Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Bax,Sr1-x )SO4 from undersaturated solution

Deng, Ning; Stack, Andrew G.; Weber, Juliane; Cao, Bo; De Yoreo, James; Hu, Yandi

doi:10.1073/pnas.1821065116

Title: Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba_x,Sr_1-x )SO₄ from undersaturated solution

Journal Article · Tue May 21 00:00:00 EDT 2019 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1821065116· OSTI ID:1546500

Deng, Ning ^[1];

^[2];

^[2]; Cao, Bo ^[1]; De Yoreo, James ^[3];

^[1]

Univ. of Houston, TX (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)

Sr-bearing marine barite [(Ba_x, Sr_1-x)SO₄] cycling has been widely used to reconstruct geochemical evolutions of paleoenvironments. However, an understanding of barite precipitation in the ocean, which is globally undersaturated with respect to barite, is missing. Moreover, the reason for the occurrence of higher Sr content in marine barites than expected for classical crystal growth processes remains unknown. Field data analyses suggested that organic molecules may regulate the formation and composition of marine barites; however, the specific organic–mineral interactions are unclear. Using in situ grazing incidence small-angle X-ray scattering (GISAXS), size and total volume evolutions of barite precipitates on organic films were characterized. The results show that barite forms on organic films from undersaturated solutions. Moreover, from a single supersaturated solution with respect to barite, Sr-rich barite nanoparticles formed on organics, while micrometer-size Sr-poor barites formed in bulk solutions. Ion adsorption experiments showed that organic films can enrich cation concentrations in the adjacent solution, thus increasing the local supersaturation and promoting barite nucleation on organic films, even when the bulk solution was undersaturated. The Sr enrichment in barites formed on organic films was found to be controlled by solid-solution nucleation rates; instead, the Sr-poor barite formation in bulk solution was found to be controlled by solid-solution growth rates. This study provides a mechanistic explanation for Sr-rich marine barite formation and offers insights for understanding and controlling the compositions of solid solutions by separately tuning their nucleation and growth rates via the unique chemistry of solution–organic interfaces.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1546500

Alternate ID(s):: OSTI ID: 1542993

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 116, Issue 27; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 28 works

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