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

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),...

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Main Authors: Yi Qiao, Liang Xu, Xiaoyang Liu, Yujing Gao, Naiyao Li, Yawen Li, Tianle Cao, Ni Yan, Zishun Liu, Gang He
Format: Article
Language:English
Published: Wiley 2025-01-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202409925
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author Yi Qiao
Liang Xu
Xiaoyang Liu
Yujing Gao
Naiyao Li
Yawen Li
Tianle Cao
Ni Yan
Zishun Liu
Gang He
author_facet Yi Qiao
Liang Xu
Xiaoyang Liu
Yujing Gao
Naiyao Li
Yawen Li
Tianle Cao
Ni Yan
Zishun Liu
Gang He
author_sort Yi Qiao
collection DOAJ
description 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.
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institution Kabale University
issn 2198-3844
language English
publishDate 2025-01-01
publisher Wiley
record_format Article
series Advanced Science
spelling doaj-art-1ca0a797ced542bc86a01543a0d5195d2025-01-13T15:29:43ZengWileyAdvanced Science2198-38442025-01-01122n/an/a10.1002/advs.202409925Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven PhotocatalysisYi Qiao0Liang Xu1Xiaoyang Liu2Yujing Gao3Naiyao Li4Yawen Li5Tianle Cao6Ni Yan7Zishun Liu8Gang He9Frontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaFrontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaFrontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaFrontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaFrontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaFrontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaSchool of Materials Science and Engineering Chang'an University Xi'an 710064 ChinaSchool of Materials Science and Engineering Chang'an University Xi'an 710064 ChinaInternational Center for Applied Mechanics State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaFrontier Institute of Science and Technology Key Laboratory of Thermo‐Fluid Science and Engineering of Ministry of Education State Key Laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University Xi'an Shaanxi Province 710054 P. R. ChinaAbstract 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.https://doi.org/10.1002/advs.202409925donor–acceptorhydrogen productionoxidative coupling reactionthrough‐space conjugationviologens
spellingShingle Yi Qiao
Liang Xu
Xiaoyang Liu
Yujing Gao
Naiyao Li
Yawen Li
Tianle Cao
Ni Yan
Zishun Liu
Gang He
Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis
Advanced Science
donor–acceptor
hydrogen production
oxidative coupling reaction
through‐space conjugation
viologens
title Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis
title_full Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis
title_fullStr Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis
title_full_unstemmed Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis
title_short Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis
title_sort donor acceptor viologens with through space conjugation for enhanced visible light driven photocatalysis
topic donor–acceptor
hydrogen production
oxidative coupling reaction
through‐space conjugation
viologens
url https://doi.org/10.1002/advs.202409925
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AT liangxu donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT xiaoyangliu donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT yujinggao donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT naiyaoli donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT yawenli donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT tianlecao donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT niyan donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT zishunliu donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis
AT ganghe donoracceptorviologenswiththroughspaceconjugationforenhancedvisiblelightdrivenphotocatalysis