{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T04:58:41Z","timestamp":1785473921219,"version":"3.56.0"},"reference-count":40,"publisher":"American Chemical Society (ACS)","issue":"7","license":[{"start":{"date-parts":[[2026,6,15]],"date-time":"2026-06-15T00:00:00Z","timestamp":1781481600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/100000048","name":"American Cancer Society","doi-asserted-by":"publisher","award":["RSG22-025-01-CDP"],"award-info":[{"award-number":["RSG22-025-01-CDP"]}],"id":[{"id":"10.13039\/100000048","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100008227","name":"Achievement Rewards for College Scientists Foundation","doi-asserted-by":"publisher","award":["NA"],"award-info":[{"award-number":["NA"]}],"id":[{"id":"10.13039\/100008227","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100013354","name":"Center for Drug Design, University of Minnesota","doi-asserted-by":"publisher","award":["NA"],"award-info":[{"award-number":["NA"]}],"id":[{"id":"10.13039\/100013354","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,7,27]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Reactive \u03b1-dicarbonyls, such as methylglyoxal (MGO), are critical biomarkers of carbonyl stress, yet their real-time monitoring is stifled by a selectivity-biocompatibility paradox. Existing probes either suffer from aldehyde promiscuity, failing to distinguish dicarbonyls from the global lipid peroxidation background, or rely on high-energy, cytotoxic excitation that precludes longitudinal study. Herein, we report the rational design of a dicyano-BODIPY platform engineered to resolve this tension through a precision-tuned acceptor-photoinduced electron transfer (a-PET) mechanism. By employing density functional theory (DFT) as a predictive blueprint, we strategically depressed the BODIPY core HOMO to \u22126.63 eV, establishing a specific energetic gradient that enforces a robust \u201coff\u201d state until triggered by reversible covalent capture of \u03b1-dicarbonyls. This electronically gated design enables longitudinal, visible-light imaging of bidirectional MGO flux in living cells, a feat inaccessible to current irreversible sensors. We further demonstrate the platform\u2019s high-fidelity performance in complex biological matrices by mapping dose-responsive MGO burden in murine brain tissue following controlled intracranial perturbation, providing a vital tool for interrogating the role of glyoxal stress in tissue-level pathologies. This work provides a generalizable electronic framework for the development of reversible-covalent sensors capable of monitoring metabolic dynamics in intact biological environments<\/jats:p>","DOI":"10.1021\/jacsau.6c00566","type":"journal-article","created":{"date-parts":[[2026,6,15]],"date-time":"2026-06-15T07:44:45Z","timestamp":1781509485000},"page":"4039-4047","source":"Crossref","is-referenced-by-count":0,"title":["Rational Design of\nan Electronically Gated Dicyano-BODIPY\nPlatform for Reversible-Covalent Imaging of Methylglyoxal"],"prefix":"10.1021","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1579-1285","authenticated-orcid":true,"given":"John M.","family":"Talbott","sequence":"first","affiliation":[{"name":"Emory University , , , ,","place":["Atlanta, Georgia, United States, 30322"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Samrat","family":"Kundu","sequence":"additional","affiliation":[{"name":"Emory University , , , ,","place":["Atlanta, Georgia, United States, 30322"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Brandon","family":"Li","sequence":"additional","affiliation":[{"name":"Emory University , , , ,","place":["Atlanta, Georgia, United States, 30322"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Leslie","family":"Hassanein","sequence":"additional","affiliation":[{"name":"Emory University School of Medicine , , , ,","place":["Atlanta, Georgia, United States, 30322"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Prakashkumar","family":"Dobariya","sequence":"additional","affiliation":[{"name":"University of Minnesota , , , ,","place":["Minneapolis, Minnesota, United States, 55455"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David","family":"Weinshenker","sequence":"additional","affiliation":[{"name":"Emory University School of Medicine , , , ,","place":["Atlanta, Georgia, United States, 30322"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8733-2029","authenticated-orcid":true,"given":"Swati S.","family":"More","sequence":"additional","affiliation":[{"name":"University of Minnesota , , , ,","place":["Minneapolis, Minnesota, United States, 55455"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9636-2222","authenticated-orcid":true,"given":"Monika","family":"Raj","sequence":"additional","affiliation":[{"name":"Emory University , , , ,","place":["Atlanta, Georgia, United States, 30322"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,6,15]]},"reference":[{"key":"2026073100191173700_cit1","doi-asserted-by":"publisher","first-page":"64","DOI":"10.1016\/j.semcancer.2017.05.010","article-title":"Methylglyoxal-derived\nstress: an emerging biological factor involved in the onset and progression\nof cancer","volume":"49","author":"Bellahcene","year":"2018","journal-title":"Semin. Cancer Biol."},{"key":"2026073100191173700_cit2","doi-asserted-by":"publisher","first-page":"667","DOI":"10.1002\/iub.1324","article-title":"Cells producing\ntheir own nemesis:\nunderstanding methylglyoxal metabolism","volume":"66","author":"Chakraborty","year":"2014","journal-title":"IUBMB\nLife"},{"key":"2026073100191173700_cit3","doi-asserted-by":"publisher","first-page":"121","DOI":"10.1016\/j.bbadis.2003.08.002","article-title":"Increased\nformation of methylglyoxal and protein glycation, oxidation and nitrosation\nin triosephosphate isomerase deficiency","volume":"1639","author":"Ahmed","year":"2003","journal-title":"Biochim.\nBiophys. Acta"},{"key":"2026073100191173700_cit4","doi-asserted-by":"publisher","first-page":"109","DOI":"10.1042\/bj3440109","article-title":"Formation of glyoxal,\nmethylglyoxal\nand 3-deoxyglucosone in the glycation of proteins by glucose","volume":"344","author":"Thornalley","year":"1999","journal-title":"Biochem. J."},{"key":"2026073100191173700_cit5","doi-asserted-by":"publisher","first-page":"1","DOI":"10.4196\/kjpp.2014.18.1.1","article-title":"Advanced glycation\nend products and diabetic complications","volume":"18","author":"Singh","year":"2014","journal-title":"Korean\nJ. Physiol. Pharmacol."},{"key":"2026073100191173700_cit6","doi-asserted-by":"publisher","first-page":"111","DOI":"10.1196\/annals.1333.014","article-title":"Dicarbonyl\nintermediates in the maillard reaction","volume":"1043","author":"Thornalley","year":"2005","journal-title":"Ann.\nN.Y. Acad. 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Lumin."},{"key":"2026073100191173700_cit37","doi-asserted-by":"publisher","DOI":"10.1002\/cbic.202400335","article-title":"Exploring the World\nof Curcumin: Photophysics, Photochemistry,\nand Applications in Nanoscience and Biology","volume":"25","author":"Ghosh","year":"2024","journal-title":"ChemBioChem."},{"key":"2026073100191173700_cit38","doi-asserted-by":"publisher","first-page":"778","DOI":"10.1111\/dme.12753","article-title":"The role\nof serum methylglyoxal on diabetic peripheral and cardiovascular autonomic\nneuropathy: the ADDITION Denmark study","volume":"32","author":"Hansen","year":"2015","journal-title":"Diabet.\nMed."},{"key":"2026073100191173700_cit39","doi-asserted-by":"publisher","first-page":"523","DOI":"10.1042\/BST20130254","article-title":"Reducing methylglyoxal as a therapeutic\ntarget for diabetic heart disease","volume":"42","author":"Vulesevic","year":"2014","journal-title":"Biochem.\nSoc. 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