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Revealing the Double‐Edged Behaviors of Heteroatom Sulfur in Carbonaceous Materials for Balancing K‐Storage Capacity and Stability
Advanced Functional Materials ( IF 19.0 ) Pub Date : 2020-11-20 , DOI: 10.1002/adfm.202006875
Yong Qian 1 , Yang Li 1 , Zheng Yi 1 , Jie Zhou 1 , Zhen Pan 1 , Jie Tian 2 , Yusong Wang 1 , Shanshan Sun 3 , Ning Lin 1 , Yitai Qian 1
Affiliation  

Heteroatoms in the carbon matrix are generally considered as active sites to enhance potassium storage capacity, while their adverse effects on ion batteries remain unclear. Herein, a series of sulfur doped carbon (SCDPx) with adjustable S content and crystallinity are accurately synthesized in the closed autoclave by controlling the ratios of precursors. Electrochemical measurements exhibit that heteroatom sulfur displays double‐edged electrochemical activities with a high initial potassium storage capacity but poor cycling stability for carbon anode. Combined with solid‐state nuclear magnetic resonance (NMR), catalytic tests, and various ex‐situ characterizations, it is demonstrated that abundant S in the carbon would not only form CSC bonds, acting as active sites to reversibly adsorb/desorb potassium ions for high capacity, but also significantly catalyze the reduction and decomposition of the electrolyte including KPF6 and ethylene carbonate/diethyl carbonate (EC/DEC) to form thicker solid electrolyte interface (SEI) and degrade electrolyte, resulting in rapid capacity decay. As a result, the optimized sample (SCDP2) with the appropriate sulfur doping content exhibits the best electrochemical performance with high capacity (688.4 mA h g−1 at 100 mA g−1), long‐term cycling stability (198.4 mA h g−1 at 2000 mA g−1 after 10 000 cycles), and excellent rate capability (238.8 mA h g−1 at 5000 mA g−1).

中文翻译:

揭示碳质材料中杂原子硫的双刃行为,以平衡钾存储容量和稳定性

碳基体中的杂原子通常被认为是增强钾储存能力的活性位点,但它们对离子电池的不利影响仍不清楚。在此,通过控制前驱体的比例,在密闭高压釜中精确地合成了具有可调节的S含量和结晶度的一系列硫掺杂碳(SCDP x)。电化学测量表明,杂原子硫表现出双刃电化学活性,具有较高的初始钾存储容量,但对碳阳极的循环稳定性较差。与固态核磁共振(NMR),催化测试,以及各种易地表征结合中,证明的是,在碳丰富S。将不仅C型小号C键可作为活性位点可逆地吸附/解吸钾离子以实现高容量,同时还显着催化包括KPF 6和碳酸亚乙酯/碳酸二乙酯(EC / DEC)在内的电解质的还原和分解,从而形成较厚的固体电解质界面( SEI)并降解电解质,导致容量快速衰减。其结果,最优化的样品(SCDP2)与合适的硫掺杂含量表现出具有高容量(688.4毫安汞柱电化学性能最好-1在100mA克-1),长期循环稳定性(198.4毫安汞柱-1在2000毫安克-1 10 000次循环后),以及优异的倍率性能(238.8毫安汞柱-1在5000毫安克-1)。
更新日期:2020-11-20
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