Wang Hong, Zhang Hefeng, Wang Junhui, Gao Yuying, Fan Fengtao, Wu Kaifeng, Zong Xu, Li Can
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Zhongshan Road 457, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2021 Mar 22;60(13):7376-7381. doi: 10.1002/anie.202014623. Epub 2021 Feb 15.
Three-dimensional (3D) organic-inorganic hybrid perovskites have demonstrated excellent capability in solar fuel production, while the two-dimensional (2D) counterparts are generally considered inferior candidates due to the high exciton binding energy and weak light absorption. Herein, contrary to our common understanding, we find that 2D perovskites can perform photocatalytic H production from HI splitting more efficiently than their 3D counterparts. We observed sharp difference between 2D perovskites crystals with organic phenylalkylammonium cations of different lengths and the 3D counterparts in their stabilization behavior in aqueous solution. Moreover, we show that the organic cations length of the 2D perovskites affects the nanostructures, optoelectronic properties, and the charge transfer process significantly, which determines the photocatalytic activity of the 2D perovskites. Among the 2D perovskites under investigation, phenylmethylammonium lead iodide with the shortest organic cations achieved the best solar-to-chemical conversion efficiency of ca. 1.57 %, which is the highest value ever reported for hybrid perovskites.
三维(3D)有机-无机杂化钙钛矿在太阳能燃料生产中展现出了卓越的能力,而二维(2D)钙钛矿由于激子结合能高和光吸收弱,通常被认为是较差的候选材料。在此,与我们的普遍认知相反,我们发现二维钙钛矿在光催化由碘化氢分解产氢方面比三维钙钛矿更高效。我们观察到,具有不同长度有机苯基烷基铵阳离子的二维钙钛矿晶体与其三维对应物在水溶液中的稳定行为存在显著差异。此外,我们表明二维钙钛矿的有机阳离子长度对纳米结构、光电性质和电荷转移过程有显著影响,这决定了二维钙钛矿的光催化活性。在所研究的二维钙钛矿中,具有最短有机阳离子的苯基甲基铵碘化铅实现了约1.57%的最佳太阳能到化学能的转换效率,这是混合钙钛矿报道过的最高值。