{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T12:02:53Z","timestamp":1791374573064,"version":"4.3.1"},"reference-count":78,"publisher":"American Chemical Society (ACS)","issue":"4","license":[{"start":{"date-parts":[[2022,2,3]],"date-time":"2022-02-03T00:00:00Z","timestamp":1643846400000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2022,2,3]],"date-time":"2022-02-03T00:00:00Z","timestamp":1643846400000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2022,2,3]],"date-time":"2022-02-03T00:00:00Z","timestamp":1643846400000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100001665","name":"Agence Nationale de la Recherche","doi-asserted-by":"publisher","award":["ANR-13-CESA-0015-01"],"award-info":[{"award-number":["ANR-13-CESA-0015-01"]}],"id":[{"id":"10.13039\/501100001665","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Corporaci\u00f3n Minera de Bolivia"}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2022,2,15]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Photochemical reactions are major pathways for the removal of Hg species from aquatic ecosystems, lowering the concentration of monomethylmercury (MMHg) and its bioaccumulation in foodwebs. Here, we investigated the rates and environmental drivers of MMHg photodegradation and inorganic Hg (IHg) photoreduction in waters of two high-altitude lakes from the Bolivian Altiplano representing meso- to eutrophic conditions. We incubated three contrasting waters in situ at two depths after adding Hg-enriched isotopic species to derive rate constants. We found that transformations mostly occurred in subsurface waters exposed to UV radiation and were mainly modulated by the dissolved organic matter (DOM) level. In parallel, we incubated the same waters after the addition of low concentrations of natural MMHg and followed the stable isotope composition of the remaining Hg species by compound-specific isotope analysis allowing the determination of enrichment factors and mass-independent fractionation (MIF) slopes (\u0394199Hg\/\u0394201Hg) during in situ MMHg photodegradation in natural waters. We found that MIF enrichment factors potentially range from \u221211 to \u221219\u2030 and average \u221214.3 \u00b1 0.6\u2030 (1 SE). The MIF slope diverged depending on the DOM level, ranging from 1.24 \u00b1 0.03 to 1.34 \u00b1 0.02 for the low and high DOM waters, respectively, and matched the MMHg MIF slope recorded in fish from the same lake. Our in situ results thus reveal (i) a relatively similar extent of Hg isotopic fractionation during MMHg photodegradation among contrasted natural waters and compared to previous laboratory experiments and (ii) that the MMHg MIF recorded in fish is characteristic for the MMHg bonding environment. They will enable a better assessment of the extent and conditions conducive to MMHg photodegradation in aquatic ecosystems.<\/jats:p>","DOI":"10.1021\/acs.est.1c04704","type":"journal-article","created":{"date-parts":[[2022,2,3]],"date-time":"2022-02-03T17:32:26Z","timestamp":1643909546000},"page":"2258-2268","source":"Crossref","is-referenced-by-count":25,"title":["In\nSitu Photochemical Transformation of Hg Species\nand Associated Isotopic Fractionation in the Water Column of High-Altitude\nLakes from the Bolivian Altiplano"],"prefix":"10.1021","volume":"56","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5753-9643","authenticated-orcid":true,"given":"Sylvain","family":"Bouchet","sequence":"first","affiliation":[{"name":"Universite de Pau et des Pays de l\u2019Adour, E2S\/UPPA, CNRS, Institut des sciences analytiques et de physico-chimie pour l\u2019environnement et les mate\u0301riaux (IPREM) , ,","place":["Pau, France, 64000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Emmanuel","family":"Tessier","sequence":"additional","affiliation":[{"name":"Universite de Pau et des Pays de l\u2019Adour, E2S\/UPPA, CNRS, Institut des sciences analytiques et de physico-chimie pour l\u2019environnement et les mate\u0301riaux (IPREM) , ,","place":["Pau, France, 64000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3063-1845","authenticated-orcid":true,"given":"Jeremy","family":"Masbou","sequence":"additional","affiliation":[{"name":"Univ. Paul Sabatier, CNRS, IRD, Observatoire Midi Pyre\u0301ne\u0301es (OMP) , , 14 avenue Edouard Belin , ,","place":["Toulouse, France, 31400"]},{"name":"Universite\u0301 de Strasbourg\/EOST\/ENGEES, CNRS UMR 7063 , , 5 rue Descartes , ,","place":["Strasbourg, France, F-67084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5218-7781","authenticated-orcid":true,"given":"David","family":"Point","sequence":"additional","affiliation":[{"name":"Univ. Paul Sabatier, CNRS, IRD, Observatoire Midi Pyre\u0301ne\u0301es (OMP) , , 14 avenue Edouard Belin , ,","place":["Toulouse, France, 31400"]},{"name":"Unidad de Calidad Ambiental (UCA) \u2212 Instituto de Ecologia - Universidad Mayor de San Andres, Campus Universitario de Cota Cota , Calle 27 , ,","place":["La Paz, Bolivia, 3161"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xavier","family":"Lazzaro","sequence":"additional","affiliation":[{"name":"Unidad de Calidad Ambiental (UCA) \u2212 Instituto de Ecologia - Universidad Mayor de San Andres, Campus Universitario de Cota Cota , Calle 27 , ,","place":["La Paz, Bolivia, 3161"]},{"name":"Universite\u0301 des Antilles, CNRS , , IRD. 61 rue Buffon , ,","place":["Paris CEDEX 5, France, 75231"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mathilde","family":"Monperrus","sequence":"additional","affiliation":[{"name":"Universite de Pau et des Pays de l\u2019Adour, E2S\/UPPA, CNRS, Institut des sciences analytiques et de physico-chimie pour l\u2019environnement et les mate\u0301riaux (IPREM) , ,","place":["Pau, France, 64000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4229-1566","authenticated-orcid":true,"given":"Ste\u0301phane","family":"Gue\u0301dron","sequence":"additional","affiliation":[{"name":"Univ. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre , ,","place":["Grenoble, France, 38000"]},{"name":"Campus Universitario de Cota-Cota , , , ,","place":["La Paz, Casilla, Bolivia, 3161"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9498-069X","authenticated-orcid":true,"given":"Dario","family":"Acha","sequence":"additional","affiliation":[{"name":"Unidad de Calidad Ambiental (UCA) \u2212 Instituto de Ecologia - Universidad Mayor de San Andres, Campus Universitario de Cota Cota , Calle 27 , ,","place":["La Paz, Bolivia, 3161"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David","family":"Amouroux","sequence":"additional","affiliation":[{"name":"Universite de Pau et des Pays de l\u2019Adour, E2S\/UPPA, CNRS, Institut des sciences analytiques et de physico-chimie pour l\u2019environnement et les mate\u0301riaux (IPREM) , ,","place":["Pau, France, 64000"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2022,2,3]]},"reference":[{"key":"2026081414082856600_cit1","doi-asserted-by":"publisher","first-page":"10485","DOI":"10.1021\/es202765m","article-title":"All-Time Releases\nof Mercury to the Atmosphere from\nHuman Activities","volume":"45","author":"Streets","year":"2011","journal-title":"Environ. 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Technol."},{"key":"2026081414082856600_cit4","doi-asserted-by":"publisher","first-page":"1332","DOI":"10.1126\/science.1230667","article-title":"The Genetic\nBasis for Bacterial Mercury\nMethylation","volume":"339","author":"Parks","year":"2013","journal-title":"Science"},{"key":"2026081414082856600_cit5","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.1500675","article-title":"Global Prevalence and Distribution of Genes and Microorganisms\nInvolved in Mercury Methylation","volume":"1","author":"Podar","year":"2015","journal-title":"Sci. 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Chem."},{"key":"2026081414082856600_cit10","doi-asserted-by":"publisher","first-page":"11672","DOI":"10.1021\/acs.est.6b03260","article-title":"Role of Settling\nParticles on Mercury Methylation in the Oxic Water Column of Freshwater\nSystems","volume":"50","author":"Gasco\u0301n\nDi\u0301ez","year":"2016","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit11","doi-asserted-by":"publisher","first-page":"355","DOI":"10.1016\/S0168-6445(03)00046-9","article-title":"Bacterial Mercury\nResistance from\nAtoms to Ecosystems","volume":"27","author":"Barkay","year":"2003","journal-title":"FEMS Microbiol. Rev."},{"key":"2026081414082856600_cit12","doi-asserted-by":"publisher","first-page":"2265","DOI":"10.4319\/lo.2004.49.6.2265","article-title":"Biological\nand Photochemical Production of Dissolved\nGaseous Mercury in a Boreal Lake","volume":"49","author":"Poulain","year":"2004","journal-title":"Limnol. Oceanogr."},{"key":"2026081414082856600_cit13","doi-asserted-by":"publisher","first-page":"6690","DOI":"10.1021\/es061046g","article-title":"Novel Reduction\nof Mercury\u00ad(II) by\nMercury-Sensitive Dissimilatory Metal Reducing Bacteria","volume":"40","author":"Wiatrowski","year":"2006","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit14","doi-asserted-by":"publisher","first-page":"1924","DOI":"10.1016\/j.apgeochem.2006.08.008","article-title":"Microbial Mercury Transformations\nin Marine, Estuarine and Freshwater Sediment Downstream of the Idrija\nMercury Mine, Slovenia","volume":"21","author":"Hines","year":"2006","journal-title":"Appl. Geochem."},{"key":"2026081414082856600_cit15","doi-asserted-by":"publisher","first-page":"303","DOI":"10.1016\/S0009-2541(02)00122-5","article-title":"Natural Attenuation\nof TCE, As, Hg\nLinked to the Heterogeneous Oxidation of Fe\u00ad(II): An AFM Study","volume":"190","author":"Charlet","year":"2002","journal-title":"Chem. Geol."},{"key":"2026081414082856600_cit16","doi-asserted-by":"publisher","first-page":"437","DOI":"10.1016\/S0045-6535(03)00545-9","article-title":"Reduction of AgI,\nAuIII, CuII, and Hg II by FeII\/FeIII\nHydroxysulfate Green Rust","volume":"53","author":"O\u2019Loughlin","year":"2003","journal-title":"Chemosphere"},{"key":"2026081414082856600_cit17","doi-asserted-by":"publisher","first-page":"457","DOI":"10.1007\/BF00342291","article-title":"Abiotic Reduction of\nMercury by Humic Substances in\nAquatic System - An Important Process for the Mercury Cycle","volume":"56","author":"Allard","year":"1991","journal-title":"Water, Air, Soil Pollut."},{"key":"2026081414082856600_cit18","doi-asserted-by":"publisher","first-page":"1479","DOI":"10.1073\/pnas.1008747108","article-title":"Mercury Reduction and Complexation by Natural Organic Matter in Anoxic\nEnvironments","volume":"108","author":"Gu","year":"2011","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"key":"2026081414082856600_cit19","doi-asserted-by":"publisher","first-page":"146","DOI":"10.1016\/j.jes.2019.11.007","article-title":"Linking the Electron Donation Capacity\nto the Molecular Composition\nof Soil Dissolved Organic Matter from the Three Gorges Reservoir Areas,\nChina","volume":"90","author":"Jiang","year":"2020","journal-title":"J. Environ. Sci."},{"key":"2026081414082856600_cit20","doi-asserted-by":"publisher","first-page":"694","DOI":"10.1038\/380694a0","article-title":"Photodegradation\nof Methylmercury in Lakes","volume":"380","author":"Seller","year":"1996","journal-title":"Nature"},{"key":"2026081414082856600_cit21","doi-asserted-by":"publisher","first-page":"2054","DOI":"10.1002\/etc.5620161010","article-title":"Photochemical Formation of Volatile\nMercury in High Arctic Lakes","volume":"16","author":"Amyot","year":"1997","journal-title":"Environ. Toxicol.\nChem."},{"key":"2026081414082856600_cit22","doi-asserted-by":"publisher","first-page":"492","DOI":"10.1016\/j.gca.2012.01.019","article-title":"Factors\nControlling the Abiotic Photo-Degradation\nof Monomethylmercury in Surface Waters","volume":"84","author":"Black","year":"2012","journal-title":"Geochim.\nCosmochim. Acta"},{"key":"2026081414082856600_cit23","doi-asserted-by":"publisher","first-page":"1212","DOI":"10.1021\/es0513234","article-title":"Photodecomposition\nof Methylmercury in an Arctic Alaskan\nLake","volume":"40","author":"Hammerschmidt","year":"2006","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit24","doi-asserted-by":"publisher","first-page":"1471","DOI":"10.1016\/j.chemosphere.2012.12.013","article-title":"Photo-Degradation of Monomethylmercury in the Presence\nof Chloride Ion","volume":"91","author":"Sun","year":"2013","journal-title":"Chemosphere"},{"key":"2026081414082856600_cit25","doi-asserted-by":"publisher","first-page":"5692","DOI":"10.1021\/es9002923","article-title":"Importance\nof Ultraviolet Radiation\nin the Photodemethylation of Methylmercury in Freshwater Ecosystems","volume":"43","author":"Lehnherr","year":"2009","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit26","doi-asserted-by":"publisher","first-page":"2664","DOI":"10.1021\/es034702a","article-title":"Effect\nof Dissolved Organic Carbon on the Photoproduction of Dissolved Gaseous\nMercury in Lakes: Potential Impacts of Forestry","volume":"38","author":"O\u2019Driscoll","year":"2004","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit27","doi-asserted-by":"publisher","first-page":"1917","DOI":"10.1016\/j.gca.2004.10.026","article-title":"Relationship\nbetween DOC Photochemistry\nand Mercury Redox Transformations in Temperate Lakes and Wetlands","volume":"69","author":"Garcia","year":"2005","journal-title":"Geochim. Cosmochim. Acta"},{"key":"2026081414082856600_cit28","doi-asserted-by":"publisher","first-page":"14","DOI":"10.1007\/s00128-017-2236-x","article-title":"Methylmercury Biogeochemistry\nin Freshwater Ecosystems:\nA Review Focusing on DOM and Photodemethylation","volume":"100","author":"Klapstein","year":"2018","journal-title":"Bull. Environ. Contam. Toxicol."},{"key":"2026081414082856600_cit29","doi-asserted-by":"publisher","first-page":"192","DOI":"10.1016\/j.gca.2020.03.027","article-title":"The Role of Fluorescent\nDissolved Organic Matter on Mercury Photoreduction Rates: A Case Study\nof Three Temperate Lakes","volume":"277","author":"Yang","year":"2020","journal-title":"Geochim. Cosmochim.\nActa"},{"key":"2026081414082856600_cit30","doi-asserted-by":"crossref","first-page":"789","DOI":"10.1007\/978-94-011-0153-0_84","article-title":"Influence of Humic Substances on Photolysis of\nDivalent Mercury in\nAqueous Solution","volume-title":"Mercury as a Global Pollutant:\nProceedings of the Third International Conference held in Whistler,\nBritish Columbia, July 10\u201314, 1994","author":"Xiao","year":"1995"},{"key":"2026081414082856600_cit31","doi-asserted-by":"publisher","first-page":"473","DOI":"10.1038\/ngeo892","article-title":"Photolytic Degradation of Methylmercury Enhanced by\nBinding to Natural Organic Ligands","volume":"3","author":"Zhang","year":"2010","journal-title":"Nat. Geosci."},{"key":"2026081414082856600_cit32","doi-asserted-by":"publisher","first-page":"392","DOI":"10.1016\/j.envpol.2017.09.049","article-title":"Methylmercury Photodemethylation\nIs Inhibited in Lakes with High Dissolved Organic Matter","volume":"232","author":"Klapstein","year":"2018","journal-title":"Environ. Pollut."},{"key":"2026081414082856600_cit33","doi-asserted-by":"publisher","first-page":"1892","DOI":"10.1039\/C5EM00305A","article-title":"Photoreduction\nof Hg\u00ad(II) and Photodemethylation\nof Methylmercury: The Key Role of Thiol Sites on Dissolved Organic\nMatter","volume":"17","author":"Jeremiason","year":"2015","journal-title":"Environ. Sci.: Processes Impacts"},{"key":"2026081414082856600_cit34","doi-asserted-by":"publisher","first-page":"6279","DOI":"10.1021\/es400373s","article-title":"Towards Universal\nWavelength-Specific Photodegradation Rate Constants for Methyl Mercury\nin Humic Waters, Exemplified by a Boreal Lake-Wetland Gradient","volume":"47","author":"Ferna\u0301ndez-Go\u0301mez","year":"2013","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit35","doi-asserted-by":"publisher","first-page":"426","DOI":"10.1021\/ez500254z","article-title":"Why Dissolved Organic\nMatter Enhances Photodegradation of Methylmercury","volume":"1","author":"Qian","year":"2014","journal-title":"Environ. Sci. Technol. Lett."},{"key":"2026081414082856600_cit36","doi-asserted-by":"publisher","first-page":"264","DOI":"10.1016\/j.watres.2018.03.055","article-title":"Probing the DOM-Mediated Photodegradation of Methylmercury by Using\nOrganic Ligands with Different Molecular Structures as the DOM Model","volume":"138","author":"Zhang","year":"2018","journal-title":"Water Res."},{"key":"2026081414082856600_cit37","doi-asserted-by":"publisher","first-page":"249","DOI":"10.1146\/annurev-earth-050212-124107","article-title":"Mercury\nIsotopes in Earth and Environmental\nSciences","volume":"42","author":"Blum","year":"2014","journal-title":"Annu. Rev. Earth Planet. Sci."},{"key":"2026081414082856600_cit38","doi-asserted-by":"publisher","first-page":"879","DOI":"10.1038\/ngeo1918","article-title":"Methylmercury Production below the\nMixed Layer in the\nNorth Pacific Ocean","volume":"6","author":"Blum","year":"2013","journal-title":"Nat. Geosci."},{"key":"2026081414082856600_cit39","doi-asserted-by":"publisher","first-page":"417","DOI":"10.1126\/science.1148050","article-title":"Mass-Dependent and -Independent Fractionation of Hg\nIsotopes by Photoreduction in Aquatic Systems","volume":"318","author":"Bergquist","year":"2007","journal-title":"Science"},{"key":"2026081414082856600_cit40","doi-asserted-by":"publisher","first-page":"950","DOI":"10.1039\/b926650j","article-title":"Experimental\nStudy of Mass-Independence of Hg Isotope Fractionation during Photodecomposition\nof Dissolved Methylmercury","volume":"25","author":"Malinovsky","year":"2010","journal-title":"J. Anal. At. Spectrom."},{"key":"2026081414082856600_cit41","doi-asserted-by":"publisher","first-page":"6704","DOI":"10.1016\/j.gca.2009.08.016","article-title":"Mercury Isotope Fractionation during Photoreduction\nin Natural Water Is Controlled by Its Hg\/DOC Ratio","volume":"73","author":"Zheng","year":"2009","journal-title":"Geochim. Cosmochim. Acta"},{"key":"2026081414082856600_cit42","doi-asserted-by":"publisher","first-page":"4246","DOI":"10.1021\/jp9111348","article-title":"Isotope Fractionation of Mercury\nduring Its Photochemical\nReduction by Low-Molecular-Weight Organic Compounds","volume":"114","author":"Zheng","year":"2010","journal-title":"J. Phys. Chem. A"},{"key":"2026081414082856600_cit43","doi-asserted-by":"publisher","first-page":"259","DOI":"10.1021\/es5034553","article-title":"Mercury\nIsotope Fractionation during\nAqueous Photo-Reduction of Monomethylmercury in the Presence of Dissolved\nOrganic Matter","volume":"49","author":"Chandan","year":"2015","journal-title":"Environ. Sci. Technol."},{"key":"2026081414082856600_cit44","doi-asserted-by":"publisher","first-page":"102","DOI":"10.1016\/j.chemgeo.2015.02.025","article-title":"Effects\nof Ultraviolet Radiation on Mercury Isotope Fractionation during Photo-Reduction\nfor Inorganic and Organic Mercury Species","volume":"405","author":"Rose","year":"2015","journal-title":"Chem.\nGeol."},{"key":"2026081414082856600_cit45","doi-asserted-by":"publisher","first-page":"2842","DOI":"10.1021\/acs.jpca.9b06308","article-title":"Mercury Isotope Fractionation during\nthe Photochemical\nReduction of Hg\u00ad(II) Coordinated with Organic Ligands","volume":"124","author":"Motta","year":"2020","journal-title":"J. Phys. Chem. A"},{"key":"2026081414082856600_cit46","doi-asserted-by":"publisher","first-page":"438","DOI":"10.3390\/geosciences8120438","article-title":"Algal Bloom Exacerbates Hydrogen\nSulfide and Methylmercury Contamination in the Emblematic High-Altitude\nLake Titicaca","volume":"8","author":"Acha\u0301","year":"2018","journal-title":"Geosciences"},{"key":"2026081414082856600_cit47","doi-asserted-by":"publisher","first-page":"262","DOI":"10.1016\/j.envpol.2017.08.009","article-title":"Mercury Contamination Level and Speciation\nInventory\nin Lakes Titicaca & Uru-Uru (Bolivia): Current Status and Future\nTrends","volume":"231","author":"Gue\u0301dron","year":"2017","journal-title":"Environ. 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