硼掺杂碳电极材料微孔内锂离子去溶剂化的第一性原理计算

doi:10.11896/cldb.25120140

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Abstract Electrochemical double-layer capacitors (EDLCs) have garnered extensive attention owing to their distinct advantages, including eco-friendliness and rapid charging kinetics, rendering them pivotal in energy storage applications. Recent studies demonstrate that ion desolvation within the internal micropores of electrode materials significantly enhances capacitance, while heteroatom doping effectively improves capacitive performance. Consequently, first-principles calculations based on density functional theory (DFT) were employed to construct boron-doped bila-yer graphene models, simulating the desolvation behavior of hydrated lithium ions confined within micropores. Structural optimization and stability analysis were performed for hydrated lithium ions (Li(H₂O)_n, n=1, 2, 3, 4) adsorbed on boron-doped monolayer graphene (MGB) and intercalated into boron-doped bilayer graphene models (BGB-x, where x denotes the interlayer spacing in Å, x=4, 5, 6, 7, 8). These computations aim to elucidate the synergistic mechanisms by which ion desolvation and boron doping enhance capacitance. Results indicate that the speciation of Li(H₂O)_n within the BGB-x interlayer is highly dependent on the interlayer spacing. Both Li and H atoms interact with the π-conjugated system of the MGB surface (Li-π and OH-π interactions). Altering the interlayer spacing disrupts this interaction equilibrium, triggering the gradual desolvation of Li(H₂O)_n. Comparative analysis reveals that the relative capacitance of Li(H₂O)₁ intercalated into BGB-x is approximately two-fold higher than that of the MGB@Li(H₂O)₄ structure. Furthermore, a decreasing trend in relative capacitance is observed with an increasing hydration number, confirming that the desolvation of Li(H₂O)_n within the micropores of boron-doped carbon electrodes significantly enhances the specific capacitance of EDLCs. This systematic investigation provides critical theoretical insights into the capacitance enhancement mechanisms of boron-doped carbon materials and offers guidance for the rational design and controllable fabrication of electrode pore structures.

Key words： boron-doped carbon material pore structure bilayer graphene desolvation first-principles calculation

Published: 10 July 2026 Online: 2026-07-24

CLC number:

TB321

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	Articles by authors
	ZHANG Xu
	LIU Kun
	SONG Yanzhao
	TANG Jupeng
	LU Xuge
	ZHANG Fengzhi
	CHEN Ran
	LIANG Qi
	XU Xu
	YANG Shaobin

Cite this article:

ZHANG Xu,LIU Kun,SONG Yanzhao, et al. First-principles Calculation of Lithium Ion Desolvation in Micropores of Boron-doped Carbon Electrode Materials[J]. Materials Reports, 2026, 40(13): 25120140-12.

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https://www.mater-rep.com/EN/10.11896/cldb.25120140 OR https://www.mater-rep.com/EN/Y2026/V40/I13/25120140

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