As one of the most promising electrode materials for capacitive deionization (CDI), the development of carbon materials with controllable pore structure and continuous mass production is essential for their practical application. Herein, a facile ultrasonic spray pyrolysis method was developed to synthesize surface-functionalized wrinkled hierarchical porous carbon spheres (HCS) with unique interconnected multi-cavity structures. The wrinkled and interconnected multi-cavity hierarchical pores of the HCS play a crucial role in providing accessible ion adsorption sites and promoting ion diffusion and storage in the “multi-cavity warehouse”. The carboxyl groups on the surface of HCS generate a negative charge that promotes the adsorption of cations. The optimized HCS possesses outstanding desalination capacity (114.25 mg g⁻¹), fast adsorption rate (6.57 mg g⁻¹ min⁻¹), and superior cycling stability (95%). Meanwhile, the HCS exhibited impressive desalination capacities in brackish water. Furthermore, the density functional theory calculation results confirmed that the synergistic effect of carboxyl groups and defects significantly enhanced the Na⁺ adsorption capacity and facilitated ion diffusion. This study extends the synthesis method of surface-functionalized hierarchical porous carbon, which is expected to facilitate the development of CDI electrode materials.

作为最有前途的电容去离子（CDI）电极材料之一，开发具有可控孔结构和连续批量生产的碳材料对其实际应用至关重要。在此，开发了一种简便的超声波喷雾热解方法来合成具有独特的互连多腔结构的表面功能化皱纹分级多孔碳球（HCS）。 HCS的褶皱且相互连接的多腔分级孔隙在提供可及的离子吸附位点以及促进离子在“多腔仓库”中扩散和存储方面发挥着至关重要的作用。 HCS表面的羧基产生负电荷，促进阳离子的吸附。优化后的HCS具有出色的脱盐能力（114.25 mg g ^{− 1} ）、快速吸附速率（6.57 mg g ^{− 1} min ^{− 1} ）和优异的循环稳定性（95%）。与此同时，HCS 展现出了令人印象深刻的苦咸水淡化能力。此外，密度泛函理论计算结果证实，羧基和缺陷的协同作用显着增强了Na ⁺吸附能力并有利于离子扩散。该研究扩展了表面功能化分级多孔碳的合成方法，有望促进CDI电极材料的发展。