SnS2/ZIF-8衍生二维多孔氮掺杂碳纳米片复合材料的锂硫电池性能研究

doi:10.15541/jim20220741

无机材料学报 ›› 2023, Vol. 38 ›› Issue (8): 938-946.DOI: 10.15541/jim20220741 CSTR: 32189.14.10.15541/jim20220741

所属专题：【能源环境】超级电容器,锂金属电池,钠离子电池和水系电池(202409)；【信息功能】MAX层状材料、MXene及其他二维材料(202409)

SnS₂/ZIF-8衍生二维多孔氮掺杂碳纳米片复合材料的锂硫电池性能研究

王新玲¹(), 周娜¹, 田亚文¹, 周明冉¹, 韩静茹¹, 申远升¹, 胡执一¹^,², 李昱¹^,²()

1.武汉理工大学材料复合新技术国家重点实验室, 武汉 430070
2.武汉理工大学纳微结构研究中心, 武汉 430070

收稿日期:2022-12-07 修回日期:2023-03-27 出版日期:2023-04-11 网络出版日期:2023-04-11
通讯作者: 李昱, 教授. E-mail: yu.li@whut.edu.cn
作者简介:王新玲(1997-), 女, 硕士研究生. E-mail: wangxinling_whut@163.com
基金资助:
国家自然科学基金(U22B6011);国家自然科学基金(22275142);国家自然科学基金(52103285);111引智计划(B20002);湖北省自然科学基金(2020CFB416)

SnS₂/ZIF-8 Derived Two-dimensional Porous Nitrogen-doped Carbon Nanosheets for Lithium-sulfur Batteries

WANG Xinling¹(), ZHOU Na¹, TIAN Yawen¹, ZHOU Mingran¹, HAN Jingru¹, SHEN Yuansheng¹, HU Zhiyi¹^,², LI Yu¹^,²()

1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
2. Nanostructure Research Centre (NRC), Wuhan University of Technology, Wuhan 430070, China

Received:2022-12-07 Revised:2023-03-27 Published:2023-04-11 Online:2023-04-11
Contact: LI Yu, professor. E-mail: yu.li@whut.edu.cn
About author:WANG Xinling (1997-), female, Master candidate. E-mail: wangxinling_whut@163.com
Supported by:
National Natural Science Foundation of China(U22B6011);National Natural Science Foundation of China(22275142);National Natural Science Foundation of China(52103285);The 111 National Project(B20002);Natural Science Foundation of Hubei Province(2020CFB416)

摘要/Abstract

摘要：

锂硫电池(LSBs)因能量密度高、原料储量丰富、环境友好等优点引起了广泛关注。然而, 多硫化物的穿梭效应、反应过程中较大的体积膨胀以及硫较差的电子电导率等缺点极大地限制了其发展。本研究设计了一种SnS₂纳米颗粒与ZIF-8衍生的花状二维多孔碳纳米片/硫复合材料(ZCN-SnS₂-S), 并研究了其作为锂硫电池正极的电化学性能。其独特的二维花状多孔结构不仅有效缓解了反应过程中的体积膨胀, 而且为Li⁺和电子的传输提供了快速通道, 杂原子N也促进了对多硫化物的吸附作用。并且负载的极性SnS₂纳米颗粒极大地增强了对多硫化物的吸附, 从而使ZCN-SnS₂-S复合材料表现出优异的电化学性能。在0.2C(1C=1675 mA·g^-1)电流密度下, ZCN-SnS₂-S电极循环100次后仍能保持948 mAh·g^-1的高可逆比容量, 容量保持率为83.7%。即使在2C的高电流密度下循环300圈, ZCN-SnS₂-S电极仍具有546 mAh·g^-1的可逆比容量。

关键词: 锂硫电池, 二维多孔氮掺杂碳纳米片, SnS₂, 多硫化物, 穿梭效应

Abstract:

Lithium-sulfur batteries (LSBs) have attracted wide attention due to their high energy density, abundant raw material reserves and environmental friendliness. However, the shuttle effect of polysulfides, the large volume expansion during the reaction, and the poor electron conductivity of sulfur greatly limit their practical development. In this work, a ZIF-8 derived flower-like two-dimensional (2D) porous carbon nanosheet/sulfur composite (ZCN-SnS₂-S) combined with SnS₂ nanoparticles is designed as the cathode for LSBs. The unique 2D flower-shaped porous structure not only effectively alleviates the volume expansion during the reaction process, but also provides a fast channel for Li⁺ and electron transport. The presence of heteroatom N further promotes the adsorption of polysulfide. In particular, the polar SnS₂ enhances the chemical adsorption on polysulfides, resulting in excellent electrochemical performance. The ZCN-SnS₂-S electrode exhibits high reversible specific capacity of 948 mAh·g^-1 after 100 cycles at 0.2C (1C=1675 mA·g^-1), demonstrating the capacity retention rate of 83.7%. Even at a high current density of 2C for 300 cycles, it still has a reversible specific capacity of 546 mAh·g^-1.

Key words: lithium-sulfur battery, 2D porous nitrogen-doped carbon nanosheet, SnS₂, polysulfide, shuttle effect

中图分类号:

TQ174

王新玲, 周娜, 田亚文, 周明冉, 韩静茹, 申远升, 胡执一, 李昱. SnS₂/ZIF-8衍生二维多孔氮掺杂碳纳米片复合材料的锂硫电池性能研究[J]. 无机材料学报, 2023, 38(8): 938-946.

WANG Xinling, ZHOU Na, TIAN Yawen, ZHOU Mingran, HAN Jingru, SHEN Yuansheng, HU Zhiyi, LI Yu. SnS₂/ZIF-8 Derived Two-dimensional Porous Nitrogen-doped Carbon Nanosheets for Lithium-sulfur Batteries[J]. Journal of Inorganic Materials, 2023, 38(8): 938-946.

图/表 15

图1 (a)ZCN-SnS2复合材料合成示意图; (b, e)ZIF-8、(c, f)ZCN和(d, g)ZCN-SnS2的FESEM照片

Fig. 1 (a) Schematics of synthetic process of ZCN-SnS2, and FESEM images of (b, e) ZIF-8, (c, f) ZCN and (d, g) ZCN-SnS2 Colorful figures are available on website

图2 ZCN样品的(a)氮气吸/脱附等温线与(b)介孔孔径分布图(插图为微孔孔径分布图); (c)ZCN-SnS2、ZCN和SnS2样品的XRD图谱; (d)ZCN样品的拉曼光谱图

Fig. 2 (a) N2 adsorption-desorption isotherm of ZCN; (b) mesoporous pore size distribution curve of ZCN with inset showing micropore pore size distribution; (c) XRD patterns of ZCN-SnS2, ZCN and SnS2; (d) Raman spectrum of ZCN

图3 ZCN-SnS2样品的(a)HRTEM, (b)SAED, (c)HAADF-STEM照片和(d~g)EDX元素分布图

Fig. 3 (a) HRTEM, (b) SAED, (c) HAADF-STEM images, and (d-g) corresponding EDX elemental mappings of ZCN-SnS2

图4 ZCN-SnS2的高分辨(a)C1s, (b)N1s, (c)Sn3d, (d)S2p XPS光谱图; SnS2的高分辨(e)Sn3d, (f)S2p XPS光谱图

Fig. 4 (a) C1s, (b) N1s, (c) Sn3d, (d) S2p XPS spectra of ZCN-SnS2, and (e) Sn3d, (f) S2p XPS spectra of SnS2

图5 (a)以ZCN-SnS2-S为电极的锂硫电池的CV曲线; 以ZCN-SnS2-S、ZCN-S、SnS2-S为电极的锂硫电池的(b)充放电曲线, (c)倍率性能和(d)0.2C下的循环性能; (e)ZCN-SnS2-S电极在2C下的循环性能

Fig. 5 (a) CV curves of Li-S battery with ZCN-SnS2-S electrode; (b) Charge-discharge curves, (c) rate performances and (d) cycling performances at 0.2C of Li-S batteries with ZCN-SnS2-S, ZCN-S and SnS2-S electrodes; (e) Cycling performance of ZCN-SnS2-S at 2C

图6 ZCN-SnS2-S、ZCN-S和SnS2-S电极的(a)阻抗谱图与(b)在较低的角频率下, 阻抗的实部和倒数指数(-1/2)之间的线性关系图; ZCN-SnS2、ZCN和SnS2样品的(c)Li2S6吸附实验照片与(d)UV-Vis吸收光谱图

Fig. 6 (a) EIS plots and (b) linear relationships between the real parts of the impedance and the reciprocal exponentials (-1/2) at the lower angular frequency of ZCN-SnS2-S, ZCN-S and SnS2-S, respectively; (c) Li2S6 adsorption plots and (d) UV-Vis absorption spectra of ZCN-SnS2, ZCN and SnS2

图S1 ZCN-SnS2样品的TGA曲线

Fig. S1 TGA curve of ZCN-SnS2

图S2 (a, b)ZCN-SnS2和(c, d)SnS2样品的FESEM照片

Fig. S2 FESEM images of (a, b) ZCN-SnS2 and (c, d) SnS2

图S3 ZCN-SnS2和SnS2样品的拉曼光谱图

Fig. S3 Raman spectra of ZCN-SnS2 and SnS2

图S4 SnS2的(a)HAADF-STEM和(b)HRTEM照片

Fig. S4 (a) HAADF-STEM and (b) HRTEM images of SnS2

图S5 (a)ZCN-SnS2-S、ZCN-S、SnS2-S样品的XRD图谱, (b)ZCN-SnS2-S样品的氮气吸/脱附等温线, (c)ZCN-SnS2-S、ZCN-S、SnS2-S样品的TGA曲线, (d)SnS2样品在1C下的循环性能。

Fig. S5 (a) XRD patterns of ZCN-SnS2-S, ZCN-S, SnS2-S, (b) nitrogen adsorption-desorption isotherm of ZCN-SnS2-S, (c) TGA curves of ZCN-SnS2-S, ZCN-S and SnS2-S, and (d) cycling performance of SnS2 at 1C

图S6 ZCN-SnS2-S样品在0.2C下的循环性能。

Fig. S6 Cycling performance of ZCN-SnS2-S at 0.2C

图S7 0.5C电流密度下循环150圈前后电极材料的FESEM照片

Fig. S7 FESEM images of electrode materials before and after 150 cycles at 0.5C current density (a, d) ZCN-SnS2-S; (b, e) ZCN-S; (c, f) SnS2-S

图S8 ZCN和SnS2混合样品的Li2S6吸附实验照片

Fig. S8 Li2S6 adsorption pictures of ZCN and SnS2 mixed samples

表S1 基于SnS2复合材料的电化学性能比较

Table S1 Comparison of electrochemical properties of SnS2 composites

Host materials	Current rate	Cycle number	Reversible capacity/(mAh·g^-1)	Ref.
ZCN-SnS₂-S	0.2C	100	948	This work
ZCN-SnS₂-S	2.0C	300	546	This work
SnS₂/CNTs/S	0.1C	100	1002.3	[1]
NG/SnS₂/TiO₂-S	0.2C	100	739	[2]
SnS₂@N-CNFs	0.2C	150	889	[3]
NHCS-SnS₂/S	1.0C	200	634	[4]
PCN-SnS₂-S	2.0C	150	650	[5]

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SnS₂/ZIF-8衍生二维多孔氮掺杂碳纳米片复合材料的锂硫电池性能研究

SnS₂/ZIF-8 Derived Two-dimensional Porous Nitrogen-doped Carbon Nanosheets for Lithium-sulfur Batteries

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