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Aggregate-forming semi-synthetic chlorophyll derivatives / Ti₃C₂Tₓ MXene hybrids for photocatalytic hydrogen evolution

Li, Y; Liu, Y; Sun, X; Zheng, T; Dall'Agnese, Y; Dall'Agnese, C; Sasaki, SI; ... Wang, XF; + view all (2021) Aggregate-forming semi-synthetic chlorophyll derivatives / Ti₃C₂Tₓ MXene hybrids for photocatalytic hydrogen evolution. Dyes and Pigments , 194 , Article 109583. 10.1016/j.dyepig.2021.109583. Green open access

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Abstract

Chlorophylls (Chls) are the most abundant natural pigments having excellent opt-electrical and semi-conductive properties. Ti3C2Tx MXene, one of the most extensively studied 2D noble metal-free co-catalyst, features outstanding electrochemical properties. This work compares three aggregate-forming chlorophyll derivatives (Chl-n; n = 1–3), namely, zinc methyl 3-devinyl-3-hydroxymethyl-pyropheophorbide-a (Chl-1), zinc dodecyl 3-devinyl-3-hydroxymethyl-pyropheophorbide-a (Chl-2) and zinc dodecyl 131-deoxo-3-devinyl-131-dicyanomethylene-3-hydroxymethyl-pyropheophorbide-a (Chl-3), as light-harvesting antenna pigments in the MXene-based photocatalytic system for hydrogen evolution under the white light illumination (λ > 420 nm). The hydrogen evolution reaction (HER) of these Chls depends on the peripheral substituent groups at the C13- and/or C17-positions of the chlorin macrocyclic π-system. Differences among these Chl-n sensitized Ti3C2Tx MXene (Chl-n@Ti3C2Tx) are compared in terms of their light-harvesting ability, morphology, charge transfer efficiency and photocatalytic performance. The best HER performance is found to be as high as 122 μmol/h/gcat with the Chl-3@Ti3C2Tx composite. This work leads the direction in synthesizing Chls in Chl/MXene hybrid structure suitable for highly efficient photocatalytic HER.

Type: Article
Title: Aggregate-forming semi-synthetic chlorophyll derivatives / Ti₃C₂Tₓ MXene hybrids for photocatalytic hydrogen evolution
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.dyepig.2021.109583
Publisher version: https://doi.org/10.1016/j.dyepig.2021.109583
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher's terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office > Institute for Materials Discovery
URI: https://discovery.ucl.ac.uk/id/eprint/10132173
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