石墨烯基聚合物复合电解质的设计、性能及其应用研究进展

杨富杰; 王亮; 阮文红; 章明秋; 容敏智

doi:10.13801/j.cnki.fhclxb.20201126.002

石墨烯基聚合物复合电解质的设计、性能及其应用研究进展

doi: 10.13801/j.cnki.fhclxb.20201126.002

杨富杰^{1, 2,},
王亮^2,,
阮文红^2, ,,
章明秋^2, ,,
容敏智^2,

1.
仲恺农业工程学院　化学化工学院，广州 510225
2.
中山大学　化学学院　聚合物复合材料及功能材料教育部重点实验室，广州 510275

基金项目: 国家自然科学基金 (52033011；51773229；51473186；52003307)；广州市科技计划项目(201802010009；201902010050)

详细信息

通讯作者:
阮文红，博士，教授，博士生导师，研究方向为聚合物复合材料及功能材料　 E-mail：cesrwh@mail.sysu.edu.cn

章明秋，博士，教授，博士生导师，研究方向为高分子及高分子复合材料的基础理论和应用基础　 E-mail：ceszmq@mail.sysu.edu.cn

中图分类号: TB332
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- 被引次数: 0
出版历程
- 收稿日期: 2020-08-24
- 录用日期: 2020-11-17
- 网络出版日期: 2020-11-26
- 刊出日期: 2021-03-15

Research progress on design, performance and application of graphene based polymer composite electrolytes

YANG Fujie^{1, 2
,},
WANG Liang^2
,,
RUAN Wenhong^{2
, ,},
ZHANG Mingqiu^{2
, ,},
RONG Minzhi^2
,

1.
College of Chemistry and Chemical Engineering, Zhongkai University of Agriculture and Engineering, Guangzhou 510225, China
2.
Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China

摘要

摘要: 固态电化学器件具有柔性好、安全性能高及能量密度高等优点，属于极有前景的新一代化学能源器件。固态电解质是实现电化学器件固态化的关键，其中石墨烯基聚合物复合电解质由传统聚合物电解质发展而来，是一类含有石墨烯纳米填料和聚合物基体的新型固态电解质，具有较高的离子电导率、良好的加工性能及优异的界面特性，现已成为固态电化学器件研发中备受关注的电解质材料。本文着重讨论了近年来石墨烯基聚合物复合电解质的结构设计、性能机制及在各种电化学储能器件中应用的研究进展。
- 石墨烯 /
- 复合材料 /
- 聚合物 /
- 固态电解质 /
- 电化学
Abstract: Solid-state electrochemical devices are considered as one of the most promising candidates for next generation chemical energy devices because of their flexibility, safety and high energy density. Solid electrolyte is a key material to achieve the goal. Graphene based polymer composite electrolyte derived from the traditional polymer electrolyte represents a new-type solid electrolyte consisting of both graphene nano-fillers and polymer matrix. In recent years, the inorganic/organic hybrid electrolytes have proved to possess high ionic conductivity, good processing ability and excellent interfacial properties, so that they received extensive attentions for working as electrolyte materials in solid-state electrochemical devices. In this review, the up-to-date research progresses in the field of graphene based polymer composite electrolytes are systematically discussed with particular emphasis on the structural design, performance mechanism and application in various electrochemical energy storage devices.
- graphene /
- composites /
- polymer /
- solid-state electrolyte /
- electrochemistry

HTML全文

图 1 氧化石墨烯(GO)的结构示意图^[11]

Figure 1. Structural schematic of graphene oxide (GO)^[11]

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图 2 SPI/PIL(NTFSI)-G/PIL膜的离子传输机制(a)^[14]; 利用功能石墨烯实现Nafion膜可调节传输特性的策略(b)^[15]

Figure 2. Ion transport mechanism in membrane of SPI/PIL(NTFSI)-G/PIL (a)^[14]; Strategy for realizing tunable transport properties of Nafion membrane using functionalized graphene (b)^[15]

SPI—Sulfonated polyimide; PILs—Protic ionic liquids; PIL(NTFSI)-G—Protic ionic liquid based composite membranes with ionic liquid modified graphene sheets; GO—Graphene oxide; SGO—Sulfonated GO; GON—GO/Nafion; SGON—SGO/Nafion

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图 3 GO-LBL自支撑薄膜制备及组装示意图^[17]

Figure 3. Schematic representation of fabrication and assembly of free-standing GO-LBL membrane^[17]

LBL—Layer-by-layer; PHS—Poly(4-vinylphenol); PAH—Poly(allylamine hydrochloride); PSS—Poly(sodium 4-styrene sulfonate)

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图 4 Li⁺/PEO络合物(a)、GO插层复合物((b)~(d))的结构及EO/GO界面上(e)锂离子的快速传输^[39]

Figure 4. Structures of ethylene oxide/lithium-ion (a), GO-intercalated composites ((b)–(d)), and fast transfer of lithium-ion at EO/GO interface (e)^[39]

EO—Ethylene oxide; PEO—Polyethylene oxide

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图 5 GO/PEO复合聚合物电解质中离子的各向异性传输行为^[42]

Figure 5. Illustration of anisotropic ion transport in GO/PEO composite electrolyte^[42]

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图 6 PAA-PEG/石墨烯、PAA-PEG/GO、PAA-PEG/石墨和PAA-PEG凝胶电解质的EIS曲线^[48]

Figure 6. EIS curves of gel electrolytes of PAA-PEG/graphene, PAA-PEG/GO, PAA-PEG/graphite and PAA-PEG^[48]

PAA—Polyacrylate; PEG—Poly(ethylene glycol); EIS—Electrochemical impedance spectroscopy

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图 7 利用激光微拉曼光谱仪对ITO电极上桥接氧化还原物质负载的GO(RS/GO)进行电化学表征: (a)含有RS/GO的ITO电极的循环伏安图(CVs);(b)循环伏安扫描期间使用反射光学显微镜成像的电极/电解质与桥接氧化石墨烯固体界面的照片; (c)电极侧电极-电解液界面的棕色(富含GO)区和黑色(富含rGO)区的拉曼光谱; (d)桥接RS/GO或RS/rGO作为扩展氧化还原界面以增强能量传递的示意图^[50]

Figure 7. Electrochemical characterization accompanied by laser micro-Raman spectroscopy study on bridged redox species-coated GO (RS/GO) on ITO electrode: (a) Cyclic voltammograms (CVs) of ITO electrode with bridged RS/GO; (b) Photographs of electrode/electrolyte solid interface with bridged GO by using reflection optical microscope imaging during cyclic voltammetry scans; (c) Raman spectra of brown (GO-rich) regions and black (rGO-rich) regions on electrode side of electrode-electrolyte interface, respectively; (d) Schematic illustration of bridged RS/GO or RS/rGO performing as extended redox interface for enhancing energy delivery^[50]

ITO—Indium tin oxide; rGO—Reduced-GO; V_d—Decomposition voltage; I_G/I_D—Intensity ratio

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图 8 PVA/H₃PO₄/SAGO和PVA/H₃PO₄凝胶电解质薄膜的拉伸应力-应变曲线^[51]

Figure 8. Typical tensile stress-strain curves of PVA/H₃PO₄/SAGO and PVA/H₃PO₄ gel electrolyte films^[51]

PVA—Poly(vinyl alcohol); SAGO—Small area GO

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图 9 甲醇分子通过剥离/定向GO纳米复合膜的扩散途径^[62]

Figure 9. Diffusion pathway of methanol molecules through an exfoliated/aligned GO nanocomposite membrane^[62]

GO_SULF—Sulfonated organo modified GO; D—Self-diffusion coefficients of water

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图 10 SPEEK-DGO界面上酸碱对之间的质子跳跃行为(左)和在120℃无水条件下的H₂/O₂单电池性能(右) (a)^[63]; 功能化GO的结构，以及在无水条件下含有PGO的PBIs的质子电导率和单一燃料电池性能(b)^[64]; SPAES与GO之间和SPAES与ABPBI-GO之间的相互作用示意图(上)，在50%湿度下的SPAES/ABPBI-GO和SPAES/GO的质子电导率(下) (c)^[65]; SPI和SPI-GOs复合膜的质子传输过程(上)及其质子电导率和直接甲醇燃料电池性能(下) (d)^[66]

Figure 10. Proton-hopping behavior between acid-base pairs at SPEEK-DGO interface (left) and performance of single cell containing the membrane with anhydrous H₂/O₂ operating under 120℃ and anhydrous conditions (right) (a)^[63]; Structure of functionalized GO, and proton conductivity and single cell performance of PBIs with PGO under anhydrous conditions (b)^[64]; Schematic drawing of interaction between SPAES matrix and GO and that between SPAES matrix and ABPBI-GO (upper), and proton conductivity of SPAES/ABPBI-GO and SPAES/GO under 50% RH conditions (bottom) (c)^[65]; Proton transport in SPI and SPI-GOs composite membranes (upper), and proton conductivities and DMFCs performance of SPI and SPI-GOs composite membranes (bottom) (d)^[66]

SPEEK—Sulfonated poly(ether ether ketone); DGO—Polydopamine-modified GO; PBI—Polybenzimidazole; Py—2,6-Pyridine; PA—Phosphoric acid; SPAES—Sulfonated poly(arylene ether sulfone); ABPBI—Poly(2,5-benzimidazole); RH—Relative humidity; SPI—Sulfonated polyimide; DMFCs—Direct methanol fuel cells

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图 11 柔性锂离子电池结构示意图(a); 柔性锂离子电池循环100次的放电容量(b)^[47]

Figure 11. Schematic drawing of flexible thin-film Li-ion battery (a); Discharge capacity during 100 cycles of flexible battery (b) ^[47]

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图 12 含有氧化石墨烯量子点(GOQDs)的凝胶复合电解质的离子传导机制及其离子电导率和锂离子电池性能^[35]

Figure 12. Ion transport mechanism and ionic conductivity of gel composite electrolyte containing graphene oxide quantum dots (GOQDs), and performance of corresponding Li-ion battery^[35]

σ—Ionic conductivity; SLE—Celgard-separator-supported liquid electrolyte; GPE—Gel polymer electrolyte; PAVM—Polymer framework comprising poly(acrylonitrile-co-vinyl acetate) and incorporated poly(methyl methacrylate); QD—Quantum dots

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