The response of PFAA mobility in highly contaminated sediment to sluice operation: Coupled effects of scour behavior and physicochemical properties

Abstract

Despite their widespread occurrence and significant environmental implications, the influence of sluice operations on the mobility of perfluoroalkyl acid (PFAA) in riverine sediments remains largely unexplored. To address this gap, a series of flume experiments were conducted to simulate the sedimentary migration of PFAA under the turbulent conditions generated by opening a sluice. Our study provides novel insights into the mechanisms by which plunging turbulence modulates the transfer of sedimentary PFAAs across the sediment‒water interface. Significant transient release effects were observed in the dissolved and suspended particulate matter (SPM) phases of PFAA, with total concentrations maintaining relative stability over extended periods following disturbance. The fluviraption of plunging turbulence increased PFAA concentrations in the surface sedimentary and porewater phases but weakened the adsorption performance of resuspended particles for the chemicals in the lower reach of the sluice. The instantaneous release of PFAA from sediment, fueled by turbulence, was identified as the primary driver of total mass transfer across the interface, increasing exponentially with the Reynolds number (Re_x, R²=0.99, p < 0.01). Notably, the peak PFAA release flux in the SPM phase lagged behind that in the dissolved phase, underscoring the dynamic interplay between phases. A structural equation model (SEM) revealed that plunging turbulence indirectly governs the cross-interface transfer of sedimentary PFAA by altering environmental physicochemical parameters and enhancing porewater diffusion. This finding underscores the complex, coupled effects of scour behavior and physicochemical properties on PFAA fate. Our study offers a unique perspective on the dynamic mechanisms underlying PFAA multimedia migration under sluice operation, contributing valuable insights for managing and regulating these emerging contaminants in aquatic environments.