Yin Hong, Deng Yiqiong, He Zhe, Xu Wenyuan, Hou Zhaohui, He Binhong, Çaha İhsan, Cunha Joao, Karimi Maryam, Yu Zhipeng
Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials, School of Chemistry and Chemical Engineering, Hunan Institute of Science and Technology, Yueyang 414006, China; International Iberian Nanotechnology Laboratory (INL), Braga 4715-330, Portugal.
Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials, School of Chemistry and Chemical Engineering, Hunan Institute of Science and Technology, Yueyang 414006, China.
J Colloid Interface Sci. 2025 Jan 15;678(Pt A):447-457. doi: 10.1016/j.jcis.2024.08.165. Epub 2024 Aug 25.
Developing efficient and cost-effective platinum-group metal-free (PGMF) catalysts for the oxygen reduction reaction (ORR) is crucial for energy conversion and storage devices. Among these catalysts, metal-nitrogen-carbon (MNC) materials, particularly cobalt single-atom catalysts (CoNC), show promise as ORR electrocatalysts. However, their ORR activity is often hindered by strong hydroxyl (OH) adsorption on the Co sites. While the impact of strain engineering on MNC electrocatalysts has been minimally explored, recent studies suggest its potential to enhance catalytic performance and optimize intrinsic activity in traditional bulk catalysts. In this context, we investigate the effect of surface strain on CoNC for ORR activity and correlate substrate-strain-induced geometric distortions with catalytic activity using experimental and theoretical methods. The findings suggest that the d-band center gap of spin states (Δε) may be a preferred descriptor for predicting strain-dependent ORR performance in MNC catalysts. Leveraging CoNC moiety placed on a substrate with an average size of 1.0 μm, we achieve performance comparable to that of commercial Pt/C catalysts when used as a cathode catalyst in zinc-air batteries. This investigation unveils the structure-function relationship of MNC electrocatalysts regarding strain engineering and provides valuable insights for future ORR activity design and enhancement.
开发用于氧还原反应（ORR）的高效且经济高效的无铂族金属（PGMF）催化剂对于能量转换和存储设备至关重要。在这些催化剂中，金属-氮-碳（MNC）材料，特别是钴单原子催化剂（CoNC），有望成为ORR电催化剂。然而，它们的ORR活性常常受到钴位点上强烈的羟基（OH）吸附的阻碍。虽然应变工程对MNC电催化剂的影响研究较少，但最近的研究表明其有潜力提高传统块状催化剂的催化性能并优化本征活性。在此背景下，我们使用实验和理论方法研究表面应变对CoNC的ORR活性的影响，并将底物应变诱导的几何畸变与催化活性相关联。研究结果表明，自旋态的d带中心间隙（Δε）可能是预测MNC催化剂中应变依赖的ORR性能的首选描述符。利用放置在平均尺寸为1.0μm的底物上的CoNC部分，当用作锌空气电池的阴极催化剂时，我们实现了与商业Pt/C催化剂相当的性能。这项研究揭示了MNC电催化剂在应变工程方面的结构-功能关系，并为未来ORR活性的设计和增强提供了有价值的见解。
