物理化学学报 >> 2024, Vol. 40 >> Issue (11): 2406026.doi: 10.3866/PKU.WHXB202406026

所属专题： 太阳燃料制备

论文 上一篇    下一篇

4-氨基-1H-咪唑-5-甲腈修饰供体-受体型氮化碳光催化剂的构建及其高效光催化产氢研究

程敬招1,2, 高诗语1,2, 程蓓1,2, 杨凯3, 王往1,2,*(), 曹少文1,2,*()   

  1. 1 武汉理工大学, 材料复合新技术国家重点实验室, 武汉 430070
    2 武汉理工大学, 湖北省先进复合材料技术创新中心, 武汉 430070
    3 江西理工大学, 化学化工学院, 江西 赣州 341000
  • 收稿日期:2024-06-20 修回日期:2024-07-25 录用日期:2024-07-26 发布日期:2024-10-14
  • 通讯作者: Email: doublewang@whut.edu.cn (王往)swcao@whut.edu.cn (曹少文)
  • 基金资助:
    国家重点研发计划项目(2022YFE0114800); 国家自然科学基金项目(22278324); 国家自然科学基金项目(52073223); 江西省“双千”人才培养计划项目(jxsq2023102141)

Construction of 4-Amino-1H-imidazole-5-carbonitrile Modified Carbon Nitride-Based Donor-Acceptor Photocatalyst for Efficient Photocatalytic Hydrogen Evolution

Jingzhao Cheng1,2, Shiyu Gao1,2, Bei Cheng1,2, Kai Yang3, Wang Wang1,2,*(), Shaowen Cao1,2,*()   

  1. 1 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
    2 Hubei Technology Innovation Center for Advanced Composites, Wuhan University of Technology, Wuhan 430070, China
    3 School of Chemistry and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China
  • Received:2024-06-20 Revised:2024-07-25 Accepted:2024-07-26 Published:2024-10-14
  • Contact: Email: doublewang@whut.edu.cn (Wang Wang)swcao@whut.edu.cn (Shaowen Cao)
  • Supported by:
    the National Key R&D Program of China(2022YFE0114800); the National Natural Science Foundation of China(22278324); the National Natural Science Foundation of China(52073223); the Jiangxi Province "Double Thousand" Talent Training Plan(jxsq2023102141)

RichHTML

8

PDF

586

赞

补充材料

1

摘要：

太阳能驱动光催化水分解制氢被认为是解决能源危机和环境污染挑战的一种极具前景的策略。光催化剂的电子性质和能带结构的调控对于提高电荷分离效率和产氢活性至关重要。基于此，本文通过将4-氨基-1H-咪唑-5-甲腈(AICN)引入氮化碳(CN)的分子骨架中，制备了基于供体-受体修饰的氮化碳共聚物。CN中掺入电子供体AICN单元可以拓宽π共轭体系并促进空间电荷分离，从而增强了光利用率并且提高了分子内电荷载流子传输速率。因此，AICN修饰的CN样品表现出更高的光催化产氢速率，最佳光催化活性可达3204 μmol·h−1·g−1。这项分子工程策略为开发高性能的氮化碳基产氢光催化剂提供了一条有效途径。

关键词: 氮化碳, 供体-受体, 分子修饰, 电荷分离, 产氢

Abstract:

Photocatalytic hydrogen generation through water splitting driven by solar energy is regarded as a highly promising strategy to tackle the challenges of the energy crisis and environmental contamination. Tuning the electronic properties and band structures of photocatalysts is critical to improving the efficiency of charge separation and the activity of hydrogen production. Herein, donor-acceptor modified polymeric carbon nitride (CN)-based copolymers are synthesized via the introduction of 4-amino-1H-imidazole-5-carbonitrile (AICN) into the molecular skeleton of CN. The incorporation of electron donor AICN units can broaden the π-conjugated system and promote the spatial charge separation in the catalysts, thus resulting in enhanced light utilization and improved intramolecular charge carrier transfer rate. As a consequence, the AICN modified CN samples exhibit an increased photocatalytic hydrogen evolution rate, and the optimal photocatalytic activity can reach 3204 μmol·h−1·g−1. This molecular engineering strategy provides an effective avenue to develop high-performance CN-based photocatalysts for hydrogen evolution.

Key words: Polymeric carbon nitride, Donor-acceptor, Molecular modification, Charge separation, Hydrogen production