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3D 多孔 Fe/N/C 球形纳米结构作为在碱性和酸性介质中都具有优异性能的氧还原电催化剂。

3D Porous Fe/N/C Spherical Nanostructures As High-Performance Electrocatalysts for Oxygen Reduction in Both Alkaline and Acidic Media.

机构信息

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.

出版信息

ACS Appl Mater Interfaces. 2017 Oct 25;9(42):36944-36954. doi: 10.1021/acsami.7b12666. Epub 2017 Oct 13.

DOI:10.1021/acsami.7b12666
PMID:28982005
Abstract

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.

摘要

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。

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