Department of Applied Chemistry, Graduate School of Engineering, Kyushu University , 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan.
Division of Chemistry and Materials Science, Graduate School of Engineering, Nagasaki University , 1-14 Bunkyo-Machi, Nagasaki 852-8521, Japan.
ACS Appl Mater Interfaces. 2016 Apr 13;8(14):9030-6. doi: 10.1021/acsami.5b06826. Epub 2016 Mar 30.
For direct methanol fuel cells (DMFCs) to be commercialized, the durability of the anodic electrocatalyst needs to be highly considered, especially under high temperature and methanol concentration conditions. Low durability caused by carbon corrosion as well as carbon monoxide (CO) poisoning of the platinum nanoparticles (Pt-NP) leads to a decrease in active Pt-NPs and increases inactive Pt-NPs covered by CO species. In this study, we deposited Pt-NPs on poly[2,2'-(2,6-pyridine)-5,5'-bibenzimidazole] (PyPBI)-wrapped nanoporous carbon (NanoPC) and coated the as-synthesized electrocatalyst with poly(vinylphosphonic acid) (PVPA). The durability of the as-synthesized NanoPC/PyPBI/Pt/PVPA was tested in 0.1 M HClO4 electrolyte at 60 °C by cycling the potential from 1.0 to 1.5 V relative to RHE, and the results indicated that NanoPC/PyPBI/Pt/PVPA showed ∼5 times better durability relative to that of the commercial CB/Pt. The methanol oxidation reaction (MOR) of the electrocatalyst was tested before and after the potential cycling in the presence of 4 or 8 M methanol at 60 °C and found that the CO tolerance of the electrocatalyst was ∼3 times higher than that of the commercial CB/Pt. Such a higher CO tolerance is due to the coating of the PVPA, which was proven by an EDX mapping measurement. The NanoPC/PyPBI/Pt/PVPA showed a high durability and CO tolerance under high temperature and high methanol concentration conditions, indicating that the electrocatalyst could be used in real fuel applications.
对于直接甲醇燃料电池(DMFC)而言,需要高度考虑阳极电催化剂的耐久性,特别是在高温和高甲醇浓度条件下。由于碳腐蚀以及铂纳米粒子(Pt-NP)的一氧化碳(CO)中毒,导致活性 Pt-NP 减少和被 CO 物种覆盖的非活性 Pt-NP 增加,从而导致耐久性降低。在这项研究中,我们将 Pt-NP 沉积在聚[2,2'-(2,6-吡啶)-5,5'-联苯并咪唑](PyPBI)包裹的纳米多孔碳(NanoPC)上,并将合成的电催化剂用聚(乙烯膦酸)(PVPA)进行涂覆。在 60°C 下,通过将相对于 RHE 的电位从 1.0 循环到 1.5V,在 0.1M HClO4 电解质中测试了所合成的 NanoPC/PyPBI/Pt/PVPA 的耐久性,结果表明 NanoPC/PyPBI/Pt/PVPA 的耐久性相对于商用 CB/Pt 提高了约 5 倍。在 60°C 下,在存在 4 或 8M 甲醇的情况下,在进行电位循环前后测试了电催化剂的甲醇氧化反应(MOR),发现电催化剂的 CO 耐受性相对于商用 CB/Pt 提高了约 3 倍。这种更高的 CO 耐受性归因于 PVPA 的涂层,这通过 EDX 映射测量得到了证明。NanoPC/PyPBI/Pt/PVPA 在高温和高甲醇浓度条件下表现出高耐久性和 CO 耐受性,表明该电催化剂可用于实际的燃料应用。