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Their typical mechanism, especially of the clinically far developed representative Triapine, is chelation of iron (Fe), with the Fe-containing enzyme ribonucleotide reductase as primary intracellular target. However, for the subclass of terminally disubstituted, nanomolar-active derivatives like Dp44mT and Me2NNMe2, recent findings suggest that the chelation, stability, and reduction properties of the copper(II) (Cu) complexes are essential for their modes of action. Consequently, it is important to elucidate whether blood serum Cu(II) is a potential metal source for these TSCs. To gain more insights, the interaction of Triapine, Dp44mT or Me2NNMe2 with purified human serum albumin (HSA) as the main pool of labile Cu(II) was investigated by UV-vis and electron paramagnetic resonance measurements. Subsequently, a size-exclusion chromatography inductively coupled plasma mass spectrometry method for the differentiation of Cu species in serum was developed, especially separating the non-labile Cu enzyme ceruloplasmin from HSA. The results indicate that the TSCs specifically chelate copper from the N-terminal Cu-binding site of HSA. Furthermore, the Cu(II)-TSC complexes were shown to form ternary HSA conjugates, most likely via histidine. Noteworthy, Fe-chelation from transferrin was not overserved, even not for Triapine. In summary, the labile Cu pool of HSA is a potential source for Cu-TSC complex formation and, consequently, distinctly influences the anticancer activity and pharmacological behavior of TSCs.<\/jats:p>","DOI":"10.1093\/mtomcs\/mfad046","type":"journal-article","created":{"date-parts":[[2023,7,27]],"date-time":"2023-07-27T12:14:43Z","timestamp":1690460083000},"source":"Crossref","is-referenced-by-count":7,"title":["Human serum albumin as a copper source for anticancer thiosemicarbazones"],"prefix":"10.1093","volume":"15","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4907-218X","authenticated-orcid":false,"given":"Martin","family":"Schaier","sequence":"first","affiliation":[{"name":"Institute of Analytical Chemistry, Faculty of Chemistry, University of Vienna , Waehringer Str. 38, A-1090 Vienna , Austria"},{"name":"Vienna Doctoral School in Chemistry (DoSChem), University of Vienna , Waehringer Str. 42, A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1944-3552","authenticated-orcid":false,"given":"Enrico","family":"Falcone","sequence":"additional","affiliation":[{"name":"Institut de Chimie, UMR 7177, CNRS, Universit\u00e9 de Strasbourg , 4 Rue Blaise Pascal, 67000 Strasbourg , France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tomas","family":"Prstek","sequence":"additional","affiliation":[{"name":"Institute of Analytical Chemistry, Faculty of Chemistry, University of Vienna , Waehringer Str. 38, A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bertrand","family":"Vileno","sequence":"additional","affiliation":[{"name":"Institut de Chimie, UMR 7177, CNRS, Universit\u00e9 de Strasbourg , 4 Rue Blaise Pascal, 67000 Strasbourg , France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8221-1044","authenticated-orcid":false,"given":"Sonja","family":"Hager","sequence":"additional","affiliation":[{"name":"Center for Cancer Research and Comprehensive Cancer Center, Medical University of Vienna , Borschkegasse 8a, A-1090 Vienna , Austria"},{"name":"Institute of Food Chemistry and Toxicology, Faculty of Chemistry, University of Vienna , Waehringer Str. 38, A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0877-1822","authenticated-orcid":false,"given":"Bernhard K","family":"Keppler","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry, Faculty of Chemistry, University of Vienna , Waehringer Str. 42, A-1090 Vienna , Austria"},{"name":"Research Cluster \u2018Translational Cancer Therapy Research\u2019 , A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6401-8646","authenticated-orcid":false,"given":"Petra","family":"Heffeter","sequence":"additional","affiliation":[{"name":"Center for Cancer Research and Comprehensive Cancer Center, Medical University of Vienna , Borschkegasse 8a, A-1090 Vienna , Austria"},{"name":"Research Cluster \u2018Translational Cancer Therapy Research\u2019 , A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1460-4919","authenticated-orcid":false,"given":"Gunda","family":"Koellensperger","sequence":"additional","affiliation":[{"name":"Institute of Analytical Chemistry, Faculty of Chemistry, University of Vienna , Waehringer Str. 38, A-1090 Vienna , Austria"},{"name":"Research Cluster \u2018Translational Cancer Therapy Research\u2019 , A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8013-0806","authenticated-orcid":false,"given":"Peter","family":"Faller","sequence":"additional","affiliation":[{"name":"Institut de Chimie, UMR 7177, CNRS, Universit\u00e9 de Strasbourg , 4 Rue Blaise Pascal, 67000 Strasbourg , France"},{"name":"Institut Universitaire de France (IUF) , 1 rue Descartes, 75231 Paris , France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8311-1632","authenticated-orcid":false,"given":"Christian R","family":"Kowol","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry, Faculty of Chemistry, University of Vienna , Waehringer Str. 42, A-1090 Vienna , Austria"},{"name":"Research Cluster \u2018Translational Cancer Therapy Research\u2019 , A-1090 Vienna , Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"286","published-online":{"date-parts":[[2023,7,28]]},"reference":[{"key":"2024012010413180700_bib1","doi-asserted-by":"crossref","first-page":"85","DOI":"10.1016\/j.jinorgbio.2018.10.006","article-title":"Synthesis and biological evaluation of biotin-conjugated anticancer thiosemicarbazones and their iron(III) and copper(II) complexes","volume":"190","author":"Kallus","year":"2019","journal-title":"J. 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