Two-dimensional (2D) metal-organic frameworks (MOFs) exhibit great promise as high-energy anode materials for next-generation lithium-ion capacitors (LICs) due to their tunable chemistry and short ion transport paths. Nevertheless, high-throughput production of ultrathin 2D MOFs and energy storage mechanism analysis are still full of challenges. Here, theoretical calculations indicate that partial introduction of Fe in Co sites can enhance interaction of metal centers with water in solvents due to the strong 3d-2p orbital binding energy, which induces ultrathin nanosheets, resulting in exposure of high-density ligand active sites, lower band gap and higher Young modulus during lithium insertion. Greatly, ultrathin 2D Co/Fe-BDC nanosheets are obtained with a bottom-up method and can be scaled up to high-throughput production. In/ex-situ results further reveal highly reversible insertion/extraction reactions accompanied by crystalline to amorphous for Co/Fe-BDC anodes. LICs with optimal Co₄Fe-BDC anode deliver high energy density (199.7 Wh kg⁻¹) and power density (10,000 W kg⁻¹), together with superior cycle lifespan. This work offers in-depth insights for the high-throughput synthesis and the storage mechanism in 2D MOFs.

二维 (2D) 金属有机框架 (MOF) 由于其可调节的化学性质和短的离子传输路径，作为下一代锂离子电容器 (LIC) 的高能阳极材料具有很大的前景。尽管如此，超薄二维MOFs的高通量生产和储能机理分析仍然充满挑战。在这里，理论计算表明，由于强大的 3d-2p 轨道结合能，在 Co 位点中部分引入 Fe 可以增强金属中心与溶剂中水的相互作用，从而诱导超薄纳米片，导致高密度配体活性位点的暴露，在锂插入过程中具有较低的带隙和较高的杨氏模量。重要的是，超薄二维 Co/Fe-BDC 纳米片是通过自下而上的方法获得的，并且可以扩大到高通量生产。原位/异位结果进一步揭示了高度可逆的插入/脱出反应，伴随着 Co/Fe-BDC 阳极的结晶到无定形。具有最佳 Co ₄ Fe-BDC 阳极的 LIC 可提供高能量密度 (199.7 Wh kg ^-1 ) 和功率密度 (10,000 W kg ^-1 )，以及出色的循环寿命。这项工作为二维 MOF 中的高通量合成和存储机制提供了深入的见解。