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 rev...

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Published in:Nature communications Vol. 16; no. 1; pp. 3634 - 13
Main Authors: Zhang, Yibo, Zhang, Si-Wei, Chu, Yue, Zhang, Jun, Xue, Haoyu, Jia, Yiran, Cao, Tengfei, Qiu, Dong, Zou, Xiaolong, Wang, Da-Wei, Tao, Ying, Zhong, Guiming, Peng, Zhangquan, Kang, Feiyu, Lv, Wei, Yang, Quan-Hong
Format: Journal Article
Language:English
Published: London Nature Publishing Group UK 16.04.2025
Nature Publishing Group
Nature Portfolio
Subjects:
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639/301/299/891
639/4077/4079/891
639/638/161/891
639/638/675
Carbon
Carbon dioxide
Defects
Design optimization
Electrochemical analysis
Electrodes
Humanities and Social Sciences
Ion pairs
Ion storage
Low temperature
Molecular sieves
Mouth
multidisciplinary
Pores
Probes
Science
Science (multidisciplinary)
Shells
Sodium
Sodium-ion batteries
Solid electrolytes
Solvation
Solvents
ISSN:2041-1723, 2041-1723
Online Access:Get full text
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Summary: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 2 but accessible to CO 2 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 2 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. Closed pores govern sodium-ion storage performance of hard carbon negative electrodes. Here, authors link pore mouth size evolution of the closed pores to the solvation structure and propose design principles for optimizing both closed pores and intrinsic defects.
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ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-025-59022-8