Significance of pH and iron-sulfur chemistry for molybdenum sequestration under sulfidic conditions

Phillips, Rachel; Singerling, Sheryl; Leng, Weinan; Xu, Jie

doi:10.1016/j.chemgeo.2023.121702

Title: Significance of pH and iron-sulfur chemistry for molybdenum sequestration under sulfidic conditions

Journal Article · 01 September 2023 · Chemical Geology

DOI: https://doi.org/10.1016/j.chemgeo.2023.121702 · OSTI ID:2204410

Phillips, Rachel ^[1]; Singerling, Sheryl ^[2]; Leng, Weinan ^[2]; Xu, Jie ^[3]

University of Texas at El Paso, TX (United States); Arizona State University, Tempe, AZ (United States); Arizona State University
Virginia Polytechnic Institute and State University (Virginia Tech), Blacksburg, VA (United States)
Arizona State University, Tempe, AZ (United States)

Molybdenum (Mo), a redox-sensitive trace metal, plays an important role in recording ancient oxygenation and deoxygenation events as a paleoredox proxy. The mobility and reactivity of Mo in aqueous conditions are closely tied to the chemistry of reduced sulfur and iron species. However, our current knowledge on the formation, structure, stability, and condensation pathways of FeMoS clusters in aqueous settings remains limited, which has driven the current study. In this study, we conducted systematic experiments investigating the interactions between dissolved Mo (initially introduced as molybdate, MoO₄^2–, or tetrathiomolybdate, MoS₄^2–), ferrous iron (Fe²⁺), and sulfide (ΣH₂S_aq) in variously defined abiotic sulfidic systems to determine the external conditions (i.e., pH, and reactant concentrations and ratios) necessary for the formation of solid-phase Fe-Mo sulfides. Solution samples of each system were monitored using ultraviolet-visible spectroscopy (UV–vis) to track the degree of thiolation of dissolved Mo species. Precipitates were analyzed using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) to determine their elemental compositions and valences, and structure (i.e., crystalline or amorphous), respectively. All FeMoS precipitates were amorphous and contained 76–90% Mo(IV) and 10–24% Mo(V) with a trend toward lower Mo(IV):Mo(V) ratios with increasing pH. The degree of Mo thiolation, which was strongly dependent on solution pH and Fe²⁺ concentrations, greatly affected the amount of Mo sequestered (i.e., an increased degree of Mo thiolation in solution led to an increased amount of Mo in the final FeMoS precipitate). Furthermore, these findings suggest that changes in pH and Fe²⁺ concentrations may be responsible for the sulfide-independent variations in Mo behavior observed in euxinic basins.

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Research Organization:: University of Texas at El Paso, TX (United States)

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

Grant/Contract Number:: SC0021995

OSTI ID:: 2204410

Journal Information:: Chemical Geology, Journal Name: Chemical Geology Vol. 638; ISSN 0009-2541

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Significance of pH and iron-sulfur chemistry for molybdenum sequestration under sulfidic conditions

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