Aggregate-forming semi-synthetic chlorophyll derivatives / Ti3C2Tx MXene hybrids for photocatalytic hydrogen evolution. (October 2021)

• Record Type: Journal Article
• Authors: Li, Yuanlin; Liu, Yanxiang; Sun, Xiaoli; Zheng, Tianfang; Dall'Agnese, Yohan; Dall'Agnese, Chunxiang; Sasaki, Shin-ichi; Tamiaki, Hitoshi; Wang, Xiao-Feng
• Is Part Of: Dyes and pigments. Volume 194(2021)
• Publication Date: 2021-10
• Subjects: Aggregates materials -- Chlorophyll derivatives -- Energy migration -- Hydrogen evolution reaction -- Ti3C2Tx MXene; Dyes and dyeing -- Periodicals; Pigments -- Periodicals; 667.2
• DOI: 10.1016/j.dyepig.2021.109583
• Languages: English
• ISSNs: 0143-7208

Abstract

Abstract: Chlorophylls (Chls) are the most abundant natural pigments having excellent opt-electrical and semi-conductive properties. Ti3 C2 T x 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 13 1 -deoxo-3-devinyl-13 1 -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 Ti3 C2 T x MXene (Chl-n@Ti3 C2 T x ) 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@Ti3 C2 T x composite. This work leads the direction in synthesizing Chls in Chl/MXene hybrid structure suitable for highly efficient photocatalytic HER. Graphical abstract: Image 1 Highlights: Three different aggregate-forming chlorophyll derivatives are compared for hydrogen evolution. Highly efficient electron-hole separation through the exciton transfer in Chl aggregates. Chl@MXene-based photocatalytic system is developed. This work leads the direction in synthesizing Chls in Chl/MXene hybrid structure suitable for HER.