Polar Aromatic Two‐dimensional Dion‐Jacobson Halide Perovskites for Efficient Photocatalytic H<sub>2</sub> Evolution
Yu Peng, Yang Zhang, Xing Wang, Xin Sui, Miao Lin, Yan Zhu, Changfei Jing, Hai Yang Yuan, Shuang Yang, Peng Fei Liu, Sheng Dai, Zhaoke Zheng, Hua Gui Yang, Yu Hou
Abstract
Abstract Polar materials with spontaneous polarization ( P s ) have emerged as highly promising photocatalysts for efficient photocatalytic H 2 evolution owing to the P s ‐enhanced photogenerated carrier separation. However, traditional inorganic polar materials often suffer from limitations such as wide band gaps and poor carrier transport, which hinders their photocatalytic H 2 evolution efficiency. Here, we rationally synthesized a series of isostructural two‐dimensional (2D) aromatic Dion–Jacobson (DJ) perovskites, namely (2‐(2‐Aminoethyl)pyridinium)PbI 4 (2‐APDPI), (3‐(2‐Aminoethyl)pyridinium)PbI 4 (3‐APDPI), and (4‐(2‐Aminoethyl)pyridinium)PbI 4 (4‐APDPI), where 2‐APDPI and 4‐APDPI crystalize in polar space groups with piezoelectric constants ( d 33 ) of approximately 40 pm V −1 and 3‐APDPI adopts a centrosymmetric structure. Strikingly, owing to the P s ‐facilitated separation of photogenerated carriers, polar 2‐APDPI and 4‐APDPI exhibit a 3.9‐ and 2.8‐fold increase, respectively, in photocatalytic H 2 evolution compared to the centrosymmetric 3‐APDPI. As a pioneering study, this work provides an efficient approach for exploring new polar photocatalysts and highlights their potential in promoting photocatalytic H 2 evolution.