ZIF-L-derived FeN–hcC catalysts with curved carbon surfaces for effective oxygen reduction reaction over the entire pH range†

IF 2.7 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Xu Dai and Zhenlu Zhao
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Abstract

The development of highly active and stable iron–nitrogen (Fe–Nx) based oxygen reduction reaction (ORR) catalysts with pH versatility is one of the future directions of electrochemical energy. However, the task of designing and controlling the three-dimensional local structure of Fe species to obtain high ORR activity and stability remains a challenge. In this study, we prepared hierarchical porous FeN–hcC (iron–nitrogen–highly curved carbon) catalysts derived from ZIF-L by a soft template method. The highly curved carbon surface possibly results in a compressive strain effect on the supported Fe–Nx active site, which can not only enhance the high exposure of the active site to improve the electrocatalytic activity, but also facilitate the stability of the Fe–Nx site during the ORR catalytic process. FeN–hcC-1 exhibited a high half-wave potential of 0.89, 0.77 and 0.82 V vs. RHE in alkaline, acidic, and neutral media, respectively. In addition, after cyclic durability tests in different electrolyte environments, good stability is still maintained, which is significantly better than the planar Fe–Nx site and Pt/C catalyst. This work provides a new synthetic strategy for the construction of highly curved surfaces of carbon materials, while inspiring a method to improve the ORR performance of ZIF-derived materials.

Abstract Image

具有弧形碳表面的 ZIF-L 型 FeN-hcC 催化剂可在整个 pH 值范围内进行有效的氧还原反应†。
开发具有 pH 适应性的高活性和稳定的铁-氮(Fe-Nx)基氧还原反应(ORR)催化剂是未来电化学能源的发展方向之一。然而,设计和控制铁物种的三维局部结构以获得高 ORR 活性和稳定性仍然是一项挑战。在本研究中,我们采用软模板法制备了源自 ZIF-L 的分层多孔 FeN-hcC(铁-氮-高弯曲碳)催化剂。高弯曲碳表面可能会对支撑的 Fe-Nx 活性位点产生压应变效应,这不仅能增强活性位点的高暴露度以提高电催化活性,还能促进 Fe-Nx 位点在 ORR 催化过程中的稳定性。在碱性、酸性和中性介质中,FeN-hcC-1 对 RHE 的半波电位分别为 0.89、0.77 和 0.82 V。此外,在不同电解质环境中进行循环耐久性测试后,仍能保持良好的稳定性,明显优于平面 Fe-Nx 位点和 Pt/C 催化剂。这项工作为构建碳材料的高弯曲表面提供了一种新的合成策略,同时也启发了一种提高 ZIF 衍生材料 ORR 性能的方法。
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来源期刊
New Journal of Chemistry
New Journal of Chemistry 化学-化学综合
CiteScore
5.30
自引率
6.10%
发文量
1832
审稿时长
2 months
期刊介绍: A journal for new directions in chemistry
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