Three-Dimensional Boron- and Nitrogen-Codoped Graphene Aerogel-Supported Pt Nanoparticles as Highly Active Electrocatalysts for Methanol Oxidation Reaction

Miaomiao Li, Quanguo Jiang, Minmin Yan, Yujie Wei, Jianbo Zong, Jianfeng Zhang, Yuping Wu, Huajie Huang

Index: 10.1021/acssuschemeng.8b00425

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Abstract

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.