Synthesis and Performance of a Novel Quasi-solid-state Electrolyte PHCN Based on Polyvinylidene Fluoride-hydrogenated Acrylate Incorparated with Mesoporous Spherical g-C3N4

doi:10.11901/1005.3093.2025.092

Chinese Journal of Materials Research

2025, Vol. 39

Issue (12): 935-944 DOI: 10.11901/1005.3093.2025.092

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Synthesis and Performance of a Novel Quasi-solid-state Electrolyte PHCN Based on Polyvinylidene Fluoride-hydrogenated Acrylate Incorparated with Mesoporous Spherical g-C₃N₄

LIANG Honghua¹, CHEN Jiangchao¹, ZHENG Wenyu¹, WU Haining¹, HUANG Yicong¹, YI Zhuoyan¹, PANG Dazhi¹, JIANG Kunpeng¹, ZHU Guisheng¹(

), XU Huarui¹^,²

^1.Engineering Research Center of Electronic Information Materials and Devices, Guangxi Key Laboratory of Information Materials, School of Materials Science and Engineering, Guilin University of Electronic Technology, Guilin 541004, China
^2.College of Petroleum and Chemical Engineering, Beibu Gulf University, Qinzhou 535011, China

Cite this article:

LIANG Honghua, CHEN Jiangchao, ZHENG Wenyu, WU Haining, HUANG Yicong, YI Zhuoyan, PANG Dazhi, JIANG Kunpeng, ZHU Guisheng, XU Huarui. Synthesis and Performance of a Novel Quasi-solid-state Electrolyte PHCN Based on Polyvinylidene Fluoride-hydrogenated Acrylate Incorparated with Mesoporous Spherical g-C₃N₄. Chinese Journal of Materials Research, 2025, 39(12): 935-944.

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Abstract

Quasi-solid-state electrolytes have garnered significant attention in lithium-ion battery research due to their potential to overcome the safety risks of liquid electrolytes and the low room-temperature ionic conductivity of solid-state electrolytes. In this work, a novel series of quasi-solid-state electrolytes named PHCN (namely PHCN-1, PHCN-2, PHCN-3, and PHCN-4) was fabricated by incorporating mesoporous spherical g-C₃N₄ into a poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix. The resulting PHCN electrolytes feature unique stationary and "instantaneous" structures, which contribute to enhanced ionic conductivity and reduced polymer crystallinity. The optimized sample, PHCN-3 (with 3% g-C₃N₄), exhibits outstanding performance: an ionic conductivity of 2.62 × 10^-3 S·cm^-1 at 30 ^oC, a Li⁺ transference number of 0.71, and a widened electrochemical stability window of approximately 4.6 V. A lithium symmetric cell employing the PHCN-3 electrolyte demonstrated exceptional cycling stability for over 2000 h at a current density of 0.2 mA·cm^-2. Furthermore, a LiFePO₄/PHCN-3-LiPF₆/Li cell maintained a high capacity retention of 88.33% after 200 cycles at a 0.5C rate. These findings indicate that the PHCN quasi-solid-state electrolytes present a promising path for the development of high-performance and safe lithium-ion batteries.

Key words: inorganic non-metallic materials quasi-solid electrolyte lithium-ion battery mesoporous spherical g-C₃N₄ “brushed” structure “stationary” structure

Received: 27 February 2025

ZTFLH:

TB332

Fund: Guilin Scientific Research and Technology Development Programme(20220120-1);Science and Technology Base and Talent Special Project of Guangxi Province(AD23023013)

Corresponding Authors: ZHU Guisheng, Tel: 13507730539, E-mail: zhuguisheng@guet.edu.cn

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	Articles by authors
	LIANG Honghua
	CHEN Jiangchao
	ZHENG Wenyu
	WU Haining
	HUANG Yicong
	YI Zhuoyan
	PANG Dazhi
	JIANG Kunpeng
	ZHU Guisheng
	XU Huarui

URL:

https://www.cjmr.org/EN/10.11901/1005.3093.2025.092 OR https://www.cjmr.org/EN/Y2025/V39/I12/935

Fig.1 Schematic diagram of the fabrication process for PHCN QSE

Fig.2 SEM images (a) and EDS spectrum (b) of mesoporous spherical g-C₃N₄, SEM image of multi-channel PVDF-HFP (c), SEM images of PHCN-3 (d) showing the fibrillated structure (e) and cross-sectional view (f)

Fig.3 N₂ adsorption-desorption isotherm (a) and pore size distribution (b) of mesoporous spherical g-C₃N₄, XRD pattern of mesoporous spherical g-C₃N₄ (c), XRD patterns (d), FTIR spectra (e), stress-strain curves (f), liquid electrolyte uptake (g), TG analysis (h), and DSC analysis (i) of PHCN-X and PVDF-HFP

Fig.4 Nyquist plots at 30 ^oC (a), Arrhenius plots (b), activation energy plots (c), chromoamperometry curve and corresponding Nyquist plots before and after polarization for PHCN-3 at 30 ^oC (d), LSV curves of PHCN-3 and PVDF-HFP quasi-solid electrolytes at 30 ^oC with a scan rate of 10 mV·s^-1 (e)

Fig.5 Galvanostatic cycling profiles of Li symmetric cells assembled with PVDF-HFP and PHCN-3 (a), and critical current density (CCD) curve for PHCN-3 (b)

Fig.6 Rate performance (a) and initial charge-discharge curves at various C-rates (b) for the LiFePO₄/PHCN-3-LiPF₆/Li cell, Cycling stability of PHCN-3 and PVDF-HFP at 0.5C and 30 ^oC (c)

Fig.7 Surface morphologies of the lithium metal anode after 500 cycles in the LiFePO₄/PHCN-3-LiPF₆/Li cell

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