Department of Chemistry, State University of New York at Stony Brook, Stony Brook, New York 11794-3400, USA.
J Am Chem Soc. 2011 Jun 29;133(25):9783-95. doi: 10.1021/ja111130t. Epub 2011 Jun 6.
We report on the synthesis, characterization, and electrochemical performance of novel, ultrathin Pt monolayer shell-Pd nanowire core catalysts. Initially, ultrathin Pd nanowires with diameters of 2.0 ± 0.5 nm were generated, and a method has been developed to achieve highly uniform distributions of these catalysts onto the Vulcan XC-72 carbon support. As-prepared wires are activated by the use of two distinctive treatment protocols followed by selective CO adsorption in order to selectively remove undesirable organic residues. Subsequently, the desired nanowire core-Pt monolayer shell motif was reliably achieved by Cu underpotential deposition followed by galvanic displacement of the Cu adatoms. The surface area and mass activity of the acid and ozone-treated nanowires were assessed, and the ozone-treated nanowires were found to maintain outstanding area and mass specific activities of 0.77 mA/cm(2) and 1.83 A/mg(Pt), respectively, which were significantly enhanced as compared with conventional commercial Pt nanoparticles, core-shell nanoparticles, and acid-treated nanowires. The ozone-treated nanowires also maintained excellent electrochemical durability under accelerated half-cell testing, and it was found that the area-specific activity increased by ~1.5 fold after a simulated catalyst lifetime.
我们报告了新型超薄 Pt 单原子层壳-Pd 纳米线核催化剂的合成、表征和电化学性能。首先,生成了直径为 2.0 ± 0.5nm 的超薄 Pd 纳米线,并开发了一种将这些催化剂高度均匀地分布在 Vulcan XC-72 碳载体上的方法。通过使用两种不同的处理方案对所制备的纳米线进行预处理,然后选择性地进行 CO 吸附,以选择性地去除不需要的有机残留物。随后,通过 Cu 欠电位沉积和随后的 Cu 原子的电置换,可靠地实现了所需的纳米线核-Pt 单原子层壳结构。对酸和臭氧处理的纳米线的比表面积和质量活性进行了评估,发现臭氧处理的纳米线保持了出色的面积和质量比活性,分别为 0.77mA/cm²和 1.83A/mg(Pt),与传统商用 Pt 纳米颗粒、核壳纳米颗粒和酸处理纳米线相比,显著提高。臭氧处理的纳米线在加速半电池测试中也保持了出色的电化学耐久性,经过模拟催化剂寿命后,发现面积比活性增加了约 1.5 倍。