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Pb Sorption at the Barite (001)–Water Interface

Journal Article · · Journal of Physical Chemistry. C
 [1];  [2];  [3];  [3];  [2];  [4]
  1. City Univ. of New York (CUNY), NY (United States). Queens College; Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. City Univ. of New York (CUNY), NY (United States). Queens College
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
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 Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-06CH11357; AC05-00OR22725; FG02-94ER14466
OSTI ID:
1776716
Alternate ID(s):
OSTI ID: 1782037
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 40 Vol. 124; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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