Extended Conjugation Tuning Carbon Nitride for Non-sacrificial H2O2 Photosynthesis and Hypoxic Tumor Therapy

被引:77
|
作者
Ma, Jin [1 ]
Peng, Xiaoxiao [1 ]
Zhou, Zhixin [1 ]
Yang, Hong [1 ]
Wu, Kaiqing [1 ]
Fang, Zhengzou [2 ]
Han, Dan [1 ]
Fang, Yanfeng [1 ]
Liu, Songqin [1 ]
Shen, Yanfei [2 ]
Zhang, Yuanjian [1 ]
机构
[1] Southeast Univ, Jiangsu Engn Lab Smart Carbon Rich Mat & Devices, Jiangsu Prov Hitech Key Lab Biomed Res, State Key Lab Bioelect,Sch Chem & Chem Engn, Nanjing 211189, Peoples R China
[2] Southeast Univ, Med Sch, Nanjing 210009, Peoples R China
基金
中国国家自然科学基金;
关键词
Carbon Nitrides; Electron Delocalization; Hydrogen Peroxide; Hypoxic Tumors; Photocatalysis; HYDROGEN-PEROXIDE PRODUCTION; PHOTODYNAMIC THERAPY; ORGANIC FRAMEWORKS; MOLECULAR-OXYGEN; FENTON REACTION; WATER; PHOTOCATALYST; GENERATION; NANOPARTICLES; NANOSHEETS;
D O I
10.1002/anie.202210856
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Artificial photocatalysis offers a clean approach for producing H2O2. However, the poor selectivity and activity of H2O2 production hamper traditional industrial applications and emerging photodynamic therapy (PDT)/chemodynamic therapy (CDT). Herein, we report a C5N2 photocatalyst with a conjugated C=N linkage for selective and efficient non-sacrificial H2O2 production in both normoxic and hypoxic systems. The strengthened delocalization of pi-electrons by linkers in C5N2 downshifted the band position, thermodynamically eliminating side H-2 evolution reaction and kinetically promoting water oxidation. As a result, C5N2 had a competitive solar-to-chemical conversion efficiency of 0.55 % in overall H2O2 production and exhibited by far the highest activity under hypoxic conditions (698 mu M h(-1)). C5N2 was further applied to hypoxic PDT/CDT with outstanding performance in apparent cancer cell death and synchronous bioimaging. The study sheds light on the photosynthesis of H2O2 by carbon nitrides for health applications.
引用
收藏
页数:9
相关论文
共 50 条
  • [11] A Minireview: The Mechanism of H2O2 Photoproduction by Graphitic Carbon Nitride
    Sun, Lu
    Li, Pengfei
    Shen, Ziye
    Pang, Yamei
    Ma, Xiaobao
    Qu, Dan
    An, Li
    Sun, Zaicheng
    ADVANCED ENERGY AND SUSTAINABILITY RESEARCH, 2023, 4 (11):
  • [12] Metal-Free Photocatalytic CO2 Reduction to CH4 and H2O2 under Non-sacrificial Ambient Conditions
    Zou, Weixin
    Cheng, Yingyi
    Ye, Yu-Xin
    Wei, Xiaoqian
    Tong, Qing
    Dong, Lin
    Ouyang, Gangfeng
    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (49)
  • [13] Simultaneous Photocatalytic CO2 Reduction and H2O Oxidation Under Non-Sacrificial Ambient Conditions
    Tong, Qing
    Tang, Yu
    Zou, Weixin
    Ye, Yu-Xin
    Dong, Lin
    Ouyang, Gangfeng
    CHEMISTRY-A EUROPEAN JOURNAL, 2024, 30 (71)
  • [14] Edge engineering of carbon nitride for enhanced sacrificial agent-free photocatalytic H2O2 evolution
    Li, Yanan
    Wang, Wei
    Wang, Yan
    He, Haichuan
    Yu, Xiao
    Xia, Dan
    Deng, Liu
    Liu, You-Nian
    CHEMICAL ENGINEERING SCIENCE, 2023, 282
  • [15] Enhanced Photocatalytic H2O2 Production over Carbon Nitride by Doping and Defect Engineering
    Wu, Shuai
    Yu, Hongtao
    Chen, Shuo
    Quan, Xie
    ACS CATALYSIS, 2020, 10 (24): : 14380 - 14389
  • [16] Extended n-conjugated system in carbon nitride by incorporating pyridine rings and N vacancies for photocatalytic H2 evolution and H2O2 production
    Ye, Baoqian
    Tang, Hua
    Liu, Qinqin
    Wang, Weikang
    Wang, Lele
    Hu, Jie
    CARBON, 2023, 204 : 465 - 474
  • [17] Zn-doped tubular graphene nitride for visible light and sacrificial-agent-free H2O2 photosynthesis in water
    Zhang, Dexu
    Peng, Xiaoying
    Zhang, Jie
    Zhu, Shixuan
    Xue, Zhihong
    Xiong, Shubin
    Xiong, Shuai
    Sheng, Bo
    He, Yiqiang
    Peng, Guiming
    Zhang, Jiadong
    APPLIED SURFACE SCIENCE, 2024, 674
  • [18] Sustainable H2O2 photosynthesis by sunlight and air
    Zhang, Hao
    Liu, Meng
    Miao, Qi
    Wu, Pan
    Liu, Changjun
    Jiang, Wei
    CHEMICAL ENGINEERING JOURNAL, 2023, 455
  • [19] Edge electronic vacancy on ultrathin carbon nitride nanosheets anchoring O2 to boost H2O2 photoproduction
    Liu, Lian-Lian
    Chen, Fei
    Wu, Jing-Hang
    Ke, Ming-Kun
    Cui, Chao
    Chen, Jie-Jie
    Yu, Han-Qing
    APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2022, 302
  • [20] ZnFe2O4/Graphitic Carbon Nitride Nano/Microcomposites for the Enhanced Electrochemical Sensing of H2O2
    Ye, Mingfu
    Yang, Chen
    Sun, Yan
    Wang, Jieyue
    Wang, Didi
    Zhao, Yijing
    Zhu, Zhu
    Liu, Pengchao
    Zhu, Jiahao
    Li, Chunsheng
    Peng, Wenxiu
    Zhang, Ning
    Dong, Yongping
    ACS APPLIED NANO MATERIALS, 2022, 5 (08) : 10922 - 10932