Oxyanion Surface Complexes Control the Kinetics and Pathway of Ferrihydrite Transformation to Goethite and Hematite

Namayandeh, Alireza; Borkiewicz, Olaf J.; Bompoti, Nefeli M.; Chrysochoou, Maria; Michel, F. Marc

doi:10.1021/acs.est.2c04971

Oxyanion Surface Complexes Control the Kinetics and Pathway of Ferrihydrite Transformation to Goethite and Hematite

Journal Article · Tue Oct 11 00:00:00 UTC 2022 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.2c04971· OSTI ID:2242508

^[1]; Borkiewicz, Olaf J. ^[2]; ^[3]; Chrysochoou, Maria ^[3]; Michel, F. Marc ^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Univ. of Connecticut, Storrs, CT (United States)

The rate and pathway of ferrihydrite (Fh) transformation at oxic conditions to more stable products is controlled largely by temperature, pH, and the presence of other ions in the system such as nitrate (NO₃^-), sulfate (SO₄^2-), and arsenate (AsO₄^3-). Although the mechanism of Fh transformation and oxyanion complexation have been separately studied, the effect of surface complex type and strength on the rate and pathway remains only partly understood. We have developed a kinetic model that describes the effects of surface complex type and strength on Fh transformation to goethite (Gt) and hematite (Hm). Two sets of oxyanion-adsorbed Fh samples were prepared, nonbuffered and buffered, aged at 70 ± 1.5 °C, and then characterized using synchrotron X-ray scattering methods and wet chemical analysis. Kinetic modeling showed a significant decrease in the rate of Fh transformation for oxyanion surface complexes dominated by strong inner-sphere (SO₄^2- and AsO₄^3-) versus weak outer-sphere (NO₃^-) bonding and the control. The results also showed that the Fh transformation pathway is influenced by the type of surface complex such that with increasing strength of bonding, a smaller fraction of Gt forms compared with Hm. In conclusion, these findings are important for understanding and predicting the role of Fh in controlling the transport and fate of metal and metalloid oxyanions in natural and applied systems.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2242508

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 22 Vol. 56; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Oxyanion Surface Complexes Control the Kinetics and Pathway of Ferrihydrite Transformation to Goethite and Hematite

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