Key Laboratory of Physics and Technology for Advanced, Batteries (Ministry of Education), College of Physics, Jilin University, Changchun, 130012, P.R. China.
Key Jilin Key Engineering Laboratory of New Energy, Materials and Technologies, Jilin University, Changchun, 130012, P.R. China.
Chemistry. 2021 Mar 17;27(16):5277-5282. doi: 10.1002/chem.202005421. Epub 2021 Feb 18.
The Z-scheme process is a photoinduced electron-transfer pathway in natural oxygenic photosynthesis involving electron transport from photosystem II (PSII) to photosystem I (PSI). Inspired by the interesting Z-scheme process, herein a photocatalytic hydrogen evolution reaction (HER) employing chlorophyll (Chl) derivatives, Chl-1 and Chl-2, on the surface of Ti C T MXene with two-dimensional accordion-like morphology, forming Chl-1@Chl-2@Ti C T composite, is demonstrated. Due to the frontier molecular orbital energy alignments of Chl-1 and Chl-2, sublayer Chl-1 is a simulation of PSI, whereas upper layer Chl-2 is equivalent to PSII, and the resultant electron transport can take place from Chl-2 to Chl-1. Under the illumination of visible light (>420 nm), the HER performance of Chl-1@Chl-2@Ti C T photocatalyst was found to be as high as 143 μmol h g , which was substantially higher than that of photocatalysts of either Chl-1@Ti C T (20 μmol h g ) or Chl-2@Ti C T (15 μmol h g ).
Z 型过程是一种在自然放氧光合作用中发生的光诱导电子转移途径，涉及电子从光系统 II（PSII）向光系统 I（PSI）的传输。受有趣的 Z 型过程的启发，本文展示了在具有二维手风琴状形貌的 Ti C T MXene 表面上利用叶绿素（Chl）衍生物 Chl-1 和 Chl-2 进行的光催化析氢反应（HER）。由于 Chl-1 和 Chl-2 的前沿分子轨道能量排列，亚层 Chl-1 模拟 PSI，而上层 Chl-2 相当于 PSII，并且可以发生从 Chl-2 到 Chl-1 的电子传递。在可见光（>420nm）照射下，发现 Chl-1@Chl-2@Ti C T 光催化剂的 HER 性能高达 143μmol h g ，明显高于 Chl-1@Ti C T（20μmol h g ）或 Chl-2@Ti C T（15μmol h g ）光催化剂的性能。
