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Elsevier, Nano Energy, (12), p. 646-656, 2015

DOI: 10.1016/j.nanoen.2015.01.043

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Carbon nitride with simultaneous porous network and O-doping for efficient solar-energy-driven Hydrogen evolution

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This paper is available in a repository.

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Abstract

Efficient charge separation and broaden light absorption are of crucial importance for solar-driven hydrogen evolution reaction (HER), and graphitic carbon nitride (g-C3N4) is a very promising photocatalyst for this reaction. Here we report a facile precursor pre-treatment method, by forming hydrogen bond-induced supramolecular aggregates, to fabricate g-C3N4 with simultaneous novel porous network and controllable O-doping. Experimental and DFT computation identified that O doping preferentially occurs on two-coordinated N position, and the porous network and O-doping synergetically promote the light harvesting and charge separation. As a result, this material shows 6.1 and 3.1 times higher HER activity (with apparent quantum efficiency of 7.8% at 420 nm) than bulk and even 3D porous g-C3N4. This work highlights that simply pre-treating the precursor can not only control the architecture but also introduce helpful foreign atoms or monomer in the matrix, which provides a useful strategy to design and fabricate highly efficient g-C3N4 photocatalyst.