State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , Changchun, Jilin 130022, China.
J Am Chem Soc. 2015 Feb 4;137(4):1436-9. doi: 10.1021/ja5129132. Epub 2015 Jan 27.
The design of a new class of non-noble-metal catalysts with oxygen reduction reaction (ORR) activity superior to that of Pt is extremely important for future fuel cell devices. Here we demonstrate a one-pot, large-scale protocol for the controlled synthesis of new one-dimensional bamboo-like carbon nanotube/Fe(3)C nanoparticle hybrid nanoelectrocatalysts, which are directly prepared by annealing a mixture of PEG-PPG-PEG Pluronic P123, melamine, and Fe(NO(3))(3) at 800 °C in N(2). The resulting hybrid electrocatalysts show very high ORR activity with a half-wave potential of 0.861 V (vs reversible hydrogen electrode) in 0.10 M KOH solution, 49 mV more positive than that of 20 wt% Pt/C catalyst. Furthermore, they exhibit good ORR activity in acidic media, with an onset potential comparable to that of the Pt/C catalyst. Most importantly, they show much higher stability and better methanol tolerance, with almost no ORR polarization curve shift and no change of the oxygen reduction peak in the cyclic voltammogram in the presence of 1.0 M methanol, than those of the commercial Pt/C catalyst in both alkaline and acidic solutions. This makes them one of the best non-noble-metal catalysts ever reported for ORR in both alkaline and acidic solutions.
设计一类具有优于 Pt 的氧还原反应 (ORR) 活性的新型非贵金属催化剂对于未来的燃料电池装置极其重要。在这里，我们展示了一种通过一锅法、大规模制备新型一维竹状碳纳米管/Fe(3)C 纳米粒子杂化纳米电催化剂的方法，该方法是通过在 N2 中 800°C 退火聚乙二醇-聚丙二醇-聚乙二醇 Pluronic P123、三聚氰胺和 Fe(NO3)3 的混合物直接制备的。所得杂化电催化剂在 0.10 M KOH 溶液中表现出非常高的 ORR 活性，半波电位为 0.861 V（相对于可逆氢电极），比 20 wt%Pt/C 催化剂正 49 mV。此外，它们在酸性介质中也表现出良好的 ORR 活性，其起始电位与 Pt/C 催化剂相当。最重要的是，与商用 Pt/C 催化剂相比，它们在碱性和酸性溶液中具有更高的稳定性和更好的甲醇耐受性，在存在 1.0 M 甲醇的情况下，几乎没有 ORR 极化曲线的偏移，循环伏安法中氧还原峰也没有变化。这使它们成为迄今为止在碱性和酸性溶液中用于 ORR 的最佳非贵金属催化剂之一。
