Nitrogen-doped graphene supported highly dispersed palladium-lead nanoparticles for synergetic enhancement of ethanol electrooxidation in alkaline medium
Nitrogen-doped graphene supported highly dispersed palladium-lead nanoparticles for synergetic enhancement of ethanol electrooxidation in alkaline medium
复制标题
氮掺杂石墨烯负载高度分散的钯铅纳米颗粒协同增强碱性介质中乙醇电氧化
DOI：
10.1016/j.electacta.2014.11.110
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发表时间：
2015-01-10
影响因子：
6.6
通讯作者：
Yao, Jiannian
中科院分区：
文献类型：
--
作者：
Wu, Peng;Huang, Yiyin;Yao, Jiannian
在这项工作中，通过一步还原法合成了一系列负载在活性炭、石墨烯和氮掺杂石墨烯上的钯和钯铅纳米颗粒。采用原子吸收光谱、x射线粉末衍射、透射电镜和x射线光电子能谱对催化剂进行了表征。结果表明，金属纳米粒子在n掺杂石墨烯表面比在石墨烯表面更均匀地分散，没有聚集现象。采用各种电化学技术来评价电催化乙醇氧化活性和耐久性。Pd/ n掺杂石墨烯乙醇电氧化的峰值电流增加到70.2 mA cm(-2)，明显高于Pd/石墨烯（38.0 mA cm(-2)），甚至超过Pd/C （51.9 mA cm(-2)）。n掺杂石墨烯载体不仅具有更快的脱氢速度，而且对Pd具有电子效应。在低电势下，Pb的引入会在催化剂表面形成丰富的含氧物质。基于Nand Pb对Pd粒子的协同作用，PdPb/ n掺杂的石墨烯催化剂（Pd: Pb = 8:1 0）对乙醇的氧化活性显著增强，达到152.3 mA cm(-2)，分别是Pd/石墨烯和Pd/C的4.0和2.9倍。催化的耐久性和稳定性也大大提高。(C) 2014 Elsevier Ltd.版权所有。
In this work, a series of palladium and palladium-lead nanoparticles supported on active carbon, graphene and nitrogen-doped graphene are synthesized via a one-step reduction method. Atomic absorption spectroscopy, X-ray powder diffraction, transmission electron microscope and X-ray photoelectron spectroscopy are used to characterize the catalysts. The results indicate that metal nanoparticles are more uniformly dispersed on the surface of N-doped graphene than those on graphene, without any aggregation. Various electrochemical techniques are carried out to evaluate the electrocatalytic ethanol oxidation activity and durability. The peak current for ethanol electrooxidation of Pd/N-doped graphene increases to 70.2 mA cm(-2), obviously higher than that of Pd/Graphene (38.0 mA cm(-2)) and even surpasses that of Pd/C (51.9 mA cm(-2)). N-doped graphene support not only possesses faster dehydrogenation but provides an electron effect to Pd. Introduction of Pb into the catalyst causes the formation of abundant oxygenated species on the catalyst surface at low potential. Based on the synergistic effect of Nand Pb towards Pd particles, the PdPb/N-doped graphene catalyst (Pd: Pb = 8:1.0) exhibits remarkably enhanced activity up to 152.3 mA cm(-2) for ethanol oxidation, which is 4.0 and 2.9 times higher than that of Pd/Graphene and Pd/C, respectively. The catalytic durability and stability are also greatly improved. (C) 2014 Elsevier Ltd. All rights reserved.