氢键化学赋能高比能锂电池关键材料

doi:10.6023/A25060204

化学学报 ›› 2025, Vol. 83 ›› Issue (11): 1451-1462.DOI: 10.6023/A25060204 上一篇

综述

氢键化学赋能高比能锂电池关键材料

周泓宇^a, 王俪颖^a, 赵宇^a, 吴泽轩^b, 李国鹏^b, 李念武^b^,^*(), 楚攀^a^,^*()

^a 中石油深圳新能源研究院有限公司广东深圳 518000
^b 北京化工大学有机无机复合材料全国重点实验室北京 100029

投稿日期:2025-06-05 发布日期:2025-08-28
通讯作者: 李念武, 楚攀

作者简介:

周泓宇, 男, 助理研究员, 于2017年获吉林大学学士学位; 2022年获吉林大学博士学位; 2023年加入中石油深圳新能源研究院有限公司, 目前主要研究方向为新型储能材料与电芯开发.

李念武, 男, 硕士生导师, 北京化工大学化学工程学院副教授, 中国颗粒协会青年理事. 于2014年南京航空航天大学获得工学博士学位, 2014年~2016年在中科院化学所从事博士后研究工作, 2017年~2018年在北京纳米能源与系统研究所任助理研究员. 目前主要研究方向为锂/钠电池负极和固态电池. 在Adv. Mater. 等期刊上发表论文80余篇, SCI总引用10000余次, H-index为40, 入选2023年科睿唯安全球高被引学者, 2024全球前2%顶尖科学家年度影响力榜. 主持国家自然科学基金青年基金和面上基金项目, 作为骨干参与国家重点研发计划. 已授权国内发明专利10项, 国际PCT专利1项.

楚攀, 中石油深圳新能源研究院有限公司高级工程师, 中国化学与物理电源行业协会储能应用分会专家委员, 中国石油学会新能源专业委员会专家委员, 中国工业节能与清洁生产协会电池回收与再利用分会专家委员, 储能领跑者联盟专家技术顾问; 长期从事能源高效利用及节能理论、新能源发电, 大规模储能技术等领域的相关工程技术研究; 参与了国内首个大规模储能方向的“国家863课题”, 主导并完成了多个集团公司的储能科技项目和储能工程项目, 近年来参与的储能项目超过50个, 在国内外权威期刊上发表SCI/EI检索论文30余篇, 并在储能领域获得了专有专利技术30余项.

基金资助:
项目受中国石油天然气股份有限公司科技项目课题(2023DJ5409); 国家自然科学基金面上项目(21975015)

Hydrogen Bond Chemistry Enabled Key Materials for High-Energy-Density Lithium Batteries

Zhou Hongyu^a, Wang Liying^a, Zhao Yu^a, Wu Zexuan^b, Li Guopeng^b, Li Nianwu^b^,^*(), Chu Pan^a^,^*()

^a PetroChina Shenzhen New Energy Research Institute Co., Ltd., Shenzhen 518000
^b State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029

Received:2025-06-05 Published:2025-08-28
Contact: Li Nianwu, Chu Pan
Supported by:
Scientific research project subject of PetroChina Company Limited(2023DJ5409); National Natural Science Foundation of China(21975015)

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摘要/Abstract

机器人、无人机、电动汽车、智能电子设备的快速发展, 促进了高比能锂电池的迅猛发展. 然而, 高比能锂电池的关键材料面临着锂离子传导差、体积膨胀大、电极/界面不稳定、化学和结构稳定性差等重要挑战. 本综述从基础化学键的角度出发, 系统总结了氢键化学在高比能锂电池关键材料设计优化中的作用. 合理构建氢键网络结构可以提升正负极材料的化学稳定性和结构稳定性, 缓解体积膨胀和提升电极/界面稳定性. 氢键可以调控电解液溶剂化结构, 增强聚合物电解质锂离子传输, 赋予聚合物电解质和粘结剂自修复功能并提升其机械性能. 最后, 指出了氢键在高比能锂电池中面临的挑战, 并对其未来的发展进行了展望.

关键词: 氢键, 离子传导, 界面, 体积膨胀, 自修复

The rapid proliferation of electric vehicles, unmanned aerial vehicles, and smart electronics has fueled escalating demand for high-energy-density lithium batteries. Current battery systems confront critical challenges: sluggish Li⁺ ion transport kinetics that constrain rate capability; structural degradation from substantial volume changes in silicon anodes and sulfur cathodes; accelerated stability deterioration through interfacial side reactions; and shortened cycle life due to chemical/structural degradation. This review, rooted in chemical bond fundamentals, systematically examines regulatory mechanisms of hydrogen bond (H-bond) chemistry—harnessing the dynamic reversibility of H-bonds (X—H…Y, where X and Y denote highly electronegative small-radius atoms like N, O, or F, with bond energies of 5~42 kJ•mol⁻¹) to overcome material limitations across battery components. For cathodes, H-bond networks between organic coatings and layered oxides suppress lattice oxygen release and transition metal dissolution, enhancing interfacial stability, while intramolecular H-bonding in organic cathodes mitigates dissolution; concurrently, self-healing binders utilizing dynamic H-bond reorganization accommodate sulfur cathode volume expansion. In electrolytes, functional enhancement is achieved through H-bond mediation: liquid electrolytes leverage atypical H-bonds (e.g., F^δ⁻—H^δ^⁺) to optimize solvation structures and reduce desolvation barriers, thereby accelerating interfacial Li⁺ ion transfer; solid-state electrolytes employ H-bond chemistry to elevate ionic conductivity and Li⁺ ion transference numbers; gel and solid polymer electrolytes exploit H-bond networks to facilitate Li⁺ conduction, inhibit dendritic growth, enhance interfacial stability, enable self-healing, improve mechanical robustness, and widen electrochemical stability windows; organic-inorganic composite electrolytes similarly utilize H-bonds to augment Li⁺ transference numbers and conductivity. Separator modifications exploit H-bond interactions with electrolytes to improve wettability and homogenize Li⁺ flux. For anodes, self-healing binders dynamically reform H-bonds to repair silicon volume-expansion cracks, while artificial solid electrolyte interphase layers utilize multi-site H-bonding to guide uniform lithium deposition. Despite these advances, three pivotal challenges persist: in-situ characterization of H-bonds requires breakthroughs in advanced analytical techniques; conceptual expansion of H-bonding principles; the need for deeper mechanistic understanding of both canonical and non-canonical H-bonding in high-energy-density battery materials. Future progress demands integration of in situ characterization, artificial intelligence-assisted design, and multiscale simulations to unlock the full potential of H-bond chemistry for next-generation batteries with ultrahigh energy density and long cycle life.

Key words: hydrogen bond, ionic transport, interphase, volume expansion, self-healing

引用此文

周泓宇, 王俪颖, 赵宇, 吴泽轩, 李国鹏, 李念武, 楚攀. 氢键化学赋能高比能锂电池关键材料[J]. 化学学报, 2025, 83(11): 1451-1462.

Zhou Hongyu, Wang Liying, Zhao Yu, Wu Zexuan, Li Guopeng, Li Nianwu, Chu Pan. Hydrogen Bond Chemistry Enabled Key Materials for High-Energy-Density Lithium Batteries[J]. Acta Chimica Sinica, 2025, 83(11): 1451-1462.

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图/表 8

图1. 氢键化学用于高比能电池示意图

Figure 1. Schematic of hydrogen bond for high-energy-density batteries

图2. (a) PPy包覆NCM正极材料的结构设计及原理示意图, (b)纯NCM、NCM@PEDOT、NCM@PPy在全固态金属锂电池中的循环性能对比图[16]

Figure 2. (a) The structural design and schematic diagram of PPy coated NCM cathode material, (b) The cycling performance of ASSLMBs paired with pure NCM, NCM@PEDOT, and NCM@PPy. Reprinted with permission from Ref.[16]. Copyright 2024, The Royal Society of Chemistry

图3. 显性和隐性溶剂化示意图. 基于电子给体的典型溶剂化壳结构(a)和阴离子受体(b), 两者溶剂化过程都会自发解离锂盐并参与溶剂化鞘的形成; 隐性溶剂和诱导剂的相互作用导致了隐形溶剂化(c); 通过分子对接激活隐性溶剂的机制(d)[35]

Figure 3. Schematic of dominant and recessive solvation. Typical solvation shell structures based on the electron donor (a) and anion receptor (b), both of which spontaneously dissociate the salt and participate in the formation of the solvation sheath; recessive solvation enabled by the interacted recessive solvent and inducer (c); activation of the recessive solvent via molecular docking mechanism (d). Reprinted with permission from Ref.[35]. Copyright 2024, Springer Nature

图4. 富含氢键的凝胶聚合物电解质与锂金属负极(LMAs)发生界面反应的示意图. (a)富含氢键的凝胶聚合物电解质与LMAs存在着严重的界面副反应; (b)通过分子封装效应可以抑制富含氢键的凝胶聚合物电解质与LMAs的界面副反应[43]

Figure 4. Schematics of interfacial reactions between hydrogen-bond-rich gel-state polymer electrolytes and LMAs. (a) The severe interfacial reactions between hydrogen-bond-rich electrolytes and LMAs. (b) The interfacial reactions between hydrogen-bond-rich electrolytes and LMAs are suppressed via the molecular encapsulation effect. Reprinted with permission from Ref.[43] Copyright 2024, Wiley-VCH

图5. 采用LHOF基固态电解质的全固态Li-O2电池示意图[20]

图6. 氢键提高电解液浸润性的机制[83]

图7. Si@PEG、Si@PANI和Si@PP的合成示意图, 以及Si NPs、PEG和PANI之间的氢键网络[95]

Figure 7. Schematic illustration of the synthesis of Si@PEG, Si@PANI, and Si@PP, and the H-bonding network between Si NPs, PEG, and PANI. Reprinted with permission from Ref.[95] Copyright 2024, Wiley-VCH

图8. (a)具有高韧性、自修复功能和弹性的动态超分子聚氨酯-脲(DSP-n)的结构设计和机理示意图; (b)分子链段在拉伸过程的运动示意图; (c) Li在裸Li和动态超分子聚氨酯-脲界面(DSIPI)@Li上的沉积示意图, 说明了DSIPI用于无枝晶和高效LMA的机制[21]

Figure 8. (a) Structural design and mechanism diagram of DSP-n featuring high toughness, self-healing capabilities, and stretchability. (b) Schematic diagram illustrating the movement of polymer chain segments during the stretching process. (c) Schematic of Li plating/stripping on bare Li and DSIPI@Li anodes, revealing the mechanism of action of DSIPI for a dendrite-free and efficient Li metal anode. Reprinted with permission from Ref.[21] Copyright 2024, Wiley-VCH

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氢键化学赋能高比能锂电池关键材料

Hydrogen Bond Chemistry Enabled Key Materials for High-Energy-Density Lithium Batteries

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