Redirecting the electron flow to coordinate oxidation and reduction reactions for efficient photocatalytic H2O2 production

被引:6
|
作者
Chen, Qichao [1 ]
Ning, Cai [2 ]
Fang, Jiawen [3 ]
Ping, Boyu [1 ]
Li, Guiyang [1 ]
Kong, Lingqiao [1 ]
Chen, Jiayi [1 ]
Sun, ZhengMing [1 ]
Wang, Jinlan [2 ]
Ruan, Qiushi [1 ]
Niu, Xianghong [4 ]
Tao, Li [1 ]
机构
[1] Southeast Univ, Sch Mat Sci & Engn, Jiangsu Key Lab Adv Met Mat, Nanjing 211189, Peoples R China
[2] Southeast Univ, Sch Phys, Nanjing 211189, Peoples R China
[3] Nanjing Univ Posts & Telecommun, Jiangsu Natl Synerget Innovat Ctr Adv Mat, Nanjing 210023, Peoples R China
[4] Nanjing Univ Posts & Telecommun, Sch Sci, Nanjing 210023, Peoples R China
基金
中国国家自然科学基金;
关键词
Singlet oxygen; Oxygen-deficient condition; Donor-acceptor structure; GRAPHITIC CARBON NITRIDE; SINGLET OXYGEN; NANOSHEETS; MECHANISMS; GENERATION;
D O I
10.1016/j.cej.2024.150581
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Energy -efficient photocatalytic production of H 2 O 2 from water holds the potential to replace the anthraquinone process. However, the impracticality of oxygen bubbling in such processes necessitates addressing the H 2 O 2 production in oxygen -deficient environments. Here, we demonstrated the generation of singlet oxygen ( 1 O 2 ) as a highly active water oxidation derivative that redirects the electron flow for H 2 O 2 production in oxygen -deficient environments. Ground -state oxygen was in -situ generated on photocatalysts and undergoes transition to 1 O 2 , surpassing other competitive electron -consuming reactions. Self -generated 1 O 2 undergoes preferential photoreduction to H 2 O 2 , benefiting from a small activation energy (0.2 eV), facilitated electron trapping rate, adjacent oxidation/reduction sites and suppressed competitive energy transfer from excited -states to air 3 O 2 . A remarkable solar -to -chemical conversion (SCC) efficiency of 0.25 % was obtained for H 2 O 2 generation in oxygendeficient conditions. This work unveils a novel concept of redirecting electron flow towards H 2 O 2 production, taking advantage of highly active in -situ generated 1 O 2 .
引用
收藏
页数:10
相关论文
共 50 条
  • [21] Pairing Oxygen Reduction and Water Oxidation for Dual-Pathway H2O2 Production
    Sun, Xin
    Yang, Jindi
    Zeng, Xiangkang
    Guo, Lijun
    Bie, Chuanbiao
    Wang, Zhuyuan
    Sun, Kaige
    Sahu, Aloka Kumar
    Tebyetekerwa, Mike
    Rufford, Thomas E.
    Zhang, Xiwang
    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2024, 63 (52)
  • [22] Aqueous Photocatalytic Glycerol Oxidation to Formic Acid Coupled to H2O2 Production with an Anthraquinone Dye
    Tacchi, Elena
    Rossi, Greta
    Natali, Mirco
    Dordevic, Luka
    Sartorel, Andrea
    ADVANCED SUSTAINABLE SYSTEMS, 2025, 9 (01):
  • [23] Near-infrared H2O2 production via dual pathways of O2 reduction and H2O oxidation
    Yingpu Bi
    Science China(Chemistry), 2023, (05) : 1239 - 1240
  • [24] Near-infrared H2O2 production via dual pathways of O2 reduction and H2O oxidation
    Yingpu Bi
    Science China Chemistry, 2023, 66 : 1239 - 1240
  • [25] Near-infrared H2O2 production via dual pathways of O2 reduction and H2O oxidation
    Bi, Yingpu
    SCIENCE CHINA-CHEMISTRY, 2023, 66 (05) : 1239 - 1240
  • [26] Catalytic properties of Cr-containing heteropolytungstates in H2O2 participated reactions: H2O2 decomposition and oxidation of unsaturated hydrocarbons with H2O2
    Kuznetsova, NI
    Kuznetsova, LI
    Likholobov, VA
    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1996, 108 (03) : 135 - 143
  • [27] Highly efficient photocatalytic H2O2 production in microdroplets: accelerated charge separation and transfer at interfaces
    Li, Kejian
    Ge, Qiuyue
    Liu, Yangyang
    Wang, Longqian
    Gong, Kedong
    Liu, Juan
    Xie, Lifang
    Wang, Wei
    Ruan, Xuejun
    Zhang, Liwu
    ENERGY & ENVIRONMENTAL SCIENCE, 2023, 16 (03) : 1135 - 1145
  • [28] P-doped melon-carbon nitride for efficient photocatalytic H2O2 production
    Xue, Lian
    Sun, Hao
    Wu, Qiang
    Yao, Weifeng
    JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2022, 615 : 87 - 94
  • [29] Extending the π-conjugation system of covalent organic frameworks for more efficient photocatalytic H2O2 production
    Deng, Maojun
    Sun, Jiamin
    Laemont, Andreas
    Liu, Chunhui
    Wang, Linyang
    Bourda, Laurens
    Chakraborty, Jeet
    Van Hecke, Kristof
    Morent, Rino
    De Geyter, Nathalie
    Leus, Karen
    Chen, Hui
    van der Voort, Pascal
    GREEN CHEMISTRY, 2023, 25 (08) : 3069 - 3076
  • [30] Gas/solid/liquid triphase interface of carbon nitride for efficient photocatalytic H2O2 production
    He, Mao
    Peng, Xiaoying
    Wu, Suqin
    Lei, Bin
    Xiong, Shuai
    Luo, Qin
    Tu, Zongxing
    Lin, Xiaoxue
    Peng, Guiming
    INORGANIC CHEMISTRY FRONTIERS, 2025,