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Acetylene and Diacetylene Functionalized Covalent Triazine Frameworks as Metal‐Free Photocatalysts for Hydrogen Peroxide Production: A New Two‐Electron Water Oxidation Pathway
Author(s) -
Chen Liang,
Wang Lei,
Wan Yangyang,
Zhang Ying,
Qi Zeming,
Wu Xiaojun,
Xu Hangxun
Publication year - 2020
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201904433
Subject(s) - diacetylene , photocatalysis , photochemistry , materials science , acetylene , covalent bond , hydrogen peroxide , catalysis , polymer , chemistry , organic chemistry , polymerization , composite material
Metal‐free polymer photocatalysts have shown great promise for photocatalytic H 2 O 2 production via two‐electron reduction of molecular O 2 . The other half‐reaction, which is the two‐electron oxidation of water, still remains elusive toward H 2 O 2 production. However, enabling this water oxidation pathway is critically important to improve the yield and maximize atom utilization efficiency. It is shown that introducing acetylene (CC) or diacetylene (CCCC) moieties into covalent triazine frameworks (CTFs) can remarkably promote photocatalytic H 2 O 2 production. This enhancement is inherent to the incorporated carbon–carbon triple bonds which are essential in modulating the electronic structures of CTFs and suppressing charge recombinations. Furthermore, the acetylene and diacetylene moieties can significantly reduce the energy associated with OH* formation and thus enable a new two‐electron oxidation pathway toward H 2 O 2 production. The study unveils an important reaction pathway toward photocatalytic H 2 O 2 production, reflecting that precise control over the chemical structures of polymer photocatalysts is vital to achieve efficient solar‐to‐chemical energy conversion.