TY - JOUR

T1 - Ab-Initio Molecular Dynamics Simulation of Condensed-Phase Reactivity

T2 - The Electrolysis of Amino Acids and Peptides

AU - Kiakojouri, Ali

AU - Nadimi, Ebrahim

AU - Frank, Irmgard

N1 - Funding Information: The study was supported by the Deutsche Forschungsgemeinschaft (DFG), grant FR1246/10-1. Part of the calculations were performed on the local cluster of the Leibniz University of Hannover at the RRZN and on the Hochstleistungsrechner Nord, HLRN, maintained by the North German Supercomputing Alliance, project nic00061.

PY - 2020/11/19

Y1 - 2020/11/19

N2 - Electrolysis is a potential candidate for a quick method of wastewater cleansing. However, it is necessary to know what compounds might be formed from bioorganic matter. We want to know if there are toxic intermediates and if it is possible to influence the product formation by the variation in initial conditions. In the present study, we use Car-Parrinello molecular dynamics to simulate the fastest reaction steps under such circumstances. We investigate the behavior of amino acids and peptides under anodic conditions. Such highly reactive situations lead to chemical reactions within picoseconds, and we can model the reaction mechanisms in full detail. The role of the electric current is to discharge charged species and, hence, to produce radicals from ions. This leads to ultra-fast radical reactions in a bulk environment, which can also be seen as redox reactions as the oxidation states change. In the case of amino acids, the educts can be zwitterionic, so we also observe complex acid-base chemistry. Hence, we obtain the full spectrum of condensed-phase chemistry.

AB - Electrolysis is a potential candidate for a quick method of wastewater cleansing. However, it is necessary to know what compounds might be formed from bioorganic matter. We want to know if there are toxic intermediates and if it is possible to influence the product formation by the variation in initial conditions. In the present study, we use Car-Parrinello molecular dynamics to simulate the fastest reaction steps under such circumstances. We investigate the behavior of amino acids and peptides under anodic conditions. Such highly reactive situations lead to chemical reactions within picoseconds, and we can model the reaction mechanisms in full detail. The role of the electric current is to discharge charged species and, hence, to produce radicals from ions. This leads to ultra-fast radical reactions in a bulk environment, which can also be seen as redox reactions as the oxidation states change. In the case of amino acids, the educts can be zwitterionic, so we also observe complex acid-base chemistry. Hence, we obtain the full spectrum of condensed-phase chemistry.

KW - Car–Parrinello molecular dynamics

KW - electrochemistry

KW - reaction intermediates

KW - reaction mechanisms

KW - wastewater cleansing

UR - http://www.scopus.com/inward/record.url?scp=85096733037&partnerID=8YFLogxK

U2 - 10.3390/molecules25225415

DO - 10.3390/molecules25225415

M3 - Article

C2 - 33228128

AN - SCOPUS:85096733037

VL - 25

JO - Molecules (Basel, Switzerland)

JF - Molecules (Basel, Switzerland)

SN - 1420-3049

IS - 22

M1 - 5415

ER -