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1Department of Chemistry, Indian Institute of Technology Hyderabad, Kandi, Sangareddy 502284, Telangana, India. arup@chy.iith.ac.in.
Abstract:
Through first-principles calculations, we investigated the role of N-site positioning in 2D COFs for modulating photocatalytic water splitting. Water activation at the pyridine N-site triggers protonation, inducing a push-pull electronic interaction, lowering the OER/HER thermodynamic barriers. Furthermore, N-atom positioning significantly alters the electron density and exciton binding energy, thereby improving the reaction thermodynamics.
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