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Title: Pb Sorption at the Barite (001)–Water Interface

Journal Article · · Journal of Physical Chemistry. C

Sorption of ions at the mineral-water interface is an important factor that determines the fate of toxic metals in the environment. Here, we use barite as a model substrate to understand the interaction of toxic-metal lead (Pb) with ionic crystals. The coverage and location of Pb sorbed to the (001) surface was measured as a function of aqueous Pb concentration ([Pb]aq) using in situ specular resonant anomalous X-ray reflectivity (RAXR) to determine the sorption capacity and process. In this work, the results show that Pb sorption occurs via incorporation (primarily within the top barite layer similar to 3 angstrom in depth) and adsorption (mostly as an inner-sphere complex at similar to 2 angstrom in height) simultaneously. Both the incorporated and adsorbed Pb coverages increase with increasing [Pb]aq up to [Pb]aq similar to 200 mu M, above which the adsorbed fraction increases more rapidly than the incorporated fraction. This enhanced adsorption has a height distribution that is further extended (>= 15 angstrom from the surface) than that observed in lower [Pb]aq. This change in distribution is interpreted as arising from additional sorption of outer-sphere species or Pb-bearing phases precipitated on the surface. Desorption experiments in Pb-free solutions show that the incorporated fraction is more resistant to removal than the adsorbed fraction, consistent with the speciation-dependent stabilities premised in the classical sorption models.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357; FG02-94ER14466; AC05-00OR22725
OSTI ID:
1776716
Alternate ID(s):
OSTI ID: 1782037
Journal Information:
Journal of Physical Chemistry. C, Vol. 124, Issue 40; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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