Infrared Irradiation-Lattice Vibration Coupling-Initiated N→Π Electronic Transition in Carbon Nitride Nanosheets for Increased Photocatalysis
文献类型：期刊论文
| 作者 | Jiang, Daochuan1; Hu, Shaonian1; Qu, Yi1; Tian, Xu1; Du, Haiwei1; Zhu, Chuhong1; Li, Zhongjun2; Yin, Lisha3; Yuan, Yupeng1; Liu, Gang4 |
| 刊名 | ADVANCED FUNCTIONAL MATERIALS
 |
| 出版日期 | 2024-01-02 |
| 页码 | 10 |
| 关键词 | carbon nitride infrared irradiation heating lattice vibration lone pairs photocatalysis |
| ISSN号 | 1616-301X |
| DOI | 10.1002/adfm.202311803 |
| 通讯作者 | Liu, Gang(gangliu@imr.ac.cn) |
| 英文摘要 | 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 |
| 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 |
| 语种 | 英语 |
| WOS记录号 | WOS:001134226900001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | National Natural Science Foundation of China ; Anhui Provincial Natural Science Foundation ; Horizontal Cooperation Project of Fuyang Municipal Government - Fuyang Normal University |
| 源URL |  |
| 专题 | 金属研究所_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. |
入库方式： OAI收割
来源：金属研究所
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