Redefining closed pores in carbons by solvation structures for enhanced sodium storage

Closed pores are widely accepted as the critical structure for hard carbon negative electrodes in sodium-ion batteries. However, the lack of a clear definition and design principle of closed pores leads to the undesirable electrochemical performance of hard carbon negative electrodes. Herein, we reveal how the evolution of pore mouth sizes determines the solvation structure and thereby redefine the closed pores. The precise and uniform control of the pore mouth sizes is achieved by using carbon molecular sieves as a model material. We show when the pore mouth is inaccessible to N<sub>2</sub> but accessible to CO<sub>2</sub> molecular probes, only a portion of solvent shells is removed before entering the pores and contact ion pairs dominate inside pores. When the pore mouth is inaccessible to CO<sub>2</sub> molecular probes, namely smaller than 0.35 nm, solvent shells are mostly sieved and dominated anion aggregates produce a thin and inorganic NaF-rich solid electrolyte interphase inside pores. Closed pores are accordingly redefined, and initial coulombic efficiency, cycling and low-temperature performance are largely improved. Furthermore, we show that intrinsic defects inside the redefined closed pores are effectively shielded from the interfacial passivation and contribute to the increased low-potential plateau capacity.

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Publication Details

Journal
Nature Communications
Published
2025-04-16
DOI
https://doi.org/10.1038/s41467-025-59022-8
Citations
81
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
59.17

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article

Redefining closed pores in carbons by solvation structures for enhanced sodium storage

Ying Tao, Dong Qiu, Tengfei Cao, Quan‐Hong Yang et al.
81 citations
Nature Communications
Advancements in Battery Materials
59.17
article

Redefining closed pores in carbons by solvation structures for enhanced sodium storage

Ying Tao, Dong Qiu, Tengfei Cao, Quan‐Hong Yang, Guiming Zhong, Zhangquan Peng, Yue Chu, Xiaolong Zou, Feiyu Kang, Wei Zhong Lv, Yiran Jia, Haoyu Xue, Jun Zhang, Dawei Wang, Yibo Zhang, Siwei Zhang
article en
81 citations

Abstract

Closed pores are widely accepted as the critical structure for hard carbon negative electrodes in sodium-ion batteries. However, the lack of a clear definition and design principle of closed pores leads to the undesirable electrochemical performance of hard carbon negative electrodes. Herein, we reveal how the evolution of pore mouth sizes determines the solvation structure and thereby redefine the closed pores. The precise and uniform control of the pore mouth sizes is achieved by using carbon molecular sieves as a model material. We show when the pore mouth is inaccessible to N<sub>2</sub> but accessible to CO<sub>2</sub> molecular probes, only a portion of solvent shells is removed before entering the pores and contact ion pairs dominate inside pores. When the pore mouth is inaccessible to CO<sub>2</sub> molecular probes, namely smaller than 0.35 nm, solvent shells are mostly sieved and dominated anion aggregates produce a thin and inorganic NaF-rich solid electrolyte interphase inside pores. Closed pores are accordingly redefined, and initial coulombic efficiency, cycling and low-temperature performance are largely improved. Furthermore, we show that intrinsic defects inside the redefined closed pores are effectively shielded from the interfacial passivation and contribute to the increased low-potential plateau capacity.

Nature CommunicationsVol. 16(1)
Tianjin University (CN), Dalian Institute of Chemical Physics (CN), Shenzhen University (CN), Chinese Academy of Sciences (CN), Tianjin Economic-Technological Development Area (CN), Tsinghua–Berkeley Shenzhen Institute (CN), Collaborative Innovation Center of Chemical Science and Engineering Tianjin (CN), Shenzhen Technology University (CN), Tianjin haihe hospital (CN), Tsinghua University (CN)
National Natural Science Foundation of China
Openalex Percentile: Top 0%
Advancements in Battery Materials
59.17
DOIOpen Access PDFOpenAlex
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