Although direct methanol fuel cells have long been regarded as promising “green” power generators for portable electronics, their further development has been largely hampered by the high cost as well as the insufficient activity of the current Pt-based anode catalysts. Herein, we present a bottom-up approach to the large-scale fabrication of three-dimensional (3D) hybrid materials made from ultrafine Pt nanoparticles as well as B- and N-codoped graphene aerogel (BN-GA). The resulting Pt/BN-GA catalyst possesses 3D cross-linked porous networks, large specific surface areas, numerous B and N active sites, homogeneous Pt dispersion, and good electrical conductivity, which are all desirable for the anode catalytic system in direct methanol fuel cells. As a consequence, outstanding electrochemical properties in terms of high catalytic activity, reliable long-term durability, and strong antitoxic ability are achieved for the Pt/BN-GA catalyst, significantly superior to those for the conventional Pt/carbon black, Pt/graphene, and Pt/graphene aerogel catalysts. Density functional theory (DFT) calculations further reveal that the dramatically enhanced catalytic performance is attributed to the strong interaction between Pt and the BN-GA support, which generates remarkable synergetic coupling effects that enable rapid kinetics for the methanol oxidation reaction.

中文翻译：

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三维硼和氮掺杂石墨烯气凝胶负载的Pt纳米颗粒作为甲醇氧化反应的高活性电催化剂

尽管直接甲醇燃料电池长期以来一直被认为是便携式电子产品的有希望的“绿色”发电机，但由于目前的Pt基阳极催化剂的高成本以及活性不足，其进一步的发展受到了很大的阻碍。在这里，我们提出了一种自底向上的方法，用于大规模制造由超细Pt纳米颗粒以及B和N掺杂的石墨烯气凝胶（BN-GA）制成的三维（3D）杂化材料。所得的Pt / BN-GA催化剂具有3D交联的多孔网络，较大的比表面积，大量的B和N活性位，均匀的Pt分散性和良好的导电性，这些都是直接甲醇燃料中阳极催化体系所需要的细胞。因此，就高催化活性而言，具有出色的电化学性能，Pt / BN-GA催化剂具有可靠的长期耐用性和强大的抗毒能力，大大优于常规Pt /炭黑，Pt /石墨烯和Pt /石墨烯气凝胶催化剂。密度泛函理论（DFT）的计算进一步表明，催化性能的显着提高归因于Pt与BN-GA载体之间的强相互作用，从而产生了显着的协同偶联效应，从而使甲醇氧化反应具有快速动力学。