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We propose an efficient method to synthesize large-scale soluble acidified graphitic carbon nitride (g-C3N4). The as-prepared material exhibits the characteristics of a poly-ammonium salt and is soluble in several solvents with good dissolution-recrystallization reversible equilibrium. The pH value- and temperature-dependent solubility of the acidified g-C3N4 facilitates its separation and purification. After dissolution, acidified g-C3N4 forms isolated ultrathin nanosheets, making it an ideal precursor for large quantities of g-C3N4 nanosheets. This study raises the possibility of liquid assembly for g-C3N4 nanosheets based composite materials, expanding the functionalization and application of g-C3N4.

Ammonia generation through N2 molecule reduction under ambient conditions has attracted tremendous attention because of the enormous energy input and continuous CO2 emissions of the traditional Haber–Bosch process. Photocatalytic and electrocatalytic N2 reduction reaction (NRR) to NH3 production using sustainable energy sources are fascinating approaches to respond to these issues. However, the state-of-the-art photocatalysis and electrocatalysis toward NH3 production is far away from the industrial requirement because of poor catalytic activity. Hence, rationally designed high-efficiency catalysts are urgently demanded to promote practical applications. Polymeric carbon nitride (PCN) has drawn considerable focus because of its unusual properties, such as visible-light response and high pyridinic nitrogen content. This Review provides the most recent progress on constructing PCN-based photocatalysts and electrocatalysts via various design strategies, including vacancy creations, doping, and incorporation, to mediate its applications in NRR. On the basis of theoretical simulations, the insights into mechanism pathways of photocatalytic and electrocatalytic NH3 evolution are presented to provide guidance for engineering PCN-based catalysts. Subsequently, the remaining challenges and future prospects of further development in this research field are also highlighted. It can be foreseen that this Review will shed some light on the development of more potential PCN-based catalysts toward NRR and offer instructive information for further understanding the structure–performance correlations.

We reviewed the recent progress made in fabricating PCN-based catalysts with various morphologies for their applications in energy chemistry.

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Polymeric carbon nitride has been considered to be an active photocathode for catalyzing the generation of H2 through water splitting. However, the application of this material in photoelectrochemical cells remains a challenge owing to the intrinsically sluggish kinetics of charge separation. Herein, a facile salt‐melt method is developed for fabricating Cu‐modified polymeric carbon nitride as an effective photocathode material for solar water splitting. Various characterization data confirm that Cu‐modified polymeric carbon nitride contains both free CuCl, derived from precursors, and coordinated Cu species incorporated into the polymeric carbon nitride, which can generate type‐II heterojunctions. This special heterojunction energy structure contributes to a significantly enhanced photocurrent density for hydrogen evolution. The proposed strategy for synthesizing the Cu‐modified polymeric carbon nitride can stimulate research for the development of highly efficient visible‐light‐active photocathodes.

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