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
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