{"title":"一种新型氮掺杂多孔碳负载g-C3N4复合材料增强光催化CO2转化","authors":"Roopesh Mekkat , Edith Mawunya Kutorglo , Milena Setka , Andrey. Prokhorov , Miroslav Šoóš","doi":"10.1016/j.jphotochem.2025.116454","DOIUrl":null,"url":null,"abstract":"<div><div>The solar light-driven CO<sub>2</sub> conversion into hydrocarbon fuels is regarded as one of the most crucial inventions to reduce CO<sub>2</sub> abundance in the atmosphere and fulfill energy needs. Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) has garnered considerable attention and emerges as a promising candidate for photocatalytic CO<sub>2</sub> reduction, owing to its visible light absorption, metal-free, and environmentally benign nature. However, its ability to effectively achieve this is currently hindered by several factors such as relatively low surface area, fast electron-hole recombination rate and limited CO<sub>2</sub> adsorption capacity, which also constrain its practical applicability. In this work, a novel photocatalyst was synthesized by incorporating a suitable amount of ZIF-8 derived N-doped porous carbon into g-C<sub>3</sub>N<sub>4</sub> without affecting its light absorption capacity. The as-prepared samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), nitrogen and CO<sub>2</sub> adsorption measurements, X-ray photoelectron spectroscopy (XPS), UV–Vis diffuse reflectance absorption spectra (UV-DRS), and photoluminescence spectroscopy (PL). Compared to g-C<sub>3</sub>N<sub>4</sub>, the optimized photocatalyst exhibited a 54-fold increase in surface area, a 3.5-fold enhancement in CO<sub>2</sub> adsorption capacity, a reduced optical bandgap, and significantly superior photocatalytic activity for CO<sub>2</sub> reduction, achieving CH<sub>4</sub> production at 70.87 μmol h<sup>−1</sup> g<sup>−1</sup> and C<sub>2</sub>H<sub>6</sub> production at 35.31 μmol h<sup>−1</sup> g<sup>−1</sup>. The enhanced activity of the composites is attributed to the synergistic effect of the N-doped carbon and g-C<sub>3</sub>N<sub>4</sub>. Thus, this approach offers a promising strategy for the future development of C<sub>3</sub>N<sub>4</sub>-based catalysts for efficient solar to fuel conversion.</div></div>","PeriodicalId":16782,"journal":{"name":"Journal of Photochemistry and Photobiology A-chemistry","volume":"467 ","pages":"Article 116454"},"PeriodicalIF":4.1000,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A novel N-doped porous carbon-supported g-C3N4 composite for enhanced photocatalytic CO2 conversion\",\"authors\":\"Roopesh Mekkat , Edith Mawunya Kutorglo , Milena Setka , Andrey. Prokhorov , Miroslav Šoóš\",\"doi\":\"10.1016/j.jphotochem.2025.116454\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The solar light-driven CO<sub>2</sub> conversion into hydrocarbon fuels is regarded as one of the most crucial inventions to reduce CO<sub>2</sub> abundance in the atmosphere and fulfill energy needs. Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) has garnered considerable attention and emerges as a promising candidate for photocatalytic CO<sub>2</sub> reduction, owing to its visible light absorption, metal-free, and environmentally benign nature. However, its ability to effectively achieve this is currently hindered by several factors such as relatively low surface area, fast electron-hole recombination rate and limited CO<sub>2</sub> adsorption capacity, which also constrain its practical applicability. In this work, a novel photocatalyst was synthesized by incorporating a suitable amount of ZIF-8 derived N-doped porous carbon into g-C<sub>3</sub>N<sub>4</sub> without affecting its light absorption capacity. The as-prepared samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), nitrogen and CO<sub>2</sub> adsorption measurements, X-ray photoelectron spectroscopy (XPS), UV–Vis diffuse reflectance absorption spectra (UV-DRS), and photoluminescence spectroscopy (PL). Compared to g-C<sub>3</sub>N<sub>4</sub>, the optimized photocatalyst exhibited a 54-fold increase in surface area, a 3.5-fold enhancement in CO<sub>2</sub> adsorption capacity, a reduced optical bandgap, and significantly superior photocatalytic activity for CO<sub>2</sub> reduction, achieving CH<sub>4</sub> production at 70.87 μmol h<sup>−1</sup> g<sup>−1</sup> and C<sub>2</sub>H<sub>6</sub> production at 35.31 μmol h<sup>−1</sup> g<sup>−1</sup>. The enhanced activity of the composites is attributed to the synergistic effect of the N-doped carbon and g-C<sub>3</sub>N<sub>4</sub>. Thus, this approach offers a promising strategy for the future development of C<sub>3</sub>N<sub>4</sub>-based catalysts for efficient solar to fuel conversion.</div></div>\",\"PeriodicalId\":16782,\"journal\":{\"name\":\"Journal of Photochemistry and Photobiology A-chemistry\",\"volume\":\"467 \",\"pages\":\"Article 116454\"},\"PeriodicalIF\":4.1000,\"publicationDate\":\"2025-04-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Photochemistry and Photobiology A-chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1010603025001947\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Photochemistry and Photobiology A-chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1010603025001947","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
A novel N-doped porous carbon-supported g-C3N4 composite for enhanced photocatalytic CO2 conversion
The solar light-driven CO2 conversion into hydrocarbon fuels is regarded as one of the most crucial inventions to reduce CO2 abundance in the atmosphere and fulfill energy needs. Graphitic carbon nitride (g-C3N4) has garnered considerable attention and emerges as a promising candidate for photocatalytic CO2 reduction, owing to its visible light absorption, metal-free, and environmentally benign nature. However, its ability to effectively achieve this is currently hindered by several factors such as relatively low surface area, fast electron-hole recombination rate and limited CO2 adsorption capacity, which also constrain its practical applicability. In this work, a novel photocatalyst was synthesized by incorporating a suitable amount of ZIF-8 derived N-doped porous carbon into g-C3N4 without affecting its light absorption capacity. The as-prepared samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), nitrogen and CO2 adsorption measurements, X-ray photoelectron spectroscopy (XPS), UV–Vis diffuse reflectance absorption spectra (UV-DRS), and photoluminescence spectroscopy (PL). Compared to g-C3N4, the optimized photocatalyst exhibited a 54-fold increase in surface area, a 3.5-fold enhancement in CO2 adsorption capacity, a reduced optical bandgap, and significantly superior photocatalytic activity for CO2 reduction, achieving CH4 production at 70.87 μmol h−1 g−1 and C2H6 production at 35.31 μmol h−1 g−1. The enhanced activity of the composites is attributed to the synergistic effect of the N-doped carbon and g-C3N4. Thus, this approach offers a promising strategy for the future development of C3N4-based catalysts for efficient solar to fuel conversion.
期刊介绍:
JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds.
All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor).
The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.