Luolei Shi, Xirui Liu, Yuqi Zhang, Yining Bao, Tianshu Ma, Linling Qin, Guoyang Cao, Changlei Wang, Chuanxiao Xiao, Xiaofeng Li and Zhenhai Yang
{"title":"钙钛矿晶界的多物理机制和调控:载流子动力学、离子迁移、热力学和热应力的见解","authors":"Luolei Shi, Xirui Liu, Yuqi Zhang, Yining Bao, Tianshu Ma, Linling Qin, Guoyang Cao, Changlei Wang, Chuanxiao Xiao, Xiaofeng Li and Zhenhai Yang","doi":"10.1039/D5EE02240A","DOIUrl":null,"url":null,"abstract":"<p >Grain boundaries (GBs), inherent in polycrystalline perovskite films and associated with numerous trap states, are widely regarded as non-radiative recombination centres 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 behaviour, 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.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 14","pages":" 7291-7301"},"PeriodicalIF":30.8000,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Multi-physics mechanisms and regulation of perovskite grain boundaries: insights into carrier dynamics, ion migration, thermodynamics, and thermal stress†\",\"authors\":\"Luolei Shi, Xirui Liu, Yuqi Zhang, Yining Bao, Tianshu Ma, Linling Qin, Guoyang Cao, Changlei Wang, Chuanxiao Xiao, Xiaofeng Li and Zhenhai Yang\",\"doi\":\"10.1039/D5EE02240A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Grain boundaries (GBs), inherent in polycrystalline perovskite films and associated with numerous trap states, are widely regarded as non-radiative recombination centres 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 behaviour, 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. 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Multi-physics mechanisms and regulation of perovskite grain boundaries: insights into carrier dynamics, ion migration, thermodynamics, and thermal stress†
Grain boundaries (GBs), inherent in polycrystalline perovskite films and associated with numerous trap states, are widely regarded as non-radiative recombination centres 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 behaviour, 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.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).