H2O2 Photosynthesis from H2O and O2 under Weak Light by Carbon Nitrides with the Piezoelectric Effect

被引:24
作者
Ma, Jin [1 ]
Peng, Cheng [2 ]
Peng, Xiaoxiao [1 ]
Liang, Sicheng [1 ]
Zhou, Zhixin [1 ]
Wu, Kaiqing [1 ]
Chen, Ran [1 ]
Liu, Songqin [1 ]
Shen, Yanfei [1 ]
Ma, Haibo [2 ]
Zhang, Yuanjian [1 ,3 ]
机构
[1] Southeast Univ, Sch Chem & Chem Engn, Jiangsu Engn Lab Smart Carbon Rich Mat & Device, Jiangsu Prov Hitech Key Lab Biomed Res,Med Sch, Nanjing 211189, Peoples R China
[2] Shandong Univ, Qingdao Inst Theoret & Computat Sci, Sch Chem & Chem Engn, Qingdao 266237, Peoples R China
[3] Southeast Univ, Zhongda Hosp, Dept Oncol, Nanjing 210009, Peoples R China
基金
中国国家自然科学基金;
关键词
HYDROGEN-PEROXIDE PRODUCTION; MOLECULAR-OXYGEN; WATER; PHOTOCATALYST; CATALYST; SEAWATER; DESIGN;
D O I
10.1021/jacs.4c07170
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Driven by the essential need of a green, safe, and low-cost approach to producing H2O2, a highly valuable multifunctional chemical, artificial photosynthesis emerges as a promising avenue. However, current catalyst systems remain challenging, due to the need of high-density sunlight, poor selectivity and activity, or/and unfavorable thermodynamics. Here, we reported that an indirect 2e(-) water oxidation reaction (WOR) in photocatalytic H2O2 production was unusually activated by C5N2 with piezoelectric effects. Interestingly, under ultrasonication, C5N2 exhibited an overall H2O2 photosynthesis rate of 918.4 mu M/h and an exceptionally high solar-to-chemical conversion efficiency of 2.6% after calibration under weak light (0.1 sun). Mechanism studies showed that the piezoelectric effect of carbon nitride overcame the high uphill thermodynamics of *OH intermediate generation, which enabled a new pathway for 2e(-) WOR, the kinetic limiting step in the overall H2O2 production from H2O and O-2. Benefiting from the outstanding sonication-assisted photocatalytic H2O2 generation under weak light, the concept was further successfully adapted to biomedical applications in efficient sono-photochemodynamic therapy for cancer treatment and water purification.
引用
收藏
页码:21147 / 21159
页数:13
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