Exploring Curvature-Induced Strain Engineering in Cobalt Single-Atom Catalysts for Enhancing Oxygen Reduction Reaction Performance

The development of efficient and cost-effective catalysts for the oxygen reduction reaction (ORR) is important for advancing energy conversion and storage technologies. Among the most promising candidates are nitrogen-coordinated single metal sites embedded in carbon supports (M–N–C).1 While strain engineering has been extensively studied for bulky catalysts, the application of this approach to M–N–C catalysts remain largely unexplored. This presentation will focus on a novel strain engineering route relaying on substrate curvature, which enables beneficial modifications of the coordination environment of cobalt centers in CoSA–N–C catalysts.2 Using a combination of experimental techniques and DFT calculations, we show that curvature-induced strain optimizes the d-band center gap of spin states (Δε d), a critical physical descriptor for ORR activity. Cobalt single-atom catalysts synthesized with optimal strain (CoSA–N–C–1.0) exhibited exceptional ORR performance, achieving an onset potential E onset = 1.05 V, robust durability, and superior methanol tolerance compared to commercial benchmark Pt/C catalysts. When employed as cathode materials in zinc-air batteries, CoSA–N–C–1.0 delivered a remarkable power density of 177 mW/cm2, demonstrating significant potential for practical energy applications. This work underscores the synergistic relationship between curvature-induced strain and traditional electronic structure modifications. The presentation will conclude with an outlook on how the proposed strain-engineering strategy can broaden the design principles for M–N–C catalysts, serving as a versatile platform for enhancing catalytic performance across a wide range of applications, from energy conversion to environmental remediation. Reference: [1] Yu, Z. P.; Si, C. W.; LaGrow, A. P.; Tai, Z. X.; Caliebe, W. A.; Tayal, A.; Sampaio, M. J.; Sousa, J. P. S.; Amorim, I.; Araujo, A.; Meng, L. J.; Faria, J. L.; Xu, J. Y.*; Li, B.*; Liu, L. F.* Iridium–Iron Diatomic Active Sites for Efficient Bifunctional Oxygen Electrocatalysis. ACS Catal., 2022, 12, 9397-9409. [2] Yin, H.; Deng, Y. Q.; He, Z.; Xu, W. Y.; Hou, Z. H.; He, B. H.; Çaha, I.; Cunha, J.; Karimi, M.; Yu, Z. P.* Strain engineering of CoSA-N-C catalyst toward enhancing the oxygen reduction reaction activity. J. Colloid Interf. Sci., 2025, 678, 447-457. Figure 1