钠离子电池硬碳负极储钠机理及优化策略

doi:10.6023/A21060284

化学学报 ›› 2021, Vol. 79 ›› Issue (12): 1461-1476.DOI: 10.6023/A21060284 上一篇下一篇

综述

钠离子电池硬碳负极储钠机理及优化策略

董瑞琪, 吴锋, 白莹^*(), 吴川^*()

北京理工大学材料学院环境科学与工程北京市重点实验室北京 100081

投稿日期:2021-06-22 发布日期:2021-08-19
通讯作者: 白莹, 吴川

作者简介:

董瑞琪, 2016年在河北工业大学获得工学学士学位, 目前为北京理工大学材料学院博士研究生, 师从吴锋院士, 主要研究方向为钠离子电池负极材料.

白莹, 北京理工大学材料学院教授. 研究兴趣包括锂/钠离子电池氧化物、聚阴离子型、硅基、碳基等电极材料、凝胶态与固态电解质, 以及电极与电解液界面稳定性、电池热分析与热安全等基本科学问题.

吴川, 北京理工大学材料学院教授. 长期从事先进能源材料的研究, 关注能量储存与转化体系及其关键材料, 包括锂离子电池、钠离子电池、铝二次电池、锂空电池、锌离子电池及其他二次电池新体系. 任Science合作期刊Energy Material Advances副主编.

基金资助:
国家自然科学基金(21975026)

Sodium Storage Mechanism and Optimization Strategies for Hard Carbon Anode of Sodium Ion Batteries

Ruiqi Dong, Feng Wu, Ying Bai(), Chuan Wu()

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

Received:2021-06-22 Published:2021-08-19
Contact: Ying Bai, Chuan Wu
Supported by:
National Natural Science Foundation of China(21975026)

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摘要/Abstract

钠离子电池因具有成本低、安全性高等优势, 被认为是一种非常适合应用于大规模储能领域的电化学储能技术. 合适的负极材料是促进钠离子电池实现商业化的关键之一. 硬碳材料由于具有丰富的碳源、低成本、无毒环保, 且储钠电位低而被认为是最可能被实用化的钠离子电池负极材料. 然而硬碳负极的实际应用中也面临着首周库伦效率低、长循环稳定性不足以及倍率性能较差等问题, 近年来众多研究者致力于硬碳负极的性能优化研究, 本Review从结构调控、形貌设计、界面构造、电解液优化四方面总结了近年来钠离子电池硬碳负极的性能优化策略研究进展, 分析了每种优化策略的优点和不足, 并进一步讨论了钠离子电池硬碳负极实用化进程中面临的瓶颈问题和挑战.

关键词: 钠离子电池, 负极, 硬碳, 性能优化, 实用化

Sodium ion batteries (SIBs) have been regarded as a very suitable electrochemical energy storage technology for large-scale energy storage due to its low cost and high safety. Suitable anode material is one of the keys to boosting the commercialization process of SIBs. Significantly, hard carbon (HC) anode is considered as the most practical anode material for SIBs due to its rich natural sources, low cost, non-toxic, environmentally friendly, and low sodium storage voltage. However, hard carbon anode also faces the problems of low initial Columbic efficiency, insufficient long cycle stability and poor rate performance, which restrict its practical application in SIBs. In recent years, extensive investigations have been done to improve the performance of hard carbon anode, herein, this review discusses the recent progress of performance optimization strategies of hard carbon anode from four aspects, including structure control, morphology design, interface manufacture, and electrolyte optimization and conducts an analysis of the merits and demerits of each optimization method. Moreover, this review also discusses the bottlenecks and challenges in the process of practical application of hard carbon anode for sodium ion batteries.

Key words: sodium ion battery, anode, hard carbon, performance optimization, practical application

引用此文

董瑞琪, 吴锋, 白莹, 吴川. 钠离子电池硬碳负极储钠机理及优化策略[J]. 化学学报, 2021, 79(12): 1461-1476.

Ruiqi Dong, Feng Wu, Ying Bai, Chuan Wu. Sodium Storage Mechanism and Optimization Strategies for Hard Carbon Anode of Sodium Ion Batteries[J]. Acta Chimica Sinica, 2021, 79(12): 1461-1476.

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图/表 12

图1. 钠离子在硬碳中储存机理示意图: (a)“插层-吸附”机制, (b) “吸附-插层”机制[56]. 已获得参考文献[56]的转载许可, 版权所有© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) 硬碳的微观结构随热解温度的变化的演变及对应的储钠机制和行为示意图[60]. 已获得参考文献[60]的转载许可, 版权所有© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) 多孔碳孔结构调整和闭孔储钠机制示意图[63]. 已获得参考文献[63]的转载许可, 版权所有© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) 不同的钠化阶段的硬碳电极的非原位WAXS曲线, (f) 硬碳储钠的“吸附—插层—孔充填”机理示意图, 灰色区域表示由于反应缓慢而未使用的容量[67]. 已获得参考文献[67]的转载许可, 版权所有© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (g)放电/充电到不同电压的硬碳电极与质子溶剂的化学反应, (h) 完全钠化的电极与乙醇反应后产生的H2的气相色谱图, (i) 硬碳中钠的稳态示意图: 在钠离子插入硬碳电极过程中伴随它们之间部分的电子转移形成准金属钠[68]. 已获得参考文献[68]的转载许可, 版权所有© 2021 Wiley-VCH GmbH

Figure 1. Schematic illustration of the mechanisms for Na-ion storage in hard carbon: (a) “intercalation-adsorption” mechanism, (b) “adsorption-intercalation” mechanism[56]. Reprinted with permission from ref. [56]. Copyright © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) Schematic illustration of the evolution of the microstructure, sodium storage mechanism and behavior with the pyrolysis temperature of HCs[60]. Reprinted with permission from ref. [60]. Copyright © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) Schematic illustration of tuning pore structure of porous carbon and sodium storage mechanism of closed pores[63]. Reprinted with permission from ref. [63]. Copyright © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) Ex-situ WAXS profiles of hard carbon electrodes at various stage of sodiation, (f) schematic diagrams of the sodium storage mechanism of “adsorption-intercalation-pore filling” in hard carbon. Gray areas indicate unused capacity because of slow kinetics[67]. Reprinted with permission from ref. [67]. Copyright © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (g) Chemical reaction of protic solvents with the HC electrode after discharged/charged to different voltages, (h) gas-chromatography chromatogram of gases with H2 after ethanol reaction with fully sodiated electrodes, (i) schematic illustration of the steady states of sodium in hard carbon: the insertion of Na+ into HC electrode accompanies by partial electron transfer between them with the formation of quasi-metallic sodium[68]. Reprinted with permission from ref. [68]. Copyright © 2021 Wiley-VCH GmbH

图2. 恒电位条件下石墨电极中Na+的稳态分布(上图)及Na+在石墨中存储的示意图(下图): (a) Na+在无空位缺陷电极中的分布, (b) Na+在存在空位缺陷电极中的分布, (c) 电流密度20 mA•g-1条件下不同电极的首周充放电曲线和 (d) HC-0.5电极的循环性能[69]. 已获得参考文献[69]的转载许可, 版权所有© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) 磷功能化前后其中P=O, P―O和P―C键形成的石墨层结构模型, (f, g) 钠离子吸附模型以及相应结合能, (h) 电流密度20 mA•g-1条件下不同电极的循环性能[100]. 已获得参考文献[100]的转载许可, 版权所有© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 2. Steady state Na+ ion distribution in graphitic electrode under constant potential conditions (top) and schematic representation of Na+ ion storage between the graphite layers (bottom). (a) Na+ ion distribution in a vacancy defect free electrode, (b) Na+ distribution in the presence of vacancy defects in the graphitic layers, (c) the first discharge-charge profiles for different electrodes at a current rate of 20 mA•g-1, (d) cycling performance for HC-0.5 electrode[69]. Reprinted with permission from ref. [69]. Copyright © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) The structure models of graphite layers before and after phosphorous-functionalized including P=O, P―O, P―C, (f, g) the Na-adsorption models and corresponding energies, (h) cycling performance for different electrodes at a current rate of 20 mA•g-1 [100]. Reprinted with permission from ref. [100]. Copyright ©2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

图3. (a, b, c) BN-CNFs电极的合成过程示意图, (d) BN-CNFs电极在10 A•g-1电流密度下的长循环性能, (e) 倍率性能[108]. 已获得参考文献[108]的转载许可, 版权所有© 2017 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) 化学预钠化和随后形成SEI膜的过程示意图. 20 mA•g-1电流密度下前三周充放电曲线(g)原始电极和(h) NaxHC电极, (i) NaxHC电极在100 mA•g-1电流密度下的长循环, 电压区间0~2 V vs. Na+/Na[113]. 已获得参考文献[113]的转载许可, 版权所有© 2020 American Chemical Society

Figure 3. (a, b, c) Fabrication process of BN-CNFs electrode, (d) cycling performance of BN-CNFs at a high current density of 10 A•g-1, (e) rate performance[108]. Reprinted with permission from ref. [108]. Copyright, © 2017 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) Schematic illustration of chemical presodiation and the subsequent SEI formation process on HC anodes. The initial three cycles of charge-discharge curves for (g) pristine HC and (h) NaxHC electrodes at a constant current of 20 mA•g-1. (i) Long-cycling performance of the NaxHC electrode at 100 mA•g-1 in the voltage range of 0~2 V vs. Na+/Na[113]. Reprinted with permission from ref. [113]. Copyright © 2020 American Chemical Society

图4. (a, b) 棉花和碳化后的棉花的SEM图像, (c, d) HCT样品的充放电曲线和循环性能[119]. 已获得参考文献[119]的转载许可, 版权所有© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) 制备的空心碳球的SEM图像, (f) 倍率性能, (g)空心碳纳米球和碳球的电化学反应过程示意图[123]. 已获得参考文献[123]的转载许可, 版权所有© 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 4. (a, b) SEM images of cotton and carbonized cotton, (c, d) charge-discharge curves and cycle performance of HCT samples[119]. Reprinted with permission from ref. [119]. Copyright © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) SEM images of the prepared hollow carbon nanospheres, (f) rate performance, (g) schemes of the electrochemical reaction process of hollow carbon nanospheres and carbon spheres[123]. Reprinted with permission from ref. [123]. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

图5. (a) SNMHCSs的合成过程, (b) 倍率性能, (c) 20 A•g-1电流密度下SNMHCSs的循环性能[131]. 已获得参考文献[131]的转载许可, 版权所有© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) HHVC的合成过程, (e, f) 不同HHVC样品的放电/充电循环性能, (g, h) 倍率性能[133]. 已获得参考文献[133]的转载许可, 版权所有© 2018 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 5. (a) The synthesis process of SNMHCSs, (b) rate performance, (c) cycle performance of SNMHCSs at the current density of 20 A•g-1 [131]. Reprinted with permission from ref. [131]. Copyright © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) The synthesis process of HHVC, (e, f) discharge/charge cycle performance of different HHVC samples, (g, h) rate performance of different HHVC samples[133]. Reprinted with permission from ref. [133]. Copyright © 2018 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 6. (a) Scheme of the pores in hard carbon filled by soft carbon, (b, c) initial discharge/charge profiles and cycle performance of all the hard-soft carbon composites with different asphalt contents, (d, e) initial discharge/charge profiles and cycle performance of all the hard-soft carbon composites with different carbonized temperatures[139]. Reprinted with permission from ref. [139]. Copyright © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 7. The electrochemical performances of hard carbon anode in different electrolyte. (a) Rate performance, (b) cycle performance at 30 mA•g-1, (c, d) initial discharge/charge profiles at different current densities, (e) long cycle performance at 2.1 A•g-1 [141]. Reprinted with permission from ref. [141]. Copyright © The Royal Society of Chemistry 2017

图8. (a) 预锂化硬碳负极在50 mA•g-1电流密度下的充放电曲线, (b) 预锂化硬碳负极在50 mA•g-1电流密度下的循环性能, (c) 预锂化硬碳负极在500 和1000 mA•g-1电流密度下的长循环性能, (d) 预锂化硬碳负极和NVP正极组装的全电池的充放电曲线, (e) 全电池的循环性能[145]. 已获得参考文献[145]的转载许可, 版权所有© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 8. (a) Initial discharge/charge profiles of pretreated hard carbon anode at 50 mA•g-1, (b) cycling performance of pretreated HC anode at a current density of 50 mA•g-1, (c) long-term cycling performance of pretreated HC at high current densities of 500 and 1000 mA•g-1, (d) full cell charge/discharge curves of NVP with pretreated and non-pretreated HC, (e) cycling performance of the full cell[145]. Reprinted with permission from ref. [145]. Copyright © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 9. Electrochemical performance of the HC anodes with different mass loadings with the ether-based electrolyte: (a) discharge/charge profiles at a current density of 0.02 A•g-1, (b) gravimetric and areal specific capacities change curves with mass loading, (c) initial Coulombic efficiencies change curve with mass loading, and (d) cycling performance at a current density of 0.2 A•g-1 [146]. Reprinted with permission from ref. [146]. Copyright © 2018, American Chemical Society

图10. (a) HCP的合成过程示意图, 薄纸, 预氧化碳纸, 硬碳纸的数码照片均显示出柔性自支撑的特征, (b) HCP的SEM图片, (c) HCP在20到2000 mA•g-1范围内不同电流密度下的倍率性能, (d) HCP在200和2000 mA•g-1电流密度下的长循环性能, (e) HCP在50 mA•g-1电流密度下–25到25 ℃范围内的充放电曲线, (f) HCP在500 mA•g-1电流密度下–15 ℃下的长循环性能[147]. 已获得参考文献[147]的转载许可, 版权所有© 2019 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim

Figure 10. (a) Schematic illustration of the preparation procedure for HCP and the digital photos of tissue, preoxidation carbonaceous paper (POCP) and HCP showing their flexible and self-supporting characteristics, (b) SEM image of HCP, (c) rate capability at various current densities from 20 to 2000 mA•g-1 of HCP, (d) long-term cycling performance at 200 and 2000 mA•g-1 of HCP, (e) GCD curves of 50 mA•g-1 of HCP at the temperature range from –25 to 25 ℃, (f) long-term cyclic stability of HCP at –15 ℃ and 500 mA•g-1 [147]. Reprinted with permission from ref. [147]. Copyright © 2019 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim

公司	技术路线	电池性能
FARADION (英国)	层状氧化物正极/硬碳负极/有机电解液, 软包电池	能量密度150~160 Wh• kg^-1, 循环寿命超3000次
NAIADES (法国)	氟磷酸钒钠正极/硬碳负极/有机电解液, 圆柱电池	能量密度90 Wh•kg^-1, 循环寿命4000次
中科海纳 (中国)	层状氧化物正极/无定型碳负极/有机电解液, 软包电池和圆柱电池	能量密度接近150 Wh• kg^-1, 循环寿命4500次以上
钠创新能源 (中国)	层状氧化物正极/硬碳负极/有机电解液, 软包电池	能量密度120 Wh•kg^-1, 循环寿命1000次
宁德时代 (中国)	普鲁士蓝正极/硬碳负极/有机电解液	能量密度160 Wh•kg^-1

表1. 钠离子电池产业化情况

Table 1. Industrialization of sodium ion batteries

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钠离子电池硬碳负极储钠机理及优化策略

Sodium Storage Mechanism and Optimization Strategies for Hard Carbon Anode of Sodium Ion Batteries

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