PEDOT导电高分子在柔性能量转化与存储器件的研究进展

doi:10.6023/A21030106

化学学报 ›› 2021, Vol. 79 ›› Issue (7): 853-868.DOI: 10.6023/A21030106 上一篇下一篇

综述

PEDOT导电高分子在柔性能量转化与存储器件的研究进展

龚陈祥^a^,^b, 程书平^a, 孟祥川^a^,^b, 胡笑添^a^,^b^,^*(), 陈义旺^a^,^b^,^c^,^*()

a 南昌大学化学学院南昌 330031
b 高分子及能源化学研究院南昌 330031
c 江西师范大学高等研究院南昌 330022

投稿日期:2021-03-22 发布日期:2021-04-27
通讯作者: 胡笑添, 陈义旺

作者简介:

龚陈祥, 南昌大学化学学院2019 级在读硕士生. 主要研究方向为导电聚合物形貌调控和大面积柔性钙钛矿太阳电池的制备研究.

胡笑添, 南昌大学特聘研究员, 中国科学院化学研究所理学博士. 主要代表性成果: 自主设计研发“卷对卷”光电器件印刷系统, 并实现大面积柔性透明电极和新型薄膜光伏器件制备; 利用柔性仿生设计, 首次实现印刷可穿戴钙钛矿太阳能电源.

陈义旺, 南昌大学和江西师范大学教授, 博士生导师, 国家杰出青年科学基金获得者, 江西师范大学副校长, 南昌大学高分子及能源化学研究院院长. 主要从事太阳电池、纳米材料、功能高分子材料等领域研究.

基金资助:
国家自然科学基金(U20A20128); 国家自然科学基金(U1801256); 国家自然科学基金(22005131); 国家自然科学基金(51833004); 国家杰出青年科学基金(51425304)

Recent Advances of PEDOT in Flexible Energy Conversion and Storage Devices

Chenxiang Gong^a^,^b, Shuping Cheng^a, Xiangchuan Meng^a^,^b, Xiaotian Hu^a^,^b(), Yiwang Chen^a^,^b^,^c()

a College of Chemistry, Nanchang University, Nanchang 330031, China
b Institute of Polymers and Energy Chemistry, Nanchang 330031, China
c Institute of Advanced Scientific Research, Jiangxi Normal University, Nanchang 330022, China

Received:2021-03-22 Published:2021-04-27
Contact: Xiaotian Hu, Yiwang Chen
Supported by:
National Natural Science Foundation of China(U20A20128); National Natural Science Foundation of China(U1801256); National Natural Science Foundation of China(22005131); National Natural Science Foundation of China(51833004); National Science Fund for Distinguished Young Scholars(51425304)

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摘要/Abstract

近年来, 柔性有机和钙钛矿光伏器件、有机薄膜晶体管和医用传感器等因其具有可穿戴性、柔性、半透明性等优点, 成为科学研究的热门领域. 利用具有优异力学性能的导电聚合物是实现这些高性能器件的有效途径之一. 在导电聚合物中, 3,4-亚乙基二氧噻吩(PEDOT)及其水性分散液3,4-亚乙基二氧噻吩:聚苯乙烯磺酸盐(PEDOT:PSS)已经被证明是最有前途替代传统金属氧化物的柔性材料, 其在器件中可作为透明电极、空穴传输层、互连器、电活性层或运动传感导体等. 综述了PEDOT及PEDOT:PSS应用柔性器件的研究现状, 包括提高电导率、机械耐受性和长期稳定性的各种策略, 揭示了性能增强的潜在机理. 最后, 论述了导电聚合物在器件制备中亟待解决的问题和未来发展方向. 本工作讨论了导电聚合物薄膜形貌的重要性, 并展望了它们在下一代柔性电子器件中的广阔前景.

关键词: PEDOT/PEDOT:PSS, 电导率, 透明电极, 柔性能源电子, 可拉伸器件

In recent years, flexible organic and perovskite photovoltaic devices, organic thin-film transistors and medical sensors have been become popular fields of scientific research due to their advantages of wearable, flexible and semi-transparent properties. Employing conductive polymer with excellent mechanical properties is one of the effective pathways to realize these high-performance devices. In conducting polymers, poly(3,4-ethylenedioxythiophene) (PEDOT) and its aqueous dispersion poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) have been demonstrated to be the most promising alternative flexible materials of conventional metal oxides. It can be used as transparent electrode, hole transport layer, interconnects, electroactive layer, or motion sensing conductor in the device. This review focused on recent research advances of flexible devices for PEDOT and PEDOT:PSS applications, including various strategies to improve electrical conductivity, mechanical tolerance and long-term stability, and reveals the potential mechanisms of performance enhancement.

Key words: PEDOT/PEDOT:PSS, electrical conductivity, transparent electrode, flexible energy electronics, stretchable device

引用此文

龚陈祥, 程书平, 孟祥川, 胡笑添, 陈义旺. PEDOT导电高分子在柔性能量转化与存储器件的研究进展[J]. 化学学报, 2021, 79(7): 853-868.

Chenxiang Gong, Shuping Cheng, Xiangchuan Meng, Xiaotian Hu, Yiwang Chen. Recent Advances of PEDOT in Flexible Energy Conversion and Storage Devices[J]. Acta Chimica Sinica, 2021, 79(7): 853-868.

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图/表 10

图1. PEDOT:PSS在能量转换领域的应用. (a) PEDOT:PSS的化学结构和优点. (b) 近年来PEDOT:PSS应用的论文发表和引用. (c) PEDOT:PSS作为透明电极在有机光伏和钙钛矿太阳电池中的应用[18,84]. (d) PEDOT:PSS在能量储存器中的应用[108,115]. (e) PEDOT:PSS在可拉伸器件中的应用[3]

Figure 1. Application of PEDOT:PSS in the field of energy conversion. (a) The chemical structure and advantages of PEDOT:PSS. (b) The manuscript of PEDOT:PSS application have been published and cited. (c) Application of PEDOT:PSS as transparent electrode in organic photovoltaic and perovskite solar cells[18,84]. (d), (e) Application of PEDOT:PSS in energy storage and stretchable device[3,108,115]

图2. 合成PEDOT或PEDOT:PSS的策略. (a) 搭配其他组分合成PEDOT纳米纤维[51]. (b) 采用“一锅”绿色聚合法合成PEDOT纳米粒子[52]. (c) 电化学聚合PC4-EDOT-COOH薄膜[53]. (d) 采用“点击化学”合成叠氮功能化的PEDOT[54]. (e) 界面聚合制备PEDOT/GO/GCE纳米纤维[57]. (f) 采用氧化-气相聚合法合成的PEDOT纳米粒子[58]

Figure 2. Diverse synthesis strategies for PEDOT and PEDOT:PSS. (a) PEDOT nanofibers are synthesized with new components[51]. (b) The PEDOT nanoparticles are synthesized by “one-pot” polymerization [52]. (c) The PC4-EDOT-COOH films by electrochemical polymerization[53]. (d) The PEDOT with azide functionalization is synthesized by “clicking chemical” [54]. (e) Fabrication of PEDOT/GO/GCE nanofibers by interfacial polymerization[57]. (f) PEDOT nanoparticles are synthesized by oxidative-vapor polymerization[58]

Scheme	Type	Solvent	σ/(S•cm^-1)	T/%	R_sh/(Ω•sq^-1)	Reference
EG	Doping	Baytron P	200	—	—	[21]
DMSO	Doping	Baytron PH500	550	95	190	[102]
EG	Doping	PH1000	1330	86	60	[68]
EG, MSA	Doping	PH1000	3560	92.5	43	[68]
	Doping	PH1000	3100	96	59	[82]
EG	Doping	PH1000	5012	73	36	[81]
H₂SO₄	Soaking (1 mol/L)	PH1000	3065	81	39	[72]
	Soaking (1 mol/L)	PH1000	3065	87	67	[72]
	Soaking (100%)	PH1000	4200	90	46	[69]
	Soaking (98%)	PH1000	3210	92	79	[71]
H₂SO₄	Transfer-printing	PH1000	4000	90	45	[70]
	Transfer-printing	PH1000	4000	86.5	33	[70]
HNO₃	Soaking	PH1000	4100	—	14	[73]
MSA	Soaking	PH1000	2540	92	50	[82]
H₂SO₄	Post-treatment	PH1000 and 4083	1700	89	—	[74]
H₂SO₄	Post-treatment	PH1000 and 4083	3000	—	—	[74]
HCOOH	Post-treatment	PH1000 and 4083	1362	—	—	[74]

表1. 不同溶剂处理的PEDOT薄膜性能参数

Table 1. Performance parameters of PEDOT films based on differential solvent treatment

PEDOT:PSS	Device structure	Scheme	PCE/%	J_SC/ (mA•cm^-2)	FF/%	V_OC/V	Reference
Transparency electrode	PET/PH1000/ZnO/Perovskite/Spiro- OMeTAD/PH1000	Nitric acid annealed	10.3	17.3	60	0.99	[25]
	PET/PH1000/Perovskite/PCBM/PTCDI/ Cr₂O₃/Cr/Au/Polyurethane	Solvent treatment	12	17.5	76	0.93	[32]
	PET/PH1000/MAPbI₃/TiO₂/Al	Solvent doping	7.60	15.0	60.0	0.80	[27]
	PET/PH1000/PEI/MAPbI₃/Spiro-OMeTAD/ Au	Solvent doping	9.73	17.2	59.7	0.95	[25]
	NOA63/PH1000/MAPbI₃/PCBM/Eutectic Ga-In blends	—	10.75	16.6	70.5	0.92	[27]
	PET/PEDOT:PSS:CFE/PEDOT:PSS/ Perovskite/PCBM/Ag	Surfactant treatment	19.0	22.38	0.79	1.08	[84]
Hole transport layer	PET/ITO/NC-PEDOT:PSS/Perovskite/PCBM/Ag	Nanocellular scaffold	19.66	22.47	0.81	1.08	[23]
	PET/ITO/PEDOT:EVA/Perovskite/PCBM/ BCP/Ag	—	19.87	21.26	0.79	1.18	[98]
	PDMS/PEDOT:PSS/Perovskite//PCBM/PEI/ PEDOT:PSS/PDMS	—	15.61	18.70	0.78	1.07	[23]
	PET/PH1000/PEDOT:PSS/Perovskite/PCBM/Rhodamine/C₆₀ /Rhodamine/LiF/Ag	Solvent treatment	8.6	17.2	57	0.86	[91]
	PET/Ag-mesh/PH1000/PEDOT:PSS/ Perovskite/PCBM/Al	Auxiliary electrode	14	19.5	80	0.91	[25]
	PEN/Graphene-Mo/PEDOT:PSS/MAPbI₃/C₆₀/BCP/LiF/Al	—	16.80	21.7	80	1.0	[27]
	PEN/ITO/PEDOT:PSS/MAPbI₃/C₆₀/BCP/LiF/Al	Metal oxide doping	17.30	21.5	83.0	0.97	[27]

表2. PEDOT:PSS应用在PSCs器件的光伏性能参数

Table 2. Photovoltaic performance parameters of PEDOT:PSS applied in PSCs devices

图3. 提升PEDOT:PSS电导率的策略. (a) PEDOT:PSS薄膜的构象重排示意图[73]. (b) 酸改性后PEDOT:PSS的构象重排示意图[69]. (c) 不同溶剂修饰提升PEDOT:PSS薄膜的电导率[74]

Figure 3. Various strategies for improving PEDOT:PSS conductivity. (a) Schematic diagram of conformation rearrangement of PEDOT:PSS films[73]. (b) Schematic diagram of conformation rearrangement of PEDOT:PSS after acid modification[69]. (c) The different solvents treatments to improve the conductivity of PEDOT:PSS films[74]

图4. 提高PEDOT:PSS薄膜机械柔韧性的策略. (a) 软聚合物掺杂提高PEDOT:PSS薄膜力学和电学性能[75]. (b) Zonyl FS-300掺杂改善PEDOT:PSS薄膜力学性能[76]. (c) 制备Ag-PEDOT:PSS复合电极的示意图[77]. (d) 制作MWCNT/PEDOT:PSS复合薄膜的流程图[78]

Figure 4. The strategies for improving mechanical flexibility of PEDOT:PSS film. (a) Soft polymer doping improves the mechanical and electrical properties of PEDOT:PSS films[75]. (b) Zonyl FS-300 doping improves the mechanical properties of PEDOT:PSS films[76]. (c) The schematic diagram of fabrication PEDOT:PSS composite electrode[77]. (d) The flow diagram of MWCNT/PEDOT:PSS composite film[78]

图5. PEDOT:PSS作为透明电极应用于柔性薄膜太阳电池. (a) PEDOT:PSS作为透明电极改善了可拉伸PSCs力学性能[32]. (b)改性PEDOT:PSS薄膜的构象发生了改善[84]. (c)改性PEDOT:PSS透明电极的力学性能得到提高[85]

Figure 5. PEDOT:PSS is employed as transparent electrode in flexible film solar cells. (a) PEDOT:PSS as a transparent electrode improves the mechanical properties of stretchable PSCs[32]. (b) The conformation of PEDOT:PSS films has been improved after modification[84]. (c) The mechanical properties of PEDOT:PSS transparent electrode are improved by modification[85]

图6. PEDOT:PSS作为界面层应用于柔性薄膜太阳电池. (a) 石墨烯衬底的柔性PSCs图像[27]. (b) 钙钛矿应力释放示意图[98]. (c) 柔性OSCs的器件结构以及能级分布[103]; (d) 柔性OSCs的结构及性能[106]

Figure 6. PEDOT:PSS is employed as the interface layer for flexible solar cells. (a) The schematic diagram of flexible PSCs based on graphene substrates[27]. (b) Schematic diagram of perovskite stress release[98]. (c) The devices structure and the energy band diagram of flexible OSCs[103]. (d) The structure and performance of flexible OSCs[106]

PEDOT:PSS	Device structure	Scheme	PCE/%	J_SC/ (mA•cm^-2)	FF/%	V_OC/V	Reference
Transparency electrode	PET/Ag-grid/PEDOT:PSS(PH1000)/ PTB7:PC₇₁BM/LiF/Al	Hybrid electrode	5.85	13.7	61	0.7	[16]
	PET/Ag-grid/PEDOT:PSS(PH1000)/ZnO/ PFN/Active layer/MoO₃/Ag	Acid treatment	6.01	13.9	60	0.72	[16]
	PEN/H₂SO₄-PEDOT:PSS(PH1000)/ PTB7-Th:PC₇₁BM/Ca/Al	Solvent doping	7.6	14.2	69	0.77	[70]
	PEN/PEI/Ag/PEDOT:PSS(PH1000)/ PTB7-Th:PC₇₁BM/MoO₃/Ag	Anti-reflection layer	9.9	16.9	74	0.79	[21]
Hole transport layer	PET/Ag-mesh/H-PEDOT:PSS/PEDOT:PSS/ PTB7:PC₇₁BM/TiO _x/Al	Hybrid electrode	6.94	14.2	67.1	0.73	[85]
	PET/Ag-grid/PH1000/ZnO/PTB7-Th:PC₇₁BM/MoO₃/Al	Auxiliary electrode	6.58	14.3	59	0.78	[16]
	PET/Acid-PH1000/PEDOT:PSS/P3HT:PCBM/Ca/Al	Acid treatment	3.92	10.2	65	0.595	[68]
	PET/Acid-PH1000/PEDOT:PSS/ PBDB-T:IT-M/Ca/Al	Acid treatment	10.12	15.5	70.3	0.93	[103]
	PET/PH1000/PEDOT:PSS/Active layer/ PDINO/Al	—	14.06	23.57	72.0	0.83	[106]
	PET/Ag-mesh/PH1000/PEDOT:PSS/ Photoactive layer/PDINO/Ag	—	10.20	20.48	67.5	0.74	[17]

表3. PEDOT:PSS应用在OSCs器件的光伏性能参数

Table 3. Photovoltaic performance parameters of PEDOT:PSS applied in OSCs devices

图7. PEDOT:PSS在其他柔性器件中的应用. (a) 有机热电(MFSOTE)矩阵性能表征示意图[114]. (b) MoS2纳米管上附着多孔PEDOT网络[117]. (c) CNT/MnO2/PEDOT (CMOP)复合阴极的制备和器件性能示意图[118]

Figure 7. Application of PEDOT:PSS in other flexible devices. (a) Schematic diagram of matrix performance characterization of organic thermoelectric (MFSOTE)[114]. (b) MoS2 nanotubes are attached to the porous PEDOT network[117]. (c) The schematic diagram of CNT/MnO2/PEDOT (CMOP) combined cathode fabrication and device performance[118]

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PEDOT导电高分子在柔性能量转化与存储器件的研究进展

Recent Advances of PEDOT in Flexible Energy Conversion and Storage Devices

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