低共熔溶剂固锂与4-叔丁基吡啶减量策略提升正式钙钛矿太阳能电池稳定性

doi:10.6023/A26030067

摘要/Abstract

正式钙钛矿太阳能电池(PSCs)凭借高效率、低成本优势在光伏领域具备广阔商业化前景, 但其空穴传输层(HTL)载流子传输效率有限与器件稳定性不足仍是制约产业化的关键问题. 传统4-叔丁基吡啶(tBP)/双三氟甲基磺酰亚胺锂(LiTFSI)掺杂体系存在tBP易挥发、Li⁺迁移等缺陷, 易引发界面劣化与性能衰减. 基于此, 本工作提出氯化胆碱-尿素-乙二醇组成的低共熔溶剂(DES)掺杂及tBP减量调控策略, 利用DES的氢键与配位作用, 实现固定Li⁺、界面缺陷钝化与载流子传输通道优化. 该策略使最优器件效率达21.15%, 暗态、热及湿度稳定性均显著提升, 25 ℃ N₂中1000 h存储效率保留97%(对照组88%), 85 ℃ N₂中T₈₀达120 h (对照组48 h), 30%~40%相对湿度空气中存储500 h后, 维持80%的初始效率(对照组60%), 为PSCs的HTL掺杂工程提供“低用量、高适配、长稳定”的有效策略.

关键词: 钙钛矿太阳能电池, Spiro-OMeTAD, 低共熔溶剂, 锂离子迁移, 稳定性

Conventional perovskite solar cells (PSCs) exhibit broad commercial prospects in the photovoltaic field due to their high power conversion efficiency (PCE) and low fabrication cost. However, the limited carrier transport efficiency of the hole transport layer (HTL) and insufficient long-term stability remain critical bottlenecks hindering their industrialization. The traditional doping system of 4-tert-butyl pyridine (tBP)/lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) has inherent drawbacks: tBP is volatile and Li⁺ tends to migrate, which easily induce interfacial degradation and device performance decay. Herein, we propose a doping strategy using a deep eutectic solvent (DES) composed of choline chloride (ChCl), urea, and ethylene glycol (EG) with a molar ratio of 1∶2∶1 at a concentration of 1 mg•mL⁻¹ into the Spiro-OMeTAD precursor solution to optimize the Spiro-OMeTAD-based HTL, combined with regulating the tBP/LiTFSI molar ratio to 2∶1 for tBP reduction. Driven by hydrogen bonding and coordination interactions, the DES achieves a synergistic mechanism of “lithium immobilization-defect passivation-molecular network enhancement”: specifically, the carbonyl groups (C=O) of urea in DES coordinate with Li⁺ to suppress thermal-induced migration, the amino groups (-NH₂) form hydrogen bonds with TFSI^- to promote LiTFSI dissociation, and the hydroxyl groups (-OH) of EG assist in stabilizing the coordination network; meanwhile, DES molecules passivate uncoordinated Pb²⁺ on the perovskite surface to reduce non-radiative recombination, and enhance the π-π stacking of Spiro-OMeTAD to optimize carrier transport channels and increase its glass transition temperature (T_g) for improved thermal stability. Benefiting from this strategy, the fabricated conventional PSCs achieve a champion PCE of 21.15%. Moreover, the devices exhibit significantly improved long-term stability under various environmental conditions: 97% of the initial PCE is retained after 1000 h of dark storage at 25 ℃ in N₂ atmosphere (vs. 88% for the control device); the T₈₀ lifetime (time to retain 80% of the initial efficiency) reaches 120 h at 85 ℃ in N₂ atmosphere (vs. 48 h for the control device); and 80% of the initial PCE is maintained after 500 h of storage at 25 ℃ and 30%~40% relative humidity in air (vs. 60% for the control device). This work provides an effective “low-dose, high-compatibility, long-stability” strategy for HTL doping engineering, which is of great significance for promoting the industrialization of PSCs.

Key words: perovskite solar cells (PSCs), Spiro-OMeTAD, deep eutectic solvent (DES), Li⁺ migration, stability

引用此文

熊相明, 张林, 徐文军, 唐景航, 杨英. 低共熔溶剂固锂与4-叔丁基吡啶减量策略提升正式钙钛矿太阳能电池稳定性[J]. 化学学报, 2026, 84(6): 888-896.

Xiangming Xiong, Lin Zhang, Wenjun Xu, Jinghang Tang, Ying Yang. Deep Eutectic Solvent-Assisted Lithium Immobilization and 4-Tert -butyl pyridine-Less Regulation Strategy for Enhancing the Stability of Conventional Perovskite Solar Cells[J]. Acta Chimica Sinica, 2026, 84(6): 888-896.

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图/表 5

图1. 1 mg•mL−1 DES掺杂HTL的作用机制. (a) DES形成与Li+固定机制; (b) DES与LiTFSI的FT-IR光谱; (c) Li 1s的XPS能谱; (d) Pb 4f的XPS能谱; (e) 钙钛矿/HTL-Control的XRD图谱; (f) 钙钛矿/HTL-DES的XRD图谱; (g) PbI2峰与(001) FAPbI3峰的强度比(*: PbI2;▲:(001) FAPbI3)

Figure 1. Mechanism of HTL doped with 1 mg•mL−1 DES. (a) DES formation and Li+ immobilization mechanism; (b) FT-IR spectra of DES and LiTFSI; (c) XPS spectrum of Li 1s; (d) XPS spectrum of Pb 4f; (e) XRD pattern of PVK/HTL-Control; (f) XRD pattern of PVK/HTL-DES; (g) Intensity ratio of PbI2 peak to (001) FAPbI3 peak (*: PbI2; ▲: (001) FAPbI3)

图2. 1 mg•mL−1 DES 掺杂HTL的载流子传输性能. (a) t5Li10-DES、t10Li14-DES、t39Li23-DES及t39Li23在干燥空气中氧化18 h后的UV吸收光谱; (b) t5Li10-DES 在干燥空气中氧化72 h后的UV吸收光谱; (c) t5Li10-DES、t39Li23-DES及t39Li23在空气中氧化72 h后UV光谱在520 nm 处的吸收峰强度; (d) t5Li10-DES、t10Li14-DES、t39Li23-DES及t39Li23在干燥空气中氧化18 h后的电导率曲线; (e) 电导率对比; (f) HTL在空气氧化过程中的电导率变化; (g) 空穴迁移率测试曲线; (h) 空穴迁移率对比; (i) PL光谱

Figure 2. Carrier transport properties of HTL doped with 1 mg•mL−1 DES. (a) UV absorption spectra of t5Li10-DES, t10Li14-DES, t39Li23-DES and t39Li23 after 18 h oxidation in dry air; (b) UV absorption spectra of t5Li10-DES after 72 h oxidation in dry air; (c) Absorption peak intensity at 520 nm of UV absorption spectra of t5Li10-DES, t39Li23-DES and t39Li23 after 72 h oxidation in air; (d) Conductivity curves of t5Li10-DES, t10Li14-DES, t39Li23-DES and t39Li23 after 18 h oxidation in dry air; (e) Conductivity comparison; (f) Conductivity variation of HTL during oxidation in air; (g) Hole mobility test curves; (h) Hole mobility comparison; (i) PL spectra

图3. 不同掺杂比例HTL的热老化性能评估. (a) 空气氧化及85 ℃热老化前后的UV吸收光谱; (b) 空气氧化及85 ℃热老化前后电导率的变化; (c) 热老化前后空穴迁移率的变化; (d) 85 ℃热老化前后的XRD图谱; (e) FT-IR光谱; (f) 85 ℃热老化前后的 FT-IR 光谱; (g) DSC 曲线; (h) PVK/HTL在85 ℃热老化前后的PL光谱; (i) PVK/HTL在空气氧化及85 ℃热老化前后的UV吸收光谱

Figure 3. Evaluation of thermal aging performance of HTLs with different doping ratios. (a) UV absorption spectra before and after oxidation in air and thermal aging at 85 ℃; (b) Variation in conductivity before and after oxidation and thermal aging at 85 ℃; (c) Variation in hole mobility before and after thermal aging; (d) XRD patterns before and after thermal aging at 85 ℃; (e) FT-IR spectra; (f) FT-IR spectra before and after thermal aging at 85 ℃; (g) DSC curves; (h) PL spectra of PVK/HTL before and after thermal aging at 85 ℃; (i) UV absorption spectra of PVK/HTL before and after oxidation and thermal aging at 85 ℃

图4. 掺杂工程调控器件光伏性能的评估. (a) 器件结构; (b) 不同掺杂浓度下的器件效率; (c) 1 mg•mL−1 DES掺杂器件的效率分布直方图; (d) 1 mg•mL−1 DES掺杂及不同tBP/LiTFSI掺杂比例下的器件光伏性能; (e) 器件J-V曲线; (f) 稳态功率输出; (g) HTL中tBP/LiTFSI物质的量比与器件效率的关系

Figure 4. Evaluation of photovoltaic performance of devices regulated by doping engineering. (a) Device structure; (b) Device efficiency with different doping concentrations; (c) Efficiency distribution histogram of devices with 1 mg•mL−1 DES doping; (d) Photovoltaic performance of devices with 1 mg•mL−1 DES doping and different tBP/LiTFSI doping ratios; (e) Device J-V curves; (f) Steady-state power output (SPO); (g) Relationship between tBP/LiTFSI molar ratio in HTL and device efficiency variation

图5. 掺杂调控器件稳定性评估. (a) 25 ℃、N2中未封装器件的暗态稳定性; (b) 85 ℃、N2氛围下未封装器件的热稳定性; (c) 25 ℃、30%~40% RH空气中未封装器件的湿度稳定性; (d) 器件稳定性综合评估

Figure 5. Stability evaluation of devices regulated by doping engineering. (a) Dark-state stability of unpackaged devices under N2 atmosphere at 25 ℃; (b) Thermal stability of unpackaged devices under N2 atmosphere at 85 ℃; (c) Humidity stability of unpackaged devices under air atmosphere at 25 ℃ and 30%~40% RH; (d) Comprehensive evaluation of device stability performance

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