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炭化温度诱导的硬碳结构演变及其储钠机制研究

Study on evolution of hard carbon structure induced by carbonization temperature and its sodium storage mechanism

  • 摘要: 以聚苯胺为前驱体,经过不同炭化温度制备硬碳材料,利用XRD、XPS、SEM和TEM对材料的形貌结构进行表征,以其为负极材料组装了钠离子半电池,并通过恒流充放电测试其电化学性能。实验结果表明,随着温度的升高,硬碳材料的碳层结构由无序到有序转变,其中石墨化程度、缺陷浓度、孔结构及层间距与炭化温度密切相关。当炭化温度为1 200℃时,硬碳材料具有发达的闭孔结构和最优的综合电化学性能,以其为负极组装的钠离子半电池,具有88%的初始库仑效率和291.7 mAh/g的比容量。非原位拉曼光谱测试结果进一步表明,随着电压从2.000 V放电至0.001 V,硬碳材料表现出“表面吸附-层间插层-闭孔填充”的储钠机制。

     

    Abstract: Using polyaniline as a precursor,a series of hard carbon materials were prepared at different carbonization temperatures. The morphology and structure of the materials were characterized using XRD,XPS,SEM and TEM. Sodium-ion half-cells were assembled with these materials as the anode,and their electrochemical performance was evaluated through galvanostatic charge-discharge tests. The results demonstrate that the carbon layer structure of hard carbon transitions from disordered to ordered with increasing temperature.The degree of graphitization,defect concentration,pore structure and interlayer spacing are critically dependent on the carbonization temperature. Key parameters such as the degree of graphitization,defect concentration,pore structure,and interlayer spacing are highly dependent on the regulation of the carbonization temperature. When the carbonization temperature is 1 200 ℃,the hard carbon material exhibits a well-developed closed pore structure and optimal overall electrochemical performance. The sodium-ion half-cells assembled with these materials as the anode demonstrate an initial Coulombic efficiency of 88% and a specific capacity of 291.7 mAh/g. Ex-situ Raman test results further reveal that as the voltage decreases from 2.000 V to 0.001 V during discharge,the material exhibits a sodium storage mechanism of "surface adsorption-intercalation into interlayers-closed pore filling.

     

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