物理化学学报 >> 2025, Vol. 41 >> Issue (6): 100052.doi: 10.1016/j.actphy.2025.100052

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调节O, S共掺杂C3N4中的活性氧生成以促进光催化降解微塑料

罗雅丹1, 郑浩1,2, 李鑫3, 李锋民1,2,*(), 唐华4, 佘希林4,*()   

  1. 1 中国海洋大学环境科学与工程学院，海洋环境与生态教育部重点实验室，海岸环境污染控制研究所，山东 青岛 266100
    2 中国海洋大学三亚海洋研究所, 海南 三亚 572000
    3 华南农业大学, 农业农村部能源植物资源与利用重点实验室, 生物质工程研究所, 广州 510642
    4 青岛大学环境科学与工程学院, 山东 青岛 266071
  • 收稿日期:2024-12-16 修回日期:2025-01-11 录用日期:2025-01-13 发布日期:2025-04-19
  • 通讯作者: Email: xlshe@qdu.edu.cn (佘希林)lifengmin@ouc.edu.cn (李锋民)
  • 基金资助:
    海南省自然科学基金(423CXTD384); 国家自然科学基金(42077115); 山东省杰出青年基金(ZR2021JQ13)

Modulating reactive oxygen species in O, S co-doped C3N4 to enhance photocatalytic degradation of microplastics

Yadan Luo1, Hao Zheng1,2, Xin Li3, Fengmin Li1,2,*(), Hua Tang4, Xilin She4,*()   

  1. 1 Institute of Coastal Environmental Pollution Control, Ministry of Education Key Laboratory of Marine Environment and Ecology, College of Environmental Science and Engineering, Ocean University of China, Qingdao 266100, Shandong Province, China
    2 Sanya Oceanographic Institute, Ocean University of China, Sanya 572000, Hainan Province, China
    3 Institute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, China
    4 School of Environmental Science and Engineering, Qingdao University, Qingdao 266071, Shandong Province, China
  • Received:2024-12-16 Revised:2025-01-11 Accepted:2025-01-13 Published:2025-04-19
  • Contact: Email: xlshe@qdu.edu.cn (Xilin She)lifengmin@ouc.edu.cn (Fengmin Li)
  • Supported by:
    the Hainan Provincial Natural Science Foundation of China(423CXTD384); the National Natural Science Foundation of China(42077115); the National Science Fund for Distinguished Young Scholars of Shandong Province(ZR2021JQ13)

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摘要：

用活性氧(ROS)光催化降解微塑料(MPs)被认为是一种环保且可持续处理水生环境中MPs污染的方法。然而，由于传统光催化剂中电荷载流子的低迁移率和快速复合率使得该手段的使用面临较大挑战。本文通过热聚合耦合热溶剂工艺成功制备了氧硫共掺杂氮化碳纳米片(OSCN)。其中，O、S共掺杂可以有效降低带隙宽度，并提高氮化碳(C3N4)的光响应效率。同时，O/S掺杂原子有效增强了电子分布的离域，提高了载流子的分离能力，进一步促进了ROS的形成并提高了材料的光催化性能。与C3N4相比，OSCN对不同类型MPs (传统的石油基MPs—聚乙烯PE和可生物降解的生物基MPs—聚乳酸PLA)的光催化降解效果和矿化率显著提高，其中PE和PLA的质量损失分别增加了32.8%和34.1%。值得注意的是，OSCN产生的•OH和1O2协同催化了PE的降解，而•OH则是引发PLA光解和水解的主要自由基。本研究对光催化技术在水环境MPs污染修复中的应用具有重要意义。

关键词: 微塑料, 光催化, 共掺杂, 氮化碳, 降解机制

Abstract:

Photocatalytic microplastic (MP) degradation via reactive oxygen species (ROS) is a considered environmentally friendly and sustainable approach for eliminating MP pollution in aquatic environments. However, it faces challenges due to the low migration and rapid recombination efficiency of charge carriers in photocatalysts. Herein, oxygen and sulfur co-doped carbon nitride (OSCN) nanosheets were synthesized through thermal polymerization coupled with a thermosolvent process. The O and S co-doping can reduce the bandgap and improve the light response of carbon nitride (C3N4). Meanwhile, O/S dopants effectively improve the delocalization of electron distribution, leading to increased carrier separation capacity, thereby promoting the formation of ROS and enhancing photocatalytic performance. Compared to C3N4, OSCN demonstrated significantly higher photocatalytic degradation and mineralization rates for MPs, including polyethylene (PE, traditional petroleum-based MPs) and polylactic acid (PLA, biodegradable bio-based MPs). Specifically, the mass loss of PE and PLA increased by 32.8% and 34.1%, respectively. Notably, •OH and 1O2 generated by OSCN synergistically catalyzed the degradation of PE, while •OH was the primary radical triggering the photolysis and hydrolysis of PLA. This study holds significant implications for the application of photocatalysis technology in the remediation of MP pollution in aquatic environments.

Key words: Microplastics, Photocatalysis, Co-doped, C3N4, Degradation mechanism