Tang Yunqi, Mak Chun Hong, Wang Chen, Fu Yu, Li Fang-Fang, Jia Guohua, Hsieh Chang-Wei, Shen Hsin-Hui, Colmenares Juan Carlos, Song Haisheng, Yuan Mingjian, Chen Yue, Hsu Hsien-Yi
School of Energy and Environment, Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, 999077, China.
Shenzhen Research Institute of City University of Hong Kong, Shenzhen, 518057, P. R. China.
Small Methods. 2022 Aug;6(8):e2200326. doi: 10.1002/smtd.202200326. Epub 2022 Jun 22.
The photocatalytic system using hydrohalic acid (HX) for hydrogen production is a promising strategy to generate clean and renewable fuels as well as value-added chemicals (such as X /X ). However, it is still challenging to develop a visible-light active and strong-acid resistive photocatalyst. Hybrid perovskites have been recognized as a potential photocatalyst for photovoltaic HX splitting. Herein, a novel environmentally friendly mixed halide perovskite MA Bi Cl I with a bandgap funnel structure is developed, i.e., confirmed by energy dispersive X-ray analysis and density functional theory calculations. Due to gradient neutral formation energy within iodine-doped MA Bi Cl , the concentration of iodide element decreases from the surface to the interior across the MA Bi Cl I perovskite. Because of the aligned energy levels of iodide/chloride-mixed MA Bi Cl I , a graded bandgap funnel structure is therefore formed, leading to the promotion of photoinduced charge transfer from the interior to the surface for efficient photocatalytic redox reaction. As a result, the hydrogen generation rate of the optimized MA Bi Cl I is enhanced up to ≈341 ± 61.7 µmol h with a Pt co-catalyst under visible light irradiation.
使用氢卤酸（HX）制氢的光催化系统是生产清洁可再生燃料以及增值化学品（如X /X ）的一种很有前景的策略。然而，开发一种可见光活性且耐强酸的光催化剂仍然具有挑战性。混合钙钛矿已被认为是用于光伏HX分解的潜在光催化剂。在此，开发了一种具有带隙漏斗结构的新型环境友好型混合卤化物钙钛矿MA Bi Cl I ，即通过能量色散X射线分析和密度泛函理论计算得到证实。由于碘掺杂的MA Bi Cl 内梯度中性形成能，碘元素的浓度在MA Bi Cl I 钙钛矿中从表面到内部逐渐降低。由于碘化物/氯化物混合的MA Bi Cl I 的能级对齐，因此形成了分级带隙漏斗结构，从而促进了光生电荷从内部到表面的转移，以进行高效的光催化氧化还原反应。结果，在可见光照射下，使用Pt助催化剂时，优化后的MA Bi Cl I 的产氢速率提高到约341 ± 61.7 μmol h 。
