Converting solar energy into hydrogen energy through a photocatalytic technology has become a hotspot of current research. Exploring and designing a photocatalyst with efficient visible light response and high activity is the core issue in the photocatalysis. As a new generation of the most promising organic semiconductor photocatalyst, graphitic carbon nitride (g-C3N4) materials has attracted great attention but still suffer from the shortcomings such as low utilization of visible light, high recombination rate of photo-generated electron-hole, and etc. By considering induced electron transfer and morphology design to overcome the above shortcomings, the directional intramolecular charge transfer, controlled electron migration and hierarchical micro-nano-structured carbon nitride material with oxygen doping and nitrogen defects are successfully designed via molecular grafting and supramolecular preassembly strategies. By using melamine as the only precursor, a hierarchical tubular carbon nitride with an internal porous coral-like architecture was successfully obtained by a self-templating method. For the first time, the three-dimensional hierarchical structure was analyzed using 3D electronic tomography. As a result, the hierarchically nanostructured g-C3N4 can achieve a highly efficient photocatalytic hydrogen production of 5.29 mmol h-1 g-1 with a high apparent quantum yield of 32.4% at 420 nm, due to the large specific surface area, short charge transfer distance, enhanced light scattering, fast mass transfer rate, and matched band gap. The mechanism and electronic structure can also be well revealed by the theoretical calculation.

Induced electron transfer and morphology design for enhanced photocatalytic hydrogen production of carbon nitride nanomaterials

ACS Fall 2020 Virtual Meeting

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