Crosslinking modification of starch improves the structural stability of hard carbon anodes for high-capacity sodium storage.

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Journal of Colloid and Interface Science Pub Date : 2025-01-15 Epub Date: 2024-09-24 DOI:10.1016/j.jcis.2024.09.191
Yangkai Sun, Tianchi Shen, Zijian He, Shurong Wang
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Abstract

Compared with the complex components of raw biomass, biomass derivatives with defined structures are more conducive to the controllable synthesis of hard carbon (HC) materials. Starch-based HC has garnered significant attention because of its cost-effectiveness; however, its practical applicability is limited by poor thermal stability. Herein, we propose a strategy for improving the stability of starch through self-assembly crosslinking modification, yielding high-performance HC. Starch and citric acid form a dense crosslinked structure through esterification between hydroxyl and carboxyl groups, effectively overcoming the poor thermal stability. The resulting HC exhibits a low specific surface area (SSA) and abundant closed pore structures, thereby enabling substantial sodium-ion storage. The optimized HC exhibits an improved reversible capacity of 378 mAh g-1 and an initial Coulombic efficiency (ICE) of 90.9 %. After 100 cycles at 0.5 C, it retains 98 % initial capacity. The assembled full-cell shows a high energy density of 248 Wh kg-1. Furthermore, the structure-performance relationship analysis reveals that the slope capacity is primarily affected by the defect concentration, while the plateau capacity is mainly determined by the closed pore structure. Galvanostatic intermittent titration technique (GITT) tests and in-situ Raman spectroscopy reveal that the sodium-ion storage mechanism in starch-based HC is "adsorption-intercalation/filling."

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淀粉的交联改性提高了用于高容量钠储存的硬碳阳极的结构稳定性。
与原料生物质的复杂成分相比,具有确定结构的生物质衍生物更有利于可控合成硬碳(HC)材料。淀粉基硬碳材料因其成本效益高而备受关注,但由于热稳定性差,其实际应用受到限制。在此,我们提出了一种通过自组装交联改性来提高淀粉稳定性的策略,从而获得高性能的碳氢化合物。淀粉和柠檬酸通过羟基和羧基之间的酯化作用形成致密的交联结构,有效克服了热稳定性差的问题。由此产生的碳氢化合物具有较低的比表面积(SSA)和丰富的封闭孔结构,从而实现了大量的钠离子存储。优化后的 HC 的可逆容量提高到 378 mAh g-1,初始库仑效率 (ICE) 为 90.9%。在 0.5 摄氏度条件下循环 100 次后,它仍能保持 98% 的初始容量。组装后的全电池显示出 248 Wh kg-1 的高能量密度。此外,结构性能关系分析表明,斜坡容量主要受缺陷浓度的影响,而高原容量则主要由封闭的孔隙结构决定。电晕静态间歇滴定技术(GITT)测试和原位拉曼光谱显示,淀粉基碳氢化合物中的钠离子存储机制是 "吸附-间隙/填充"。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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