Oxide- and Silicate-Water Interfaces and Their Roles in Technology and the Environment

José Leobardo Bañuelos, Eric Borguet, Gordon E. Brown, Randall T. Cygan, James J. Deyoreo, Patricia M. Dove, Marie Pierre Gaigeot, Franz M. Geiger, Julianne M. Gibbs, Vicki H. Grassian, Anastasia G. Ilgen, Young Shin Jun, Nadine Kabengi, Lynn Katz, James D. Kubicki, Johannes Lützenkirchen, Christine V. Putnis, Richard C. Remsing, Kevin M. Rosso, Gernot RotherMarialore Sulpizi, Mario Villalobos, Huichun Zhang

Research output: Contribution to journalReview articlepeer-review

63 Scopus citations

Abstract

Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic- and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by "anomalies" or "non-idealities" such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surface-sensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide- and silicate-water interfaces. This critical review discusses how science progresses from understanding ideal solid-water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. We anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.

Original languageEnglish
Pages (from-to)6413-6544
Number of pages132
JournalChemical Reviews
Volume123
Issue number10
DOIs
StatePublished - May 24 2023

Funding

V.H.G. was supported by the Army Research Office/Army Research Laboratory via grant #W911NF-19-1-0078 to the University of California, San Diego (VHG). Any errors and opinions are not those of the Army Research Office or Department of Defense and are attributable solely to the author(s). A.G.I. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under Field Work Proposal number 21-015452 at Sandia National Laboratories. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA-0003525. We would like to acknowledge Eric Lundin at Sandia for help creating and editing graphics included in this manuscript. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Y.-S.J. is grateful for the support received from the U.S. National Science Foundation’s Environmental Chemical Sciences program (CHE-1905077), the American Chemical Society’s Petroleum Research Fund (62756-ND5), and the U.S. Department of Energy Office of Science (DE-SC0023390). N.K. acknowledges support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division (Geosciences Program) under award number DE-SC0012186. K.M.R. acknowledges support from the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division through its Geosciences program at Pacific Northwest National Laboratory (FWP #56674). G.R. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division. M.V. acknowledges the financial support of CONACyT through project 2016-CB 283416, as well as to the LANGEM, Geology Institute, UNAM. M.S. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy-EXC 2033-390677874-RESOLV. We all appreciate Prof. James C. Ballard’s careful review of the entire article and acknowledge the McKelvey School of Engineering at Washington University in St. Louis for editorial support. We also thank Gabrial Goldner (Georgia State University) for her immense help with cataloguing, organizing, and inserting the many references into the manuscript. We also gratefully acknowledge Drs. Louise Criscenti and Kevin Leung at Sandia for technical review of this manuscript prior to submission and Andrea Heacock-Reyes at Sandia for copy editing portions in this manuscript.

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