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Main Authors: Saldana-Robles, Adriana, Damian, Cesar, von Spakovsky, Michael R., Reynolds Jr, William T.
Format: Preprint
Published: 2024
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Online Access:https://arxiv.org/abs/2410.05157
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author Saldana-Robles, Adriana
Damian, Cesar
von Spakovsky, Michael R.
Reynolds Jr, William T.
author_facet Saldana-Robles, Adriana
Damian, Cesar
von Spakovsky, Michael R.
Reynolds Jr, William T.
contents Water contamination by arsenic(V) constitutes a major public-health concern, underscoring the need for models that capture both equilibrium and transient adsorption behaviour. A framework that can do so is the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework, which is used here to describe the uptake of As(V) on graphene oxide (GO) across pollutant concentrations of 25-350 mg/L. A non-equilibrium equation of motion derived from the steepest-entropy-ascent principle for a five-component system (water, arsenic, two GO functional groups, and protons is solved with an energy eigenstructure generated by a Replica-Exchange Wang-Landau algorithm and then extrapolated to relevant contaminant concentrations via an artificial neural network. Without recourse to empirical rate laws, the model predicts the time-dependent adsorption capacity, the stable-equilibrium arsenic concentration, and the pH dependence of removal efficiency. Equilibrium capacities are reproduced within 5 % of experimental isotherms, and the characteristic adsorption time aligns with the reported kinetics. These results indicate that SEAQT framework provides a thermodynamically consistent, fully predictive tool for designing and optimising adsorbent-based water-treatment technologies.
format Preprint
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institution arXiv
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spellingShingle Steepest-Entropy-Ascent Framework for Predicting Arsenic Adsorption on Graphene Oxide Surfaces -- A Case Study
Saldana-Robles, Adriana
Damian, Cesar
von Spakovsky, Michael R.
Reynolds Jr, William T.
Chemical Physics
Water contamination by arsenic(V) constitutes a major public-health concern, underscoring the need for models that capture both equilibrium and transient adsorption behaviour. A framework that can do so is the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework, which is used here to describe the uptake of As(V) on graphene oxide (GO) across pollutant concentrations of 25-350 mg/L. A non-equilibrium equation of motion derived from the steepest-entropy-ascent principle for a five-component system (water, arsenic, two GO functional groups, and protons is solved with an energy eigenstructure generated by a Replica-Exchange Wang-Landau algorithm and then extrapolated to relevant contaminant concentrations via an artificial neural network. Without recourse to empirical rate laws, the model predicts the time-dependent adsorption capacity, the stable-equilibrium arsenic concentration, and the pH dependence of removal efficiency. Equilibrium capacities are reproduced within 5 % of experimental isotherms, and the characteristic adsorption time aligns with the reported kinetics. These results indicate that SEAQT framework provides a thermodynamically consistent, fully predictive tool for designing and optimising adsorbent-based water-treatment technologies.
title Steepest-Entropy-Ascent Framework for Predicting Arsenic Adsorption on Graphene Oxide Surfaces -- A Case Study
topic Chemical Physics
url https://arxiv.org/abs/2410.05157