锂/钠离子电池硬碳负极材料的研究进展

doi:10.15541/jim20230365

无机材料学报 ›› 2024, Vol. 39 ›› Issue (1): 32-44.DOI: 10.15541/jim20230365

锂/钠离子电池硬碳负极材料的研究进展

胡梦菲¹^,²(), 黄丽萍¹, 李贺², 张国军¹(), 吴厚政²()

1.东华大学材料科学与工程学院, 功能材料研究中心纤维材料改性国家重点实验室, 上海 201620
2.赛迈科先进材料股份有限公司, 湖州 313100

收稿日期:2023-08-10 修回日期:2023-11-02 出版日期:2024-01-20 网络出版日期:2023-11-10
通讯作者: 张国军, 教授. E-mail: gjzhang@dhu.edu.cn;
吴厚政, 博士. E-mail: wuhz@sinosteelamc.com
作者简介:胡梦菲(1993-), 女, 博士. E-mail: mfhu1993@163.com
基金资助:
浙江省领军型创新创业团队(2022R01017)

Research Progress on Hard Carbon Anode for Li/Na-ion Batteries

HU Mengfei¹^,²(), HUANG Liping¹, LI He², ZHANG Guojun¹(), WU Houzheng²()

1. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Institute of Functional Material, College of Material Science and Engineering, Donghua University, Shanghai 201620, China
2. SIAMC Advanced Materials Corporation, Huzhou 313100, China

Received:2023-08-10 Revised:2023-11-02 Published:2024-01-20 Online:2023-11-10
Contact: ZHANG Guojun, professor. E-mail: gjzhang@dhu.edu.cn;
WU Houzheng, PhD. E-mail: wuhz@sinosteelamc.com
About author:About author:HU Mengfei (1993-), female, PhD. E-mail: mfhu1993@163.com
Supported by:
Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2022R01017)

摘要/Abstract

摘要：

随着锂离子电池的发展和钠离子电池的兴起, 硬碳材料作为一种新型负极材料, 受到了广泛关注。硬碳来源丰富, 价格便宜, 具有比锂离子电池石墨负极更高的储锂容量和优异的倍率性能, 并且是最有商业化潜质的钠离子电池负极材料。然而, 硬碳普遍存在电池首周库仑效率低的问题, 且对于硬碳的储锂/钠机制仍存在争论, 其比容量仍有较大的提升空间。近年来, 研究人员围绕硬碳负极材料的电化学机理展开了各种研究和模型假设, 针对硬碳负极存在的问题, 提出了各种解决策略。本文介绍了硬碳的基本结构和常用的制备方法, 并结合硬碳的优势, 梳理了硬碳在锂离子电池和钠离子电池中的应用情况, 重点介绍了其在快充、包覆等细分领域的应用进展, 并分别针对硬碳提升比容量和改善首周库仑效率的需求, 归纳了孔结构设计、元素掺杂、优化材料与电解液界面等不同改性策略。

关键词: 负极材料, 锂离子电池, 钠离子电池, 硬碳, 综述

Abstract:

With rapid development of lithium ion batteries (LIB) and sodium ion batteries (SIB), hard carbon (HC) as new anode material has earned much attention. Besides its rich precursor sources and low cost, HC has higher Li⁺ storage capacity and better rate performance than graphite for LIB. Furthermore, it is also recognized as the most commercially potential anode material for SIB. However, low initial Coulombic efficiency is a common issue for HC. In addition, it is believed that the specific capacity can be further improved with the clarification of the Li/Na ion storage mechanism. In recent years, many researches on electrochemical mechanism have been conducted with some model assumptions proposed for better understanding the mechanism. This review introduced the structures and preparation approaches of HC as well as its application in LIB and SIB. The advantages, especially in fast charging, coating and other subdivision were discussed, and the different modification strategies such as pore structure design, doping, optimizing interface between electrode and electrolyte were summarized, aiming at the increase of capacity and the improvement of Coulombic efficiency of batteries.

Key words: anode material, lithium ion battery, sodium ion battery, hard carbon, review

中图分类号:

TQ152

胡梦菲, 黄丽萍, 李贺, 张国军, 吴厚政. 锂/钠离子电池硬碳负极材料的研究进展[J]. 无机材料学报, 2024, 39(1): 32-44.

HU Mengfei, HUANG Liping, LI He, ZHANG Guojun, WU Houzheng. Research Progress on Hard Carbon Anode for Li/Na-ion Batteries[J]. Journal of Inorganic Materials, 2024, 39(1): 32-44.

图/表 9

图1 锂/钠离子电池硬碳负极材料的应用与改性策略概览

Fig. 1 Over-view on the application and modification strategies of hard carbon in Li/Na ion batteries

图2 硬碳、软碳和石墨的形成机制[3]

Fig. 2 Formation scheme of hard carbon, soft carbon and graphite[3]

图3 生物质碳源及其性能

Fig. 3 Biomass carbon precursors and their properties (a) General biomass carbon precursors; (b) Rate performance and Coulombic efficiency of carbon from coffee waste in LIB[16]; (c) Schematic of synthesis and proposed mechanism of pitch/lignin-derived carbon[22]

图4 (a) 硬碳储锂/钠离子的三种方式[28]及(b) 硬碳储钠的四种模型[39]

Fig. 4 (a) Three different mechanisms of lithium/sodium ion storage in hard carbon[28], and (b) four different models of sodium storage in hard carbon[39]

图5 硬碳在快充领域的应用

Fig. 5 Hard carbon in fast-charging application (a) Schematic of ion diffusion pathways in carbon fiber (CF); (b) Lithium-ion diffusion coefficient of CF and carbon sphere (CS) measured by potentiostatic intermittent titration technique (PITT); (c) Cycling performance of Li||CF and Li||graphite cells[45]; (d) Z'-ω0.5 plots in low-frequency region calculated from electrochemical impedance spectroscopy (EIS) measurement; (e) DLi and electrical conductivity plots of CNFs[47] in which the mass ratio of polyacrylonitrile to pitch can be tuned as 10/0, 9/1, 7/3, and 5/5 for PAN-800, PCTP9-1, PCTP7-3, PCTP5-5, respectively; (f) Rate performance of N-GCNs in LIBs from 0.1 to 20 A·g-1 (CE: Coulombic efficiency)[49]

图6 硬碳用作负极材料包覆层

Fig. 6 Hard carbon as coating layer for anode (a) Multistep heating in different carbonization procedures; (b) Charge-discharge profiles of the sample with carbonization 2# in (a)[50]; (c) Illustration of resorcinol-formaldehyde resin (RF) coated nano Si[53]; (d) TEM image of Si-C-G-15 composite; (e) PITT results of Si-C-G-15 and capacity contributions of each component (AC: amorphous carbon; NG: natural graphite; SiNPs: silicon nano-particles)[54]

图7 元素掺杂策略和预氧化策略

Fig. 7 Doping and pre-oxidation strategies (a) Schematic illustration of fabrication process of S-NCNFs; (b) TEM image of S-NCNFs and corresponding S, N, and C elemental mappings[62]: (c) Capacity of hard carbon derived from pitch (HCP) with and without pre-oxidization[64]; (d) Specfic capacity and initial Coulombic efficiency of lignin spheres hard carbon (LSHC) with pre-oxidation at different temperatures[65]

图8 (a) (左)典型多孔碳和(右)分子筛型碳及界面双电层示意图, (b) 多孔碳和(c) 分子筛型碳的前两周充放电曲线[66]

Fig. 8 (a) Schematic showing the control of the nanopores in a typical porous carbon (left) to produce molecular sieve carbon (right), and comparison between their different IEDLs, charge/discharge curves for first two cycles of (b) porous carbon and (c) molecular seive carbon anodes[66]

图9 提高首周库仑效率的方案

Fig. 9 Strategies for improving initial Coulombic efficiency (a) Schematic of the influence of ALD-Al2O3 coating on hard carbon[67]; (b) Charge/discharge curves of P-doped C (PO/C) and C prepared at 800 ℃ without doping (C-800) at 0.1 A·g-1; (c) Illustration of different compositions of the SEI on the surface of PO/C electrode[68]; (d) Illustration of closed pore in hard carbon; (e) Galvanostatic initial discharge-charge profiles of HC-21-x (x: pyrolysis temperature)[70]; (f) Schematic illustration of Na storage mechanism in HC-GLC electrode[73]

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锂/钠离子电池硬碳负极材料的研究进展

Research Progress on Hard Carbon Anode for Li/Na-ion Batteries

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