化工进展 ›› 2024, Vol. 43 ›› Issue (7): 4148-4154.DOI: 10.16085/j.issn.1000-6613.2023-0988

• 资源与环境化工 • 上一篇    

具有碳空位超薄g-C3N4纳米片可见光下产过氧化氢

石家汀(), 王辉, 蒲凯凯, 赵婷, 聂丽君, 郑娜, 高宇航, 薛坤坤, 石建惠()   

  1. 太原理工大学环境科学与工程学院,山西 太原 030024
  • 收稿日期:2023-06-16 修回日期:2023-07-20 出版日期:2024-07-10 发布日期:2024-08-14
  • 通讯作者: 石建惠
  • 作者简介:石家汀(1998—),女,硕士研究生,研究方向为光催化产过氧化氢。E-mail:shijiating313@163.com
  • 基金资助:
    国家自然科学基金(52100101)

Enhanced hydrogen peroxide production performance in visible light from ultra-thin g-C3N4 nanosheets with carbon vacancies

SHI Jiating(), WANG Hui, PU Kaikai, ZHAO Ting, NIE Lijun, ZHENG Na, GAO Yuhang, XUE Kunkun, SHI Jianhui()   

  1. College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2023-06-16 Revised:2023-07-20 Online:2024-07-10 Published:2024-08-14
  • Contact: SHI Jianhui

摘要:

光催化产过氧化氢(H2O2)作为一种绿色可持续发展技术,相比于工业上常用的蒽醌法,具有清洁无污染、安全、低能耗及低成本等优点。石墨相氮化碳(g-C3N4)作为一种无机非金属材料,是一种很有前景的产H2O2光催化剂。然而,块体g-C3N4存在光生电子空穴复合严重以及光生电荷迁移能力弱等问题,导致其光催化产H2O2效率低。为了提高g-C3N4的光催化产H2O2活性。本文通过简单的连续两步高温煅烧制备了含有碳空位的超薄g-C3N4纳米片(CNS580),通过X射线衍射仪、扫描电子显微镜、原子力显微镜、电子顺磁共振仪、紫外可见漫反射、瞬态光电流、电化学阻抗谱测试等对光催化剂进行了一系列的结构形貌、光吸收性能以及电化学性能表征。结果表明,该光催化剂具有超薄纳米片结构,厚度约为2.15nm,可提高光生电荷的传输效率;同时引入的碳空位可捕获光生电子,这将改善其光生电子空穴的分离能力。在光催化产H2O2的实验中,CNS580光催化反应6h,其产H2O2浓度可达到0.091mmol/L,是块体g-C3N4的4.13倍。此外,讨论并提出CNS580光催化产H2O2可能的机理。

关键词: 石墨相氮化碳, 超薄纳米片, 碳空位, 可见光, 过氧化氢

Abstract:

Photocatalytic production of hydrogen peroxide (H2O2), as a green and sustainable technology, has the advantages of clean and pollution-free, safety, low energy consumption and low cost compared with the anthraquinone method commonly used in industry. Graphitic phase carbon nitride (g-C3N4), as an inorganic nonmetallic material, is a promising H2O2 producing photocatalyst. However, bulk g-C3N4 suffers from severe photogenerated electrons-holes complexation and weak photogenerated charge transfer ability, resulting in its low photocatalytic H2O2 production efficiency. In order to improve the photocatalytic H2O2 production activity of g-C3N4, ultrathin g-C3N4 nanosheets containing carbon vacancies (CNS580) were prepared by simple sequential two-step high-temperature calcination in this paper, and the structure and morphology, light absorption properties and electrochemical properties of photocatalysts were characterized by XRD, SEM, AFM, ESR, UV-Vis, TPC and EIS. The results showed that the photocatalyst had an ultrathin nanosheet structure with a thickness of about 2.15nm, which could improve the transmission efficiency of photogenerated charge. Meanwhile, the introduced carbon vacancies could capture photogenerated electrons, which would improve its photogenerated electrons-holes separation ability. In the experiment of photocatalytic H2O2 production, the H2O2 production concentration by CNS580via photocatalytic reaction for 6h could reach 0.091mmol/L, which was 4.13 times higher than that of the bulk g-C3N4. In addition, the possible mechanism of photocatalytic H2O2 production for CNS580 was discussed and proposed.

Key words: graphitic phase carbon nitride, ultra-thin nanosheets, carbon vacancy, visible light, hydrogen peroxide

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