Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries. However, an elaborate structure that could simultaneously endow active materials with promoted reaction reversibility, accelerated kinetic and restricted volume change still remains a huge challenge. Herein, a novel chemical interaction motivated structure design strategy has been proposed, and a chemically bonded Co(CO₃)_0.5OH·0.11H₂O@MXene (CoCH@MXene) layered-composite was fabricated for the first time. In such a composite, the chemical interaction between Co²⁺ and MXene drives the growth of smaller-sized CoCH crystals and the subsequent formation of interwoven CoCH wires sandwiched in-between MXene nanosheets. This unique layered structure not only encourages charge transfer for faster reaction dynamics, but buffers the volume change of CoCH during lithiation-delithiation process, owing to the confined crystal growth between conductive MXene layers with the help of chemical bonding. Besides, the sandwiched interwoven CoCH wires also prevent the stacking of MXene layers, further conducive to the electrochemical performance of the composite. As a result, the as-prepared CoCH@MXene anode demonstrates a high reversible capacity (903.1 mAh g⁻¹ at 100 mA g⁻¹) and excellent cycling stability (maintains 733.6 mAh g⁻¹ at 1000 mA g⁻¹ after 500 cycles) for lithium ion batteries. This work highlights a novel concept of layer-by-layer chemical interaction motivated architecture design for futuristic high performance electrode materials in energy storage systems.

合理的架构设计已被证明是提高电池电极材料电化学性能的有效策略。然而，能够同时赋予活性材料促进反应可逆性、加速动力学和限制体积变化的精细结构仍然是一个巨大的挑战。在此，提出了一种新的化学相互作用驱动结构设计策略，并首次制备了化学键合的 Co(CO ₃ ) _0.5 OH·0.11H ₂ O@MXene (CoCH@MXene) 层状复合材料。在这种复合材料中，Co ²⁺之间的化学相互作用和 MXene 驱动更小尺寸的 CoCH 晶体的生长以及随后夹在 MXene 纳米片之间的交织 CoCH 线的形成。这种独特的层状结构不仅促进电荷转移以加快反应动力学，而且在锂化-脱锂过程中缓冲 CoCH 的体积变化，这是由于在化学键的帮助下导电 MXene 层之间的晶体生长受限。此外，夹层交织的 CoCH 线还可以防止 MXene 层的堆叠，进一步有利于复合材料的电化学性能。其结果是，所制备的COCH @ MXene阳极演示了高可逆容量（毫安903.1克^-1在100mA克^-1）和优异的循环稳定性（维持733.6毫安克^-1在 1000 mA g ^-1 500 次循环后）锂离子电池。这项工作突出了储能系统中未来高性能电极材料的逐层化学相互作用驱动架构设计的新概念。