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二维过渡金属硼化物（MBene）作为新型金属离子电池电极材料，具有MB、M2B、M2B2等多种相结构，然而现有研究对于M2B相体系的探索仍显匮乏。本研究聚焦于M2B相MBene的设计，首次构建了硫（S）官能团化的Zr2BS2和Nb2BS2两种全新材料，系统揭示了其作为锂/钠离子电池负极材料的性能机制。通过第一性原理的计算方法，证实Zr2BS2和Nb2BS2两种材料具备优异的结构稳定性，并且在钠离子电池中展现出较高的理论比容量（分别为624 mA h g-1;和616 mA h g-1）以及较低的扩散势垒（Na+扩散势垒低至0.131 eV和0.088 eV）。同时，其较低的开路电压（0.38 V和0.21 V）可有效抑制枝晶生长，兼具高容量与安全性。本研究不仅完善了M2B相MBene体系的系统性研究，更为开发高容量、快充型钠离子电池负极材料提供了理论指导。Two-dimensional transition metal borides (MBene), as emerging electrode materials for metal-ion batteries, exhibit diverse phase structures including MB, M2B, and M2B2. However, current research remains insufficient in exploring the M2B-phase system. This study focuses on the design of M2B-phase MBenes, pioneering the construction of two novel sulfur-functionalized materials, Zr2BS2 and Nb2BS2, while systematically elucidating their performance mechanisms as anode materials for lithium/sodium-ion batteries. Through first-principles calculations, both Zr2BS2 and Nb2BS2 demonstrate exceptional structural stability and superior electrochemical properties in sodium-ion battery applications. Specifically, they exhibit high theoretical specific capacities (624 mA h g-1 and 616 mA h g-1) and remarkably low diffusion energy barriers for Na⁺ (0.131 eV and 0.088 eV). Moreover, their low open-circuit voltages (0.38 V and 0.21 V) effectively suppress dendrite growth, achieving an optimal balance between high capacity and operational safety. This work not only establishes a theoretical framework for MBene-based anode design but also provides critical insights into the correlation between surface functionalization, structural stability, and ion transport kinetics. The findings offer valuable guidance for developing other two-dimensional materials and non-layered systems, while contributing to mechanistic understanding of charge-discharge processes in transition metal dichalcogenide TMD-based lithium/sodium-ion batteries.
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