Transition metal sulfides with hierarchical (ball in ball) micro/nanoporous structures have drawn wide spread interests for various applications, such as energy storage, catalysis, solar cells, owing to their unique features and intriguing properties. However, precise control of synthesizing process for hierarchical porous nanospheres of transition metal sulfides remains a big challenge. In addition, the charging and discharging process of transition metal sulfides in electrochemical storage is still a black box. Herein we design and precise control of synthesizing a transition metal sulfide with hierarchical porous nanosphere structure, namely cobalt sulfide hierarchical porous nanospheres (HPNs). Brownian snowball mechanism is put forward to explain the formation mechanism of CoS samples, which is supported by first-principles calculations. The proposed Brownian snowball mechanism helps us understand the formation process and facilitates comprehensive and precise manipulation, a key requirement for industrial scale-up. The CoS hierarchical porous nanospheres with a specific surface area of approximately 140 m²/g possess a total specific capacitance of 1310 F/g and 932 F/g at a current density of 5 A/g when used as electrode materials for electrochemical capacitors. The capacitance reflected hybrid electrical energy storage and is separated into double layer charging and the Faradaic contribution from the OH⁻ ions reactions with surface atoms. It is demonstrated that Faradaic capacitance dominates in CoS hierarchical porous nanospheres exceeding 770 F/g by an analysis of the voltammetric sweep data.

具有分层（球形）微/纳米孔结构的过渡金属硫化物因其独特的特性和令人着迷的特性而在各种应用中引起了广泛的关注，例如能量存储，催化，太阳能电池。然而，精确控制过渡金属硫化物的分级多孔纳米球的合成过程仍然是一个巨大的挑战。另外，电化学存储中过渡金属硫化物的充放电过程仍然是一个黑匣子。本文中，我们设计并精确控制了具有分级多孔纳米球结构的过渡金属硫化物的合成，即硫化钴分级多孔纳米球（HPNs）。提出了布朗雪球机制来解释CoS样本的形成机理，并得到第一性原理的支持。拟议的布朗雪球机制有助于我们理解形成过程并促进全面而精确的操纵，这是工业规模扩大的关键要求。具有约140 m比表面积的CoS分层多孔纳米球² / g用作电化学电容器的电极材料时，在5 A / g的电流密度下具有1310 F / g和932 F / g的总比电容。电容反射混合式电能储存，并被分离成双层充电，并从OH法拉第贡献^-与表面原子离子的反应。通过伏安扫描数据的分析表明，法拉第电容在CoS分层多孔纳米球中的含量超过770 F / g。