Removal of Water-Soluble Inorganic Arsenicals with Phosphorene Oxide Nanoadsorbents: A First-Principles Study

22 April 2021, Version 2
This content is a preprint and has not undergone peer review at the time of posting.


A complete picture of the phosphorene oxide (PhosO) sorption properties for the simultaneous removal of inorganic As(III) and As(V) pollutants from water has been developed using first-principles calculations. Calculated adsorption energies, competitive adsorption with co-existing species, energy decomposition analyses (ALMO-EDA), implicitly/explicitly solvated geometries, and adsorption free energies provide deep insights into the adsorption mechanism as well as the origin of the strong selectivity sorption ability. The PhosO nanoadsorbents establish inner-sphere surface complexes with arsenicals even under competition with water molecules. These proposed structures also show a strong affinity with the highly mobile As(III), where energy saving is achieved by avoiding the pre oxidation process to convert As(III) into As(V) as requested in related materials. Results show that electrostatic driving forces govern the adsorption of neutral arsenicals, while the interplay between electrostatic and polarization phenomena drives the uptake of anionic arsenicals. By computing the adsorption strength as a function of the oxidation degree, the optimum adsorption efficiency is reached with a 25% in the content of oxidizing groups. In this oxidation degree, the strong repulsive surface charge at high pH turns the PhosO nanoadsorbents convenient to recycle via simple treatment with alkaline eluents. Finally, the adsorption ability remains thermodynamically allowed in a wide range of ambient temperatures (enthalpically governed reaction). Conceptually understanding the sorption properties of phosphorene-oxide-based materials towards arsenic pollutants provides a useful framework for future water treatment technologies.


dft calculations
water pollution remediation
water pollution treatment
Water pollution
Arsenic Contaminated Groundwater
arsenic species
arsenic groundwater aquifers
phosphorene oxides
phosphorene nanoribbons
Phosphorene NanoribbonsPassivated phosphorene nanoribbons
Energy Decomposition Analysis methods
energy decomposition analysis scheme
atoms-in-molecules analysis
Adsorbents Performance
Nanotechnology Papers
computational chemistry
environmental pollution
first principles modeling
computational modeling
CM5 charges
free energy
conceptual density functional theory
chemical potential
molecular hardness


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