Substitution of lead with tin suppresses ionic transport in halide perovskite optoelectronics.
Substitution of lead with tin suppresses ionic transport in halide perovskite optoelectronics.
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DOI：
10.1039/d3ee03772j
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发表时间：
2024-01-23
影响因子：
32.5
通讯作者：
Stranks, Samuel D.
中科院分区：
文献类型：
--
作者：
Dey, Krishanu;Ghosh, Dibyajyoti;Pilot, Matthew;Pering, Samuel R.;Roose, Bart;Deswal, Priyanka;Senanayak, Satyaprasad P.;Cameron, Petra J.;Islam, M. Saiful;Stranks, Samuel D.
尽管具有垂直电荷传输的各种钙钛矿光电子器件的性能快速上升，但离子迁移的影响仍然是限制卤化铅钙钛矿器件的长期操作稳定性的常见且长期存在的阿喀琉斯之踵。然而，锡（Sn）取代对铅（Pb）卤化物钙钛矿的离子动力学的影响的理解仍然有限。在这里，我们采用扫描速率相关的电流-电压测量铅和混合铅-锡钙钛矿太阳能电池显示，短路电流损失在较低的扫描速率，这可以追溯到存在的移动的离子，存在于两种钙钛矿。为了了解离子迁移的动力学，我们进行了扫描速率相关的滞后分析和温度相关的阻抗谱测量，这表明抑制离子迁移的Pb-Sn设备相比，他们的Pb-唯一的类似物。通过将这些实验观察结果与混合Pb-Sn钙钛矿的第一性原理计算相联系，我们揭示了Sn空位在增加碘离子迁移势垒中所起的关键作用，这是由于局部结构扭曲。这些结果突出了Sn取代在减轻卤化物钙钛矿中不期望的离子迁移方面的有益效果，对未来的器件开发具有潜在的影响。移动的离子导致卤化铅钙钛矿装置的装置性能和稳定性两者的劣化。这项研究提供了直接的证据，在含锡的钙钛矿组合物中的离子迁移效应的实质性抑制。
Despite the rapid rise in the performance of a variety of perovskite optoelectronic devices with vertical charge transport, the effects of ion migration remain a common and longstanding Achilles’ heel limiting the long-term operational stability of lead halide perovskite devices. However, there is still limited understanding of the impact of tin (Sn) substitution on the ion dynamics of lead (Pb) halide perovskites. Here, we employ scan-rate-dependent current–voltage measurements on Pb and mixed Pb–Sn perovskite solar cells to show that short circuit current losses at lower scan rates, which can be traced to the presence of mobile ions, are present in both kinds of perovskites. To understand the kinetics of ion migration, we carry out scan-rate-dependent hysteresis analyses and temperature-dependent impedance spectroscopy measurements, which demonstrate suppressed ion migration in Pb–Sn devices compared to their Pb-only analogues. By linking these experimental observations to first-principles calculations on mixed Pb–Sn perovskites, we reveal the key role played by Sn vacancies in increasing the iodide ion migration barrier due to local structural distortions. These results highlight the beneficial effect of Sn substitution in mitigating undesirable ion migration in halide perovskites, with potential implications for future device development. Mobile ions cause deterioration in both device performance and stability of lead halide perovskite devices. This study provides direct evidence for substantial suppression of ionic migration effects in tin-containing perovskite compositions.
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影响因子：
44.1
作者：
Freysoldt, Christoph;Grabowski, Blazej;Van de Walle, Chris G.
通讯作者：
Van de Walle, Chris G.
影响因子：
11.5
作者：
Cao, H.;Zhang, Z.;Wang, M.
通讯作者：
Wang, M.
影响因子：
16.6
作者：
Eames, Christopher;Frost, Jarvist M.;Barnes, Piers R. F.;O'Regan, Brian C.;Walsh, Aron;Islam, M. Saiful
通讯作者：
Islam, M. Saiful
影响因子：
16.6
作者：
Bi C;Wang Q;Shao Y;Yuan Y;Xiao Z;Huang J
通讯作者：
Huang J
影响因子：
29.4
作者：
Dey, Krishanu;Roose, Bart;Stranks, Samuel D.
通讯作者：
Stranks, Samuel D.