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Tailoring Phase Purity in the 2D/3D Perovskite Heterostructures Using Lattice Mismatch
ACS Energy Letters ( IF 19.3 ) Pub Date : 2022-01-04 , DOI: 10.1021/acsenergylett.1c02580 Min Xiong 1 , Wenjun Zou 1 , Ke Fan 2 , Chaochao Qin 3 , Sibo Li 1 , Linfeng Fei 1 , Jizhong Jiang 4 , Haitao Huang 2 , Liang Shen 4 , Feng Gao 5 , Alex K.-Y. Jen 6 , Kai Yao 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2022-01-04 , DOI: 10.1021/acsenergylett.1c02580 Min Xiong 1 , Wenjun Zou 1 , Ke Fan 2 , Chaochao Qin 3 , Sibo Li 1 , Linfeng Fei 1 , Jizhong Jiang 4 , Haitao Huang 2 , Liang Shen 4 , Feng Gao 5 , Alex K.-Y. Jen 6 , Kai Yao 1
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Although the fabrication of two-dimensional (2D)/three-dimensional (3D) halide perovskite heterostructures has been employed to balance the long-term stability and high efficiency of perovskite solar cells, the formation of metastable quasi-2D perovskites remains the most serious challenge. Here, we demonstrate that large lattice mismatch derived from halide and cation differences between 2D and 3D perovskites are key to avoiding the formation of unintended 2D phases in the preparation of 2D/3D bulk heterostructure because the phase transformation becomes less thermodynamically favorable. Specifically, by employing chloride 2D perovskite (PYA)2PbCl4 (PYA = propargylammonium) crystals into a 3D precursor solution, we achieve a phase-pure 2D/3D heterojunction with clean type-I band alignment, which exhibits greatly reduced charge recombination. Furthermore, the incorporation of alkyne perovskites is also shown to suppress iodine diffusion and formation due to their exceptional iodine capture capacity. The resultant 2D/3D heterostructured devices exhibited enhanced efficiencies and stabilities compared with their 3D counterparts.
中文翻译：
使用晶格失配调整 2D/3D 钙钛矿异质结构中的相纯度
尽管已经采用二维（2D）/三维（3D）卤化物钙钛矿异质结构来平衡钙钛矿太阳能电池的长期稳定性和高效率，但亚稳态准二维钙钛矿的形成仍然是最严重的挑战。在这里，我们证明了由 2D 和 3D 钙钛矿之间的卤化物和阳离子差异引起的大晶格失配是避免在 2D/3D 体异质结构制备过程中形成意外 2D 相的关键，因为相变在热力学上变得不太有利。具体来说，通过采用氯化物 2D 钙钛矿 (PYA) 2 PbCl 4（PYA = 炔丙基铵）晶体进入 3D 前体溶液，我们实现了具有干净的 I 型能带排列的相纯 2D/3D 异质结，其表现出电荷复合大大减少。此外，由于其出色的碘捕获能力，炔烃钙钛矿的掺入也显示出抑制碘的扩散和形成。与 3D 对应物相比，所得 2D/3D 异质结构器件表现出更高的效率和稳定性。
更新日期：2022-01-14
中文翻译：
使用晶格失配调整 2D/3D 钙钛矿异质结构中的相纯度
尽管已经采用二维（2D）/三维（3D）卤化物钙钛矿异质结构来平衡钙钛矿太阳能电池的长期稳定性和高效率，但亚稳态准二维钙钛矿的形成仍然是最严重的挑战。在这里，我们证明了由 2D 和 3D 钙钛矿之间的卤化物和阳离子差异引起的大晶格失配是避免在 2D/3D 体异质结构制备过程中形成意外 2D 相的关键，因为相变在热力学上变得不太有利。具体来说，通过采用氯化物 2D 钙钛矿 (PYA) 2 PbCl 4（PYA = 炔丙基铵）晶体进入 3D 前体溶液，我们实现了具有干净的 I 型能带排列的相纯 2D/3D 异质结，其表现出电荷复合大大减少。此外，由于其出色的碘捕获能力，炔烃钙钛矿的掺入也显示出抑制碘的扩散和形成。与 3D 对应物相比，所得 2D/3D 异质结构器件表现出更高的效率和稳定性。
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