Molecular Stitching in Polysaccharide Precursor for Fabricating Hard Carbon with Ultra‐High Plateau Capacity of Sodium Storage,Advanced Materials

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Molecular Stitching in Polysaccharide Precursor for Fabricating Hard Carbon with Ultra‐High Plateau Capacity of Sodium Storage
Advanced Materials ( IF 27.4 ) Pub Date : 2025-03-25 , DOI: 10.1002/adma.202420251
Zhenzhuang Wen ₁ , Ruiguang Zhao ₁ , Tongtong Tian ₁ , Tao Zhang ₁ , Xin Wang ₁ , Xinyi Yang ₁ , Wanqing Song ₁ , Yanan Chen _{1,

2,

3} , Jia Ding _{1,

2,

3} , Wenbin Hu _{1,

2,

3}

Affiliation

High energy density of sodium‐ion batteries (SIBs) requires high low‐voltage capacity and initial Coulombic efficiency for hard carbon. However, simultaneously achieving both characteristics is a substantial challenge. Herein, a unique molecular stitching strategy is proposed to edit the polymeric structure of common starch for synthesizing cost‐effective hard carbon (STHC‐MS). A mild air‐heating treatment toward starch is employed to trigger the esterification reaction between carboxyl and hydroxy groups, which can effectively connect the branched polysaccharide chains thereby constructing a highly cross‐linked polymeric network. In contrast with the pristine branched‐chain starch, the cross‐linking structured precursor evolves into highly twisted graphitic lattices creating a large population of closed ultramicro‐pores (<0.3 nm) enabling the storage of massive sodium clusters. Resultantly, STHC‐MS delivers a reversible capacity of 348 mAh g−1 with a remarkable low‐voltage (below 0.1 V) capacity of 294 mAh g−1, which becomes more attractive by combining the high initial Coulombic efficiency of 93.3%. Moreover, STHC‐MS exhibits outstanding stability of 0.008% decay per cycle over 4800 cycles at 1 A g−1. STHC‐MS||Na3V2(PO3)4 full cells achieve an energy density of 266 Wh kg−1, largely surpassing the commercial hard carbon‐based counterpart. This work opens the avenue of molecular‐level modulation in organic precursors for developing high‐performance hard carbon in SIBs.

中文翻译：

多糖前驱体中的分子拼接用于制备具有超高钠储存能力的硬碳

钠离子电池（SIB）的高能量密度需要高低压容量和硬碳的初始库仑效率。然而，同时实现这两个特性是一项巨大的挑战。在此，提出了一种独特的分子拼接策略来编辑常见淀粉的聚合物结构，以合成具有成本效益的硬碳（STHC-MS）。对淀粉采用温和的空气加热处理来触发羧基和羟基之间的酯化反应，这可以有效地连接支链多糖链，从而构建高度交联的聚合物网络。与原始支链淀粉相比，交联结构前驱体演变成高度扭曲的石墨晶格，形成大量封闭的超微孔（<0.3 nm），从而能够储存大量的钠簇。因此，STHC-MS 可提供 348 mAh g-1 的可逆容量和 294 mAh g-1 的显著低电压（低于 0.1 V）容量，结合 93.3% 的高初始库仑效率，它变得更加有吸引力。此外，STHC-MS 在 1 A g-1 下，在 4800 次循环中表现出每个循环 0.008% 衰减的出色稳定性。STHC-MS ||Na3V2（PO3）4 全电池的能量密度为 266 Wh kg-1，大大超过了商业硬碳基电池。这项工作为在 SIB 中开发高性能硬碳开辟了有机前驱体分子水平调制的途径。

更新日期：2025-03-25

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