Tailoring the edge defects and morphology of g-C3N4 for efficient CO2 conversion to cyclic carbonates

IF 4 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Structure Pub Date : 2025-06-11 DOI:10.1016/j.molstruc.2025.142982

Jiale Ni, Zicheng Yang, Binxuan Hong, Yi Feng, Jianfeng Yao

{"title":"Tailoring the edge defects and morphology of g-C3N4 for efficient CO2 conversion to cyclic carbonates","authors":"Jiale Ni, Zicheng Yang, Binxuan Hong, Yi Feng, Jianfeng Yao","doi":"10.1016/j.molstruc.2025.142982","DOIUrl":null,"url":null,"abstract":"<div><div>This research endeavors to optimize the morphology and edge defects of g-C3N4 through straightforward pyrolysis of rationally chosen precursors, with the objective of increasing the CO2 conversion efficiency. Our findings reveal that employing melamine and urea as precursors yields tubular g-C3N4 (CN tube), featuring an increased surface area and a greater density of edge defects than melamine-derived bulk g-C3N4 and urea-derived layered g-C3N4. As a result, the obtained CN tube can deliver an impressive yield of 98 % for CO2 cycloaddition with epichlorohydrin at 12 h under mild conditions of 80 °C and 0.1 MPa CO2 pressure, significantly outperforming those derived from melamine (53 %) or urea (66 %) alone. This investigation demonstrated the pivotal role of a tubular architecture and enriched edge defects in facilitating the thermally driven CO2 fixation process to produce cyclic carbonates.</div></div>","PeriodicalId":16414,"journal":{"name":"Journal of Molecular Structure","volume":"1344 ","pages":"Article 142982"},"PeriodicalIF":4.0000,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Structure","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022286025016552","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

This research endeavors to optimize the morphology and edge defects of g-C₃N₄ through straightforward pyrolysis of rationally chosen precursors, with the objective of increasing the CO₂ conversion efficiency. Our findings reveal that employing melamine and urea as precursors yields tubular g-C₃N₄ (CN tube), featuring an increased surface area and a greater density of edge defects than melamine-derived bulk g-C₃N₄ and urea-derived layered g-C₃N₄. As a result, the obtained CN tube can deliver an impressive yield of 98 % for CO₂ cycloaddition with epichlorohydrin at 12 h under mild conditions of 80 °C and 0.1 MPa CO₂ pressure, significantly outperforming those derived from melamine (53 %) or urea (66 %) alone. This investigation demonstrated the pivotal role of a tubular architecture and enriched edge defects in facilitating the thermally driven CO₂ fixation process to produce cyclic carbonates.

查看原文本刊更多论文

调整g-C3N4的边缘缺陷和形态，以有效地将二氧化碳转化为循环碳酸盐

本研究通过合理选择前驱体的直接热解，优化g-C3N4的形貌和边缘缺陷，以提高CO2转化效率。我们的研究结果表明，采用三聚氰胺和尿素作为前体制备的管状g-C3N4 （CN管）比三聚氰胺衍生的块状g-C3N4和尿素衍生的层状g-C3N4具有更大的表面积和更大的边缘缺陷密度。结果表明，在80°C和0.1 MPa CO2压力的温和条件下，与环氧氯丙烷进行12 h的CO2环加成反应，CN管的收率达到98%，明显优于单独使用三聚氰胺（53%）或尿素（66%）的CN管。该研究证明了管状结构和富集的边缘缺陷在促进热驱动CO2固定过程中产生环状碳酸盐的关键作用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Molecular Structure 化学-物理化学

CiteScore

7.10

自引率

15.80%

发文量

2384

审稿时长

45 days

期刊介绍： The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.