Emergent Behavior at the Calcite–Water Interface during Reactive Transport in a Simple Microfluidic Channel

Abdilla, Bektur; Minahan, Daniel J.; Gleghorn, Jason P.; Kim, YoungJae; Lee, Sang Soo; Fenter, Paul; Sturchio, Neil C.

doi:10.1021/acsearthspacechem.1c00424

Emergent Behavior at the Calcite–Water Interface during Reactive Transport in a Simple Microfluidic Channel

Journal Article · Thu Apr 07 00:00:00 EDT 2022 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.1c00424· OSTI ID:1879892

Abdilla, Bektur ^[1]; Minahan, Daniel J. ^[1]; Gleghorn, Jason P. ^[1]; Kim, YoungJae ^[2]; ^[2]; ^[2]; ^[1]

Univ. of Delaware, Newark, DE (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

Geochemical reactive transport processes in natural mineral-fluid systems may produce a wide array of emergent phenomena that are difficult to predict from basic principles and to reproduce in model systems. In this study, we present experimental results obtained from a simple microfluidic system with which we explored the consequences of reacting the calcite (104) cleavage surface with an acidic Pb-bearing solution (pH = 3.5, [Pb]_total = 5 mM) as a function of flow rate. This system is relevant to passive remediation systems for Pb-rich acid mine drainage. We observed periodic banding in the amounts of Pb sorption at flow velocities ≥ 926 μm s^-1, where the band spacing was spatially correlated with the amount of calcite dissolution and the development of micropyramidal topography on the calcite (104) surface. The equivalent coverage of Pb deposited in these Pb-rich bands was at least several monolayers per unit cell, yet there was no evidence for precipitation of any secondary Pb phase implying incorporation of Pb within the near-surface calcite lattice. We also observed spatial variations in nucleation and growth of euhedral secondary Pb-carbonate minerals hydrocerusite and cerussite at flow rates ≤ 278 μm s^-1,. These findings demonstrate potential for exploiting the rich phenomenology afforded by the interplay among transport phenomena and chemical kinetics in experimental systems designed to yield deeper insights into geochemical self-organization.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (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

OSTI ID:: 1879892

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 4 Vol. 6; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Emergent Behavior at the Calcite–Water Interface during Reactive Transport in a Simple Microfluidic Channel

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