Institut National de la Recherche Scientifique-Énergie Matériaux et Télécommunications , Varennes, Quebec J3X 1S2, Canada.
Ballard Power Systems Inc. , Burnaby, British Columbia V5J 5J8, Canada.
ACS Appl Mater Interfaces. 2017 Oct 25;9(42):36944-36954. doi: 10.1021/acsami.7b12666. Epub 2017 Oct 13.
Exploring inexpensive and high-performance nonprecious metal catalysts (NPMCs) to replace the rare and expensive Pt-based catalyst for the oxygen reduction reaction (ORR) is crucial for future low-temperature fuel cell devices. Herein, we developed a new type of highly efficient 3D porous Fe/N/C electrocatalyst through a simple pyrolysis approach. Our systematic study revealed that the pyrolysis temperature, the surface area, and the Fe content in the catalysts largely affect the ORR performance of the Fe/N/C catalysts, and the optimized parameters have been identified. The optimized Fe/N/C catalyst, with an interconnected hollow and open structure, exhibits one of the highest ORR activity, stability and selectivity in both alkaline and acidic conditions. In 0.1 M KOH, compared to the commercial Pt/C catalyst, the 3D porous Fe/N/C catalyst exhibits ∼6 times better activity (e.g., 1.91 mA cm for Fe/N/C vs 0.32 mA cm for Pt/C, at 0.9 V) and excellent stability (e.g., no any decay for Fe/N/C vs 35 mV negative half-wave potential shift for Pt/C, after 10000 cycles test). In 0.5 M HSO, this catalyst also exhibits comparable activity and better stability comparing to Pt/C catalyst. More importantly, in both alkaline and acidic media (RRDE environment), the as-synthesized Fe/N/C catalyst shows much better stability and methanol tolerance than those of the state-of-the-art commercial Pt/C catalyst. All these make the 3D porous Fe/N/C nanostructure an excellent candidate for non-precious-metal ORR catalyst in metal-air batteries and fuel cells.
探索廉价且高性能的非贵金属催化剂(NPMCs)来替代稀有且昂贵的 Pt 基催化剂对于未来的低温燃料电池设备至关重要。在此,我们通过简单的热解法开发了一种新型高效的 3D 多孔 Fe/N/C 电催化剂。我们的系统研究表明,催化剂的热解温度、比表面积和 Fe 含量极大地影响了 Fe/N/C 催化剂的 ORR 性能,并且已经确定了最佳参数。优化后的 Fe/N/C 催化剂具有互联的中空和开放结构,在碱性和酸性条件下均表现出最高的 ORR 活性、稳定性和选择性之一。在 0.1 M KOH 中,与商业 Pt/C 催化剂相比,3D 多孔 Fe/N/C 催化剂表现出约 6 倍的更好的活性(例如,在 0.9 V 时,Fe/N/C 为 1.91 mA cm,而 Pt/C 为 0.32 mA cm)和出色的稳定性(例如,在 10000 次循环测试后,Fe/N/C 没有任何衰减,而 Pt/C 的负半波电位偏移为 35 mV)。在 0.5 M HSO 中,与 Pt/C 催化剂相比,该催化剂也表现出相当的活性和更好的稳定性。更重要的是,在碱性和酸性介质(RRDE 环境)中,与最先进的商业 Pt/C 催化剂相比,所合成的 Fe/N/C 催化剂表现出更好的稳定性和甲醇耐受性。所有这些都使 3D 多孔 Fe/N/C 纳米结构成为金属空气电池和燃料电池中非贵金属 ORR 催化剂的优秀候选者。