Modulating the oxidation states of transition metal species has been regarded as a promising strategy to tune the redox activity and achieve more active sites in electrode materials. In this work, a unique three-dimensional (3D) honeycomb-like cobalt sulfide (Co_xS_y) network organized by cross-linked nanosheets (Co_xS_y-T NSs) was prepared via a simple triethanolamine (TEOA)-assisted self-templating strategy. Interestingly, it has been found for the first time that the introduction of TEOA in the reaction effectively increases the ratio of high-valence Co³⁺ in the final product. Benefiting from the synergetic effect of the tailored high-valence Co³⁺ with the 3D network structure, the Co_xS_y-T NS electrode exhibits a maximum specific capacity of 351 mAhg⁻¹ (2635 F g⁻¹) at 5 A g⁻¹ as well as excellent cycling stability. Furthermore, with the solid-state asymmetric supercapacitor (ASC) constructed based on the Co_xS_y-T NSs and activated carbon (AC) electrodes, a high energy density up to 81.62 W h kg⁻¹ has been achieved at the power density of 0.81 kW kg⁻¹ and 96.2% capacitance is preserved after 7000 cycles, indicating robust cycling stability. This result high lights the simple approach of simultaneously tailoring high valence metal species and constructing 3D network structure toward high performance electrode materials for energy sto rage and conversion.

调节过渡金属物质的氧化态已被认为是一种有前途的策略，可调节氧化还原活性并在电极材料中获得更多的活性位。在这项工作中，通过简单的三乙醇胺（TEOA）辅助制备了由交联的纳米片（Co _x S _y -T NSs）组织的独特的三维（3D）蜂窝状硫化钴（Co _x S _y）网络。自我模板化策略。有趣的是，首次发现在反应中引入TEOA有效地提高了最终产物中高价Co ³⁺的比例。受益于量身定制的高价Co ³⁺的协同效应凭借3D网络结构，Co _x S _y -T NS电极在5 A g ^-1下显示的最大比容量为351 mAhg ^-1（2635 F g ^-1），并且具有出色的循环稳定性。此外，使用基于Co _x S _y -T NSs和活性炭（AC）电极构造的固态不对称超级电容器（ASC），在功率密度下已实现高达81.62 W h kg ^-1的高能量密度的0.81 kW kg ^-17000次循环后保留96.2％的电容，表明强大的循环稳定性。该结果使人们轻松掌握了同时定制高价金属种类和针对高性能电极材料构建3D网络结构以进行能量存储和转换的简单方法。