| Affiliation: | 1. 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;2. Institute for Materials Discovery, University College London, London, WC1E 7JE UK;3. Key Laboratory of Physics and Technology for Advanced, Batteries (Ministry of Education), College of Physics, Jilin University, Changchun, 130012 P.R. China;4. Graduate School of Life Sciences, Ritsumeikan University, Kusatsu, Shiga, 5258577 Japan |
| Abstract: | 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 Ti3C2Tx MXene with two-dimensional accordion-like morphology, forming Chl-1@Chl-2@Ti3C2Tx 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@Ti3C2Tx photocatalyst was found to be as high as 143 μmol h−1 gcat−1, which was substantially higher than that of photocatalysts of either Chl-1@Ti3C2Tx (20 μmol h−1 g−1) or Chl-2@Ti3C2Tx (15 μmol h−1 g−1). |
