Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis
The selectivity of electrochemical sensors to ascorbic acid (AA), dopamine (DA), and uric acid (UA) remains an open challenge in the field of biosensing. In this study, the selective mechanisms for detecting AA, DA, and UA molecules on the graphene and graphene oxide substrates were illustrated thro...
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doaj-57ff4eab997b42e3a439d9c3d03275022021-04-14T23:05:33ZengMDPI AGSensors1424-82202021-04-01212773277310.3390/s21082773Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population AnalysisKittiya Prasert0Thana Sutthibutpong1Theoretical and Computational Physics Group, Department of Physics, Faculty of Science, King Mongkut’s University of Technology Thonburi (KMUTT), Bangkok 10140, ThailandCenter of Excellence in Theoretical and Computational Science (TaCS-CoE), Faculty of Science, King Mongkut’s University of Technology Thonburi (KMUTT), 126 Pracha Uthit Rd., Bang Mod, Thung Khru, Bangkok 10140, ThailandThe selectivity of electrochemical sensors to ascorbic acid (AA), dopamine (DA), and uric acid (UA) remains an open challenge in the field of biosensing. In this study, the selective mechanisms for detecting AA, DA, and UA molecules on the graphene and graphene oxide substrates were illustrated through the charge population analysis from the density functional theory (DFT) calculation results. Our substrate models contained the 1:10 oxygen per carbon ratio of reduced graphene oxide, and the functionalized configurations were selected according to the formation energy. Geometry optimizations were performed for the AA, DA, and UA on the pristine graphene, epoxy-functionalized graphene, and hydroxyl-functionalized graphene at the DFT level with vdW-DF2 corrections. From the calculations, AA was bound to both epoxy and hydroxyl-functionalized GO with relatively low adsorption energy, while DA was adsorbed stronger to the electronegative epoxy groups. The strongest adsorption of UA to both functional groups corresponded to the largest amount of electron transfer through the pi orbitals. Local electron loss created local electric fields that opposed the electron transfer during an oxidation reaction. Our analysis agreed with the results from previous experimental studies and provided insight into other electrode modifications for electrochemical sensing.https://www.mdpi.com/1424-8220/21/8/2773density functional theoryAA, UA, and DA detectionsgraphene oxide |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Kittiya Prasert Thana Sutthibutpong |
spellingShingle |
Kittiya Prasert Thana Sutthibutpong Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis Sensors density functional theory AA, UA, and DA detections graphene oxide |
author_facet |
Kittiya Prasert Thana Sutthibutpong |
author_sort |
Kittiya Prasert |
title |
Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis |
title_short |
Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis |
title_full |
Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis |
title_fullStr |
Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis |
title_full_unstemmed |
Unveiling the Fundamental Mechanisms of Graphene Oxide Selectivity on the Ascorbic Acid, Dopamine, and Uric Acid by Density Functional Theory Calculations and Charge Population Analysis |
title_sort |
unveiling the fundamental mechanisms of graphene oxide selectivity on the ascorbic acid, dopamine, and uric acid by density functional theory calculations and charge population analysis |
publisher |
MDPI AG |
series |
Sensors |
issn |
1424-8220 |
publishDate |
2021-04-01 |
description |
The selectivity of electrochemical sensors to ascorbic acid (AA), dopamine (DA), and uric acid (UA) remains an open challenge in the field of biosensing. In this study, the selective mechanisms for detecting AA, DA, and UA molecules on the graphene and graphene oxide substrates were illustrated through the charge population analysis from the density functional theory (DFT) calculation results. Our substrate models contained the 1:10 oxygen per carbon ratio of reduced graphene oxide, and the functionalized configurations were selected according to the formation energy. Geometry optimizations were performed for the AA, DA, and UA on the pristine graphene, epoxy-functionalized graphene, and hydroxyl-functionalized graphene at the DFT level with vdW-DF2 corrections. From the calculations, AA was bound to both epoxy and hydroxyl-functionalized GO with relatively low adsorption energy, while DA was adsorbed stronger to the electronegative epoxy groups. The strongest adsorption of UA to both functional groups corresponded to the largest amount of electron transfer through the pi orbitals. Local electron loss created local electric fields that opposed the electron transfer during an oxidation reaction. Our analysis agreed with the results from previous experimental studies and provided insight into other electrode modifications for electrochemical sensing. |
topic |
density functional theory AA, UA, and DA detections graphene oxide |
url |
https://www.mdpi.com/1424-8220/21/8/2773 |
work_keys_str_mv |
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