PEO基Li+-g-C3N4 复合固态电解质的制备及其电化学性能

doi:10.19799/j.cnki.2095-4239.2022.0345

储能科学与技术 ›› 2022, Vol. 11 ›› Issue (11): 3463-3469.doi: 10.19799/j.cnki.2095-4239.2022.0345

PEO基Li⁺-g-C₃N₄ 复合固态电解质的制备及其电化学性能

张林森¹^,²^,³(), 王士奇¹, 王利霞¹^,²^,³, 宋延华¹^,²^,³

^1.郑州轻工业大学材料与化学工程学院
^2.郑州轻工业大学陶瓷材料研究中心
^3.河南省陶瓷基;新能源材料国际联合实验室，河南郑州 450001

收稿日期:2022-06-22 修回日期:2022-07-19 出版日期:2022-11-05 发布日期:2022-11-09
通讯作者: 张林森 E-mail:hnzhanglinsen@163.com
作者简介:张林森（1979—），男，博士，教授，从事固态电解质的研究，E-mail： hnzhanglinsen@163.com。
基金资助:
国家自然科学基金面上项目(82172564);河南省科技攻关项目(222102240041)

Synthesis and performances of Li⁺ modified g-C₃N₄ for PEO-based composite solid electrolyte

Linsen ZHANG¹^,²^,³(), Shiqi WANG¹, Lixia WANG¹^,²^,³, Yanhua SONG¹^,²^,³

^1.School of Material and Chemical Engineering, Zhengzhou University of Light Industry
^2.Ceramic Materials Research Center, Zhengzhou University of Light Industry
^3.Henan International Joint Laboratory of Ceramic Energy Materials, Zhengzhou 450001, Henan, China

Received:2022-06-22 Revised:2022-07-19 Online:2022-11-05 Published:2022-11-09
Contact: Linsen ZHANG E-mail:hnzhanglinsen@163.com

摘要/Abstract

摘要：

利用g-C₃N₄表面丰富的官能团进行锂化，得到锂化氮化碳(L-g-C₃N₄)材料，并以双三氟甲基磺酰亚胺锂(LiTFSI)为锂盐，聚环氧乙烯(PEO)为聚合物基体，采用流延-热压法制备Li⁺-g-C₃N₄复合固态电解质。借助透射电子显微镜(TEM)、X射线衍射仪(XRD)、红外光谱仪(FT-IR)、差示扫描量热法(DSC)、线性循环伏安(LSV)、直流极化曲线、交流阻抗谱以及充放电测试等手段对复合固态电解质进行表征和测试。对比分析相同质量分数g-C₃N₄复合固态电解质与L-g-C₃N₄复合固态电解质的电化学性能，同时对不同L-g-C₃N₄含量的复合固态电解质的电化学性能进行研究。结果表明，添加质量分数为10% L-g-C₃N₄的复合固态电解质在60 ℃时的离子电导率为3.95×10^-4 S/cm，锂离子迁移数为0.639，电化学窗口为4.5 V以上。以复合固态电解质组装Li/LiFePO₄全固态电池，在60 ℃以0.5 C充放电，电池的首次放电比容量为163.76 mAh/g，循环80次后容量仍有160.10 mAh/g，容量保持率为97.8 %。

关键词: 锂离子电池, PEO基固态电解质, 离子电导率, 氮化碳

Abstract:

The rich functional groups on the surface of g-C₃N₄ were used for lithiation to acquire lithiated g-C₃N₄ (L-g-C₃N₄). Bistrifluoromethane sulfonimide lithium salt as the lithium salt and polyvinyl epoxide as the polymer matrix was used to prepare L-g-C₃N₄ composite solid electrolytes using the casting-hot-pressing method. Transmission electron microscopy, X-ray diffractometer, infrared spectrometer, differential scanning calorimetry, linear cyclic voltammetry, DC polarization curve, electrochemical impedance spectroscopy and charge-discharge tests were used to characterize and test the composite solid electrolytes. g-C₃N₄ composite solid electrolyte and L-g-C₃N₄ composite solid electrolyte were compared and their electrochemical properties were evaluated. Simultaneously, composite solid electrolytes with different L-g-C₃N₄ content levels were also studied. The results revealed that the composite solid electrolyte's ionic conductivity is 3.95 × 10^-4 S/cm, the Li⁺ migration number is 0.639, and the electrochemical window is higher than 4.5 V. The Li/LiFePO₄ all-solid-state batteries were gathered with composite solid electrolytes. The battery's initial specific discharge capacity was 163.76 mAh/g for the first discharge when charged-discharged with 0.5 C in 2.5-4.0 V at 60 ℃. After 80 cycles, the capacity was still 160.10 mAh/g, and the capacity retention rate was 97.8%.

Key words: Li-ion batteries, PEO-based solid electrolyte, ionic conductivity, carbon nitride (g-C₃N₄)

中图分类号:

TM 912.9

张林森, 王士奇, 王利霞, 宋延华. PEO基Li⁺-g-C₃N₄ 复合固态电解质的制备及其电化学性能[J]. 储能科学与技术, 2022, 11(11): 3463-3469.

Linsen ZHANG, Shiqi WANG, Lixia WANG, Yanhua SONG. Synthesis and performances of Li⁺ modified g-C₃N₄ for PEO-based composite solid electrolyte[J]. Energy Storage Science and Technology, 2022, 11(11): 3463-3469.

图/表 11

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材料	C_g	CPE-T	CPE-P	R_b	离子电导率/(S/cm)
PEO-LiTFSI	3.330×10^-18	2.767×10^-6	0.80952	702.1	5.14×10^-6
5%-g-C₃N₄	1.835×10^-17	5.273×10^-6	0.89533	23.35	9.81×10^-5
5%-L-g-C₃N₄	6.810×10^-18	1.092×10^-5	0.85373	14.2	2.17×10^-4
10%-L-g-C₃N₄	3.571×10^-16	2.423×10^-5	0.83146	6.3	3.95×10^-4
15%-L-g-C₃N₄	2.174×10^-16	1.341×10^-5	0.85308	16.87	2.16×10^-4

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PEO基Li⁺-g-C₃N₄ 复合固态电解质的制备及其电化学性能

Synthesis and performances of Li⁺ modified g-C₃N₄ for PEO-based composite solid electrolyte

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