Tailoring photoactivity of polymeric carbon nitride via donor-π-acceptor network

Molecular doping approach can effectively modulate the charge transfer kinetics of polymeric carbon nitride (PCN) photocatalyst. Herein, we show that doping of PCN with a strong electron-withdrawing 2,3-diaminopyridine (DAP) induces the formation of donor-π-acceptor (D-π-A) network. As formed D-π-A...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2022-08, Vol.310, p.121347, Article 121347
Main Authors: Bhoyar, Toshali, Kim, Dong Jin, Abraham, B. Moses, Tonda, Surendar, Manwar, Nilesh R., Vidyasagar, Devthade, Umare, Suresh S.
Format: Article
Language:English
Subjects:
2,3-Diaminopyridine
Carbon
Carbon nitride
Catalysts
Charge transfer
Current carriers
Donor-π-acceptor
Doping
Free energy
Heterocyclic compounds
Hydrogen
Hydrogen evolution
Hydrogen production
Optoelectronics
Photocatalysis
Photocatalyst
Polymeric carbon nitride
Theoretical analysis
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Summary:Molecular doping approach can effectively modulate the charge transfer kinetics of polymeric carbon nitride (PCN) photocatalyst. Herein, we show that doping of PCN with a strong electron-withdrawing 2,3-diaminopyridine (DAP) induces the formation of donor-π-acceptor (D-π-A) network. As formed D-π-A type network demonstrated a photocatalytic hydrogen production activity of 6.56 mmolg−1 h−1, which is 4.5-times greater than the pure PCN. The optoelectronic features characterized by spectroscopic techniques indicate rapid separation of photoexcited charge carriers and extended light-harvesting ability of DAP-doped PCN. Further, the theoretical analysis revealed that DAP-doped PCN has near-ideal hydrogen adsorption free energy of − 0.11 eV, which supports the excellent hydrogen production performance. Importantly, the hydrogen production activity demonstrated here outperforms several state-of-art molecular-doped PCN-based catalysts. This study sheds light on the effective production of PCN-based D-π-A networks using conjugated heterocyclic compounds. [Display omitted] •Donor-π-acceptor (D-π-A) type polymeric carbon nitride is realized by doping 2,3-diaminopyridine moiety.•Intramolecular charge transfer (ICT) in D-π-A type network facilitates rapid dissociation of charge-carriers.•D-π-A type network shows near ideal hydrogen adsorption free energy of −0.11 eV.•Photocatalytic hydrogen production activity of D-π-A type PCN is 4.5-times greater than bulk PCN catalyst.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2022.121347