Abstract Pt and Pt-based catalysts are deemed as the popular anode catalysts for direct methanol fuel cells due to their high electrocatalytic activity for methanol oxidation. The structure of the catalyst support is critical to the electrocatalytic performance of the catalysts. In this work, a kind of high-quality graphene (electrochemically exfoliated graphene) with the intact surface is exploited as the catalyst support instead of the popularly used reduced graphene oxide. Pt nanoparticles are successfully synthesized on electrochemically exfoliated graphene and exhibit better methanol electro-oxidation activity than those on reduced graphene oxide. To further raise the electrocatalytic performance of Pt catalysts, the substrate surface is modified by conductive polyaniline. It is found that the interaction of electrochemically exfoliated graphene with polyaniline is much different from the interaction of reduced graphene oxide with polyaniline. The intact surface structure of electrochemically exfoliated graphene is favorable for the combination with polyaniline by π-π interactions, which releases more N species for the growth of Pt nanoparticles. The synergistic interaction of Pt and N species can facilitate the dispersion of Pt nanocrystals as well as the electron transport through Pt-based hybrids, thereby further promoting the electrocatalytic properties of Pt catalysts for methanol oxidation.

中文翻译：

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通过聚苯胺改性增强电化学剥离石墨烯-Pt 的甲醇电氧化活性

摘要 Pt 和 Pt 基催化剂因其对甲醇氧化的高电催化活性而被认为是直接甲醇燃料电池的常用阳极催化剂。催化剂载体的结构对催化剂的电催化性能至关重要。在这项工作中，一种具有完整表面的高质量石墨烯（电化学剥离石墨烯）被用作催化剂载体，而不是普遍使用的还原氧化石墨烯。Pt 纳米粒子在电化学剥离的石墨烯上成功合成，并且表现出比还原氧化石墨烯更好的甲醇电氧化活性。为了进一步提高Pt催化剂的电催化性能，基体表面采用导电聚苯胺进行改性。发现电化学剥离的石墨烯与聚苯胺的相互作用与还原氧化石墨烯与聚苯胺的相互作用有很大不同。电化学剥离的石墨烯完整的表面结构有利于通过 π-π 相互作用与聚苯胺结合，从而释放更多的 N 物种用于 Pt 纳米粒子的生长。Pt 和 N 物种的协同相互作用可以促进 Pt 纳米晶体的分散以及通过 Pt 基杂化物的电子传输，从而进一步提高 Pt 催化剂对甲醇氧化的电催化性能。电化学剥离的石墨烯完整的表面结构有利于通过 π-π 相互作用与聚苯胺结合，从而释放更多的 N 物种用于 Pt 纳米粒子的生长。Pt 和 N 物种的协同相互作用可以促进 Pt 纳米晶体的分散以及通过 Pt 基杂化物的电子传输，从而进一步提高 Pt 催化剂对甲醇氧化的电催化性能。电化学剥离石墨烯的完整表面结构有利于通过 π-π 相互作用与聚苯胺结合，从而释放出更多的 N 物种用于 Pt 纳米颗粒的生长。Pt 和 N 物种的协同相互作用可以促进 Pt 纳米晶体的分散以及通过 Pt 基杂化物的电子传输，从而进一步提高 Pt 催化剂对甲醇氧化的电催化性能。