论文总字数：25379字

摘 要

随着时代进步，高性能储能设备的研究愈发成为热点，传统锂离子电池已经因为其缺陷，限制了其商业化的进程。于是本论文也基于综合硫和硒的电化学性能优势的研究方向来研究锂硫化硒电池。本论文针对锂硫化硒电池的正极材料进行改性处理，以CoP-C-N@CC作为正极宿主材料负载SeS₂制备电池正极。

本论文针对传统锂硫化硒电池进行正极材料的改性处理。实验首先通过水热法，得到亲水性、高导电性碳布（CC），作为ZIF-67（Co-MOFs）生长基底。然后以硝酸钴和二甲基咪唑合成具有自支撑柔性氮掺杂钴阵列，经碳化处理的到Co-C-N@CC；然后与亚磷酸钠在管式炉中加热处理得到CoP-C-N@CC。然后负载硫化硒得到SeS₂@CoP-C-N@CC作为正极材料。通过了XRD衍射物相分析，SEM形貌分析，XPS能谱分析，电化学循环性能、充放电曲线、能量效率、倍率性能等测试。

实验结果表明，成功制备正极材料SeS₂@CoP-C-N@CC之后经过测试，提高了对于活性物质的吸附能力，提升了锂硫电池的循环性能，减弱了穿梭效应。

关键词：锂硫电池；锂硫化硒电池；MOF；金属磷化物；正极材料；穿梭效应

CoP composite electrode for high performance Li-SeS₂ battery

Abstract

With the advancement of the times, the research of high-performance energy storage equipment has become a hot spot. Traditional lithium-ion batteries have limited the commercialization process because of their defects. Therefore, this paper also studies lithium selenide batteries based on the research direction of the advantages of electrochemical properties of sulfur and selenium. In this thesis, the positive electrode material of lithium selenide battery was modified, and the positive electrode was prepared by loading SeS2 with CoP-C-N@CC as the positive host material.

This paper is aimed at the modification of cathode materials for traditional lithium selenide batteries. First, a hydrothermal method was used to obtain a hydrophilic, highly conductive carbon cloth (CC) as a ZIF-67 (Co-MOFs) growth substrate. Then, a self-supporting flexible nitrogen-doped cobalt array was synthesized with cobalt nitrate and dimethylimidazole, and carbonized to Co-C-N@CC; and then heat treated with sodium phosphite in a tube furnace to obtain CoP-C-N@CC. Selenium sulfide was then loaded to obtain SeS₂@CoP-C-N@CC as a positive electrode material. Through XRD diffraction phase analysis, SEM morphology analysis, XPS energy spectrum analysis, electrochemical cycle performance, charge and discharge curve, energy efficiency, rate performance and other tests.

The experimental results show that after the successful preparation of the positive electrode material SeS₂@CoP-C-N@CC, the adsorption capacity of the active material is improved, the cycle performance of the lithium-sulfur battery is improved, and the shuttle effect is weakened.

Key words: Lithium-sulfur battery; lithium selenide battery; MOF; cathode material;shuttle effect

目 录

摘 要 I

Abstract II

第一章 绪论 1

1.1 前言 1

1.2 锂硫电池概述 2

1.2.1 硫的存在形态、物理化学性质 2

1.2.2 锂硫电池的工作原理 2

1.2.3 锂硫电池的主要瓶颈 3

1.3 锂硒电池概述 4

1.3.1 锂硒电池的主要问题 5

1.4 锂硫化硒（Li-SeS₂）电池 5

1.4.1 Li-SeS₂ 电池正极的改性策略 6

1.5 金属磷化物 8

1.6 金属有机框架（MOFs） 9

1.7 本论文研究目的及内容 10

第二章 实验部分 11

2.1 实验药品 11

2.2 实验仪器 12

2.2 实验流程 12

2.2.1 亲水碳布（CFC）的制备 12

2.2.2 合成自支撑柔性氮掺杂钴阵列（Co-C-N@CC） 12

2.2.3 制备自支撑柔性氮掺杂磷化钴阵列（CoP-C-N@CC） 13

2.2.4 制备正极材料 SeS2@CoP-C-N@CC 13

2.3 实验表征方法 13

2.3.1 扫描电子显微镜形貌分析 13

2.3.2 X 射线衍射物相分析 13

2.3.3 X 射线光电子能谱 14

第三章 性能表征 15

3.1 结构形貌分析 15

3.2 物相的分析 15

3.3 化学组成分析 16

3.4 电化学性能分析 16

3.4.1 循环性能 16

3.4.2 倍率性能 17

第四章 结论与展望 19

4.1 结论 19

4.2实验展望 19

参考文献 20

致谢 25

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