Interface engineering resulting in good contact, enhanced transport capability, and matched energy levels is indispensable and critical for the development of high-performance planar perovskite solar cells (PSCs). Here, we report an excellent electron-transporting layer (ETL) that can simultaneously enhance the stability and efficiency of n-i-p planar PSCs. Large π-conjugated graphdiyne (GD) was introduced into cross-linkable fullerene [6,6]-phenyl-C61-butyric styryl dendron ester (PCBSD) to improve the film orientation. Raman spectroscopy and 2D grazing incidence X-ray diffraction (GIXRD) measurements revealed that a strong π–π stacking interaction occurred between GD and cross-linkable PCBSD (C-PCBSD), generating a face-on stacked composite film. The orientated C-PCBSD:GD films was favorable for the growth and crystallization of the subsequent perovskite films and provided the merits of superior electron mobility, efficient charge extraction and energy-level tailoring. In addition, the thermally annealed C-PCBSD:GD film provided an adhesive film network with sufficient solvent resistance. Consequently, the perovskite devices delivered a power conversion efficiency of 20.19% with obviously improved cell stability. This indicates a potential application of GD-modified cross-linkable fullerene as an ETL in n-i-p structure PSCs. The finding opens a new route to deposit the fullerene films with ordered orientation by 2D materials with large π-conjugation, and thus to control the subsequent perovskite crystallization.

界面工程带来良好的接触，增强的运输能力以及相匹配的能级是必不可少的，对于开发高性能平面钙钛矿太阳能电池（PSC）至关重要。在这里，我们报告了一个出色的电子传输层（ETL），它可以同时提高压区平面PSC的稳定性和效率。将大的π共轭石墨二炔（GD）引入可交联的富勒烯[6,6]-苯基-C61-丁苯乙烯基树枝状酯（PCBSD）中以改善薄膜取向。拉曼光谱和2D掠入射X射线衍射（GIXRD）测量表明，GD与可交联PCBSD（C-PCBSD）之间发生了强烈的π-π堆叠相互作用，从而产生了面朝上堆叠的复合膜。定向的C-PCBSD：GD膜有利于后续钙钛矿膜的生长和结晶，并具有优异的电子迁移率，有效的电荷提取和能级调整的优点。另外，热退火的C-PCBSD：GD膜提供了具有足够耐溶剂性的粘合膜网络。因此，钙钛矿器件可提供20.19％的功率转换效率，并明显改善了电池的稳定性。这表明GD改性的可交联富勒烯作为ETL在压区结构PSC中的潜在应用。这一发现开辟了一条新的途径，即通过具有大π共轭的2D材料沉积有序取向的富勒烯薄膜，从而控制随后的钙钛矿结晶。高效的电荷提取和能级调整。另外，热退火的C-PCBSD：GD膜提供了具有足够耐溶剂性的粘合膜网络。因此，钙钛矿器件可提供20.19％的功率转换效率，并明显改善了电池的稳定性。这表明GD改性的可交联富勒烯作为ETL在压区结构PSC中的潜在应用。这一发现开辟了一条新的途径，即通过具有大π共轭的2D材料沉积有序取向的富勒烯薄膜，从而控制随后的钙钛矿结晶。高效的电荷提取和能级调整。另外，热退火的C-PCBSD：GD膜提供了具有足够耐溶剂性的粘合膜网络。因此，钙钛矿器件可提供20.19％的功率转换效率，并明显改善了电池的稳定性。这表明GD改性的可交联富勒烯作为ETL在压区结构PSC中的潜在应用。这一发现开辟了一条新的途径，即通过具有大π共轭的2D材料沉积有序取向的富勒烯薄膜，从而控制随后的钙钛矿结晶。19％具有明显改善的细胞稳定性。这表明GD改性的可交联富勒烯作为ETL在压区结构PSC中的潜在应用。这一发现开辟了一条新的途径，即通过具有大π共轭的2D材料沉积有序取向的富勒烯薄膜，从而控制随后的钙钛矿结晶。19％具有明显改善的细胞稳定性。这表明GD改性的可交联富勒烯作为ETL在压区结构PSC中的潜在应用。这一发现开辟了一条新的途径，即通过具有大π共轭的2D材料沉积有序取向的富勒烯薄膜，从而控制随后的钙钛矿结晶。