Li, Y; Sun, Y; Zheng, T; Dall'Agnese, Y; Dall'Agnese, C; Meng, X; Sasaki, S-I; ... Wang, X-F; + view all Li, Y; Sun, Y; Zheng, T; Dall'Agnese, Y; Dall'Agnese, C; Meng, X; Sasaki, S-I; Tamiaki, H; Wang, X-F; - view fewer (2021) Chlorophyll based organic heterojunction on Ti3C2Tx MXenes nano‐sheets for efficient hydrogen production. Chemistry - A European Journal , 27 (16) pp. 5277-5282. 10.1002/chem.202005421.

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Abstract

Z‐scheme process is a photo‐induced electron transfer pathway in natural oxygenic photosynthesis involving the electron transport from photosystem II (PSII) to PSI. Inspired by the interesting Z‐scheme process, here we demonstrated a photocatalytic hydrogen evolution reaction (HER) employing chlorophyll derivatives, Chl‐1 and Chl‐2, on the surface of Ti3C2Tx MXenes with two‐dimensional accordion‐like morphology forming Chl‐1@Chl‐2@Ti3C2Tx composite. Due to the frontier molecular orbital energy alignments of Chl‐1 and Chl‐2, the sublayer Chl‐1 is a simulation of PSI whereas the 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 photocatalysts was found to be as high as 143 μmol/h/gcat , which was substantially higher than that of photocatalysts of either Chl‐1@Ti3C2Tx (20 μmol/h/g) or Chl‐2@Ti3C2Tx (15 μmol/h/g).

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