Donor–Acceptor Viologens with Through-Space Conjugation for Enhanced Visible-Light-Driven Photocatalysis

Yi Qiao; Liang Xu; Xiaoyang Liu; Yujing Gao; Naiyao Li; Yawen Li; Tianle Cao; Ni Yan; Zishun Liu; Gang He

doi:10.1002/advs.202409925

Donor–Acceptor Viologens with Through-Space Conjugation for Enhanced Visible-Light-Driven Photocatalysis

Yi Qiao, Liang Xu, Xiaoyang Liu, Yujing Gao, Naiyao Li, Yawen Li^*, Tianle Cao, Ni Yan, Zishun Liu^*, Gang He^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

10 Citations (Scopus)

7 Downloads (CityUHK Scholars)

Abstract

A series of novel donor–acceptor (D–A) type viologens with through-space conjugation (TSC) are synthesized. The synergistic effect of D–A conjugation and TSC endow these compounds with a narrower energy gap, excellent redox properties, strong absorption in the visible range (up to 450 nm), and high efficiency of intramolecular charge transfer (ICT). These compounds also exhibit a long-lived charge separation state and stable radical formation. Considering their impressive photophysical and redox properties, TSC viologens with D–A conjugation are explored for visible-light-driven photocatalysis. As a catalyst in oxidative coupling reactions under visible light, compound 9 can achieve a yield of 94%, attributed to its strong ICT effect. Additionally, hybridized into graphitic carbon nitride (g-C₃N₄), compound 9 enhances hydrogen production performance under visible light, achieving an H₂ generation rate of 4102 µmol h⁻¹g⁻¹. This study highlights the potential applications of TSC viologens in photocatalytic systems. © 2024 The Author(s). Advanced Science published by Wiley-VCH GmbH.

Original language	English
Article number	2409925
Journal	Advanced Science
Volume	12
Issue number	2
Online published	21 Nov 2024
DOIs	https://doi.org/10.1002/advs.202409925
Publication status	Published - 13 Jan 2025
Externally published	Yes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

donor–acceptor
hydrogen production
oxidative coupling reaction
through-space conjugation
viologens

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abstract = "A series of novel donor–acceptor (D–A) type viologens with through-space conjugation (TSC) are synthesized. The synergistic effect of D–A conjugation and TSC endow these compounds with a narrower energy gap, excellent redox properties, strong absorption in the visible range (up to 450 nm), and high efficiency of intramolecular charge transfer (ICT). These compounds also exhibit a long-lived charge separation state and stable radical formation. Considering their impressive photophysical and redox properties, TSC viologens with D–A conjugation are explored for visible-light-driven photocatalysis. As a catalyst in oxidative coupling reactions under visible light, compound 9 can achieve a yield of 94%, attributed to its strong ICT effect. Additionally, hybridized into graphitic carbon nitride (g-C₃N₄), compound 9 enhances hydrogen production performance under visible light, achieving an H2 generation rate of 4102 µmol h−1g−1. This study highlights the potential applications of TSC viologens in photocatalytic systems. {\textcopyright} 2024 The Author(s). Advanced Science published by Wiley-VCH GmbH.",

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author = "Yi Qiao and Liang Xu and Xiaoyang Liu and Yujing Gao and Naiyao Li and Yawen Li and Tianle Cao and Ni Yan and Zishun Liu and Gang He",

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T1 - Donor–Acceptor Viologens with Through-Space Conjugation for Enhanced Visible-Light-Driven Photocatalysis

AU - Qiao, Yi

AU - Xu, Liang

AU - Liu, Xiaoyang

AU - Gao, Yujing

AU - Li, Naiyao

AU - Li, Yawen

AU - Cao, Tianle

AU - Yan, Ni

AU - Liu, Zishun

AU - He, Gang

PY - 2025/1/13

Y1 - 2025/1/13

N2 - A series of novel donor–acceptor (D–A) type viologens with through-space conjugation (TSC) are synthesized. The synergistic effect of D–A conjugation and TSC endow these compounds with a narrower energy gap, excellent redox properties, strong absorption in the visible range (up to 450 nm), and high efficiency of intramolecular charge transfer (ICT). These compounds also exhibit a long-lived charge separation state and stable radical formation. Considering their impressive photophysical and redox properties, TSC viologens with D–A conjugation are explored for visible-light-driven photocatalysis. As a catalyst in oxidative coupling reactions under visible light, compound 9 can achieve a yield of 94%, attributed to its strong ICT effect. Additionally, hybridized into graphitic carbon nitride (g-C₃N₄), compound 9 enhances hydrogen production performance under visible light, achieving an H2 generation rate of 4102 µmol h−1g−1. This study highlights the potential applications of TSC viologens in photocatalytic systems. © 2024 The Author(s). Advanced Science published by Wiley-VCH GmbH.

AB - A series of novel donor–acceptor (D–A) type viologens with through-space conjugation (TSC) are synthesized. The synergistic effect of D–A conjugation and TSC endow these compounds with a narrower energy gap, excellent redox properties, strong absorption in the visible range (up to 450 nm), and high efficiency of intramolecular charge transfer (ICT). These compounds also exhibit a long-lived charge separation state and stable radical formation. Considering their impressive photophysical and redox properties, TSC viologens with D–A conjugation are explored for visible-light-driven photocatalysis. As a catalyst in oxidative coupling reactions under visible light, compound 9 can achieve a yield of 94%, attributed to its strong ICT effect. Additionally, hybridized into graphitic carbon nitride (g-C₃N₄), compound 9 enhances hydrogen production performance under visible light, achieving an H2 generation rate of 4102 µmol h−1g−1. This study highlights the potential applications of TSC viologens in photocatalytic systems. © 2024 The Author(s). Advanced Science published by Wiley-VCH GmbH.

KW - donor–acceptor

KW - hydrogen production

KW - oxidative coupling reaction

KW - through-space conjugation

KW - viologens

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DO - 10.1002/advs.202409925

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Donor–Acceptor Viologens with Through-Space Conjugation for Enhanced Visible-Light-Driven Photocatalysis

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Research Keywords

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