Semiconductor polymeric graphitic carbon nitride (g-C3N4) photocatalysts have attracted dramatically growing attention in the field of the visible-light-induced hydrogen evolution reaction (HER) because of their facile synthesis, easy functionalization, attractive electronic band structure, high physicochemical stability and photocatalytic activity. This review article presents a panorama of the latest advancements in the rational design and development of g-C3N4 and g-C3N4-based composite photocatalysts for HER application. Concretely, the review starts with the development history, synthetic strategy, electronic structure and physicochemical characteristics of g-C3N4 materials, followed by the rational design and engineering of various nanostructured g-C3N4 (e.g. thinner, highly crystalline, doped, and porous g-C3N4) photocatalysts for HER application. Then a series of highly efficient g-C3N4 (e.g., metal/g-C3N4, semiconductor/g-C3N4, metal organic framework/g-C3N4, carbon/g-C3N4, conducting polymer/g-C3N4, sensitizer/g-C3N4) composite photocatalysts are exemplified. Lastly, this review provides a comprehensive summary and outlook on the major challenges, opportunities, and inspiring perspectives for future research in this hot area on the basis of pioneering works. It is believed that the emerging g-C3N4-based photocatalysts will act as the “holy grail” for highly efficient photocatalytic HER under visible-light irradiation.

Semiconductor polymeric graphitic carbon nitride photocatalysts: the “holy grail” for the photocatalytic hydrogen evolution reaction under visible light

Polymeric carbon nitride (C3N4) has emerged as the most promising candidate for metal-free photocatalysts but is plagued by low activity due to the poor quantum efficiency and low specific surface area. Exfoliation of bulk crystals into ultrathin nanosheets has proven to be an effective and widely used strategy for enabling high photocatalytic performances; however, this process is complicated, time-consuming, and costly. Here, we report a simple bottom-up method to synthesize porous few-layer C3N4, which involves molecule self-assembly into layered precursors, alcohol molecules intercalation, and subsequent thermal-induced exfoliation and polycondensation. The as-prepared few-layer C3N4 expose more active sites and greatly enhance the separation of charge carriers, thus exhibiting a 26-fold higher hydrogen evolution activity than bulk counterpart. Furthermore, we find that both the high activity and selectivity for the oxidative coupling of amines to imines can be obtained under visible light that surpass those of other metal-free photocatalysts so far.

Molecule Self-Assembly Synthesis of Porous Few-Layer Carbon Nitride for Highly Efficient Photoredox Catalysis.

Three-dimensional porous g-C3N4 for highly efficient photocatalytic overall water splitting

Tri-s-triazine-based crystalline carbon nitride nanosheets (CCNNSs) have been successfully extracted via a conventional and cost-effective sonication-centrifugation process. These CCNNSs possess a highly defined and unambiguous structure with minimal thickness, large aspect ratios, homogeneous tri-s-triazine-based units, and high crystallinity. These tri-s-triazine-based CCNNSs show significantly enhanced photocatalytic hydrogen generation activity under visible light than g-C3 N4 , poly (triazine imide)/Li+ Cl- , and bulk tri-s-triazine-based crystalline carbon nitrides. A highly apparent quantum efficiency of 8.57% at 420 nm for hydrogen production from aqueous methanol feedstock can be achieved from tri-s-triazine-based CCNNSs, exceeding most of the reported carbon nitride nanosheets. Benefiting from the inherent structure of 2D crystals, the ultrathin tri-s-triazine-based CCNNSs provide a broad range of application prospects in the fields of bioimaging, and energy storage and conversion.

Tri-s-triazine-Based Crystalline Carbon Nitride Nanosheets for an Improved Hydrogen Evolution.

2D Nanomaterials, with unique structural and electronic features, have shown enormous potential toward photocatalysis fields. However, the photocatalytic behavior of pristine 2D photocatalysts are still unsatisfactory, and far below the requirements of practical applications. In this regard, surface defect engineering can serve as an effective means to tune photoelectric parameters of 2D photocatalysts through tailoring the local surface microstructure, electronic structure, and carrier concentration. In this review, recent progress in the design of surface defects with the classified anion vacancy, cation vacancy, vacancy associates, pits, distortions, and disorder on 2D photocatalysts to boost the photocatalytic performance is summarized. The strategies for controlling defects formation and technique to distinguish various surface defects are presented. The crucial roles of surface defects for photocatalysis performance optimization are proposed and advancement of defective 2D photocatalysts toward versatile applications such as water oxidation, hydrogen production, CO2 reduction, nitrogen fixation, organic synthesis, and pollutants removal are discussed. Surface defect modulated 2D photocatalysts thus represent a powerful configuration for further development toward photocatalysis.

Surface Defect Engineering in 2D Nanomaterials for Photocatalysis

Dr. Y. F. Li, Dr. R. X. Jin, Prof. Y. Xing, Dr. X. C. Liu Jilin Provincial Key Laboratory of Advanced Energy Materials Department of Chemistry Northeast Normal University Changchun 130024, P. R. China E-mail: xingy202@nenu.edu.cn Dr. J. Q. Li, Dr. S. Y. Song State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022, P. R. China E-mail: songsy@ciac.ac.cn Prof. M. Li Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission & Ministry of Education South-Central University for Nationalities Wuhan 430074, P. R. China Prof. R. C. Jin Department of Chemistry Carnegie Mellon University Pittsburgh, PA 15213, USA

Macroscopic Foam‐Like Holey Ultrathin g‐C3N4 Nanosheets for Drastic Improvement of Visible‐Light Photocatalytic Activity

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Macroscopic Foam‐Like Holey Ultrathin g‐C3N4 Nanosheets for Drastic Improvement of Visible‐Light Photocatalytic Activity