Structural Regulation of Pt-Based Anode Catalysts and their Electrocatalytical Performance

铂基催化剂是燃料电池和石油化工等领域广泛应用的催化剂。由于铂的资源匮乏、储量有限、价格昂贵，因此如何提高铂基催化剂的催化活性和稳定性，减少在使用过程中的损失，提高其利用效率是相关应用领域一直持续研究的重要课题。铂基材料在燃料电池电催化反应过程中具有过电位高，易毒化，选择性差，易于团聚等缺陷。而研究表明铂基催化剂的活性与其粒径尺寸、分散性、表面结构和电子结构密切相关。本论文旨在提高铂基材料的活性与抗毒化能力，从合金化效应，载体效应，形貌调控等方面，充分发挥铂和其他金属间以及金属氧化物载体之间的协同作用，改善催化剂表面特性从而制备出高性能的燃料电池阳极催化剂。主要研究工作包括以下两个部分： (1...Platium-base catalysts are widely used in the field of fuel cell, petrochemical industry and other important areas. Being limited by the shortage of stock and high price, it is always very necessary to improve the activity, stability and utilization efficiency of Pt-base catalysts in related application fields. High overpotential, surface poisoning, low selectivity and agglomeration were main shor...学位：理学硕士院系专业：化学化工学院_物理化学学号：2052013115161

盐封后碳化钼电催化剂的制备及其氢析出性能（英文）

碳化钼具有低廉的价格、优越的催化性能以及良好的稳定性而被人们认为是极好的可以替代Pt等贵金属的氢析出反应（HER）催化剂。本工作采用钼酸钠和2,6-二氨基吡啶为反应原料,之后不断进行...supported by the National Key Research and Development Program of China(2017YFA0206500);; the National Natural Science Foundation of China(21773198,U1705253)~

The Preparation Method and Methanol Electrocatalytic Activity of Ternary PtRhSn/GN

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.国家自然科学基金(21273180;21361140374;21321062