Li Jun-Kang, Zhao Haobo, Zhang Yang, Ma Jing-Jing, Wang Fen-Fen, Zhao Shu-Na, Li Jun, Zang Shuang-Quan
Henan Key Laboratory of Crystalline Molecular Functional Materials, College of Chemistry and Pingyuan Laboratory, Zhengzhou University, Zhengzhou, 450001, China.
Department of Chemistry and Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Tsinghua University, Beijing, 100084, China.
Adv Sci (Weinh). 2025 Feb;12(6):e2412387. doi: 10.1002/advs.202412387. Epub 2024 Dec 16.
Curvature-induced interfacial electric field effects and local strain engineering offer a powerful approach for optimizing the intrinsic catalytic activity of single-atom catalysts (SACs). Investigations into the surface curvature on SACs are still ongoing, and the impact of the concave surface is often overlooked. In this work, theoretical calculations indicate that curved surfaces, particularly those with concavity, can optimize the electronic structures of single Fe sites and facilitate the reductive release of *OH. A carbon sphere featuring uniformly oriented channels and a chiral multi-shelled carbon hollow nanosphere are selected as carbon matrices due to their accessible concave and/or convex surfaces. After loading Fe species, the resulting catalysts with Fe SA in curved surfaces exhibit excellent oxygen reduction reaction activity (E = ≈0.89 V), strong methanol tolerance, and favorable long-term stability. Impressively, a solid-state flexible Zn-air battery based on this catalyst exhibits a remarkable durability over 40 h with a high peak power density of 122.1 mW cm and excellent charge-discharge performance at different bending angles. This work offers in-depth insights into the rational design of carbon supports with highly curved surfaces, offering new opportunities for the microenvironmental regulation of SACs at the atomic level.
曲率诱导的界面电场效应和局部应变工程为优化单原子催化剂（SACs）的本征催化活性提供了一种强有力的方法。对SACs表面曲率的研究仍在进行中，而凹面的影响常常被忽视。在这项工作中，理论计算表明，弯曲表面，特别是具有凹面的表面，可以优化单个铁位点的电子结构，并促进*OH的还原释放。由于具有可及的凹面和/或凸面，具有均匀取向通道的碳球和手性多壳碳空心纳米球被选作碳基质。负载铁物种后，所得的在弯曲表面含有铁单原子的催化剂表现出优异的氧还原反应活性（E = ≈0.89 V）、强甲醇耐受性和良好的长期稳定性。令人印象深刻的是，基于这种催化剂的固态柔性锌空气电池在40小时以上表现出卓越的耐久性，具有122.1 mW cm的高峰值功率密度，并且在不同弯曲角度下具有优异的充放电性能。这项工作为具有高度弯曲表面的碳载体的合理设计提供了深入见解，为在原子水平上对SACs进行微环境调控提供了新机会。
