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We validate a scheme for producing results in the thermodynamic limit by correcting results obtained on finite lithium clusters containing only 40\u2013100 atoms, which enables the use of hybrid density functionals, random-phase approximation, and correlated wavefunction theories, such as coupled-cluster theory and auxiliary-field quantum Monte Carlo. We find that the high-level theories agree to within 2\u20135 kcal\/mol and can, therefore, serve as benchmarks for more affordable methods. Using our reference data, we demonstrate that generalized gradient approximation functionals, such as PBE, are not sufficiently accurate for reaction barrier heights, and we identify \u03c9B97X-V as an especially promising functional for the interfacial chemistry of electrolyte solvents at lithium metal anodes.<\/jats:p>","DOI":"10.1063\/5.0335668","type":"journal-article","created":{"date-parts":[[2026,10,6]],"date-time":"2026-10-06T11:53:51Z","timestamp":1791287631000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Adsorption energies and decomposition barrier heights for ethylene carbonate on the surface of lithium from cluster-based quantum chemistry"],"prefix":"10.1063","volume":"165","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9059-4911","authenticated-orcid":false,"given":"Ethan A.","family":"Vo","sequence":"first","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7965-379X","authenticated-orcid":false,"given":"Hung T.","family":"Vuong","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5556-4079","authenticated-orcid":false,"given":"Zachary K.","family":"Goldsmith","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3714-2753","authenticated-orcid":false,"given":"Hong-Zhou","family":"Ye","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry, University of Maryland 2 , College Park, Maryland 20742,","place":["USA"]},{"name":"Institute for Physical Science and Technology, University of Maryland 3 , College Park, Maryland 20742,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yujing","family":"Wei","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5499-9775","authenticated-orcid":false,"given":"Sohang","family":"Kundu","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5230-2631","authenticated-orcid":false,"given":"Ardavan","family":"Farahvash","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7814-6072","authenticated-orcid":false,"given":"Garvit","family":"Agarwal","sequence":"additional","affiliation":[{"name":"Schr\u00f6dinger, Inc. 4 , New York, New York 10036,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1708-9342","authenticated-orcid":false,"given":"Richard A.","family":"Friesner","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7445-2136","authenticated-orcid":false,"given":"Timothy C.","family":"Berkelbach","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Columbia University 1 , New York, New York 10027,","place":["USA"]},{"name":"Initiative for Computational Catalysis, Flatiron Institute 5 , New York, New York 10010,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,10,6]]},"reference":[{"key":"2026100607534809500_c1","doi-asserted-by":"publisher","first-page":"11708","DOI":"10.1021\/ja0164529","article-title":"Theoretical studies to understand surface chemistry on carbon anodes for lithium\u2013ion batteries: Reduction mechanisms of ethylene carbonate","volume":"123","year":"2001","journal-title":"J.\u00a0Am. 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