羟基功能化分子工程消除二维相壁垒实现高效宽带隙及全钙钛矿叠层太阳能电池

引用本文: 刘彬彬, 陈杨, 贾天赐, 陈辰, 吴章豪, 刘毓辉, 翟宇航, 马天舒, 王长擂. 羟基功能化分子工程消除二维相壁垒实现高效宽带隙及全钙钛矿叠层太阳能电池[J]. 物理化学学报, 2026, 42(1): 100128. doi: 10.1016/j.actphy.2025.100128 shu

Citation: Binbin Liu, Yang Chen, Tianci Jia, Chen Chen, Zhanghao Wu, Yuhui Liu, Yuhang Zhai, Tianshu Ma, Changlei Wang. Hydroxyl-functionalized molecular engineering mitigates 2D phase barriers for efficient wide-bandgap and all-perovskite tandem solar cells[J]. Acta Physico-Chimica Sinica, 2026, 42(1): 100128. doi: 10.1016/j.actphy.2025.100128 shu

羟基功能化分子工程消除二维相壁垒实现高效宽带隙及全钙钛矿叠层太阳能电池

苏州大学光电科学与工程学院, 苏州纳米科技协同创新中心, 江苏省先进光学制造技术重点实验室, 教育部现代光学技术重点实验室, 江苏苏州 215006

通讯作者: 马天舒，Emails:tsma@suda.edu.cn; 王长擂，Emails:cl.wang@suda.edu.cn

基金项目:
国家自然科学基金(62005188)，江苏省高校自然科学研究项目(22KJA480003)，唐仲英基金会，国家资助博士后研究人员计划(GZB20240516)，苏州大学大学生创新创业训练计划(202310285029Z)资助

摘要: 全钙钛矿叠层太阳能电池展现出突破单结器件效率极限的潜力，通过最大化利用太阳光谱和减少热弛豫损失，其理论转换效率可超过44%。宽带隙钙钛矿太阳能电池(WBG PSCs)是叠层光伏技术的核心元件，其性能在过去十年取得飞速进展。然而，这类器件仍然面临着严重的开路电压(V_OC)损失问题，主要归因于界面复合损失和载流子传输损耗，其中关键诱因是在表面钝化过程中形成的绝缘性二维(2D)钙钛矿相。因此，本文引入多功能分子添加剂4-羟基苯乙基碘化铵(p-OHPEAI)，以解决高电压和高效电荷提取之间的核心矛盾。不同于传统的苯乙基碘化铵(PEAI)处理会形成绝缘二维相并因其分子垂直取向导致反向内建电场(阻碍电荷输运)，p-OHPEAI通过氨基(–NH₃)和羟基(–OH)的协同作用，实现了分子在钙钛矿表面的平行吸附构型。这种构型有效抑制了绝缘二维相的形成，同时钝化了配位不足的卤素离子和铅空位缺陷，显著降低非辐射复合。此外，p-OHPEAI的分子极性会在钙钛矿层/电子传输层界面诱导产生内建偶极矩，优化了能级匹配并加速了电子提取过程。将p-OHPEAI应用于1.77 eV宽带隙钙钛矿太阳能电池，器件的开路电压达到1.344 V，相应的开路电压损失仅为0.426 V，在已经报道的1.75–1.80 eV带隙范围内的反式结构器件中处于领先水平。优化后的器件光电转换效率(PCE)达到19.24%，显著优于PEAI钝化器件。将该策略应用于全钙钛矿叠层太阳能电池(TSCs)，实现了28.50%的冠军效率(认证效率为28.19%)。同时，叠层器件展现出优异的运行稳定性，在350 h持续光照后仍能保持90%以上的初始效率，充分验证了羟基钝化策略的可靠性。本研究通过在钝化分子中引入羟基官能团，开发了一种兼具缺陷钝化与电荷传输保障的普适性策略，成功解决了钙钛矿电池高电压与高效载流子提取之间的矛盾。

关键词:

English

Hydroxyl-functionalized molecular engineering mitigates 2D phase barriers for efficient wide-bandgap and all-perovskite tandem solar cells

School of Optoelectronic Science and Engineering, Collaborative Innovation Center of Suzhou Nano Science and Technology, Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province, Key Lab of Modern Optical Technologies of Education Ministry of China, Soochow University, Suzhou 215006, Jiangsu Province, China

Corresponding author: Tianshu Ma, ; Changlei Wang,

Received Date: 19 April 2025
Revised Date: 11 June 2025
Available Online: 03 July 2025

Abstract: All-perovskite tandem solar cells (TSCs) demonstrate exceptional potential to overcome the single-junction efficiency limit through enhanced photon harvesting across the solar spectrum and suppressed thermalization effects, achieving theoretical power conversion efficiencies surpassing 44%. Wide-bandgap perovskites solar cells (WBG PSCs) are crucial for tandem photovoltaics, and have witnessed exponential progress during the last decade. However, these devices suffer from severe open-circuit voltage (V_OC) deficits, primarily due to interfacial recombination and carrier transport losses. A major contributor to these losses is the uncontrolled formation of insulating two-dimensional (2D) perovskite phases during surface passivation. Here, we introduce 4-hydroxyphenylethyl ammonium iodide (p-OHPEAI) as a multifunctional molecular additive to address this critical trade-off. Unlike conventional phenethyl ammonium iodide (PEAI), which forms the insulating 2D phase and the invert electric field by vertical molecular orientation that impedes charge extraction, the hydroxyl group (–OH) in p-OHPEAI enables parallel molecular adsorption on perovskite surfaces via synergistic interactions between amino (–NH₃) and –OH groups. This configuration effectively eliminates the formation of insulating 2D perovskite phase, passivates undercoordinated halide and lead vacancies, reducing non-radiative recombination. Additionally, the polarity of p-OHPEAI generates a dipole moment at the perovskite/electron transport layer (ETL) interface, optimizing energy-level alignment and facilitating electron extraction. By incorporating p-OHPEAI into 1.77 eV WBG PSCs, we achieved a remarkable V_OC of 1.344 V, corresponding to a minimal voltage deficit of 0.426 V, which is among the lowest reported V_OC-deficit values for the inverted WBG PSCs with bandgaps ranging from 1.75 to 1.80 eV. The optimized device delivered a power conversion efficiency (PCE) of 19.24%, demonstrating superior performance compared to conventional PEAI-passivated cells. When integrated into all-perovskite TSCs, this strategy enabled a champion PCE of 28.50% (with a certified efficiency of 28.19%). Furthermore, the devices exhibited excellent operational stability, maintaining over 90% of their initial efficiency after 350 h of continuous illumination, highlighting the robustness of the hydroxyl-driven passivation approach. The introduction of hydroxyl groups in passivation molecules provides a versatile strategy to balance defect suppression and charge transport, bridging the gap between high voltage and efficient carrier extraction.

Key words:

Wide-bandgap perovskite solar cell
/ All-perovskite tandem solar cell; Open-circuit voltage deficit
/ Energy alignment
/ Charge transport

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沈阳化工大学材料科学与工程学院沈阳 110142

羟基功能化分子工程消除二维相壁垒实现高效宽带隙及全钙钛矿叠层太阳能电池

通讯作者: 马天舒，Emails:tsma@suda.edu.cn; 王长擂，Emails:cl.wang@suda.edu.cn

English

Hydroxyl-functionalized molecular engineering mitigates 2D phase barriers for efficient wide-bandgap and all-perovskite tandem solar cells

Corresponding author: Tianshu Ma, ; Changlei Wang,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

羟基功能化分子工程消除二维相壁垒实现高效宽带隙及全钙钛矿叠层太阳能电池

通讯作者: 马天舒，Emails:tsma@suda.edu.cn; 王长擂，Emails:cl.wang@suda.edu.cn

English

Hydroxyl-functionalized molecular engineering mitigates 2D phase barriers for efficient wide-bandgap and all-perovskite tandem solar cells

Corresponding author: Tianshu Ma, ; Changlei Wang,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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