Pacific Northwest National Laboratory, Richland, Washington 99352, USA.
J Am Chem Soc. 2011 Mar 2;133(8):2541-7. doi: 10.1021/ja107719u. Epub 2011 Feb 8.
Carbon-supported precious metal catalysts are widely used in heterogeneous catalysis and electrocatalysis, and enhancement of catalyst dispersion and stability by controlling the interfacial structure is highly desired. Here we report a new method to deposit metal oxides and metal nanoparticles on graphene and form stable metal-metal oxide-graphene triple junctions for electrocatalysis applications. We first synthesize indium tin oxide (ITO) nanocrystals directly on functionalized graphene sheets, forming an ITO-graphene hybrid. Platinum nanoparticles are then deposited, forming a unique triple-junction structure (Pt-ITO-graphene). Our experimental work and periodic density functional theory (DFT) calculations show that the supported Pt nanoparticles are more stable at the Pt-ITO-graphene triple junctions. Furthermore, DFT calculations suggest that the defects and functional groups on graphene also play an important role in stabilizing the catalysts. These new catalyst materials were tested for oxygen reduction for potential applications in polymer electrolyte membrane fuel cells, and they exhibited greatly enhanced stability and activity.
负载贵金属催化剂在多相催化和电催化中得到了广泛的应用,通过控制界面结构来提高催化剂的分散性和稳定性是非常重要的。在这里,我们报道了一种在石墨烯上沉积金属氧化物和金属纳米颗粒并形成稳定的金属-金属氧化物-石墨烯三结合体的新方法,用于电催化应用。我们首先在功能化石墨烯片上直接合成氧化铟锡(ITO)纳米晶体,形成 ITO-石墨烯杂化材料。然后沉积铂纳米颗粒,形成独特的三结合结构(Pt-ITO-石墨烯)。我们的实验工作和周期性密度泛函理论(DFT)计算表明,在 Pt-ITO-石墨烯三结合体中,负载的 Pt 纳米颗粒更稳定。此外,DFT 计算表明,石墨烯上的缺陷和官能团对稳定催化剂也起着重要作用。这些新型催化剂材料被用于氧还原反应,以潜在应用于聚合物电解质膜燃料电池,它们表现出了极大的稳定性和活性增强。