{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,7,30]],"date-time":"2025-07-30T11:16:58Z","timestamp":1753874218524,"version":"3.41.2"},"reference-count":95,"publisher":"AIP Publishing","issue":"12","funder":[{"DOI":"10.13039\/501100001871","name":"Funda\u00e7\u00e3o para a Ci\u00eancia e a Tecnologia","doi-asserted-by":"publisher","award":["UIDB\/04046\/2020","UIDP\/04046\/2020","PTDC\/QUI-QFI\/29236\/2017","PTDC\/QUI-QFI\/31896\/2017"],"award-info":[{"award-number":["UIDB\/04046\/2020","UIDP\/04046\/2020","PTDC\/QUI-QFI\/29236\/2017","PTDC\/QUI-QFI\/31896\/2017"]}],"id":[{"id":"10.13039\/501100001871","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":["pubs.aip.org"],"crossmark-restriction":true},"short-container-title":[],"published-print":{"date-parts":[[2021,3,28]]},"abstract":"<jats:p>The photoreduction of a Keggin type lacunary tungstomolybdophosphate, \u03b1-(Bu4N)4[H3PW9Mo2O39], in acetonitrile, led to the formation of a monoreduced lacunary heteropoly anion, or a one electron reduced \u201cheteropoly blue\u201d species, whereby the added \u201cblue\u201d electron was captured by the molybdenum atoms. The magnetic properties and behavior of the \u201cblue\u201d electron were studied by a modified Evans nuclear magnetic resonance method (small downshift of the 31P signal) and variable-temperature electron paramagnetic resonance (g = 1.936 for MoV). The intermolecular exchange of the \u201cblue\u201d electron was limited by a geometrical factor, which requires the contact between Mo caps to exchange it between the heteropoly couple. The intramolecular exchange of the \u201cblue\u201d electron between Mo atoms was rather fast (5.3 \u00d7 109 s\u22121), with a rate of more than six orders of magnitude larger than the intermolecular exchange rate. Density functional theory was used to determine the most prevalent protonation sites in the mixed lacunary isomers with the aim of studying the intramolecular electron transfer pathway in the isolated [H4PW9Mo2O39]4\u2212 species. The singly occupied molecular orbital (SOMO) is essentially localized in one of the two nonequivalent molybdenum sites. The kinetics of the intramolecular electron exchange equilibrium MoV + MoVI \u2192 MoVI + MoV between the two molybdenum atoms bridged by an oxygen atom was found to be fast in agreement with the experimental result. The transition state is of mixed-valence type, with the SOMO delocalized over the Mo\u2014O\u2014Mo group. Spectroscopic parameters were found to be in fair agreement with experimental results.<\/jats:p>","DOI":"10.1063\/5.0039092","type":"journal-article","created":{"date-parts":[[2021,3,22]],"date-time":"2021-03-22T10:23:28Z","timestamp":1616408608000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["A lacunary tungstomolybdophosphate as an electronic pendulum: The \u201cblue\u201d electron under examination"],"prefix":"10.1063","volume":"154","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5754-7328","authenticated-orcid":false,"given":"Nuno A. G.","family":"Bandeira","sequence":"first","affiliation":[{"name":"BioISI - Biosystems and Integrative Sciences Institute, Departamento de Qu\u00edmica e Bioqu\u00edmica, Faculdade de Ci\u00eancias, Universidade de Lisboa 1 , Campo Grande, Ed. C8, 1749-016 Lisboa, Portugal"}]},{"given":"Huizhang","family":"Liu","sequence":"additional","affiliation":[{"name":"BioISI - Biosystems and Integrative Sciences Institute, Departamento de Qu\u00edmica e Bioqu\u00edmica, Faculdade de Ci\u00eancias, Universidade de Lisboa 1 , Campo Grande, Ed. C8, 1749-016 Lisboa, Portugal"},{"name":"Jiangsu TOP New Materials Ltd. 2 , Maba Economic Zone, Xuyi, Jiangsu, People\u2019s Republic of China"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6872-3569","authenticated-orcid":false,"given":"Maria Jos\u00e9","family":"Calhorda","sequence":"additional","affiliation":[{"name":"BioISI - Biosystems and Integrative Sciences Institute, Departamento de Qu\u00edmica e Bioqu\u00edmica, Faculdade de Ci\u00eancias, Universidade de Lisboa 1 , Campo Grande, Ed. 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