Photocatalytic Abstraction of Hydrogen Atoms from Water Using Hydroxylated Graphitic Carbon Nitride for Hydrogenative Coupling Reactions

Employing pure water, the ultimate green source of hydrogen donor to initiate chemical reactions that involve a hydrogen atom transfer (HAT) step is fascinating but challenging due to its large H−O bond dissociation energy (BDEH‐O=5.1 eV). Many approaches have been explored to stimulate water for hy...

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Bibliographic Details
Published in:Angewandte Chemie 2022-06, Vol.134 (24), p.n/a
Main Authors: Zhang, Dongsheng, Ren, Pengju, Liu, Wuwen, Li, Yaru, Salli, Sofia, Han, Feiyu, Qiao, Wei, Liu, Yu, Fan, Yingzhu, Cui, Yi, Shen, Yanbin, Richards, Emma, Wen, Xiaodong, Rummeli, Mark H., Li, Yongwang, Besenbacher, Flemming, Niemantsverdriet, Hans, Lim, Tingbin, Su, Ren
Format: Article
Language:English
Subjects:
Carbon
Carbon nitride
Chemical reactions
Chemistry
Coupling
Coupling Reaction
Dehydrogenation
Energy of dissociation
Free energy
Heat of formation
Heterogeneous Photocatalysis
Hydrogen
Hydrogen Atom Transfer
Hydrogen atoms
Hydrogen peroxide
Irradiation
Light irradiation
Pharmaceutical industry
Renewable energy
Solar radiation
Surface Hydroxylation
Water
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Summary:Employing pure water, the ultimate green source of hydrogen donor to initiate chemical reactions that involve a hydrogen atom transfer (HAT) step is fascinating but challenging due to its large H−O bond dissociation energy (BDEH‐O=5.1 eV). Many approaches have been explored to stimulate water for hydrogenative reactions, but the efficiency and productivity still require significant enhancement. Here, we show that the surface hydroxylated graphitic carbon nitride (gCN−OH) only requires 2.25 eV to activate H−O bonds in water, enabling ion of hydrogen atoms via dehydrogenation of pure water into hydrogen peroxide under visible light irradiation. The gCN−OH presents a stable catalytic performance for hydrogenative N−N coupling, pinacol‐type coupling and dehalogenative C−C coupling, all with high yield and efficiency, even under solar radiation, featuring extensive impacts in using renewable energy for a cleaner process in dye, electronic, and pharmaceutical industries. Using water as hydrogen donor is very challenging for hydrogen atom transfer reaction. Compared with gCN, the surface hydroxylated graphitic carbon nitride (gCN−OH) shows the activation of H−O bonds in water under visible light irradiation, thus rendering water as hydrogen donor for multiple reductions involving a hydrogen atom transfer (HAT) step and the oxidation of water to H2O2.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202204256