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双金属和氮共掺杂的球形多孔碳在碱性介质中对氧还原反应具有高效的催化性能。

Bimetal- and nitrogen-codoped spherical porous carbon with efficient catalytic performance towards oxygen reduction reaction in alkaline media.

机构信息

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China; Faculty of Chemistry, Northeast Normal University, Changchun 130024, China.

Faculty of Chemistry, Northeast Normal University, Changchun 130024, China.

出版信息

J Colloid Interface Sci. 2019 Jan 15;534:655-664. doi: 10.1016/j.jcis.2018.09.066. Epub 2018 Sep 19.

Abstract

Nonprecious-metal electrocatalysts have been intensively investigated, but how to keep a balance between their sustainability and competitive performance for the oxygen reduction reaction (ORR) is still a big challenge for energy applications. In this work, a type of bimetal- and nitrogen-codoped mesoporous carbon electrocatalyst (FeCo-N/C-800) was successfully synthesized via a simple hydrothermal method, followed by a calcination process at 800 °C in nitrogen atmosphere and an acid-etching process. The obtained FeCo-N/C-800 can act as a high-performance ORR catalyst with high onset and half-wave potentials (0.94 and 0.85 V), a large limiting current density (5.94 mA cm) and a four-electron reaction process in 0.1 M KOH solution, which can be comparable with commercial Pt/C catalyst. Additionally, the FeCo-N/C-800 exhibited superior long-term durability and high methanol tolerance. The excellent electrocatalytic performance of the FeCo-N/C-800 can be ascribed to the mesoporous structure (bimodal pores system), the synergetic interaction of the multiple ORR active sites, suitable N-doping level and the highly conductive carbon matrix. These structural features can promote efficiently the mass and electron transfer, provide abundant active sites for the adsorption and reaction of oxygen molecules, and thus improve the reaction kinetics. The present study not only provides a strategy for the synthesis of carbon-based electrocatalyst with high ORR catalytic activity and stability, but also demonstrates that the bimetal- and nitrogen-codoped carbon materials could be a class of competitive candidate for non-noble metal-based electrocatalysts.

摘要

非贵金属电催化剂受到了广泛的研究,但如何在可持续性和竞争性能之间取得平衡,对于能源应用来说仍然是一个巨大的挑战。在这项工作中,通过一种简单的水热法,随后在氮气气氛中 800°C 的煅烧过程和酸刻蚀过程,成功合成了一种双金属和氮共掺杂介孔碳电催化剂(FeCo-N/C-800)。所得到的 FeCo-N/C-800 可以作为一种高性能的 ORR 催化剂,具有高起始电位和半波电位(0.94 和 0.85 V)、大极限电流密度(5.94 mA cm)和在 0.1 M KOH 溶液中四电子反应过程,可与商业 Pt/C 催化剂相媲美。此外,FeCo-N/C-800 表现出优异的长期耐久性和高甲醇耐受性。FeCo-N/C-800 的优异电催化性能可归因于介孔结构(双模态孔系统)、多种 ORR 活性位点的协同相互作用、合适的 N 掺杂水平和高导电性碳基质。这些结构特征可以有效地促进质量和电子转移,为氧分子的吸附和反应提供丰富的活性位点,从而提高反应动力学。本研究不仅为合成具有高 ORR 催化活性和稳定性的碳基电催化剂提供了一种策略,还证明了双金属和氮共掺杂碳材料可能成为一类有竞争力的非贵金属基电催化剂候选材料。

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