Enabling Fast Interfacial Desolvation Kinetics in Hard Carbon Anodes via Boric Acid-Crosslinked Binder Network

As a key auxiliary component for electrode fabrication, the binder not only serves as the macroscopic scaffold that holds electrode constituents together, but also acts as a bridge governing electrode−electrolyte contact. While hard carbon (HC) offers efficient sodium storage capacity and superior cycling stability due to its unique hybrid ordered-disordered structure, its rate performance is often constrained by sluggish sodium-ion desolvation kinetics at the interface. To achieve uniform regulation of desolvation rates, we designed a crosslinked multifunctional binder, NaPAB, by incorporating boron centers with vacant orbitals into a sodium polyacrylic acid backbone. This creates a 3D network with Lewis acidic sites that uniformly cover the electrode interface, aligning with the desolvation region. These boron sites coordinate with solvent molecules via Lewis acid−base interactions, weakening Na + −solvent binding and thereby lowering the desolvation energy barrier, accelerating interfacial kinetics, and reducing in-plane heterogeneity. The improved uniformity alleviates local ionic flux disparities and suppresses kinetically driven sodium plating, enabling rapid and stable Na + insertion. Meanwhile, the crosslinked network enhances mechanical integrity by connecting hard-carbon particles and mitigating stress. The sodium-salt moieties offer partial Na + compensation to reduce first-cycle irreversibility. Additionally, boron sites facilitate the formation of a robust solid−electrolyte interphase (SEI), suppressing side reactions and ensuring long-term transport stability. Consequently, the NaPAB-based hard carbon anode exhibits a high initial Coulombic efficiency (ICE) of 89.06% and significantly enhanced rate capability in half-cells, with sodium plating effectively mitigated even after high-rate cycling. This work demonstrates that precisely regulating the interfacial microenvironment via a functionalized binder network is a promising strategy, offering a new perspective for optimizing the electrochemical performance of hard carbon.

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Journal
ACS Applied Energy Materials
Published
2026-06-28
DOI
https://doi.org/10.1021/acsaem.6c01107
Primary Topic
Advancements in Battery Materials
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article
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article

Enabling Fast Interfacial Desolvation Kinetics in Hard Carbon Anodes via Boric Acid-Crosslinked Binder Network

X Wang, Jinbao Zhao, Ruilai Ye, Xueying Yang et al.
ACS Applied Energy Materials
Advancements in Battery Materials
article

Enabling Fast Interfacial Desolvation Kinetics in Hard Carbon Anodes via Boric Acid-Crosslinked Binder Network

X Wang, Jinbao Zhao, Ruilai Ye, Xueying Yang, Qichen Chen, Yinghang Gao, Zhibin Lin, Peng Zhang, Shuang Liu
article en

Abstract

As a key auxiliary component for electrode fabrication, the binder not only serves as the macroscopic scaffold that holds electrode constituents together, but also acts as a bridge governing electrode−electrolyte contact. While hard carbon (HC) offers efficient sodium storage capacity and superior cycling stability due to its unique hybrid ordered-disordered structure, its rate performance is often constrained by sluggish sodium-ion desolvation kinetics at the interface. To achieve uniform regulation of desolvation rates, we designed a crosslinked multifunctional binder, NaPAB, by incorporating boron centers with vacant orbitals into a sodium polyacrylic acid backbone. This creates a 3D network with Lewis acidic sites that uniformly cover the electrode interface, aligning with the desolvation region. These boron sites coordinate with solvent molecules via Lewis acid−base interactions, weakening Na + −solvent binding and thereby lowering the desolvation energy barrier, accelerating interfacial kinetics, and reducing in-plane heterogeneity. The improved uniformity alleviates local ionic flux disparities and suppresses kinetically driven sodium plating, enabling rapid and stable Na + insertion. Meanwhile, the crosslinked network enhances mechanical integrity by connecting hard-carbon particles and mitigating stress. The sodium-salt moieties offer partial Na + compensation to reduce first-cycle irreversibility. Additionally, boron sites facilitate the formation of a robust solid−electrolyte interphase (SEI), suppressing side reactions and ensuring long-term transport stability. Consequently, the NaPAB-based hard carbon anode exhibits a high initial Coulombic efficiency (ICE) of 89.06% and significantly enhanced rate capability in half-cells, with sodium plating effectively mitigated even after high-rate cycling. This work demonstrates that precisely regulating the interfacial microenvironment via a functionalized binder network is a promising strategy, offering a new perspective for optimizing the electrochemical performance of hard carbon.

ACS Applied Energy Materials
Xiamen University (CN), China Tobacco (CN), Tan Kah Kee Innovation Laboratory (CN), Collaborative Innovation Center of Chemistry for Energy Materials (CN)
Openalex Percentile: Top 11%
Advancements in Battery Materials
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