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作 者:朱复春[1] 游乐星[1] 瞿希铭 张斌伟[1] 张宗成[1] 姜艳霞[1] 孙世刚[1]
机构地区:[1]厦门大学化学化工学院,固体表面物理化学国家重点实验室,福建厦门361005
出 处:《厦门大学学报(自然科学版)》2015年第5期685-692,共8页Journal of Xiamen University:Natural Science
基 金:国家自然科学基金(21273180,21361140374,21321062)
摘 要:本研究通过多元醇还原法制备了石墨烯(graphene,GN)负载的Pt及Pt基多元催化剂:Pt/GN、PtRh/GN、PtSn/GN、PtRhSn/GN.X射线粉末衍射(XRD)和透射电镜(TEM)结果表明,所制备的催化剂分布均匀,Pt/GN和PtRh/GN具有立方体形状,PtSn/GN呈现三维网络形貌,PtRhSn/GN则为立方体延伸的三维网络.循环伏安研究表明,Rh的加入提升了甲醇电催化氧化的活性,而Sn的加入明显降低了甲醇在Pt上的起始氧化电位,负移达到106mV.电化学原位红外光谱研究进一步证明,Rh和Sn的加入使得Pt基催化剂对甲醇氧化的起始氧化电位负移;Rh的加入使得CO谱峰强度增大,而Sn的加入明显降低了CO谱峰强度.三元催化剂PtRhSn/GN很好地综合了Rh和Sn的电子效应及协同效应特点,相比于Pt/GN催化剂,起始氧化电位负移60mV,且催化活性达到其1.57倍,表明该三元催化剂在直接甲醇燃料电池中将会有较好的应用前景.Pt/GN,PtRh/GN,PtSn/GN and PtRhSn/GN catalysts were synthesized through a polyol method.The results of transmission electron microscopy(TEM)and X-ray diffraction(XRD)indicated that the as-synthesized catalysts were uniformly dispersed on the graphene(GN)surface.Both Pt/GN and PtRh/GN were composed of homogeneous cubics,while PtSn/GN showed threedimensional network morphology(TDNM)and PtRhSn/GN presented a cubic extended TDNM.Electrochemical cyclic voltammetric(CV)result revealed that the additive element Rh was able to promote the activity,while Sn lowered the onset potential as much as106 mV compared with Pt/GN catalyst for methanol electro-oxidation.In-situ electrochemical Fourier transform infrared spectroscopy(FT-IR)results showed that Rh and Sn could lower the onset potential,and Sn declined the CO peak intensity while Rh increased it.The electronic effect and synergistic effect between the additive element Rh,Sn and Pt make ternary PtRhSn/GN a promising lowPt catalyst for direct methanol fuel cells,which shows a peak current of 1.57 times as much and the onset potential shifting negatively by 60 mV compared with Pt/GN.
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