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One of the most frequent ways to widen the adsorption range of carbon nitride (CN) is to add a well-known photosensitizer into its basic structure. So far, such attachments have been accomplished by using weak van der Waals forces. However, using strong covalent bonding to attach such photosensitizer with CN is yet to be determined. Here, for the first time, we covalently bonded porphyrin (5,10,15,20-tetrakis(4-(2,4-diamino-1,3,5-triazinyl) phenyl)-Porphyrin (TDP)), a renowned photosensitizer, effectively with CN by thermally balanced molecular strategy. A photoreaction system was set up for the deoxygenated conversion of CO2 to CO under visible light, where cobalt acted as a redox controller to speed up the charge transportation, while CN-TDP worked as a CO2 activating photocatalyst. The subsequent photocatalyst has a broader absorbance range, a greater specific surface area, and intramolecular organic connections that help to decrease the electron-hole pairs’ recombination rate. Furthermore, the average weight ratio between urea and TDP was well-tuned, resulting in a fantastic CO2 photoconversion for CN-TDP7.0 compared to the blank sample. This substantial increase in photocatalytic activity predicts a significant shift in CN’s specific surface area, band gap, chemical composition, and structure, as well as the efficient separation of photogenerated charge carriers from the ground state (HOMO) to the excited state (LUMO), making it a top candidate for CO2 photoreduction. At the same time, this approach paves the path for the bottom-up fabrication of carbon nitride nanosheets.

Being one of the foremost enticing and intriguing innovations, heterogeneous photocatalysis has also been used to effectively gather, transform, and conserve sustainable sun‘s radiation for the production of efficient and clean fossil energy as well as a wide range of ecological implications. The generation of solar fuel‐based water splitting and CO2 photoreduction is excellent for generating alternative resources and reducing global warming. Developing an inexpensive photocatalyst can effectively split water into hydrogen (H2), oxygen (O2) sources, and carbon dioxide (CO2) into fuel sources, which is a crucial problem in photocatalysis. The metal‐free g‐C3N4 photocatalyst has a high solar fuel generation potential. This review covers the most recent advancements in g‐C3N4 preparation, including innovative design concepts and new synthesis methods, and novel ideas for expanding the light absorption of pure g‐C3N4 for photocatalytic application. Similarly, the main issue concerning research and prospects in photocatalysts based g‐C3N4 was also discussed. The current dissertation provides an overview of comprehensive understanding of the exploitation of the extraordinary systemic and characteristics, as well as the fabrication processes and uses of g‐C3N4.

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Light-driven heterogeneous photocatalysis has gained great significance for generating solar fuel; the challenging charge separation process and sluggish surface catalytic reactions significantly restrict the progress of solar energy conversion using a semiconductor photocatalyst. Herein, we propose a novel and feasible strategy to incorporate dihydroxy benzene (DHB) as a conjugated monomer within the framework of urea containing CN (CNU-DHBx) to tune the electronic conductivity and charge separation due to the aromaticity of the benzene ring, which acts as an electron-donating species. Systematic characterizations such as SPV, PL, XPS, DRS, and TRPL demonstrated that the incorporation of the DHB monomer greatly enhanced the photocatalytic CO2 reduction of CN due to the enhanced charge separation and modulation of the ionic mobility. The significantly enhanced photocatalytic activity of CNU–DHB15.0 in comparison with parental CN was 85 µmol/h for CO and 19.92 µmol/h of the H2 source. It can be attributed to the electron–hole pair separation and enhance the optical adsorption due to the presence of DHB. Furthermore, this remarkable modification affected the chemical composition, bandgap, and surface area, encouraging the controlled detachment of light-produced photons and making it the ideal choice for CO2 photoreduction. Our research findings potentially offer a solution for tuning complex charge separation and catalytic reactions in photocatalysis that could practically lead to the generation of artificial photocatalysts for efficient solar energy into chemical energy conversion.

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Summary Conjugated monomer 2,6‐dimethylindole (DMI) was integrated into the triazine framework of polymeric carbon nitride (PCN) via molecular engineering. As‐prepared samples were utilized for photocatalytic evolution of hydrogen (H2) through water splitting and photodegradation of RhB dye under visible light. The integration of this monomer DMI has been dominated within the internal framework of PCN and operated as a substitution reaction membrane, retarding an appropriate control and promote the charge density in π‐electron conjugated system. It also promotes the charge transferring and separation to elevate the photocatalytic activity of PCN under visible light. The HER for pure PCN was found as 77.9 μmol/h, while for PCN‐DMI18.0 was predicted at 701.2 μmol/h, which is exclusively output approximately nine times higher than that of pure PCN respectively. Besides, the pseudo‐order kinetic constant of PCN‐DMI18.0 degradation of RhB was multiple times higher when contrasted to pristine PCN.

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