Capacitive deionization (CDI) has aroused significant concern for its application in treating low-concentration brackish water. However, some carbonaceous materials suffer from the limited salt adsorption capacity (SAC), sluggish adsorption kinetics, and inferior selectivity to particular ions. Hence, we develop the well-dispersed few-layered two-dimensional pseudocapacitive material MoS₂ connected with a robust 3D conductive architecture constructed by carbon nanotubes (CNT) and carbon spheres (CS) (MoS₂@CNT-CS). The enhanced dispersibility and expanded interlayer of MoS₂ nanosheets provide sufficient faradic effective sites for ion storage and transfer, while the interlaced carbonaceous network affords improved hydrophilicity, convenient electron transport path, and low charge transfer resistance for fast charge transportation and permeation. Therefore, the asymmetric hybrid CDI cell (CNT-CS for anode and MoS₂@CNT-CS for cathode) delivers a prominent SAC (25.35 mg g⁻¹), fast SAR (3.9 mg g⁻¹ min⁻¹), enhanced desalination kinetics, and favorable cycling stability. In addition, the specific ion selectivity of MoS₂@CNT-CS electrode was evaluated systematically in the equimolar multi-salt solutions, and a selectivity order of Ca²⁺ > Na⁺ > Mg²⁺ > K⁺ was obtained. The molecular dynamic (MD) calculation provides the lowest intercalation energy for Ca²⁺ (−2.55 eV), further confirming the strong interaction and preferable pseudocapacitive deionization of MoS₂@CNT-CS electrode to Ca²⁺ over other cations.

电容去离子（CDI）在处理低浓度微咸水方面的应用引起了人们的极大关注。然而，一些含碳材料的盐吸附能力（SAC）有限，吸附动力学缓慢，对特定离子的选择性较差。因此，我们开发了分散良好的少层二维赝电容材料 MoS ₂，该材料与由碳纳米管 (CNT) 和碳球 (CS) (MoS ₂ @CNT-CS)构建的坚固的 3D 导电结构相连。MoS ₂增强的分散性和扩展的中间层纳米片为离子存储和传输提供了足够的法拉第有效位点，而交错的碳质网络提供了更好的亲水性、方便的电子传输路径和低电荷传输阻力，以实现快速电荷传输和渗透。因此，不对称混合 CDI 电池（阳极的CNT-CS 和阴极的MoS ₂ @CNT-CS）提供显着的 SAC（25.35 mg g ^-1）、快速 SAR（3.9 mg g ^-1  min ^-1）、增强的脱盐动力学和良好的循环稳定性。此外，在等摩尔多盐溶液中系统地评估了 MoS ₂ @CNT-CS 电极的特定离子选择性，选择性顺序为 Ca ²⁺  > Na ⁺ > Mg ²⁺  > K ⁺获得。分子动力学 (MD) 计算为 Ca ²⁺ (-2.55 eV)提供了最低的嵌入能量，进一步证实了 MoS ₂ @CNT-CS 电极对 Ca ²⁺的强相互作用和更好的赝电容去离子作用，而不是其他阳离子。