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

IF 30.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Luolei Shi, Xirui Liu, Yuqi Zhang, Yining Bao, Tianshu Ma, Linling Qin, Guoyang Cao, Changlei Wang, Chuanxiao Xiao, Xiaofeng Li and Zhenhai Yang
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引用次数: 0

摘要

多晶钙钛矿薄膜中固有的晶界(GBs)与许多陷阱态相关,被广泛认为是降低钙钛矿太阳能电池(PSCs)性能的非辐射复合中心。目前对gb - psc的研究仅限于载流子动力学,缺乏全面的多物理场视角,包括含gb - psc的热生成/输运/耗散和内应力形成/积累。在此,我们通过光电-电热-应力耦合模拟和精心设计的实验,通过整合载流子输运、离子迁移、热力学和热应力分析,系统地阐明了GBs的多物理机制。值得注意的是,电学模拟结果表明,gb通常会降低器件性能的原因可归因于它们在载流子传输中的有益作用被载流子重组损失所取代。此外,含gb的PSC表现出不同的离子动力学行为,离子优先积聚在gb或钙钛矿颗粒内,进一步影响PSC的效率和稳定性。更重要的是,我们证明了用宽带隙材料填充或钝化GB和表面GB凹槽有效地减轻了性能下降。热应力模拟进一步表明,含gb的psc比不含gb的psc产生更多的热量,导致器件工作温度升高,在gb处局部热应力积累,并加速性能下降。实验结果证实,用合适的材料钝化gb,同时缓解了导热性不均匀性和热应力积累,为研究含gb psc的多物理场机制提供了新的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Multi-physics mechanisms and regulation of perovskite grain boundaries: insights into carrier dynamics, ion migration, thermodynamics, and thermal stress†

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.

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来源期刊
Energy & Environmental Science
Energy & Environmental Science 化学-工程:化工
CiteScore
50.50
自引率
2.20%
发文量
349
审稿时长
2.2 months
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).
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