Yin Zhengxuan, Xiong Lixin, Su Neil Qiang
Center for Theoretical and Computational Chemistry, State Key Laboratory of Advanced Chemical Power Sources, Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Department of Chemistry, Nankai University, Tianjin 300071, China.
J Chem Theory Comput. 2024 Sep 3. doi: 10.1021/acs.jctc.4c00789.
The lithium-oxygen (Li-O) battery, renowned for its exceptionally high theoretical energy density, is poised to revolutionize next-generation energy storage systems. However, its practical application depends on overcoming several challenges, particularly the high cathode overpotential, which significantly diminishes the battery's energy efficiency and durability. This study delves into the interactions at the cathode surface during oxygen reduction and evolution reactions (ORR/OER), extending the analysis beyond the initial reaction stages to encompass the extensive charge-discharge process. We introduce and define the concepts of intrinsic equilibrium potential and intrinsic overpotential, demonstrating that these critical parameters are predominantly influenced by the growth of discharge products, rather than the catalysts, thereby underscoring the inherent properties of the battery. This shift in focus from merely enhancing cathode catalysts to understanding and leveraging the intrinsic characteristics of the battery discharge process opens new avenues for optimizing and enhancing the performance of large-scale Li-O batteries. Furthermore, our findings indicate potential broader applications to other metal-oxygen systems, paving the way for the design of high-capacity, high-efficiency energy storage technologies.
锂氧（Li-O）电池以其极高的理论能量密度而闻名，有望彻底改变下一代储能系统。然而，其实际应用取决于克服几个挑战，特别是高阴极过电位，这会显著降低电池的能量效率和耐久性。本研究深入探讨了氧还原和析氧反应（ORR/OER）过程中阴极表面的相互作用，将分析范围从初始反应阶段扩展到涵盖广泛的充放电过程。我们引入并定义了本征平衡电位和本征过电位的概念，表明这些关键参数主要受放电产物生长的影响，而非催化剂，从而突出了电池的固有特性。这种从单纯增强阴极催化剂到理解和利用电池放电过程固有特性的重点转变，为优化和提高大规模Li-O电池的性能开辟了新途径。此外，我们的研究结果表明其在其他金属-氧系统中可能有更广泛的应用，为设计高容量、高效率的储能技术铺平了道路。
