调节纤维素衍生硬碳的氧官能度以实现优异的钠储存,Journal of Materials Chemistry A

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调节纤维素衍生硬碳的氧官能度以实现优异的钠储存
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-01-30 , DOI: 10.1039/d3ta07775f
Boyang Zhao ₁ , Xiaotian Li ₁ , Lei Shang ₁ , Chuang Qiu ₁ , Renlu Yuan ₁ , Haiyan Liu ₂ , Tao Liu ₂ , Ang Li ₁ , Xiaohong Chen ₁ , Huaihe Song ₁

Affiliation

纤维素由于其成本低廉且资源丰富，是用于钠离子电池负极的硬碳的重要前体。然而，如何调节纤维素基碳材料的结构以提高低压高原储钠能力仍然是一个巨大的挑战。这里，我们选择一种高聚合度、低结晶度的纤维素作为碳源。采用预氧化来裂解纤维素糖苷键并诱导分子链交联。纤维素的氧化交联过程产生更多的CO [双键，长度为m-破折号]

并保留更多的C-O。在热解过程中，会产生更窄和更长的石墨微晶结构，从而形成更大的闭孔。由具有最佳氧官能度含量的前体制备的硬碳样品表现出最低的比表面积（8.7 m ² g ^-1）和最高的闭孔体积。优化后平台容量大幅提升，实现了优异的储钠性能。可逆容量达到了426.8 mA hg ^-1的惊人值，其中平台容量占72.1%，达到307.5 mA hg ^-1。这项研究为钠离子电池领域具有相当大平台容量的硬碳负极的合理设计提供了宝贵的见解。

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Regulating oxygen functionalities of cellulose-derived hard carbon toward superior sodium storage

Cellulose is an important precursor for hard carbon for use in sodium-ion battery anodes, owing to its low cost and abundant resource. However, how to modulate the structure of cellulose-based carbon materials which possesses increased low-voltage plateau Na-storage capacity is still a great challenge. Herein, we select a kind of cellulose with high polymerization degree and low crystallinity as the carbon source. Pre-oxidation was employed to cleave the cellulose glycosidic bond and induce cross-linking of the molecular chains. The oxidative crosslinking process of cellulose produces more C [double bond, length as m-dash]

O and retains more C–O. During pyrolysis, narrower and longer graphite microcrystalline structures are generated, resulting in the formation of larger closed pores. The hard carbon samples prepared from the precursor with the optimal oxygen functionality content exhibit the lowest specific surface area (8.7 m² g⁻¹) and the highest closed pore volume. After optimization, there is a substantial increase in the plateau capacity, and excellent sodium storage performance is achieved. The reversible capacity achieves an impressive value of 426.8 mA h g⁻¹, with the plateau capacity accounting for 72.1% and reaching 307.5 mA h g⁻¹. This research provides valuable insights into the rational design of hard carbon anodes with a substantial plateau capacity in the field of sodium-ion batteries.

更新日期：2024-01-30

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