A New Paradigm for Brine Thermodynamics: Inverse Electrochemical Probing of Activity Using Reverse Electrodialysis 

Inverse electrochemical probing of thermodynamic activity in hypersaline brines using reverse electrodialysis | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Inverse electrochemical probing of thermodynamic activity in hypersaline brines using reverse electrodialysis Moulay Rachid Babaa This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8574892/v2 This work is licensed under a CC BY 4.0 License Status: Posted Version 2 posted You are reading this latest preprint version Show more versions Abstract Hypersaline electrolytes are difficult to characterize because strong non-ideality decouples concentration from chemical potential, while conventional electrochemical sensors often fail at high ionic strength. Here we introduce a model-based framework that treats reverse electrodialysis (RED) as an electrochemical transducer for inverse thermodynamic probing: deviations of stack open-circuit voltage (OCV) from an ideal-solution Nernst baseline encode the non-ideal chemical-potential state of complex brines. We couple a permselectivity-corrected RED electrochemical model with multi-ion Pitzer thermodynamics and perform seasonal simulations for hypersaline brine–treated wastewater systems representative of inland saline environments. Systematic OCV deviations define a measurable residual voltage, ΔEγ, that isolates activity-coefficient contributions and constrains mean ionic activity-coefficient contrasts between the concentrated and dilute streams. Using the resulting mapping between ΔEγ and γ±, we show that OCV measurements can, in principle, be inverted to infer effective NaCl-equivalent activity (thermodynamic salinity) in real time. Despite large seasonal changes in composition and total salt load, hypersaline brines exhibit constrained effective activities of 1.00–1.11 mol kg −1 , substantially lower than implied by concentration-only assumptions. This proof-of-concept establishes, for the first time, a direct mapping between electrochemical voltage observables (ΔEγ) and reduced thermodynamic descriptors governing activity-coefficient contrasts (γ ± ), positioning RED/ED stacks as electrochemical transducers for activity-based sensing and diagnostics in non-ideal, multi-ionic electrolytes, with implications for hypersaline brine geochemistry and management. Physical Chemistry electrolyte non-ideality ionic activity Pitzer model reverse electrodialysis hypersaline brines environmental diagnostics Full Text Additional Declarations The authors declare potential competing interests as follows: The author is the applicant on a pending international patent application related to reverse electrodialysis as an inverse thermodynamic probe. Supplementary Files BabaaSI.pdf Cite Share Download PDF Status: Posted Version 2 posted You are reading this latest preprint version Show more versions Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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probe.","formattedTitle":"\u003cp\u003e\u003cstrong\u003eInverse electrochemical probing of thermodynamic activity in hypersaline brines using reverse electrodialysis\u003c/strong\u003e\u003c/p\u003e","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"electrolyte non-ideality, ionic activity, Pitzer model, reverse electrodialysis, hypersaline brines, environmental diagnostics","lastPublishedDoi":"10.21203/rs.3.rs-8574892/v2","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8574892/v2","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003e\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003eHypersaline electrolytes are difficult to characterize because strong non-ideality decouples concentration from chemical potential, while conventional electrochemical sensors often fail at high ionic strength. Here we introduce a model-based framework that treats reverse electrodialysis (RED) as an electrochemical transducer for inverse thermodynamic probing: deviations of stack open-circuit voltage (OCV) from an ideal-solution Nernst baseline encode the non-ideal chemical-potential state of complex brines. We couple a permselectivity-corrected RED electrochemical model with multi-ion Pitzer thermodynamics and perform seasonal simulations for hypersaline brine–treated wastewater systems representative of inland saline environments. Systematic OCV deviations define a measurable residual voltage, ΔEγ, that isolates activity-coefficient contributions and constrains mean ionic activity-coefficient contrasts between the concentrated and dilute streams. Using the resulting \u0026nbsp;mapping\u0026nbsp;between ΔEγ\u0026nbsp;and γ±, we show that OCV measurements can, in principle, be inverted to infer effective NaCl-equivalent activity (thermodynamic salinity) in real time. Despite large seasonal changes in composition and total salt load, hypersaline brines exhibit constrained effective activities of 1.00–1.11 mol kg\u003csup\u003e−1\u003c/sup\u003e, substantially lower than implied by concentration-only assumptions.\u0026nbsp;This proof-of-concept establishes, for the first time, a direct mapping between electrochemical voltage observables (ΔEγ) and reduced thermodynamic descriptors governing activity-coefficient contrasts (γ\u003csub\u003e±\u003c/sub\u003e), positioning RED/ED stacks as electrochemical transducers for activity-based sensing and diagnostics in non-ideal, multi-ionic electrolytes, with implications for hypersaline brine geochemistry and management.\u003c/p\u003e","manuscriptTitle":"Inverse electrochemical probing of thermodynamic activity in hypersaline brines using reverse electrodialysis","msid":"","msnumber":"","nonDraftVersions":[{"code":2,"date":"2026-01-26 15:16:55","doi":"10.21203/rs.3.rs-8574892/v2","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}},{"code":1,"date":"2026-01-13 03:16:38","doi":"10.21203/rs.3.rs-8574892/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"17d1728d-7d97-412f-b5c3-f532a5952d2a","owner":[],"postedDate":"January 26th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":61307466,"name":"Physical Chemistry"}],"tags":[],"updatedAt":"2026-01-17T21:38:21+00:00","versionOfRecord":[],"versionCreatedAt":"2026-01-26 15:16:55","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v2","identity":"rs-8574892","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8574892","identity":"rs-8574892","version":["v2"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}