{"refrec":{"BRefID":349361,"RR":"<b>Henriques Pereira, D.P.; Leethaus, J.; Beyazay, T.; Nascimento Vieira, A.; Kleinermanns, K.; Tüysüz, H.; Martin, W.F.; Preiner, M.</b> (2022). Role of geochemical protoenzymes (geozymes) in primordial metabolism: specific abiotic hydride transfer by metals to the biological redox cofactor NAD<sup>+</sup>. <i>The FEBS Journal 289(11)</i>: 3148-3162. <a href=\"https://dx.doi.org/10.1111/febs.16329\" target=\"_blank\">https://dx.doi.org/10.1111/febs.16329</a>","BEntID":347056,"PublicFlag":1,"CheckedFlag":0,"wosflag":1,"vabbflag":1,"RefStringPartII":". <i>The FEBS Journal 289(11)</i>: 3148-3162. <a href=\"https://dx.doi.org/10.1111/febs.16329\" target=\"_blank\">https://dx.doi.org/10.1111/febs.16329</a>","DocTypID":8,"DocType":"Journal article","MarineFlag":0,"FreshFlag":0,"BrackishFlag":0,"TerrestrialFlag":0,"Authorstring":"Henriques Pereira, D.P.; Leethaus, J.; Beyazay, T.; Nascimento Vieira, A.; Kleinermanns, K.; Tüysüz, H.; Martin, W.F.; Preiner, M.","OrigTitleTranslFlag":0,"Authorstringtrunc":"Henriques Pereira, D.P. <i>et al.</i>","Englishabstract":"Hydrogen gas, H<sub>2</sub>, is generated in serpentinizing hydrothermal systems, where it has supplied electrons and energy for microbial communities since there was liquid water on Earth. In modern metabolism, H<sub>2</sub> is converted by hydrogenases into organically bound hydrides (H<sup>–</sup>), for example, the cofactor NADH. It transfers hydrides among molecules, serving as an activated and biologically harnessed form of H<sub>2</sub>. In serpentinizing systems, minerals can also bind hydrides and could, in principle, have acted as inorganic hydride donors—possibly as a geochemical protoenzyme, a ‘geozyme’— at the origin of metabolism. To test this idea, we investigated the ability of H<sub>2</sub> to reduce NAD<sup>+</sup> in the presence of iron (Fe), cobalt (Co) and nickel (Ni), metals that occur in serpentinizing systems. In the presence of H<sub>2</sub>, all three metals specifically reduce NAD<sup>+</sup> to the biologically relevant form, 1,4-NADH, with up to 100% conversion rates within a few hours under alkaline aqueous conditions at 40 °C. Using Henry's law, the partial pressure of H<sub>2</sub> in our reactions corresponds to 3.6 m<span class=\"smallCaps\">m</span>, a concentration observed in many modern serpentinizing systems. While the reduction of NAD<sup>+</sup> by Ni is strictly H<sub>2</sub>-dependent, experiments in heavy water (<sup>2</sup>H<sub>2</sub>O) indicate that native Fe can reduce NAD<sup>+</sup> both with and without H<sub>2</sub>. The results establish a mechanistic connection between abiotic and biotic hydride donors, indicating that geochemically catalysed, H<sub>2</sub>-dependent NAD<sup>+</sup> reduction could have preceded the hydrogenase-dependent reaction in evolution.","AbstractOtherLang":null,"BibLvlCode":"AS","StandardTitle":"Role of geochemical protoenzymes (geozymes) in primordial metabolism: specific abiotic hydride transfer by metals to the biological redox cofactor NAD<sup>+</sup>","OrigTitleLangCode":"en","OrigTitleLangCodeExtended":"eng","OrigTitleLangID":15,"DateLastModified":{"date":"2024-12-10 01:33:17.368041","timezone_type":1,"timezone":"+01:00"},"UserAccessRight":null,"UserAccID":null,"AuthorKeywords":"cofactors; electron donors; hydrogen; hydrogenase; NADH; origin of life; reduction; serpentinizing systems","OtherDescriptors":null,"Notes":null,"AnaPub":2022,"MonPub":null,"DateUpdate":"2023-01-11","DateCreate":"2022-01-27","SecASFANote":null,"ConfID":null,"PeerRev":1,"VlizCoreFlag":1,"WoScode":"WOS:000737317300001","VABBcode":null,"OpenAcc":1,"DOI":"10.1111/febs.16329"},"refs":null,"anarec":{"AnaID":349361,"PubliDate":2022,"Pagination":"3148-3162","XtraPublOfAnaID":null,"ISBN":null,"Volume":"289","Issue":"11","BRefMon":null,"BRefMonRR":null,"BRefXtra":null,"BRefXtraRR":null,"SerBRefID":235768,"SerRR":"The FEBS Journal. 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