With the rapid development of flexible optoelectronic devices, recyclability is highly desirable for alleviating resource waste and environmental pollution, but remains challenging. Here, a fully closed-loop recyclable crosslinked polyimide (RCPI) was fabricated via carboxyl ligand exchange between the CPI with pendent carboxyl groups and the cyclic Ti-oxo cluster (CTOC) with labile carboxyl ligands, which could be reconverted into reprocessable CPI and CTOC solution by pivalic acid. The RCPI-based embedded AgNWs@RCPI electrode shows comparable high conductivity, transparency and low roughness with ITO (indium tin oxide)/glass electrode, and meanwhile outstanding mechanical robustness. The related flexible organic solar cells (FOSCs) provided a high efficiency of 14.78% and maintained ~97% of the initial efficiency after 5000 bending cycles at a small bending radius of 1 mm. Moreover, the recyclability of the RCPI still retains after being manufactured into the FOSCs. This work provides a promising strategy for recyclable flexible optoelectronic devices.

随着柔性光电器件的快速发展，可回收性对于减轻资源浪费和环境污染是非常可取的，但仍然具有挑战性。在这里，通过具有悬垂羧基的 CPI 和具有不稳定羧基配体的环状 Ti-氧簇 (CTOC) 之间的羧基配体交换，制备了一种完全闭环的可回收交联聚酰亚胺 (RCPI)，可以将其重新转化为可再加工的 CPI 和 CTOC新戊酸溶液。基于 RCPI 的嵌入式 AgNWs@RCPI 电极显示出与 ITO（氧化铟锡）/玻璃电极相当的高导电性、透明度和低粗糙度，同时具有出色的机械强度。相关的柔性有机太阳能电池（FOSC）提供了 14 倍的高效率。在 1 mm 的小弯曲半径下 5000 次弯曲循环后，78% 并保持初始效率的约 97%。此外，RCPI 的可回收性在制造成 FOSC 后仍然保留。这项工作为可回收的柔性光电器件提供了一种有前景的策略。