. In addition, PtRu nanoparticles decoration on MWNTs was also prepared by similar process. All samples were characterized by X-ray diffraction (XRD), fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), high resolution transmission electron microscopy (HRTEM), energy dispersive X-ray spectroscopy (EDX), inductively coupled plasma mass spectroscopy (ICP), and thermo gravimetric analysis (TGA). The performance of electrocatalyst was examined by cyclic voltammetry (CV), and methanol oxidation reaction (MOR). High Pt loading (≈40 wt.%) could be achieved on surface functionalized MWNTs. Acid oxidation does not have great effect to change particle size. However, thiolation has great effect to change particle size. Particle size as small as 3.77 nm could be observed on thiolized sample. The presence of S2p peak from XPS confirmed that surface thiolation process was successful. On the CV test, low Pt loading sample has higher ESA than high Pt loading sample. On MOR test, PtRu sample has very high forward scan peak current (If). Highest If could be found on PtRu/r3s2MWNTs sample which has If 337 mA. These results indicate that MWNTs surface functionalization and microwave-assisted polyol heating synthesis could be a promising method for preparation of Pt electrocatalyst for fuel cell application.

並列關鍵字

functionalized electrocatalysts Pt MWCNTs:Ru

參考文獻


Balasubramanian, K., Burghard, M., Chemically Functionalized Carbon Nanotubes, Small., 1, 180-192, 2005.
Chen, C. M., Chen, M., Yu, H. W., Lu, S. C., Chen, C. F., Rapid and Homogeneous Dispersion of Pt Catalyst Particles on Multi-Walled Carbon Nanotubes by Temperature-Controlled Microwave Polyol Method, Japanese Journal of Applied Physics., 47, 2324-2329, 2008.
Croy, J. R., Mostafa, S., Heinrich, H., Cuenya, B. R., Size-selected Pt Nanoparticles Synthesized via Micelle Encapsulation: Effect of Pretreatment and Oxidation State on the Activity for Methanol Decomposition and Oxidation, Catalysis Letters., 131, 21-32, 2009.
Cui, S. K., and Guo, D. J., Highly dispersed Pt nanoparticles immobilized on 1,4-benzenediamine-modified multi-walled carbon nanotube for methanol oxidation, Journal of Colloid and Interface Science., 333, 300-303, 2009.
Doris, E. Chemically functionalization of carbon nanotubes, ESF Nanocarb09 Research Conference., Italy, 2009.

延伸閱讀