Sorption of arsenate(Ⅴ) to naturally occurring secondary iron minerals formed at different conditions: The relationship between sorption behavior and surface structure

Abstract

Arsenic (As) is a problematic pollutant that can cause cancer and other chronic diseases due to its potential toxicity. Iron (oxyhydr)oxides can readily sorb As and play important roles in the geochemical cycle of As. Attention has mainly been given to the affinity and mechanism of As sorption by synthetic pure iron (oxyhydr)oxides, and little is known about the relationship between As behavior and multicomponent secondary iron minerals (SIMs) naturally formed in acid mine drainage (AMD). To investigate this relationship, we performed sorption kinetics, isotherm and competitive sorption experiments to investigate As(V) sorption behaviors on naturally formed SIMs harvested from different runoff zones of an abandoned coal mine. Several spectroscopic analyses were used to evaluate the structural and component changes and phase transformation. Three environmental SIMs formed at nascent (n-SIM), transient (t-SIM) and mature (m-SIM) stages were determined to be similar in the element components of Fe, S and O but different in structure. As(V) sorption behaviors on these environmental SIMs followed a pseudo-second-order kinetic model, and the sorption extent followed the sequence of n-SIM > t-SIM > m-SIM. As(V) sorption is not significantly influenced by Na+/Ca2+ concentration or ionic strength except for that of PO43−, and it slightly decreases as the Cr(Ⅲ) concentration increases but increases with increasing Sb(Ⅲ)/(V) concentration. The results of spectral analyses indicate that As(V) immobilization mainly depends on exchange with SO42− and surface complexation, along with the phase transformation of schwertmannite/jarosite to goethite and other phases. These findings are helpful for better understanding the geochemical behaviors of As(V) associated with environmental SIMs.