As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

Semiconductor-based photocatalysis is considered to be an attractive way for solving the worldwide energy shortage and environmental pollution issues. Since the pioneering work in 2009 on graphitic carbon nitride (g-C3N4) for visible-light photocatalytic water splitting, g-C3N4 -based photocatalysis has become a very hot research topic. This review summarizes the recent progress regarding the design and preparation of g-C3N4 -based photocatalysts, including the fabrication and nanostructure design of pristine g-C3N4 , bandgap engineering through atomic-level doping and molecular-level modification, and the preparation of g-C3N4 -based semiconductor composites. Also, the photo-catalytic applications of g-C3N4 -based photocatalysts in the fields of water splitting, CO2 reduction, pollutant degradation, organic syntheses, and bacterial disinfection are reviewed, with emphasis on photocatalysis promoted by carbon materials, non-noble-metal cocatalysts, and Z-scheme heterojunctions. Finally, the concluding remarks are presented and some perspectives regarding the future development of g-C3N4 -based photocatalysts are highlighted.

Polymeric Photocatalysts Based on Graphitic Carbon Nitride

A review on g-C3N4-based photocatalysts

Graphitic carbon nitride (g-C3N4), as an intriguing earth-abundant visible light photocatalyst, possesses a unique two-dimensional structure, excellent chemical stability and tunable electronic structure. Pure g-C3N4 suffers from rapid recombination of photo-generated electron–hole pairs resulting in low photocatalytic activity. Because of the unique electronic structure, the g-C3N4 could act as an eminent candidate for coupling with various functional materials to enhance the performance. According to the discrepancies in the photocatalytic mechanism and process, six primary systems of g-C3N4-based nanocomposites can be classified and summarized: namely, the g-C3N4 based metal-free heterojunction, the g-C3N4/single metal oxide (metal sulfide) heterojunction, g-C3N4/composite oxide, the g-C3N4/halide heterojunction, g-C3N4/noble metal heterostructures, and the g-C3N4 based complex system. Apart from the depiction of the fabrication methods, heterojunction structure and multifunctional application of the g-C3N4-based nanocomposites, we emphasize and elaborate on the underlying mechanisms in the photocatalytic activity enhancement of g-C3N4-based nanocomposites. The unique functions of the p–n junction (semiconductor/semiconductor heterostructures), the Schottky junction (metal/semiconductor heterostructures), the surface plasmon resonance (SPR) effect, photosensitization, superconductivity, etc. are utilized in the photocatalytic processes. Furthermore, the enhanced performance of g-C3N4-based nanocomposites has been widely employed in environmental and energetic applications such as photocatalytic degradation of pollutants, photocatalytic hydrogen generation, carbon dioxide reduction, disinfection, and supercapacitors. This critical review ends with a summary and some perspectives on the challenges and new directions in exploring g-C3N4-based advanced nanomaterials.

Graphitic carbon nitride based nanocomposites: a review

Graphitic carbon nitride, g-C3N4, is a polymeric material consisting of C, N, and some impurity H, connected via tris-triazine-based patterns. Compared with the majority of carbon materials, it has electron-rich properties, basic surface functionalities and H-bonding motifs due to the presence of N and H atoms. It is thus regarded as a potential candidate to complement carbon in material applications. In this review, a brief introduction to g-C3N4 is given, the methods used for synthesizing this material with different textural structures and surface morphologies are described, and its physicochemical properties are referred. In addition, four aspects of the applications of g-C3N4 in catalysis are discussed: (1) as a base metal-free catalyst for NO decomposition, (2) as a reference material in differentiating oxygen activation sites for oxidation reactions over supported catalysts, (3) as a functional material to synthesize nanosized metal particles, and (4) as a metal-free catalyst for photocatalysis. Th...

Graphitic Carbon Nitride: Synthesis, Properties, and Applications in Catalysis

Palladium modified mesoporous graphitic carbon nitride polymer (Pd/mpg-C 3 N 4 ) was fabricated and used for the degradation of bisphenol A (BPA) in water. Doping Pd on the surface of mpg-C 3 N 4 enhanced the light absorbance in the range of UV–vis region. Most of the embedded Pd was present as Pd 0 and could act as electron traps and facilitate the separation of photogenerated holes and electron pairs. As a result, the photocatalytic performance was improved significantly. The reaction rate constant ( k obs ) increased with the Pd loading on the surface of mpg-C 3 N 4 and the maximum was achieved with 1.50% Pd. Almost 100% of BPA (20 mg L −1 ) was photodegraded by the solids of 0.5 g L −1 Pd/mpg-C 3 N 4 after irradiation with simulated solar light for 360 min. The Pd/mpg-C 3 N 4 exhibited very stable and high efficient photocatalytic activity to BPA in a wide range of pH 3.08–11.00. It also displayed high photocatalytic activity without photocorrosion after reuse for many times. Hydroxyl radicals, photogenerated holes, and superoxide radical species were responsible for the photodegradation while the superoxide radical species were more predominant in the Pd/mpg-C 3 N 4 reaction system.

Photodegradation of bisphenol A by highly stable palladium-doped mesoporous graphite carbon nitride (Pd/mpg-C3N4) under simulated solar light irradiation

The integration of cathodic hydrogen evolution reaction (HER) with thermodynamically favorable anodic oxidation reactions offers a sustainable alternative for electrochemical valorization. Herein, the atomic Ni modified CoP electrocatalyst featuring an elaborate ordered macroporous superstructure with abundant built-in mesopores has been developed from the ordered macroporous ZIF-67 single crystals, of which the distinctive structural advantages lead to a high HER performance. When the catalyst further underwent an electrochemical reconstruction, an outstanding activity with high Faradaic efficiency up to 96% of formate for ethylene glycol oxidation reaction (EGOR) can be afforded in alkaline electrolyte, as well as in the complex electrolyte of polyethylene terephthalate (PET) plastic hydrolysate. Remarkably, an exotic energy-saving pair-electrolysis system coupling HER and EGOR was explored in the PET plastic hydrolysate by employing this bifunctional electrocatalyst for concurrent H 2 and commodity chemical production. Our work may showcase the rational structural engineering of advanced electrocatalysts for multiple electrochemical applications. • Atomic Ni-modified CoP electrocatalyst with ordered macroporous superstructure was prepared. • A low overpotential of 119 mV @ 10 mA cm −2 for alkaline HER can be achieved. • A high formate Faradaic efficiency of 96 % for EGOR can be obtained. • An energy-saving pair-electrolysis system was explored for concurrent H 2 production and PET plastic upcycling. 

Ordered Macroporous Superstructure of Bifunctional Cobalt Phosphide With Heteroatomic Modification for Paired Hydrogen Production and Polyethylene Terephthalate Plastic Recycling

The heterogenized metallomacrocycles with atomically dispersed active sites are identified as the promising candidates for electrocatalytic CO2 reduction reaction (CO2RR), where their unique heterointerface with interaction between sp2 carbon and macrocyclic molecules is important but remains vague. Herein, based on well-structured nickel phthalocyanine and porphyrin with the same functional groups (MeNiPc and MeNiPp), the influences of heterointerfacial effect on catalytic performances are systematically disclosed. Through the molecular structure-induced self-adaptive adsorption with optimized heterointerfacial distance, MeNiPc/graphene reveals a high CO Faradaic efficiency of ~99% in a wide potential window, greatly outperforming the MeNiPp/graphene counterpart (≤29.6%). Detailed measurements and theoretical calculations decipher that the higher CO2RR activity of MeNiPc/graphene is attributed to the unique electronic structures of the Ni-N4 configurations suitable for well-suited heterointerfacial charge transfer and rapid CO desorption. Additionally, the extended research confirms the universality of heterointerface engineering on boosting the catalytic performances. 

New insight into heterointerfacial effect for heterogenized metallomacrocycle catalysts in executing electrocatalytic CO2 reduction

Heterointerface engineering of Ru/RuS2 on N/S-doped hollow mesoporous carbon for promoting alkaline hydrogen evolution

Surveying the electrocatalytic CO2-to-CO activity of heterogenized metallomacrocycles via accurate clipping at the molecular level

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