多孔聚合物在锂金属负极保护中的研究进展

doi:10.6023/A20100462

化学学报 ›› 2021, Vol. 79 ›› Issue (4): 378-387.DOI: 10.6023/A20100462 上一篇下一篇

综述

多孔聚合物在锂金属负极保护中的研究进展

庄容^a, 许潇洒^a, 曲昌镇^a, 徐顺奇^b, 于涛^a, 王洪强^a^,^*(), 徐飞^a^,^*

a 西北工业大学材料学院凝固技术国家重点实验室纳米能源材料研究中心西安 710072
b 德累斯顿工业大学化学与食品学院德累斯顿 01062

投稿日期:2020-10-09 发布日期:2020-11-19
通讯作者: 王洪强, 徐飞

作者简介:

庄容, 2020年毕业于北京化工大学, 获工学硕士学位, 目前在徐飞副教授指导下攻读博士学位. 研究兴趣为COFs材料的功能化设计与合成及其在储能方向的应用.

许潇洒, 2017年毕业于陕西师范大学, 获工学硕士学位, 目前在王洪强教授和徐飞副教授指导下攻读博士学位, 研究兴趣为纳米晶功能化的COFs材料及其储能性能研究.

王洪强, 教授、博士生导师, 德国洪堡学者、欧盟玛丽居里学者及国家高层次人才青年项目入选者. 2015年加入西北工业大学. 主要面向高性能钙钛矿光电器件、光电化学水分解以及可充电电池等新能源器件用关键材料, 开展亚稳超纳材料的瞬态极端制造与应用研究.

徐飞, 西北工业大学材料学院副教授、博士生导师、洪堡学者, 于2009年和2015年在中山大学分别获得学士和博士学位, 2012~2014年在日本分子科学研究所从事联合培养博士研究, 2018~2020年在德累斯顿工业大学从事洪堡博士后研究. 主要研究方向为功能多孔聚合物和炭材料的创新制备及在电化学储能与吸附等领域的研究.

† These authors contributed equally to this work

基金资助:
国家自然科学基金(51702262); 国家自然科学基金(51972270); 国家自然科学基金(51872179); 国家自然科学基金(51672225); 陕西省自然科学基金重点项目(2020JZ-07); 陕西省重点研发计划(2019TSLGY07-03)

Recent Progress of Porous Polymers for Lithium Metal Anodes Protection

Rong Zhuang^a, Xiaosa Xu^a, Changzhen Qu^a, Shunqi Xu^b, Tao Yu^a, Hongqiang Wang^a^,^*(), Fei Xu^a^,^*

a State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an 710072, China
b Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden 01062, Germany

Received:2020-10-09 Published:2020-11-19
Contact: Hongqiang Wang, Fei Xu
About author:
* E-mail: feixu@nwpu.edu.cn; Tel.: 029-88460684; Fax: 029-88460684
Supported by:
National Natural Science Foundation of China(51702262); National Natural Science Foundation of China(51972270); National Natural Science Foundation of China(51872179); National Natural Science Foundation of China(51672225); Natural Science Foundation of Shaanxi Province(2020JZ-07); Key Research and Development Program of Shaanxi Province(2019TSLGY07-03)

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摘要/Abstract

锂金属负极具有极高的理论比容量和最低的还原电位, 因此锂金属电池被认为是最具潜力的高比能储能器件之一. 然而, 充放电过程中不受控制的枝晶生长、不稳定的界面反应与巨大的体积变化导致锂金属负极库伦效率低与循环稳定性差, 同时枝晶刺穿隔膜也会带来安全隐患, 这些问题极大地制约着锂金属电池的实际应用. 多孔聚合物由于比表面积大、密度低、孔结构与微化学环境易裁剪等特点, 能够有效促进锂离子传输和均匀沉积, 已逐渐成为“无枝晶”锂金属电池研究领域的“新宠”. 然而, 相关的研究依然处于起步阶段, 本综述从人工固体电解质界面膜、隔膜修饰层与锂负极结构设计三个方面对多孔聚合物在锂金属电池负极保护中的研究进行了介绍与评述.

关键词: 锂金属电池, 锂枝晶, 负极保护, 多孔聚合物, 孔结构

Lithium metal batteries (LMBs) are regarded as one of the most promising candidates for next-generation high-energy-density devices, due to the high theoretical specific capacity and low electrochemical potential of lithium metal anode. However, the uncontrollable growth of Li dendrite, unstable Li/electrolyte interface and infinite volume fluctuation during charge/discharge process give rise to low Coulombic efficiency, poor cycle stability and even serious safety hazard from internal short-circuit via dendrite penetration through separators. These multifaceted problems severely hinder the practical applications of LMBs. Featured by high specific surface area, low density, controllable pore structure, and flexible molecular design of pore surface/skeleton functionality, porous polymers have received growing attention in electrochemical energy storage, especially for lithium anode protection. The nanopores and tailored functionalities could allow for facilitated Li ion transport, while inhibiting anions and regulating the grain size and distribution of LiF. The large pores are conducive to accommodating lithium deposition and lowing of local current density. Consequently, porous polymers have become the “new favorite” in the field of “dendrite-free” LMBs recently, which show great potential for stabilizing Li metal anode. However, explorations in this field still remain in their infancy, and the objective of this review is to briefly summarize the research progress of porous polymers, especially crystalline covalent organic frameworks for lithium metal anodes protection, by means of constructing the artificial solid electrolyte interphase layer, coating separator with functional layers and designing metal anode structure.

Key words: lithium metal battery, Li dendrite, anode protection, porous polymer, pore structure

引用此文

庄容, 许潇洒, 曲昌镇, 徐顺奇, 于涛, 王洪强, 徐飞. 多孔聚合物在锂金属负极保护中的研究进展[J]. 化学学报, 2021, 79(4): 378-387.

Rong Zhuang, Xiaosa Xu, Changzhen Qu, Shunqi Xu, Tao Yu, Hongqiang Wang, Fei Xu. Recent Progress of Porous Polymers for Lithium Metal Anodes Protection[J]. Acta Chimica Sinica, 2021, 79(4): 378-387.

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图/表 9

图1. 锂枝晶生长机理示意图[4]

Figure 1. Mechanism illustration of Li dendrite growth[4]

图2. 多孔聚合物在锂金属负极保护中的应用

Figure 2. The application of porous polymers for lithium metal anodes protection

图3. (a) COF的制备过程以及锂沉积/脱镀示意图. (b) COF保护锂负极在对称电池中的恒流循环图[8]. (c) COF-LZU1诱导锂沉积示意图[9]

Figure 3. (a) Preparation scheme of COF and the schematic diagram of Li plating/stripping. (b) Galvanostatic cycling profile of polished Li and COF-Li in a symmetrical cell[8]. (c) Schematic of inducing Li deposition via COF-LZU1[9]

图4. (a) COF-LiF的电化学制备示意图. (b)在极低N/P比和有限电解液的条件下, LiCOF-LiF@Li|NCM在0.15 C下的循环性能和库伦效率. (c)在1~30 mA•cm–2的电流密度和5 mAh•cm–2的沉积容量下, LiCOF-LiF@Li的锂沉积/剥离图. (d)锂化TpPa-COF结构中Li+的迁移过程示意图[11]

Figure 4. (a) Schematic illustration of the electrochemical preparation of the COF-LiF hybrid interphase layer. (b) Cycling stability and coulombic efficiency of LiCOF-LiF@Li|NCM at 0.15 C under limited N/P ratios and electrolytes conditions. (c) Li deposition/dissolution profiles of LiCOF-LiF@Li at current densities from 1 mA•cm–2 to 30 mA•cm–2 with a deposition capacity of 5 mAh•cm–2. (d) Schematic illustration of the fast Li+ transport process through the optimized structures of the lithiated TpPa-COF[11]

图5. (a)二维mPPy-GO异质结构的制备示意图. (b) mPPy-GO电极在电流密度为0.5 mA•cm–2和锂沉积容量为0.5 mAh•cm–2时的库伦效率. (c)以mPPy-GO-Li为负极, LiCoO2为正极所组装全电池的循环性能[50]

Figure 5. (a) Schematic of the fabrication of 2D mPPy-GO heterostructure. (b) Ultralong time Coulombic efficiency test of mPPy-GO electrode with capacity of 0.5 mAh•cm–2 at 0.5 mA•cm–2. (c) Long-term cycling stability of full batteries based on mPPy-GO-Li anode with LiCoO2 cathodes[50]

图6. (a)溶剂化/去溶剂化Li+、阴离子和阳离子通过不同隔膜的迁移示意图. (b) PEO/N-rGO/PVDF-HFP//COF-1双层膜组装的Li||Li对称电池的锂离子迁移数(内部插图为离子迁移数的测试电池示意图). (c) Li-Li4Ti5O12全电池和(d) Li-LiFePO4全电池的循环性能[13]

Figure 6. (a) Schematic diagram of solvated/desolvated Li+ and the transport of cations and anions through different membranes. (b) The Li-ion transference number of the Li||Li cell with double-layer PEO/N-rGO/PVDF-HFP//COF-1 membrane (Inset of (b): the corresponding configuration of the cells for testing the ion transference number). The cycling performance of Li-Li4Ti5O12 full battery (c) and Li-LiFePO4 full battery (d)[13]

图7. (a) COF-LZU1的结构示意图和Li+在2D COF-LZU1中的迁移图. (b) Li+遵循高尔顿板模型的沉积示意图. (c) Li+迁移数的测试. (d) 在不同电解液体系中, 使用常规隔膜和COF-LZU1/PP隔膜的锂||锂对称电池的电化学性能对比[14]

Figure 7. (a) Schematic of the structure of COF-LZU1 and Li-ion transport in the stacked 2D COF-LZU1. (b) Schematic of Li-ion deposition following the principle of Galton Board model. (c) Measurements of Li-ion transference numbers. (d) Comparison of electrochemical performance of Li||Li symmetric batteries with conventional separator and COF-LZU1/PP separator using different electrolyte[14]

图8. (a) 3D PPS在电场中的电动效应. (b)以Li@3D PPS@Cu为负极, LiFePO4为正极所组装全电池的循环性能[15]. (c)用于碱金属负极的三维MXene-MF制备流程图. (d) 3D MXene-MF电极在电流密度为50 mA•cm–2和锂沉积容量为50 mAh•cm–2时的库伦效率. (e)基于MXene-MF-Li电极的对称电池在电流密度为10 mA•cm–2和锂沉积容量为10 mAh•cm–2时的循环性能[17]

Figure 8. (a) Electrokinetic phenomena in 3D PPS under an electric field. (b) Cycling performance of full cells using Li@3D PPS@Cu as the anodes and a high-areal-capacity LiFePO4 as the cathodes[15]. (c) Schematic illustration of the fabrication process of 3D MXene-MF scaffold for alkali metal anode. (d) Coulombic efficiency of 3D MXene-MF electrode at high current density of 50 mA•cm–2 for 50 mAh•cm–2. (e) Long-life symmetric cells galvanostatic cycling of MXene-MF-Li electrode at 10 mA•cm–2 with Li deposition capacity of 10 mAh•cm–2 [17]

材料	电流密度/ (mA•cm^–2)	容量/(mAh•cm^–2)	电解液	循环寿命	参考文献
COF	1	1	1 mol/L LiTFSI in DOL/DME (1∶1,V/V)	400 h	[8]
COF-LZU1	0.5	0.5	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 1% (w) LiNO₃	2000 h	[9]
TpPa-COF	10	5	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 1% (w) LiNO₃	200 h	[11]
AP-CTF-LiF	5	1	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 2% (w) LiNO₃	280 h	[12]
mPPy-GO	5	1	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 1% (w) LiNO₃	400 h	[50]
PEO/N-rGO/PVDF-HFP//COF-1	1	1	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 1% (w) LiNO₃	2200 h	[13]
2D COF-LZU1	1	1	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 2% (w) LiNO₃	1000 h	[14]
3D PPS	4	2	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 1% (w) LiNO₃	300 h	[15]
PMF	10	1	1 mol/L LiTFSI in DOL/DME (1∶1,V/V)	50 h	[16]
3D MXene-MF	10	10	1 mol/L LiTFSI in DOL/DME (1∶1,V/V) with 1% (w) LiNO₃	3800 h	[17]

表1. 多孔聚合物应用于锂金属负极保护中的电化学性能

Table 1. The electrochemical performance of porous polymer in lithium metal anodes protection

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多孔聚合物在锂金属负极保护中的研究进展

Recent Progress of Porous Polymers for Lithium Metal Anodes Protection

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