题目：Multi-Physics Mechanisms and Regulation of Perovskite Grain Boundaries: Insights into Carrier Dynamics, Ion Migration, Thermodynamics, and Thermal Stress
作者：Luolei Shi,ab Xirui Liu,c Yuqi Zhang,ab Yining Bao,ab Tianshu Ma,ab Linling Qin,ab Guoyang Cao,*ab Changlei Wang,ab Chuanxiao Xiao,*c Xiaofeng Li,*ab and Zhenhai Yang*ab
单位：
a. School of Optoelectronic Science and Engineering & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006, China
b.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, China
c. Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315000, China
Abstract: Grain boundaries (GBs), inherent in polycrystalline perovskite films and associated with numerous trap states, are widely regarded as non-radiative recombination centers that degrade the performance of perovskite solar cells (PSCs). Current research on GBs is limited to carrier dynamics, which, however, lacks a comprehensive multi-physics perspective encompassing thermal generation/transport/dissipation and internal-stress formation/accumulation in GB-containing PSCs. Herein, we systematically elucidate the multi-physics mechanisms of GBs by integrating carrier-transport, ion-migration, thermodynamics, and thermal-stress analyses through opto-electro-thermal-stress coupled simulations and well-designed experiments. Notably, electrical simulation results reveal that the reason why GBs generally degrade device performance can be attributed to their beneficial role in carrier transport being surpassed by carrier recombination losses. Additionally, GB-containing PSCs exhibit distinct ion dynamic behavior, with ions accumulating preferentially at GBs or within perovskite grains, further compromising PSC efficiency and stability. More importantly, we demonstrate that filling or passivating GBs and surface GB grooves with wide-bandgap materials effectively mitigates performance degradation. Thermal-stress simulations further show that GB-containing PSCs generate more heat than their GB-free counterparts, leading to elevated device operating temperatures, localized thermal-stress accumulation at GBs, and accelerated performance degradation. Experimental results confirm that passivating GBs with suitable materials simultaneously alleviates thermal conductivity inhomogeneity and thermal-stress accumulation, offering new insights into the multi-physics mechanisms of GB-containing PSCs.
摘要：晶界作为多晶钙钛矿薄膜的关键固有特征，因其丰富的缺陷态被普遍视为非辐射复合中心，严重限制钙钛矿太阳能电池的性能。当前针对晶界的研究多局限于载流子动力学层面，然而在实际包含晶界的钙钛矿太阳能电池中，热的生成/传导/耗散与内应力的形成/累积等多物理场耦合作用机制尚未得到系统性阐释。本研究通过构建光-电-热-应力多物理场耦合仿真模型并开展实验验证，结合载流子输运、离子迁移、热力学及热应力多维度分析，首次揭示了晶界的多物理耦合机制。电学模拟结果表明：晶界对器件性能的负面影响主要源于载流子复合损耗，在多数情况下，这种负面影响会显著大于其对载流子输运的促进效应。此外，包含晶界的器件呈现独特的离子动力学行为，离子会优先在晶界或晶粒内部聚集，进一步加剧器件效率与稳定性的衰退。研究还发现：采用宽带隙材料填充或钝化晶界及其表面沟槽可显著抑制由此引发的性能衰退。热-应力仿真进一步揭示：相较于无晶界体系，含晶界的钙钛矿太阳能电池因产热加剧导致器件工作温度显著升高，且热应力在晶界处呈现局部聚集特征，进而加速性能衰减。实验数据证实：选择合适材料进行晶界钝化可同时改善热导率分布非均匀性与热应力聚集现象，为理解含晶界钙钛矿电池的多物理场协同作用机制提供了新视角。
影响因子：32.4
链接：//pubs.rsc.org/en/content/articlelanding/2025/ee/d5ee02240a