物理化学学报 >> 2024, Vol. 40 >> Issue (11): 2406021.doi: 10.3866/PKU.WHXB202406021

所属专题: 太阳燃料制备

论文 上一篇    下一篇

熔融中间体运输导向合成富氨基g-C3N4纳米片用于高效光催化产H2O2

陈郭强1, 郑子璇1, 钟威2, 王国宏1, 吴新鹤1,*()   

  1. 1 湖北师范大学化学化工学院污染物分析与资源化技术湖北省重点实验室, 湖北 黄石 435002
    2 深圳技术大学新材料与新能源学院, 广东 深圳 518118
  • 收稿日期:2024-06-17 修回日期:2024-07-15 录用日期:2024-07-16 发布日期:2024-10-14
  • 通讯作者: Email: wuxinhe@hbnu.edu.cn; Tel.: +86-714-6515602 (吴新鹤)
  • 基金资助:
    国家自然科学基金(22302061); 国家自然科学基金(22075072); 湖北省自然科学基金(2022CFC060); 2023年国家级大学生创新创业训练计划(202324)

Molten Intermediate Transportation-Oriented Synthesis of Amino-Rich g-C3N4 Nanosheets for Efficient Photocatalytic H2O2 Production

Guoqiang Chen1, Zixuan Zheng1, Wei Zhong2, Guohong Wang1, Xinhe Wu1,*()   

  1. 1 Hubei Key Laboratory of Pollutant Analysis and Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002, Hubei Province, China
    2 College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, Guangdong Province, China
  • Received:2024-06-17 Revised:2024-07-15 Accepted:2024-07-16 Published:2024-10-14
  • Contact: Email: wuxinhe@hbnu.edu.cn; Tel.: +86-714-6515602 (Xinhe Wu)
  • Supported by:
    the National Natural Science Foundation of China(22302061); the National Natural Science Foundation of China(22075072); Hubei Provincial Natural Science Foundation of China(2022CFC060); the 2023 National Undergraduate Training Programs for Innovation and Entrepreneurship(202324)

摘要:

为避免使用当前g-C3N4纳米片合成策略中的外加辅助,如模板、强酸、强碱等,本研究设计了一种g-C3N4熔融中间体运输的创新模式,在没有任何外加物质辅助情况下,成功一步合成富含氨基g-C3N4纳米片。该创新模式具体包括先将三聚氰胺放置在倒置坩埚的顶部平台上,随后进行一步煅烧。在煅烧过程中,三聚氰胺及其随后形成的g-C3N4中间体转变为熔融状态,并沿倒置坩埚外表面逐渐向下流动。这种熔融中间体运输模式可以有效减少其团聚,并使其依次分批聚合成富含氨基的g-C3N4纳米片。此外,所得富氨基g-C3N4纳米片的光催化产H2O2速率显著提高,约为85.8 μmol·L–1·h–1,是传统块体g-C3N4的2倍,这主要是因为除了其纳米片结构具有较大的比表面积外,富氨基结构可以有效增强对O2原料和*OOH中间体的吸附,并加速*OOH高效转化为H2O2。该探究提供了一种创新模式来合成富含氨基的g-C3N4纳米片,并深入探究了其光催化机理。

关键词: 光催化, 氮化碳纳米片, 富氨基, 中间体运输, 产过氧化氢

Abstract:

To eliminate the additional assistance of previously reported strategies for the synthesis of g-C3N4 nanosheets such as templates, strong acids and alkalis, in this study, an innovative pattern for transportation of molten g-C3N4 intermediates, without any additional substance assistance, has been resoundingly established to produce amino-rich g-C3N4 nanosheets. The innovative pattern concretely contains the preliminary placement of melamine onto the top platform of an inverted crucible and their subsequent one-step calcination. During the calcination process, melamine and its subsequently formed g-C3N4 intermediate can transform into a molten state and gradually stream down along the outer surface of inverted crucible. This molten intermediate transportation pattern contributes to remarkably resist severe aggregation, resulting in the final polymerization into amino-rich g-C3N4 nanosheets in sequence. Moreover, the resultant amino-rich g-C3N4 nanosheets exhibit an evidently enhanced photocatalytic H2O2-production rate of ca. 85.8 μmol·L–1·h–1, over 2 times superior to bulk g-C3N4, mainly due to the fact that in addition to their nanosheet structures with enhanced specific surface areas, their amino-rich structures can efficiently reinforce the adsorption of O2 and *OOH intermediates to accelerate their effective transformation into H2O2. This work delivers an innovative pattern to synthesize amino-rich g-C3N4 nanosheets with an insight into the photocatalytic mechanism.

Key words: Photocatalysis, g-C3N4 nanosheets, Amino-rich, Intermediate transportation, H2O2 production