DFT Study of Selectivity in Photoelectrocatalytic C–H Arene Aminations

Location

Science Center Perlik Commons

Document Type

Poster - Open Access

Start Date

5-13-2022 12:00 PM

End Date

5-13-2022 2:00 PM

Abstract

The topic of photoelectrocatalytic (PEC) C-H amination of arenes is important to the scientific community because of the clear benefits for sustainability and drug synthesis. The purpose of this study was to explain the regioselectivity of C–N bond formation in the photoelectrocatalytic C–H amination of arenes.. Generally, the para isomer is expected to dominate, but Zhang et al. (2019) presented an uncommon case with high ortho selectivity. Thus, the goal of our study was to understand why this is taking place and how the newer methods stray away from the normal para selectivity. We used Density Functional Theory (DFT) calculations to study the transition states forming the C–N bonds..When the transition state energies of C–N bond formation at different positions of the aromatic ring were compared, the lowest energy transition state was the ortho, in good agreement with the experimental observation that ortho is the major product. We also found that C–N formation at the meta position is the least preferred. Future work will focus on locating more possible variations of the transition states and studying the role of hexafluoroisopropanol (HFIP) solvent.

Keywords:

Computational chemistry, Arene aminations, Photoelectrocatalysis

Notes

Presenters: Ophelia Ortíz and Sofia Bielinski Leitão

Major

Chemistry and Biochemistry

Award

STRONG

Project Mentor(s)

Shuming Chen, Chemistry

2022

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May 13th, 12:00 PM May 13th, 2:00 PM

DFT Study of Selectivity in Photoelectrocatalytic C–H Arene Aminations

Science Center Perlik Commons

The topic of photoelectrocatalytic (PEC) C-H amination of arenes is important to the scientific community because of the clear benefits for sustainability and drug synthesis. The purpose of this study was to explain the regioselectivity of C–N bond formation in the photoelectrocatalytic C–H amination of arenes.. Generally, the para isomer is expected to dominate, but Zhang et al. (2019) presented an uncommon case with high ortho selectivity. Thus, the goal of our study was to understand why this is taking place and how the newer methods stray away from the normal para selectivity. We used Density Functional Theory (DFT) calculations to study the transition states forming the C–N bonds..When the transition state energies of C–N bond formation at different positions of the aromatic ring were compared, the lowest energy transition state was the ortho, in good agreement with the experimental observation that ortho is the major product. We also found that C–N formation at the meta position is the least preferred. Future work will focus on locating more possible variations of the transition states and studying the role of hexafluoroisopropanol (HFIP) solvent.