发表机构
Kyung Hee University（庆熙大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过第一性原理计算发现亚氮化物电子化合物Ba$_3$N可实现超低势垒钠离子传输，兼具平坦低电位平台与安全裕度，为高倍率钠存储电极提供了新设计范式。
AI 中文摘要
电子化合物是一类离子晶体，其中过剩电子在间隙空位中离域而非束缚于特定原子位点，表现出奇异的物理化学行为，但其作为电化学储能主体的潜力在很大程度上尚未被探索。在此，利用全面的第一性原理计算，我们证明了准一维亚氮化物电子化合物Ba$_3$N为克服钠离子电池负极中长期存在的性能权衡提供了一条引人注目的途径。钠自发嵌入开放的链间通道形成了热力学稳定的相，产生了异常平坦的低电位平台，避免了硬碳的高电位倾斜损耗，同时保留了防止枝晶形成的基本安全裕度。至关重要的是，巡回的间隙阴离子电子海通过抑制位点特异性轨道相互作用动态地平坦化势能景观，实现了具有极低迁移势垒的超快钠离子传输。这项工作建立了一种利用电子化合物化学实现超快电池电极的设计范式。
英文摘要
Electrides, ionic crystals in which excess electrons are delocalized within interstitial voids rather than bound to specific atomic sites, exhibit exotic physicochemical behaviors, yet their potential as electrochemical energy-storage hosts remains largely unexplored. Here, using comprehensive first-principles calculations, we demonstrate that the quasi-one-dimensional subnitride electride Ba$_3$N offers a compelling route to overcome the long-standing performance trade-offs in sodium-ion battery anodes. Spontaneous Na intercalation into the open interchain channels establishes thermodynamically stable phases, generating an exceptionally flat low-potential plateau that avoids the high-potential sloping losses of hard carbon while preserving an essential safety margin against dendrite formation. Crucially, the itinerant interstitial anionic electron sea dynamically flattens the potential landscape by suppressing site-specific orbital interactions, enabling ultrafast Na ion transport with an exceptionally low migration barrier. This work establishes a design paradigm for harnessing electride chemistry to achieve ultrafast battery electrodes.
Comments9 pages, 5 figures
