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

被引:44
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
相关论文
共 96 条
[11]   An organic perspective on photocatalytic production of hydrogen peroxide [J].
Freese, T. ;
Meijer, J. T. ;
Feringa, B. L. ;
Beil, S. B. .
NATURE CATALYSIS, 2023, 6 (07) :553-558
[12]   Dual-defect enhanced piezocatalytic performance of C3N5 for multifunctional applications [J].
Fu, Cheng ;
Wu, Tao ;
Sun, Guowei ;
Yin, Guofeng ;
Wang, Chan ;
Ran, Guoxia ;
Song, Qijun .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2023, 323
[13]   Promoting Piezocatalytic H2O2 Production in Pure Water by Loading Metal-Organic Cage-Modified Gold Nanoparticles on Graphitic Carbon Nitride [J].
Fu, Meng ;
Luo, Jinghong ;
Shi, Bo ;
Tu, Shuchen ;
Wang, Zihao ;
Yu, Changlin ;
Ma, Zequn ;
Chen, Xingyuan ;
Li, Xiangming .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2024, 63 (02)
[14]   Mechanochemistry for ammonia synthesis under mild conditions [J].
Han, Gao-Feng ;
Li, Feng ;
Chen, Zhi-Wen ;
Coppex, Claude ;
Kim, Seok-Jin ;
Noh, Hyuk-Jun ;
Fu, Zhengping ;
Lu, Yalin ;
Singh, Chandra Veer ;
Siahrostami, Samira ;
Jiang, Qing ;
Baek, Jong-Beom .
NATURE NANOTECHNOLOGY, 2021, 16 (03) :325-+
[15]   Photo-Driven Quasi-Topological Transformation Exposing Highly Active Nitrogen Cation Sites for Enhanced Photocatalytic H2O2 Production [J].
Hao, Feini ;
Yang, Chao ;
Lv, Ximeng ;
Chen, Fangshuai ;
Wang, Shengyao ;
Zheng, Gengfeng ;
Han, Qing .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (50)
[16]   Discovery of Key TIPS-Naphthalene for Efficient Visible-to-UV Photon Upconversion under Sunlight and Room Light** [J].
Harada, Naoyuki ;
Sasaki, Yoichi ;
Hosoyamada, Masanori ;
Kimizuka, Nobuo ;
Yanai, Nobuhiro .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2021, 60 (01) :142-147
[17]   C-Doped KNbO3 single crystals for enhanced piezocatalytic intermediate water splitting [J].
He, Jiaqing ;
Gao, Feng ;
Wang, Haowei ;
Liu, Fangyan ;
Lin, Jiahui ;
Wang, Biao ;
Liu, Chuan ;
Huang, Feng ;
Lin, Zhang ;
Wang, Mengye .
ENVIRONMENTAL SCIENCE-NANO, 2022, 9 (06) :1952-1960
[18]   Production of Hydrogen Peroxide by Photocatalytic Processes [J].
Hou, Huilin ;
Zeng, Xiangkang ;
Zhang, Xiwang .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2020, 59 (40) :17356-17376
[19]   Orthogonal Charge Transfer by Precise Positioning of Silver Single Atoms and Clusters on Carbon Nitride for Efficient Piezocatalytic Pure Water Splitting [J].
Hu, Cheng ;
Hu, Jingcong ;
Zhu, Zijian ;
Lu, Yue ;
Chu, Shengqi ;
Ma, Tianyi ;
Zhang, Yihe ;
Huang, Hongwei .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (43)
[20]   Exceptional Cocatalyst-Free Photo-Enhanced Piezocatalytic Hydrogen Evolution of Carbon Nitride Nanosheets from Strong In-Plane Polarization [J].
Hu, Cheng ;
Chen, Fang ;
Wang, Yonggang ;
Tian, Na ;
Ma, Tianyi ;
Zhang, Yihe ;
Huang, Hongwei .
ADVANCED MATERIALS, 2021, 33 (24)