染料敏化太阳能电池氧化还原电对

doi:10.16085/j.issn.1000-6613.2025-0633

化工进展 ›› 2025, Vol. 44 ›› Issue (S1): 350-367.DOI: 10.16085/j.issn.1000-6613.2025-0633

• 材料科学与技术 • 上一篇

染料敏化太阳能电池氧化还原电对

管思颖(), 问金月, 焦守政(), 郝雨薇, 孙志成

北京印刷学院印刷与包装工程学院，印刷电子工程技术研究中心，北京 102600

收稿日期:2025-04-29 修回日期:2025-08-29 出版日期:2025-10-25 发布日期:2025-11-24
通讯作者: 焦守政
作者简介:管思颖（1999—），女，硕士研究生，研究方向为印刷电子材料。E-mail：884676098@qq.com。
基金资助:
国家自然科学基金(22278037);国家自然科学基金(62371051);国家自然科学基金(61971049);国家自然科学基金(62211530446);北京市教育委员会科技研究计划(KM202310015005);北京市自然科学基金(2252034);材料科学与工程学科建设项目(21090124010);博士科研启动基金(27170124011);博士科研启动基金(20190225001);博士科研启动基金(Ed2025001);北京市高等教育学会项目(MS2022094)

Redox couple electrolyte in dye-sensitized solar cells

GUAN Siying(), WEN Jinyue, JIAO Shouzheng(), HAO Yuwei, SUN Zhicheng

Beijing Engineering Research Center of Printed Electronics, School of Printing and Packaging Engineering, Beijing Institute of Graphic Communication, Beijing 102600, China

Received:2025-04-29 Revised:2025-08-29 Online:2025-10-25 Published:2025-11-24
Contact: JIAO Shouzheng

摘要/Abstract

摘要：

回顾了染料敏化太阳能电池（DSSC）的发展与工作原理，介绍了电解液氧化还原电对在染料再生与其在电路闭合中的作用及其对开路电压（V_OC）、短路电流（J_SC）和填充因子（FF）的影响。本文阐述了能级匹配与动力学准则：以染料分子能级的“边界”与氧化还原电位、TiO₂导带位置解释再生与注入驱动力，结合介体扩散与对电极催化说明电流与填充因子来源。研究了近几年I⁻/I $3 -$ 、Co（Ⅱ）/Co（Ⅲ）、Cu（Ⅰ）/Cu（Ⅱ）、2,2,6,6-四甲基-1-哌啶氧化物（TEMPO）/TEMPO⁺、四甲基对苯二酚/苯醌（HQ/BQ）与Br $3 -$ /Br⁻等体系的电位区间、光谱自吸收、扩散黏度与稳定性。结果说明，非碘体系整体更有利于获得高V_oc与低自吸收，Cu/Co介体在低驱动力快速再生策略下的室内能量采集优势突出，进行比较后的优点体现在：可精确调控电位并兼顾扩散/选择性、与高活性对电极协同降低界面阻抗、在AM1.5G（光强1000W/m²）与1000lx条件下保持较高效率，最后对室内光伏DSSC在物联网（IoT）领域的可持续发展及应用进行了展望。

关键词: 染料敏化太阳能电池, 氧化还原电对, 非碘体系电解质, 室内光伏, 光电转换效率

Abstract:

This review surveyed the development and operating principles of dye-sensitized solar cells (DSSC), introduced the role of electrolyte redox couples in dye regeneration and electrochemical circuit closure, and analyzed their influence on the open-circuit voltage (V_OC), short-circuit current density (J_SC) and fill factor (FF). The energetic and kinetic design rules were elucidated, i.e., regeneration and injection driving forces were rationalized by aligning the dyes' frontier molecular orbitals with the redox potential and the TiO₂ conduction band, while current generation and FF were further governed by mediator diffusion and the catalytic activity of the counter electrode. The recent I⁻/I $3 -$ , Co(Ⅲ)/Co(Ⅱ), Cu(Ⅰ)/Cu(Ⅱ), TEMPO/TEMPO⁺, hydroquinone/benzoquinone (HQ/BQ) and Br₃⁻/Br⁻ systems were comparatively examined with respect to formal potential windows, visible-light self-absorption, diffusivity/viscosity and stability. The analysis showed that non-iodide mediators were, in general, more favorable for achieving higher V_OC with reduced spectral competition. Cu-based and Co-based shuttles operated under low-overpotential and fast-regeneration conditions exhibited pronounced advantages for indoor energy harvesting. Relative to iodide, the key merits included electronically tunable potentials with balanced diffusion/selectivity, synergistic compatibility with high-activity counter electrodes that lowered interfacial impedance and robust efficiencies under AM 1.5G and 1000lx illumination. Finally, the prospects of DSSC indoor photovoltaics for sustainable Internet-of-Things (IoT) power supplies were outlined.

Key words: dye-sensitized solar cells, redox couple, non-iodine-based electrolyte systems, indoor photovoltaics, photovoltaic conversion efficiency

中图分类号:

TM914.4

管思颖, 问金月, 焦守政, 郝雨薇, 孙志成. 染料敏化太阳能电池氧化还原电对[J]. 化工进展, 2025, 44(S1): 350-367.

GUAN Siying, WEN Jinyue, JIAO Shouzheng, HAO Yuwei, SUN Zhicheng. Redox couple electrolyte in dye-sensitized solar cells[J]. Chemical Industry and Engineering Progress, 2025, 44(S1): 350-367.

图/表 19

图1 部分代表性氧化还原电对的能级示意图

表1 Br3-/Br-氧化还原电对电解质在全光强下获得的光电转换效率

3 -

/Br^-

曙红Y

ADEKA-3

1.05

2.6

3.9

[27]

[29]

表1 Br3-/Br-氧化还原电对电解质在全光强下获得的光电转换效率

氧化还原电对

染料

氧化还原电位(vs. NHE)/V

效率/%

参考文献

3 -

/Br^-

曙红Y

ADEKA-3

1.05

2.6

3.9

[27]

[29]

DMBIBr/Br₂

TC306

1.10

5.2

[28]

表2 钴配合物电解质电池在全光强下获得的光电转换效率

ADEKA-1/LEG4

SA246

SA634

X73

Y123

0.62

14.30

9.4

8.2

8.1

11.3

[33]

[34]

[35]

[38]

[40]

C218

Y123

0.57

12.3

12.6

10.3

8.0

[31]

[36]

[37]

[39]

表3 铁配合物电解质电池在全光强下获得的光电转换效率

RR9

[三(2-苯基吡啶)铱2(4,4′-双(二乙基膦甲基)-2,2′-联吡啶)]PF₆

1.37

1.90

0.80

[43]

[45]

图2 敏化剂和铜配合物的能级图以及采用这些材料器件的光电流-电压特性[51]

图3 新DSSC架构示意图、敏化TiO2电极和基于PEDOT半导体对电极的DSSC在AM 1.5G条件下和1000lx室内光下的J-V特性曲线[9]

表4 铜配合物电解质电池在全光强下获得的光电转换效率

染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
N719 Y123 D35	0.93	1.4 10.3 7.5	[47] [49] [51]
Y123	0.97	10.3	[50]
Y123	0.9	10.3	[49]
LEG4	0.59	9.0	[48]
Y123 D35和XY1 WS-72 L350 XY1和L1 MS5和XY1b SL9和SL10	0.87	10.00 11.3；28.9（1000lx） 11.6 11.2；28.4（1000lx） 11.5；34（1000lx） 13.5；34.5（1000lx） 15.20	[49] [9] [52] [53] [6] [54] [4]

图4 DSSC中[VO(salen)]0/1+ ([VO]0/1+)电对的氧化还原介导过程[63]Φ—功函数；E1/2—半波电位；kex—电子交换速率常数；k0—标准电荷转移速率常数

图5 Ni(Ⅲ/Ⅳ)合成方案及N719敏化纳米TiO2薄膜和0.1mol/L 3Ni(Ⅱ/Ⅲ)的光吸收光谱[66]

表5 其他金属配合物电解质在全光强下获得的光电转换效率

染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
D205和D131	0.84	5.4	[63]
N719	0.58	2	[64]
MK2	0.49	4.4	[68]
Z907	1.20	2.62	[69]
Z907	0.49	1.48	[69]

表6 氮氧自由基类氧化还原电对电解质在全光强下获得的光电转换效率

D149

Y123

N719

Y123

0.80

5.4

3.9

6.0

2.1

[70]

[71]

[73]

[74]

表7 硫脲/过硫醚、巯盐/过硫醚氧化还原电对电解质在全光强下获得的光电转换效率

含三苯胺取代的六噻吩π-共轭染料/SQ2染料（PMI-6T-TPA/SQ2）

PP2-NDI

PMI-acac

0.49

1.33

2.27

0.098

[75]

[76]

[77]

表8 对苯二酚/对苯醌氧化还原电对电解质在全光强下获得的光电转换效率

染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
N719 CM309	0.50	8.4 6.2	[79] [80]
LEG4	0.95	1.3	[81]
LEG4	0.47	2.5	[81]
LEG4	0.58	2.0	[81]

表9 卤间化合物氧化还原电对电解质在全光强下获得的光电转换效率

氧化还原电对	染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
NMBI/[BuPy]IBr₂（NMBI为N-甲基苯并咪唑，BuPy为丁基咪唑）	N3	0.50	6.4	[85]
(I^-, Br^-)/(I $3 -$ , I₂Br^-)	N719	0.56	7.06	[86]

表9 卤间化合物氧化还原电对电解质在全光强下获得的光电转换效率

氧化还原电对	染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
NMBI/[BuPy]IBr₂（NMBI为N-甲基苯并咪唑，BuPy为丁基咪唑）	N3	0.50	6.4	[85]
(I^-, Br^-)/(I $3 -$ , I₂Br^-)	N719	0.56	7.06	[86]

图6 I-/(SeCN)2的性能优势[83]

表10 拟卤素氧化还原电对电解质在全光强下获得的光电转换效率

氧化还原电对	染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
SeCN^-/(SeCN) $3 -$	N3 Z907 Ru(deeb)(bpy)₂(PF₆)₂	0.50	20（IPCE） 7.5 0.65（IPCE）	[87] [88] [89]
SCN^-/(SCN) $3 -$	N3 Ru(deeb)(bpy)₂(PF₆)₂	0.77	4 0.51（IPCE）	[87] [83]
(I^-, SeCN^-)/(I $3 -$ , I₂SeCN^-)	N719	0.46	6.2	[89]
(I^-, SCN^-)/(I $3 -$ , I₂SCN^-)	N719	0.46	8.42和8.46	[89]

表10 拟卤素氧化还原电对电解质在全光强下获得的光电转换效率

氧化还原电对	染料	氧化还原电位(vs. NHE)/V	效率/%	参考文献
SeCN^-/(SeCN) $3 -$	N3 Z907 Ru(deeb)(bpy)₂(PF₆)₂	0.50	20（IPCE） 7.5 0.65（IPCE）	[87] [88] [89]
SCN^-/(SCN) $3 -$	N3 Ru(deeb)(bpy)₂(PF₆)₂	0.77	4 0.51（IPCE）	[87] [83]
(I^-, SeCN^-)/(I $3 -$ , I₂SeCN^-)	N719	0.46	6.2	[89]
(I^-, SCN^-)/(I $3 -$ , I₂SCN^-)	N719	0.46	8.42和8.46	[89]

图7 全印刷DSCC和传统DSSC的结构及全印刷DSSC的过程

图8 MXene/rGO三维插层结构的合成和DSSC效果的示意图

表11 目前染料敏化太阳能电池常见电解液氧化还原电对对比

氧化还原电对	氧化还原电位 (vs. NHE)/V	优点	局限	参考文献
I⁻/I $3 -$	0.35~0.4	再生快、工艺成熟	具有腐蚀性、可见区自吸收、V_oc受限，在室内光下表现逊于金属配合物	[20-24]
Co(Ⅱ/Ⅲ)联吡啶/菲咯啉	可调（0.55~0.9）	电位可设计、可降低自吸收、室内表现好	分子尺寸大、扩散慢、可能导致复合加剧，存在稳定性方面的问题	[32-40]
Cu(Ⅰ/Ⅱ)联吡啶	0.85~1.0	高V_oc、低驱动力再生可行、室内纪录保持者	配体稳定性与长时稳定性需要继续优化	[47-57]
TEMPO/TEMPO⁺	0.8~0.9	高V_oc、低驱动力再生	存在稳定性与挥发性问题、长期寿命待提高	[70-74]
HQ/BQ	0.5~1.0（取决于取代）	透明度高、低自吸收	存在长期稳定性与电极选择性问题	[79-81]
SeCN⁻/(SeCN) $3 -$ 、SCN⁻/(SCN) $3 -$	可调	可降低自吸收、部分条件下提升V_oc	体系选择性强、通用性与稳定性待验证	[87-89]

表11 目前染料敏化太阳能电池常见电解液氧化还原电对对比

氧化还原电对	氧化还原电位 (vs. NHE)/V	优点	局限	参考文献
I⁻/I $3 -$	0.35~0.4	再生快、工艺成熟	具有腐蚀性、可见区自吸收、V_oc受限，在室内光下表现逊于金属配合物	[20-24]
Co(Ⅱ/Ⅲ)联吡啶/菲咯啉	可调（0.55~0.9）	电位可设计、可降低自吸收、室内表现好	分子尺寸大、扩散慢、可能导致复合加剧，存在稳定性方面的问题	[32-40]
Cu(Ⅰ/Ⅱ)联吡啶	0.85~1.0	高V_oc、低驱动力再生可行、室内纪录保持者	配体稳定性与长时稳定性需要继续优化	[47-57]
TEMPO/TEMPO⁺	0.8~0.9	高V_oc、低驱动力再生	存在稳定性与挥发性问题、长期寿命待提高	[70-74]
HQ/BQ	0.5~1.0（取决于取代）	透明度高、低自吸收	存在长期稳定性与电极选择性问题	[79-81]
SeCN⁻/(SeCN) $3 -$ 、SCN⁻/(SCN) $3 -$	可调	可降低自吸收、部分条件下提升V_oc	体系选择性强、通用性与稳定性待验证	[87-89]

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染料敏化太阳能电池氧化还原电对

Redox couple electrolyte in dye-sensitized solar cells

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染料敏化太阳能电池氧化还原电对

Redox couple electrolyte in dye-sensitized solar cells​

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Redox couple electrolyte in dye-sensitized solar cells