Role of an Ice Surface in the Photoreaction of Coumarins
文献类型：期刊论文
| 作者 | Zhang, Shizhong2; Zhang, Chuanbiao3; Fu, Yang4; Li, Linhai; Huang, Chuanbing; Lin, Yang; Zhu, Chongqin6; Francisco, Joseph S.; He, Zhiyuan7; Zhou, Xin1,8 |
| 刊名 | LANGMUIR
 |
| 出版日期 | 2022 |
| 卷号 | 38期号:37页码:11346-11353 |
| ISSN号 | 0743-7463 |
| 关键词 | SINGLE-CRYSTALS CHEMISTRY WATER PHOTOCHEMISTRY CYCLOADDITION ADSORPTION REACTIVITY CHLORIDE COMPLEX LIGHT |
| DOI | 10.1021/acs.langmuir.2c01637 |
| 英文摘要 | Ice affects many chemical reactions in nature, which greatly influences the atmosphere, climate, and life. However, the exact mechanism of ice in these chemical reactions remains elusive. For example, it is still an open question as to whether ice can act as a catalyst to greatly enhance the reactivity and selectivity, which is essential for the production of some natural compounds in our planet. Here, we discover that ice can lead to high efficiency and stereoselectivity of the [2 + 2] photodimerization of coumarin and its derivatives. The conversion of the [2 + 2] photodimerization of coumarins enhanced by ice is dozens of times higher than that in the unfrozen saturated solution, and the reaction displays a high syn-head-head stereoselectivity (> 95%) in comparison with those in the absence of the ice. Note that almost no reaction occurs in the crystal powder and melt of the coumarins, indicating that the role of ice in the photodimerization reaction is not simply due to the usual mechanisms found in the freezing concentration. We further reveal that the reaction rate is found to be proportional to the total area of the ice surface and follows Michaelis-Menten-like kinetics, indicating that the ice surface catalyzes the reaction. Molecular dynamics simulations demonstrate that ice surfaces can induce reactants to form a two-dimensional liquid-crystal-ordered layer with a suitable intermolecular distance and unique side-by-side packing, facilitating stereoselective photodimerization for syn-head-head dimers. These findings give evidence that ice-surface-induced molecular assembly may play an important role in atmospheric heterogeneous photoreaction processes. |
| 学科主题 | Chemistry ; Materials Science |
| 语种 | 英语 |
| 源URL | [http://ir.itp.ac.cn/handle/311006/27847]  |
| 专题 | 理论物理研究所_理论物理所1978-2010年知识产出 |
| 作者单位 | 1.Beijing Inst Technol, Sch Mat Sci & Engn, Beijing 100081, Peoples R China 2.Chinese Acad Sci, Inst Chem, Key Lab Green Printing, Beijing Natl Lab Mol Sci, R China, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Sch Future Technol, Beijing 100049, Peoples R China 4.Heze Univ, Coll Phys & Elect Engn, Heze 274015, Peoples R China 5.Chinese Acad Sci, Inst Theoret Phys, Beijing 100190, Peoples R China 6.Zhu, Chongqin; Francisco, Joseph S.] Beijing Normal Univ, Coll Chem, Key Lab Theoret & Computat Photochem Minist Educ, Beijing 100190, Peoples R China 7.Univ Penn, Dept Earth & Environm Sci, Philadelphia, PA 19104 USA 8.Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100049, Peoples R China 9.Univ Chinese Acad Sci, CAS Ctr Excellence Topol Quantum Computat, Beijing 100049, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhang, Shizhong,Zhang, Chuanbiao,Fu, Yang,et al. Role of an Ice Surface in the Photoreaction of Coumarins[J]. LANGMUIR,2022,38(37):11346-11353. |
| APA | Zhang, Shizhong.,Zhang, Chuanbiao.,Fu, Yang.,Li, Linhai.,Huang, Chuanbing.,...&Wang, Jianjun.(2022).Role of an Ice Surface in the Photoreaction of Coumarins.LANGMUIR,38(37),11346-11353. |
| MLA | Zhang, Shizhong,et al."Role of an Ice Surface in the Photoreaction of Coumarins".LANGMUIR 38.37(2022):11346-11353. |
入库方式： OAI收割
来源：理论物理研究所
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