Infrared Irradiation-Lattice Vibration Coupling-Initiated N→Π Electronic Transition in Carbon Nitride Nanosheets for Increased Photocatalysis

doi:10.1002/adfm.202311803

IMR OpenIR

	Infrared Irradiation-Lattice Vibration Coupling-Initiated N→Π Electronic Transition in Carbon Nitride Nanosheets for Increased Photocatalysis
	Jiang, Daochuan 1; Hu, Shaonian 1; Qu, Yi 1; Tian, Xu 1; Du, Haiwei 1; Zhu, Chuhong 1; Li, Zhongjun 2; Yin, Lisha 3; Yuan, Yupeng 1; Liu, Gang 4
通讯作者	Liu, Gang(gangliu@imr.ac.cn)
	2024-01-02
发表期刊	ADVANCED FUNCTIONAL MATERIALS
ISSN	1616-301X
页码	10
摘要	Enabling n ->pi* electronic transition in graphitic carbon nitride (g-CN) can significantly enhance its photocatalytic performance by extending visible light absorption. However, achieving this transition remains a grand challenge due to the selection rule that restricts it to planar tri-s-triazine units of g-CN. Here, an effective strategy to induce the n ->pi* transition in g-CN nanosheets by coupling infrared irradiation with lattice vibrations is presented. Theoretical simulations reveal two prominent vibration modes perpendicular to tri-s-triazine units at 219 and 737 cm-1 can promote the corrugation of tri-s-triazine units and facilitate the n ->pi* electronic transition when coupled with infrared irradiation. Additionally, these vibrational modes enable the efficient exfoliation of bulk g-CN into 2D nanosheets by overcoming the interplanar binding energy. Through femtosecond transient absorption spectra (fs-TAS), the n ->pi* transition prolongs the lifetime of photocatalytically active shallow electron trapping states and charge separation states in g-CN is demonstrated. Accordingly, the activated n ->pi* electronic transition and prolonged lifetime of photocatalytically active charges lead to an H2 generation rate of 2485 mu mol h-1 gcat-1, approximate to 40 times higher than that of the bulk counterpart. This work highlights the effectiveness of coupling lattice vibrations with infrared irradiation to drive the n ->pi* transition for enhanced visible-light photocatalysis. The lattice vibration modes perpendicular to heptazine units in g-CN, which induce both bulk exfoliation into nanosheets and the formation of corrugated heptazine building blocks, are identified as the origin of n ->pi* electronic transition. This transition enables extended visible light absorption and a prolonged lifetime of photocatalytically active charges, thereby resulting in a remarkable 40-fold enhancement of photocatalytic H2 generation.image
关键词	carbon nitride infrared irradiation heating lattice vibration lone pairs photocatalysis
资助者	National Natural Science Foundation of China ; Anhui Provincial Natural Science Foundation ; Horizontal Cooperation Project of Fuyang Municipal Government - Fuyang Normal University
DOI	10.1002/adfm.202311803
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; Anhui Provincial Natural Science Foundation[2108085QE192] ; Horizontal Cooperation Project of Fuyang Municipal Government - Fuyang Normal University[SXHZ202102] ; [52072001] ; [12174080] ; [22102002] ; [51825204]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001134226900001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：43[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/183166
专题	中国科学院金属研究所
通讯作者	Liu, Gang
作者单位	1.Anhui Univ, Sch Mat Sci & Engn, Key Lab Struct & Performance Funct Hybrid Mat, Minist Educ, Hefei 230601, Peoples R China 2.Hefei Univ Technol, Sch Phys, Hefei 230009, Peoples R China 3.Nanjing Tech Univ, Inst Adv Mat, Nanjing 211816, Peoples R China 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Jiang, Daochuan,Hu, Shaonian,Qu, Yi,et al. Infrared Irradiation-Lattice Vibration Coupling-Initiated N→Π Electronic Transition in Carbon Nitride Nanosheets for Increased Photocatalysis[J]. ADVANCED FUNCTIONAL MATERIALS,2024:10.
APA	Jiang, Daochuan.,Hu, Shaonian.,Qu, Yi.,Tian, Xu.,Du, Haiwei.,...&Liu, Gang.(2024).Infrared Irradiation-Lattice Vibration Coupling-Initiated N→Π Electronic Transition in Carbon Nitride Nanosheets for Increased Photocatalysis.ADVANCED FUNCTIONAL MATERIALS,10.
MLA	Jiang, Daochuan,et al."Infrared Irradiation-Lattice Vibration Coupling-Initiated N→Π Electronic Transition in Carbon Nitride Nanosheets for Increased Photocatalysis".ADVANCED FUNCTIONAL MATERIALS (2024):10.