Abstract

Photocatalytic hydrogen evolution from water has triggered an intensive search for metal-free semiconducting photocatalysts. However, traditional semiconducting materials suffer from limited hydrogen evolution efficiency owing to low intrinsic electron transfer, rapid recombination of photogenerated carriers, and lack of artificial microstructure. Herein, we report a metal-free half-metallic carbon nitride for highly efficient photocatalytic hydrogen evolution. The introduced half-metallic features not only effectively facilitate carrier transfer but also provide more active sites for hydrogen evolution reaction. The nanosheets incorporated into a micro grid mode resonance structure via in situ pyrolysis of ionic liquid, which show further enhanced photoelectronic coupling and entire solar energy exploitation, boosts the hydrogen evolution rate reach up to 1009 μmol g−1 h−1. Our findings propose a strategy for micro-structural regulations of half-metallic carbon nitride material, and meanwhile the fundamentals provide inspirations for the steering of electron transfer and solar energy absorption in electrocatalysis, photoelectrocatalysis, and photovoltaic cells.

Highlights

  • Photocatalytic hydrogen evolution from water has triggered an intensive search for metalfree semiconducting photocatalysts

  • Among the above metal-free semiconducting materials, photocatalysts with large number of exposed active sites, low resistance for carrier transfer and wide solar light response have been identified as promising candidates for hydrogen evolution reaction (HER)[10]

  • The density functional theory (DFT) prediction was implemented and the calculated results show that the layered carbon nitride [C(CN)3] has the expected intrinsic halfmetallicity and suitable band gap (2.06–2.33 eV) to harvest more solar energy (Supplementary Fig. 1)[14]

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Summary

Introduction

Photocatalytic hydrogen evolution from water has triggered an intensive search for metalfree semiconducting photocatalysts. Among the above metal-free semiconducting materials, photocatalysts with large number of exposed active sites, low resistance for carrier transfer and wide solar light response have been identified as promising candidates for hydrogen evolution reaction (HER)[10]. The designed various nanostructures are widely used in solar cells to enhance light absorption[15,16,17,18] In our system, this artificial nanotube array acts as micro grid mode resonance to tune optoelectronic coupling process for enhanced utilization of solar energy and the template to control the size of carbon nitride nanosheets.

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