MOE Laboratory of Bioinorganic and Synthetic Chemistry, KLGHEI of Environment and Energy Chemistry, School of Chemistry and Chemical Engineering, Sun Yat-sen University, Guangzhou 510275, China.
J Am Chem Soc. 2013 Jul 24;135(29):10703-9. doi: 10.1021/ja403101r. Epub 2013 Jul 9.
Low cost, high activity, and long-term durability are the main requirements for commercializing fuel cell electrocatalysts. Despite tremendous efforts, developing non-Pt anode electrocatalysts with high activity and long-term durability at low cost remains a significant technical challenge. Here we report a new type of hybrid Pd/PANI/Pd sandwich-structured nanotube array (SNTA) to exploit shape effects and synergistic effects of Pd-PANI composites for the oxidation of small organic molecules for direct alcohol fuel cells. These synthesized Pd/PANI/Pd SNTAs exhibit significantly improved electrocatalytic activity and durability compared with Pd NTAs and commercial Pd/C catalysts. The unique SNTAs provide fast transport and short diffusion paths for electroactive species and high utilization rate of catalysts. Besides the merits of nanotube arrays, the improved electrocatalytic activity and durability are especially attributed to the special Pd/PANI/Pd sandwich-like nanostructures, which results in electron delocalization between Pd d orbitals and PANI π-conjugated ligands and in electron transfer from Pd to PANI.
低成本、高活性和长期耐久性是商业化燃料电池电催化剂的主要要求。尽管付出了巨大的努力，但开发具有低成本、高活性和长期耐久性的非 Pt 阳极电催化剂仍然是一个重大的技术挑战。在这里，我们报告了一种新型的混合 Pd/PANI/Pd 三明治结构纳米管阵列 (SNTA)，以利用 Pd-PANI 复合材料的形状效应和协同效应，用于小分子的氧化，以用于直接醇燃料电池。与 Pd NTAs 和商业 Pd/C 催化剂相比，这些合成的 Pd/PANI/Pd SNTAs 表现出显著提高的电催化活性和耐久性。独特的 SNTAs 为电活性物质提供了快速的传输和短的扩散路径以及催化剂的高利用率。除了纳米管阵列的优点外，电催化活性和耐久性的提高尤其归因于特殊的 Pd/PANI/Pd 三明治状纳米结构，这导致 Pd d 轨道和 PANI π 共轭配体之间的电子离域以及电子从 Pd 到 PANI 的转移。
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