Ka kopo ela hloko tšebeliso ea formic acid

Sengoloa sena se hlahlobiloe ho latela mekhoa le maano a bohlophisi ba Science X. Bahlophisi ba totobalitse litšobotsi tse latelang ha ba ntse ba netefatsa botšepehi ba litaba:
Phetoho ea tlelaemete ke bothata ba tikoloho lefatšeng ka bophara. Sesosa se seholo sa phetoho ea tlelaemete ke ho chesoa ho feteletseng ha mafura a khale. Li hlahisa carbon dioxide (CO2), khase e futhumatsang lefatše e tlatsetsang ho futhumaleng ha lefatše. Ka lebaka lena, mebuso lefatšeng ka bophara e ntse e theha maano a ho fokotsa likhase tse joalo tsa carbon. Leha ho le joalo, ho fokotsa likhase tsa carbon feela ho ka 'na ha se ke ha lekana. Khase ea carbon dioxide le eona e hloka ho laoloa. googletag.cmd.push(function() { googletag.display('div-gpt-ad-1449240174198-2′); });
Ntlheng ena, bo-rasaense ba sisinya phetoho ea lik'hemik'hale ea carbon dioxide hore e be metsoako e ekelitsoeng ka boleng joalo ka methanol le formic acid (HCOOH). Ho hlahisa ea morao-rao, ho hlokahala mohloli oa li-ion tsa hydride (H-), tse lekanang le proton e le 'ngoe le lielektrone tse peli. Mohlala, para ea reduction-oxidation ea nicotinamide adenine dinucleotide (NAD+/NADH) ke jenereithara le pokello ea hydride (H-) lits'ebetsong tsa baeloji.
Khahlanong le boemo bona, sehlopha sa bafuputsi se etelletsoeng pele ke Moprofesa Hitoshi Tamiaki oa Univesithi ea Ritsumeikan, Japane, se ntlafalitse mokhoa o mocha oa lik'hemik'hale se sebelisa metsoako ea NAD+/NADH e kang ruthenium ho fokotsa CO2 ho HCOOH. Liphetho tsa thuto ea bona li phatlalalitsoe koranteng ea ChemSusChem ka la 13 Pherekhong 2023.
Moprofesa Tamiaki o hlalosa lebaka leo a entseng dipatlisiso tsa hae ka lona. “Haufinyane ho bontshitswe hore ruthenium complex e nang le mohlala wa NAD+, [Ru(bpy)2(pbn)](PF6)2, e fokotseha ka di-electron tse pedi ka photochemical. E entse hore ho be le mofuta o tsamaellanang wa NADH complex [Ru (bpy) )2 (pbnHH)](PF6)2 moo ho nang le triethanolamine ka hara acetonitrile (CH3CN) tlasa lesedi le bonahalang,” o boletse jwalo.
"Ho phaella moo, ho butsoela CO2 ho ba tharollo ea [Ru(bpy)2(pbnHH)]2+ ho nchafatsa [Ru(bpy)2(pbn)]2+ 'me ho hlahisa li-ion tsa li-formate (HCOO-). Leha ho le joalo, lebelo la eona la tlhahiso le tlase haholo. Le lekhutšoanyane. Ka hona, ho fetolela H- ho CO2 ho hloka sistimi e ntlafalitsoeng ea catalytic."
Ka hona, bafuputsi ba batlisisitse di-reagent tse fapaneng le maemo a karabelo a thusang ho fokotsa mosi wa carbon dioxide. Ho latela diteko tsena, ba sisintse phokotso ya dielektrone tse pedi tse bakwang ke lesedi ya para ya redox [Ru(bpy)2(pbn)]2+/[Ru(bpy)2(pbnHH)]2+ boteng ba 1, 3-. Dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH). Ho feta moo, metsi (H2O) ho CH3CN ho ena le triethanolamine a ntlafaditse chai haholo.

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Ho phaella moo, bafuputsi ba boetse ba batlisitse mekgwa e ka bang teng ya karabelo ba sebedisa mekgwa e kang nuclear magnetic resonance, cyclic voltammetry le UV-visible spectrophotometry. Ho itshetlehile ka sena, ba ile ba nahana: Taba ya pele, ha ho etswa photoexcitation ya [Ru(bpy)2(pbn)]2+, free radical [RuIII(bpy)2(pbn•-)]2+*, e theolwang ke phokotso e latelang: BIH Get [RuII(bpy)2(pbn•-)]2+ le BIH•+. Ka mora moo, H2O e hlahisa proton ya ruthenium complex ho theha [Ru(bpy)2(pbnH•)]2+ le BI•. Sehlahiswa se hlahang se arolwa ho theha [Ru(bpy)2(pbnHH)]2+ mme se kgutlela ho [Ru(bpy)2(pbnHH)]2+. Ya pele e fokotswa ke BI• ho hlahisa [Ru(bpy)(bpy•−)(pbnHH)]+. Motsoako ona ke sesebelisoa se sebetsang sa ho baka khase se fetolang H- ho ba CO2, se hlahisang HCOO- le formic acid.
Bafuputsi ba bontšitse hore karabelo e sisintsweng e na le palo e phahameng ea phetoho (palo ea li-moles tsa carbon dioxide tse fetotsoeng ke mole e le 'ngoe ea catalyst) - 63.
Bafuputsi ba thabetse lintho tsena tse sibolotsoeng 'me ba tšepa ho nts'etsapele mokhoa o mocha oa ho fetola matla (letsatsi hore e be matla a lik'hemik'hale) ho hlahisa thepa e ncha e ka nchafatsoang.
“Mokhoa oa rona o tla boela o fokotse kakaretso ea carbon dioxide Lefatšeng 'me o thuse ho boloka potoloho ea carbon. Ka hona, o ka fokotsa ho futhumala ha lefatše nakong e tlang,” Moprofesa Tamiaki o ile a eketsa. “Ho phaella moo, mahlale a macha a ho tsamaisa hydride ea tlhaho a tla re fa metsoako ea bohlokoa.”
Tlhahisoleseding e batsi: Yusuke Kinoshita et al., Phetiso ya hydride ya tlhaho e bakwang ke lesedi ho CO2** e tsamaiswang ke di-complex tsa ruthenium e le mehlala ya banyalani ba redox ba NAD+/NADH, ChemSusChem (2023). DOI: 10.1002/cssc.202300032

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Nako ea poso: Tshitwe-04-2023