Both direct formic acid fuel cells (DFAFCs) and direct methanol fuel cells (DMFCs) are promising power-generation technologies for various electronic devices, while their large-scale commercial applications are largely precluded by the lack of advanced noble metal catalysts with high activity and acceptable cost. Herein, we report a simple and scalable strategy to prepare nanosized Pd crystals anchored on three-dimensional (3D) boron- and nitrogen-codoped graphene aerogels (Pd/BNG) as multifunctional electrocatalysts for formic acid and methanol oxidation reactions. The resulting Pd/BNG catalyst possesses a series of distinctive structural merits adapted to the anode fuel cell catalytic systems, such as large specific surface areas, 3D interconnected porous frameworks, uniform Pd distribution, abundant B and N active sites, and excellent electrical conductivity. Compared with the conventional Pd/carbon black and Pd/graphene catalysts, the newly designed 3D Pd/BNG architecture exhibits dramatically enhanced electrocatalytic performance, including large electrochemically active surface areas, high mass activity, and good long-term stability. Density functional theory calculation further discloses that there is a strong electronic interaction between Pd and the BNG substrate, which effectively enhances the antitoxic ability of Pd/BNG toward CO intermediates and thereby promotes the electrocatalytic reaction kinetics.

中文翻译：

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在三维硼和氮共混的石墨烯气凝胶上固定纳米级Pd，作为甲酸和甲醇氧化反应的高活性多功能电催化剂

直接甲酸燃料电池（DFAFC）和直接甲醇燃料电池（DMFC）都是用于各种电子设备的有前途的发电技术，而它们的大规模商业应用在很大程度上由于缺乏具有高活性和高活性的高级贵金属催化剂而被排除在外。可接受的费用。本文中，我们报告了一种简单且可扩展的策略，以制备锚固在三维（3D）硼和氮共混的石墨烯气凝胶（Pd / BNG）上的纳米级Pd晶体，作为甲酸和甲醇氧化反应的多功能电催化剂。所得的Pd / BNG催化剂具有一系列与阳极燃料电池催化系统相适应的独特结构优点，例如较大的比表面积，3D互连的多孔骨架，均匀的Pd分布，丰富的B和N活性位点，以及出色的导电性。与传统的Pd /炭黑和Pd /石墨烯催化剂相比，新设计的3D Pd / BNG结构具有显着增强的电催化性能，包括大的电化学活性表面积，高质量活性和良好的长期稳定性。密度泛函理论计算进一步揭示了Pd与BNG底物之间存在很强的电子相互作用，有效增强了Pd / BNG对CO中间体的抗毒能力，从而促进了电催化反应动力学。质量活性高，长期稳定性好。密度泛函理论计算进一步揭示了Pd与BNG底物之间存在很强的电子相互作用，有效增强了Pd / BNG对CO中间体的抗毒能力，从而促进了电催化反应动力学。质量活性高，长期稳定性好。密度泛函理论计算进一步揭示了Pd与BNG底物之间存在很强的电子相互作用，有效增强了Pd / BNG对CO中间体的抗毒能力，从而促进了电催化反应动力学。