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A Pt-Fe Carbon Nitride Nano-electrocatalyst for Polymer Electrolyte Membrane Fuel Cells and Direct-Methanol Fuel Cells: Synthesis, Characterization, and Electrochemical Studies

机译:用于聚合物电解质膜燃料电池和直接甲醇燃料电池的Pt-Fe碳氮化碳纳米电催化剂:合成,表征和电化学研究

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摘要

This report describes the preparation of a new nano-electrocatalyst for applications in polymer electrolyte fuel cells operating with H_2 and methanol. The nano-electrocatalyst, having the composition K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)], consists of a distribution of Pt and Fe bimetallic clusters supported on carbon nitride nanoparticles. This material was synthesized by thermal treatment of a zeolitic inorganic-organic polymer electrolyte-like (Z-IOPE) precursor, prepared by reacting H_2PtCl_6 and K_3Fe(CN)_6 in the presence of sucrose, as organic binder, in a water solution. This reaction allows the desired material to be prepared by means of a sol→gel process followed by a gel→plastic transition. The morphology and surface properties of K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)] were studied via scanning and high-resolution transmission electron microscopies and X-ray photoelectron spectroscopy. Far-infrared, mid-infrared, and micro-Raman-laser spectroscopies, as well as X-ray diffraction studies, together with detailed compositional data reveal the structural information and describe the interactions characterizing the mass activity of the K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)] system. This material has structural and morphological features that are very different to those usually found in commercially available electrocatalysts for application in H_2 polymer electrolyte membrane fuel cells (PEMFCs) and direct methanol fuel cells (DMFCs). K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)] consists of active bimetallic catalytic sites supported on a mixture of a and graphitic carbon nitride-like nanoparticles. The studies performed by cyclic voltammetry with the thin-film rotating-disk electrode indicate that the performance of K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)] and of the EC-20 reference material is a) equal to -255 and -216 A g~(-1) Pt, respectively, in the oxygen-reduction reaction at 0.75 V; and b) equal to 967 and 533 Ag~(-1) Pt, respectively, in the hydrogen-oxidation reaction at potentials lower than 0.2 V. The activation potential of K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)] is about 15 mV higher than that of the EC-20 reference. In conclusion, the proposed synthesis route is general and promising for the development of new, improved nano-electrocatalysts for low-temperature fuel cells such as PEMFCs and DMFCs.
机译:该报告描述了一种新的纳米电催化剂的制备方法,该催化剂可用于使用H_2和甲醇的聚合物电解质燃料电池中。具有组成K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)]的纳米电极催化剂由负载在氮化碳纳米颗粒上的Pt和Fe双金属簇的分布组成。该材料是通过对沸石类无机-有机聚合物电解质样(Z-IOPE)前体进行热处理而合成的,该前体是通过在有机溶剂中存在蔗糖的情况下使H_2PtCl_6和K_3Fe(CN)_6在水溶液中反应来制备的。该反应允许通过溶胶→凝胶法,然后进行凝胶→塑性转变来制备所需的材料。通过扫描和高分辨率透射电子显微镜以及X射线光电子能谱研究了K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)]的形貌和表面性质。远红外,中红外和微拉曼激光光谱学以及X射线衍射研究以及详细的组成数据共同揭示了结构信息,并描述了表征K_(0.12)[Pt_1Fe_ (1.6)C_(55)N_(0.12)]系统。这种材料的结构和形态特征与通常用于商业化的用于H_2聚合物电解质膜燃料电池(PEMFC)和直接甲醇燃料电池(DMFC)的电催化剂中发现的结构和形态特征非常不同。 K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)]由活性双金属催化位点组成,该催化位点负载在α和石墨状碳氮化物类纳米颗粒的混合物上。通过循环伏安法对薄膜转盘电极进行的研究表明,K_(0.12)[Pt_1Fe_(1.6)C_(55)N_(0.12)]和EC-20参考材料的性能相同在0.75V的氧还原反应中分别为-255和-216A g〜(-1)Pt。 b)在低于0.2 V的氢氧化反应中分别等于967和533 Ag〜(-1)Pt。K_(0.12)[Pt_1Fe_(1.6)C_(55)N_( 0.12)]比EC-20参考电压高约15 mV。总之,所提出的合成路线是通用的,对于开发用于低温燃料电池(如PEMFC和DMFC)的新型,改进的纳米电催化剂是有前途的。

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