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Unraveling the Formation Mechanisms of Highly Oriented Tin Perovskite with a 3D-over-2D Heterostructure
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-09-03 , DOI: 10.1021/acsenergylett.4c01725 Yuanze Xu 1 , Juno Kim 2 , Shripathi Ramakrishnan 1 , Taiyi Chen 1 , Xiaoyu Zhang 1 , Yugang Zhang 3 , Andrew J. Musser 2 , Qiuming Yu 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-09-03 , DOI: 10.1021/acsenergylett.4c01725 Yuanze Xu 1 , Juno Kim 2 , Shripathi Ramakrishnan 1 , Taiyi Chen 1 , Xiaoyu Zhang 1 , Yugang Zhang 3 , Andrew J. Musser 2 , Qiuming Yu 1
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Tin-based perovskites (TinPVKs) have become the most promising candidates for lead-free perovskite solar cells, owing to its low toxicity and improved photovoltaic performance. However, due to the absence of 4f shell, TinPVKs suffer from uncontrolled crystallization, limiting the power conversion efficiency (PCE) of tin perovskite solar cells (TinPSCs). Here, we systematically study the ligand regulated crystallization process of TinPVK. We find that with elongated spin time, TinPVK crystals undergo reorientation and lateral growth. 3D α-phase FASnI3 and 2D (n = 2) and 2D (n = 1) phases emerge sequentially to form a “3D-over-2D” heterostructure via a proposed “diffusion-propagation” mechanism. TinPSCs exhibit improved open circuit voltage (VOC) due to favorable energy level alignment of the 3D-over-2D heterostructure, with a champion PCE value of 13.07% and T80 value of over 1200 h. This work provides mechanistic insights on controlled crystallization and heterostructure formation of TinPVKs, paving the way toward high-efficiency TinPSCs.
中文翻译：
揭示具有 3D-over-2D 异质结构的高取向锡钙钛矿的形成机制
锡基钙钛矿（TinPVK）因其低毒性和改进的光伏性能而成为无铅钙钛矿太阳能电池最有前途的候选者。然而，由于缺乏4f壳，TinPVK会出现不受控制的结晶，限制了锡钙钛矿太阳能电池（TinPSC）的功率转换效率（PCE）。在这里，我们系统地研究了TinPVK的配体调控结晶过程。我们发现，随着旋转时间的延长，TinPVK 晶体会发生重新取向和横向生长。 3D α相 FASnI 3和 2D ( n = 2) 和 2D ( n = 1) 相依次出现，通过提出的“扩散传播”机制形成“3D-over-2D”异质结构。由于 3D-over-2D 异质结构的有利能级排列，TinPSC 表现出更高的开路电压 ( V OC )，冠军 PCE 值为 13.07%， T 80值超过 1200 h。这项工作提供了有关 TinPVK 的受控结晶和异质结构形成的机制见解，为高效 TinPSC 铺平了道路。
更新日期：2024-09-03
中文翻译：
揭示具有 3D-over-2D 异质结构的高取向锡钙钛矿的形成机制
锡基钙钛矿（TinPVK）因其低毒性和改进的光伏性能而成为无铅钙钛矿太阳能电池最有前途的候选者。然而，由于缺乏4f壳，TinPVK会出现不受控制的结晶，限制了锡钙钛矿太阳能电池（TinPSC）的功率转换效率（PCE）。在这里，我们系统地研究了TinPVK的配体调控结晶过程。我们发现，随着旋转时间的延长，TinPVK 晶体会发生重新取向和横向生长。 3D α相 FASnI 3和 2D ( n = 2) 和 2D ( n = 1) 相依次出现，通过提出的“扩散传播”机制形成“3D-over-2D”异质结构。由于 3D-over-2D 异质结构的有利能级排列，TinPSC 表现出更高的开路电压 ( V OC )，冠军 PCE 值为 13.07%， T 80值超过 1200 h。这项工作提供了有关 TinPVK 的受控结晶和异质结构形成的机制见解，为高效 TinPSC 铺平了道路。
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