Evaluating the Ability of External Electric Fields to Accelerate Reactions in Solution

被引:2
|
作者
Aziz, Miriam [1 ]
Prindle, Claudia R. [1 ]
Lee, Woojung [1 ]
Zhang, Boyuan [2 ]
Schaack, Cedric [3 ]
Steigerwald, Michael L. [1 ]
Zandkarimi, Fereshteh [1 ,4 ,5 ]
Nuckolls, Colin [1 ]
Venkataraman, Latha [1 ,4 ,6 ]
机构
[1] Columbia Univ, Dept Chem, New York, NY 10027 USA
[2] Fairfield Univ, Dept Chem, Fairfield, CT 06824 USA
[3] Wake Forest Univ, Dept Chem, Winston Salem, NC 27109 USA
[4] Columbia Univ, Dept Chem, New York, NY 10027 USA
[5] Columbia Univ, Mass Spectrometry Core Facil, Dept Chem, New York, NY 10027 USA
[6] Columbia Univ, Dept Appl Phys & Appl Math, New York, NY 10027 USA
来源
JOURNAL OF PHYSICAL CHEMISTRY B | 2024年 / 128卷 / 39期
关键词
CATALYSIS; SELECTIVITY; CHEMISTRY; GLYCEROL;
D O I
10.1021/acs.jpcb.4c04864
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
This study investigates the catalytic effects of external electric fields (EEFs) on two reactions in solution: the Menshutkin reaction and the Chapman rearrangement. Utilizing a scanning tunneling microscope-based break-junction (STM-BJ) setup and monitoring reaction rates through high-performance liquid chromatography connected to a UV detector (HPLC-UV) and ultraperformance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry (UPLC-q-ToF-MS), we observed no rate enhancement for either reaction under ambient conditions. Density functional theory (DFT) calculations indicate that electric field-induced changes in reactant orientation and the minimization of activation energy are crucial factors in determining the efficacy of EEF-driven catalysis. Our findings suggest that the current experimental setups and field strengths are insufficient to catalyze these reactions, underscoring the importance of these criteria in assessing the reaction candidates.
引用
收藏
页码:9553 / 9560
页数:8
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