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聚乙烯吡咯烷酮修饰的石墨碳纳米纤维作为直接甲醇燃料电池中铂钌催化剂的理想载体

Poly(vinylpyrrolidone)-modified graphite carbon nanofibers as promising supports for PtRu catalysts in direct methanol fuel cells.

作者信息

Hsin Yu Lin, Hwang Kuo Chu, Yeh Chuin-Tih

机构信息

Department of Chemistry, National Tsing Hua University, Hsinchu, Taiwan.

出版信息

J Am Chem Soc. 2007 Aug 15;129(32):9999-10010. doi: 10.1021/ja072367a. Epub 2007 Jul 21.

Abstract

Carbon nanomaterials, including herringbone graphite carbon nanofibers (GNFH), multiwalled carbon nanotubes (MWCNT), and carbon black, were surface-modified by a new poly(vinylpyrrolidone) (PVP) grafting process as well as by the conventional acid-oxidation (AO) process, and characterized by FTIR, TGA, Raman, HRTEM, XRD, and XPS measurements. Pt nanoparticles of 1.8 nm were evenly deposited on all PVP-grafted carbon nanomaterials. The effects of the two surface modification processes on the dispersion, average Pt nanoparticle sizes, the electrocatalytic performance, and electrical conductivities of Pt-carbon nanocomposites in direct methanol oxidation were systematically studied and compared. It was found that the PVP-grafted carbon nanomaterials have much less loss in the electric conductivity and thus better electrocatalytic performance, 17-463% higher, than their corresponding acid oxidation-treated nanocomposites. The electrocatalytic performance of the Pt-carbon nanocomposites decreases in the following order: Pt-PVP-GNFH > Pt-PVP-MWCNTarc > Pt-AO-MWCNTarc > Pt-PVP-MWCNTCVD > Pt-AO-MWCNTCVD > Pt-XC-72R > Pt-AO-GNFH, with the Pt-PVP-GNFH nanocomposite having approximately 270% higher performance than that of the Pt-Vulcan XC-72R nanocomposite. In addition, PtRu-PVP-GNFH shows even better (50% higher) electrocatalytic activity than the Pt-PVP-GNFH nanocomposite at a 0.6 V applied voltage.

摘要

包括人字形石墨碳纳米纤维(GNFH)、多壁碳纳米管(MWCNT)和炭黑在内的碳纳米材料,通过一种新的聚乙烯吡咯烷酮(PVP)接枝工艺以及传统的酸氧化(AO)工艺进行表面改性,并通过傅里叶变换红外光谱(FTIR)、热重分析(TGA)、拉曼光谱、高分辨率透射电子显微镜(HRTEM)、X射线衍射(XRD)和X射线光电子能谱(XPS)测量进行表征。1.8纳米的铂纳米颗粒均匀沉积在所有PVP接枝的碳纳米材料上。系统研究并比较了这两种表面改性工艺对铂-碳纳米复合材料在直接甲醇氧化中的分散性、平均铂纳米颗粒尺寸、电催化性能和电导率的影响。结果发现,PVP接枝的碳纳米材料的电导率损失要小得多,因此其电催化性能比相应的酸氧化处理的纳米复合材料高17 - 463%。铂-碳纳米复合材料的电催化性能按以下顺序降低:Pt-PVP-GNFH > Pt-PVP-MWCNTarc > Pt-AO-MWCNTarc > Pt-PVP-MWCNTCVD > Pt-AO-MWCNTCVD > Pt-XC-72R > Pt-AO-GNFH,其中Pt-PVP-GNFH纳米复合材料的性能比Pt-Vulcan XC-72R纳米复合材料高约270%。此外,在0.6 V的外加电压下,PtRu-PVP-GNFH的电催化活性比Pt-PVP-GNFH纳米复合材料还要好(高50%)。

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