{"id":{"repo_id":"mit","oai_identifier":"oai:dspace.mit.edu:1721.1/122158"},"canonical_url":"https://search.dev.ndltd.org/etd/mit/oai:dspace.mit.edu:1721.1/122158","repository":{"repo_id":"mit","name":"MIT","base_url":"https://dspace.mit.edu/oai/request"},"display":{"title":"Electrochemical engineering considerations for gas evolution in molten sulfide electrolytes","abstract":"The current interrupt and galvanostatic electrochemical impedance spectroscopy techniques were utilized to characterize the ohmic, charge transfer, and mass transfer over-potential behavior of gas evolving electrodes in aqueous, molten chloride, and molten sulfide electrolyte solutions under steady-state natural convective flow conditions as a means to gain access to thermodynamic, physicochemical, and hydrodynamic properties of these systems. Previous efforts purposely chose operating conditions under which one or more sources of overpotential were negligible to facilitate analysis of the total overpotential observed at the expense of maintaining operating conditions of industrial relevance. This work represents a preliminary effort to understand the fundamental material properties of a molten sulfide electrolyte, by application of materials-blind electrochemical techniques that were validated on previously well characterized systems-oxygen evolution in aqueous KOH and chlorine evolution in eutectic LiCl-KCl-CsCl. For the first time, values are reported for the saturation concentration of dissolved sulfur gas, an approximate range of Schmidt number for dissolved sulfur, and natural convection limiting current densities in a molten sulfide electrolyte consisting of Cu₂S-BaS-La₂S₃ at 1300°C.","abstract_html":"The current interrupt and galvanostatic electrochemical impedance spectroscopy techniques were utilized to characterize the ohmic, charge transfer, and mass transfer over-potential behavior of gas evolving electrodes in aqueous, molten chloride, and molten sulfide electrolyte solutions under steady-state natural convective flow conditions as a means to gain access to thermodynamic, physicochemical, and hydrodynamic properties of these systems. Previous efforts purposely chose operating conditions under which one or more sources of overpotential were negligible to facilitate analysis of the total overpotential observed at the expense of maintaining operating conditions of industrial relevance. This work represents a preliminary effort to understand the fundamental material properties of a molten sulfide electrolyte, by application of materials-blind electrochemical techniques that were validated on previously well characterized systems-oxygen evolution in aqueous KOH and chlorine evolution in eutectic LiCl-KCl-CsCl. For the first time, values are reported for the saturation concentration of dissolved sulfur gas, an approximate range of Schmidt number for dissolved sulfur, and natural convection limiting current densities in a molten sulfide electrolyte consisting of Cu₂S-BaS-La₂S₃ at 1300°C.","abstract_has_math":false,"creators":["Chmielowiec, Brian John."],"institution":"Massachusetts Institute of Technology","degree_name":"Doctoral","degree_level":null,"degree_discipline":null,"degree_department":"Massachusetts Institute of Technology. Department of Materials Science and Engineering","school":null,"contributors":[],"advisors":["Antoine Allanore."],"committee_chairs":[],"committee_members":[],"year":2019,"date_issued":"2019","date_published":"2019","updated_at":"2026-07-22T22:21:48Z","subjects":["Materials Science and Engineering."],"languages":["eng"],"rights":["MIT theses are protected by copyright. They may be viewed, downloaded, or printed from this source but further reproduction or distribution in any format is prohibited without written permission."],"rights_urls":["http://dspace.mit.edu/handle/1721.1/7582"],"identifier_entries":[]},"links":{"outbound_url":"https://hdl.handle.net/1721.1/122158","outbound_label":"Handle","outbound_source":"dc:identifier.uri"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor.advisor","label":"Advisor","values":["Antoine Allanore."]},{"key":"dc:contributor.department","label":"Department","values":["Massachusetts Institute of Technology. Department of Materials Science and Engineering","MatSci"]},{"key":"dc:contributor.other","label":"Dc Contributor Other","values":["Massachusetts Institute of Technology. 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They may be viewed, downloaded, or printed from this source but further reproduction or distribution in any format is prohibited without written permission."]},{"key":"dc:rights.uri","label":"Rights URI","values":["http://dspace.mit.edu/handle/1721.1/7582"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier.uri","label":"Identifier URI","values":["https://hdl.handle.net/1721.1/122158"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["Thesis: Sc. D., Massachusetts Institute of Technology, Department of Materials Science and Engineering, 2019","Cataloged from PDF version of thesis.","Includes bibliographical references."]},{"key":"dc:description.abstract","label":"Abstract","values":["The current interrupt and galvanostatic electrochemical impedance spectroscopy techniques were utilized to characterize the ohmic, charge transfer, and mass transfer over-potential behavior of gas evolving electrodes in aqueous, molten chloride, and molten sulfide electrolyte solutions under steady-state natural convective flow conditions as a means to gain access to thermodynamic, physicochemical, and hydrodynamic properties of these systems. Previous efforts purposely chose operating conditions under which one or more sources of overpotential were negligible to facilitate analysis of the total overpotential observed at the expense of maintaining operating conditions of industrial relevance. This work represents a preliminary effort to understand the fundamental material properties of a molten sulfide electrolyte, by application of materials-blind electrochemical techniques that were validated on previously well characterized systems-oxygen evolution in aqueous KOH and chlorine evolution in eutectic LiCl-KCl-CsCl. For the first time, values are reported for the saturation concentration of dissolved sulfur gas, an approximate range of Schmidt number for dissolved sulfur, and natural convection limiting current densities in a molten sulfide electrolyte consisting of Cu₂S-BaS-La₂S₃ at 1300°C."]},{"key":"dc:description.degree","label":"Dc Description Degree","values":["Sc. D."]},{"key":"dc:title","label":"Title","values":["Electrochemical engineering considerations for gas evolution in molten sulfide electrolytes"]}]}],"canonical_facts":{"dc:contributor.advisor":["Antoine Allanore."],"dc:contributor.department":["Massachusetts Institute of Technology. Department of Materials Science and Engineering","MatSci"],"dc:contributor.other":["Massachusetts Institute of Technology. Department of Materials Science and Engineering."],"dc:creator":["Chmielowiec, Brian John."],"dc:date.accessioned":["2019-09-16T21:17:45Z"],"dc:date.available":["2019-09-16T21:17:45Z"],"dc:date.issued":["2019"],"dc:description":["Thesis: Sc. D., Massachusetts Institute of Technology, Department of Materials Science and Engineering, 2019","Cataloged from PDF version of thesis.","Includes bibliographical references."],"dc:description.abstract":["The current interrupt and galvanostatic electrochemical impedance spectroscopy techniques were utilized to characterize the ohmic, charge transfer, and mass transfer over-potential behavior of gas evolving electrodes in aqueous, molten chloride, and molten sulfide electrolyte solutions under steady-state natural convective flow conditions as a means to gain access to thermodynamic, physicochemical, and hydrodynamic properties of these systems. Previous efforts purposely chose operating conditions under which one or more sources of overpotential were negligible to facilitate analysis of the total overpotential observed at the expense of maintaining operating conditions of industrial relevance. This work represents a preliminary effort to understand the fundamental material properties of a molten sulfide electrolyte, by application of materials-blind electrochemical techniques that were validated on previously well characterized systems-oxygen evolution in aqueous KOH and chlorine evolution in eutectic LiCl-KCl-CsCl. For the first time, values are reported for the saturation concentration of dissolved sulfur gas, an approximate range of Schmidt number for dissolved sulfur, and natural convection limiting current densities in a molten sulfide electrolyte consisting of Cu₂S-BaS-La₂S₃ at 1300°C."],"dc:description.degree":["Sc. D."],"dc:identifier.uri":["https://hdl.handle.net/1721.1/122158"],"dc:language.iso":["eng"],"dc:publisher":["Massachusetts Institute of Technology"],"dc:rights":["MIT theses are protected by copyright. They may be viewed, downloaded, or printed from this source but further reproduction or distribution in any format is prohibited without written permission."],"dc:rights.uri":["http://dspace.mit.edu/handle/1721.1/7582"],"dc:subject":["Materials Science and Engineering."],"dc:title":["Electrochemical engineering considerations for gas evolution in molten sulfide electrolytes"],"dc:type":["Thesis"],"thesis:degree_name":["Doctoral"]},"updated_at":"2026-07-22T22:21:48Z"}