Efficient visible light photocatalysis enabled by the interaction between dual cooperative defect sites

被引:43
作者
Qi, Rongjie [1 ,2 ]
Yu, Pengfei [3 ,4 ]
Zhang, Jiachen [5 ]
Guo, Weiqi [1 ,2 ]
He, Yaoyu [1 ,2 ]
Hojo, Hajime [6 ]
Einaga, Hisahiro [6 ]
Zhang, Qun [5 ]
Liu, Xiaosong [3 ,4 ,7 ]
Jiang, Zhi [1 ,2 ]
Shangguan, Wenfeng [1 ,2 ]
机构
[1] Shanghai Jiao Tong Univ, Res Ctr Combust & Environm Technol, Shanghai 200240, Peoples R China
[2] Shanghai Jiao Tong Univ, Ctr Hydrogen Sci, Shanghai 200240, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China
[4] Chinese Acad Sci, Ctr Excellence Superconducting Elect CENSE, Shanghai, Peoples R China
[5] Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Dept Chem Phys, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[6] Kyushu Univ, Fac Engn Sci, Dept Energy & Mat Sci, 6-1 Kasuga Koen, Kasuga, Fukuoka 8168580, Japan
[7] Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 200031, Peoples R China
基金
中国国家自然科学基金;
关键词
Dual defect; Nitrogen defects; Single-site copper; Long-wavelength visible light; Photocatalytic hydrogen production; GRAPHITIC CARBON NITRIDE; X-RAY-ABSORPTION; HYDROGEN EVOLUTION; SINGLE-ATOM; TIO2; H-2; NANOCRYSTALS; SPECTROSCOPY; COCATALYST; FRAMEWORKS;
D O I
10.1016/j.apcatb.2020.119099
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Modifying photocatalyst with defects offers effective pathway to tailor light absorption properties, but may result in more sluggish kinetics. Therefore, enhanced light absorption often could not guarantee increased activity. Here, we report a dual defect strategy to extend light absorption with minimal loss in charge dynamics. Fine-tuned amount of dual defect, i.e., nitrogen defects and single-site copper, is simultaneously generated in polymer carbon nitride(PCN) through in-situ vapor diffusion method. Surface nitrogen defect extends the light absorption to long-wavelength via sub-band absorption. The interaction between nitrogen and single-site copper at certain concentration retains the charge dynamics by making the photogenerated electrons more delocalized through the newly-formed copper-nitrogen bonds. As a result, champion modified PCN exhibits robust hydrogen production activity, roughly 4.5-fold greater than the pristine counterpart in both visible and full light ranges. More intriguingly, this synergism provides PCN with efficient visible light activity even in faint tailing optical absorption region( > 450 nm).
引用
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页数:12
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