In situ surface-enhanced Raman spectroscopy monitoring of molecular reorientation in plasmon-mediated chemical reactions

被引:13
作者
Zhou, Binbin [1 ,4 ]
Zhong, Jing [1 ,4 ]
Tang, Xinxue [1 ,2 ,3 ]
Liu, Jia-hua [1 ,2 ,3 ]
Shen, Junda [1 ,2 ,3 ]
Wang, Chong [1 ,4 ]
Ou, Weihui [1 ,4 ]
Wang, Hao [6 ]
Liu, Lu [1 ,3 ,5 ]
Pan, Jie [1 ,2 ,3 ]
Lu, Jian [1 ,3 ,4 ,5 ,7 ,8 ]
Li, Yang Yang [1 ,2 ,3 ,7 ]
机构
[1] City Univ Hong Kong, Natl Precious Met Mat Engn Res Ctr, Kowloon, Hong Kong Branch, Hong Kong 99907, Peoples R China
[2] City Univ Hong Kong, Ctr Super Diamond & Adv Films COSDAF, Kowloon, Hong Kong 99907, Peoples R China
[3] City Univ Hong Kong, Dept Mat Sci & Engn, Kowloon, Hong Kong 99907, Peoples R China
[4] City Univ Hong Kong, Dept Mech Engn, Kowloon, Hong Kong 99907, Peoples R China
[5] Hong Kong Ctr Cerebro Caradiovasular Hlth Engn CO, Shatin, Hong Kong 99907, Peoples R China
[6] Univ Hong Kong, Dept Chem, Kowloon, Hong Kong 99907, Peoples R China
[7] City Univ Hong Kong, Ctr Adv Struct Mat, Greater Bay Joint Div, Shenyang Natl Lab Mat Sci,Shenzhen Res Inst, Shenzhen 518057, Peoples R China
[8] CityU Shenzhen Futian Res Inst, Shenzhen 518045, Peoples R China
关键词
In situ analysis; Photocatalysis; Raman spectroscopy; Molecular reorientation; Hot carriers; SILVER; AMINOTHIOPHENOL; ORIENTATION; WAVELENGTH; ENERGY; GOLD; AG;
D O I
10.1016/j.jcat.2022.06.028
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
Understanding the molecular orientation is crucial for revealing the mechanism of chemical reactions. However, how to accurately monitor the molecular orientation remains a great challenge because of the motion of the molecules during the chemical reaction. Here, surface-enhanced Raman spectroscopy (SERS) was used to monitor the molecular reorientation from the plasmon-catalyzed conversion of p-aminothiophenol (PATP) to p,p'-dimercaptoazobenzene (DMAB). Spectral change due to molecular reorientation, which is often overlooked, is clearly extracted through the protonation of the PATP molecules to suppress the conversion of PATP to DMAB. Meanwhile, by monitoring the Raman features, the reaction process and molecular reorientation are simultaneously recorded, offering fresh insights on the long-standing puzzle that why the conversion to DMAB is suppressed with concentrated PATP: this is because the over-crowded PATP adsorbed on the substrate hampered its own space-taking reorientation (similar to the space-steric effect) which is a prerequisite for producing DMAB. (C) 2022 Published by Elsevier Inc.
引用
收藏
页码:527 / 533
页数:7
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