Although platinum and its derivatives are generally recognized as the most efficient anode materials for direct methanol fuel cells, their high usage costs and poor poison tolerance largely hamper the large-scale commercial application. Here, we present a convenient bottom-up approach to the fabrication of well-dispersive Pt nanoparticles grown on 3D nitrogen- and sulfur-codoped graphene nanoribbon (Pt/NS-GNR) architectures via a self-assembly process. With a series of intriguing structural features, including large specific surface area, 3D interpenetrating porous carbon networks, a large presence of N and S dopants and homogeneous dispersion of ultrafine Pt nanoparticles, the obtained Pt/NS-GNR hybrid possesses a large electrochemically active surface area, high electrocatalytic activity, reliable long-term durability, as well as good antitoxic ability toward methanol oxidation reaction, far surpassing those of conventional Pt catalysts deposited on commercial carbon black, carbon nanotubes, graphene, and undoped graphene nanoribbon supports. Theoretical simulations further reveal that there are strong electronic interactions between metal and matrix, which could not only immobilize the Pt particles onto the 3D NS-GNR frameworks but also weaken the CO adsorption on the catalytic sites, thereby synergistically promoting the methanol oxidation catalytic efficiency.

虽然铂及其衍生物被普遍认为是直接甲醇燃料电池最有效的负极材料，但其高昂的使用成本和较差的毒害耐受性在很大程度上阻碍了其大规模商业应用。在这里，我们提出了一种方便的自下而上的方法，通过自组装工艺在 3D 氮和硫共掺杂石墨烯纳米带(Pt/NS-GNR) 结构上制备良好分散的 Pt 纳米粒子。具有一系列有趣的结构特征，包括大比表面积、3D 互穿多孔碳网络、大量的 N 和 S掺杂剂和超细 Pt 纳米粒子的均匀分散，获得的 Pt/NS-GNR 杂化物具有大的电化学活性表面积、高电催化活性、可靠的长期耐久性，以及对甲醇氧化反应良好的抗毒能力，远远超过那些传统的铂催化剂沉积在商业炭黑、碳纳米管、石墨烯和未掺杂的石墨烯纳米带载体上。理论模拟进一步表明，金属与基体之间存在强电子相互作用，这不仅可以将 Pt 颗粒固定在 3D NS-GNR 骨架上，还可以减弱催化位点上的 CO 吸附，从而协同提高甲醇氧化催化效率。