The roles of Fe oxyhydroxide coating and chemical aging in pyrogenic carbon nanoparticle transport in unsaturated porous media

Abstract

Pyrogenic carbon (PyC) nanoparticles are widespread in the environment, which is important to global carbon cycle. PyC can exist for millions of years and undergo various environmental aging processes. To better understand the roles of Fe oxyhydroxides and water content on the pristine and aged PyC transport, adsorption and column experiments were conducted under three saturations (100%, 70%, and 40%) and three pH (5, 7, and 9) in both clean and Fe oxyhydroxide-coated sand. At high water saturations (100% and 70%), the mobility of both the pristine and aged PyC was enhanced at high pH due to strong electrostatic repulsion, and the aged PyC showed higher mobility than the pristine PyC because of its more negative charge and hydrophilic surface. The coating of Fe oxyhydroxides on sand decreased the mobility of both the pristine and aged PyC due to weak electrostatic repulsion, large specific surface area, and high roughness. At low saturation (40%), solution pH showed little effect on both the pristine and aged PyC mobility, and water saturation became the main factor affecting PyC mobility. Almost no pristine or aged PyC transported out from the Fe oxyhydroxide-coated sand column because Fe oxide increased the roughness of the sand surface, which led to a sharp increase in the air-water-solid interface and retention sites. This study demonstrates that water content, environmental aging, and Fe oxyhydroxides are significant in the fate and transport of PyC nanoparticles in environments, which provides a good fundamental understanding for the assessment of pyrogenic carbon application in environmental protection and carbon sequestration.