Lesi sihloko sibuyekezwe ngokuhambisana nezinqubo nezinqubomgomo zokuhlela zeSayensi X. Abahleli bagcizelele lezi zimfanelo ezilandelayo ngenkathi beqinisekisa ubuqotho bokuqukethwe:
Ukushintsha kwesimo sezulu kuyinkinga yemvelo yomhlaba wonke. Okubangela ukuguquka kwesimo sezulu ukushiswa ngokweqile kwamafutha angaphansi komhlaba. Akhiqiza i-carbon dioxide (CO2), igesi ebamba ukushisa ebangela ukufudumala komhlaba. Ngenxa yalokhu, ohulumeni emhlabeni wonke bathuthukisa izinqubomgomo zokunciphisa ukukhishwa okunjalo kwekhabhoni. Kodwa-ke, ukunciphisa nje ukukhishwa kwekhabhoni kungase kunganele. Ukukhishwa kwekhabhoni dioxide nakho kudinga ukulawulwa. googletag.cmd.push(function() { googletag.display('div-gpt-ad-1449240174198-2′); });
Kulokhu, ososayensi baphakamisa ukuguqulwa kwamakhemikhali kwe-carbon dioxide kube yi-value-added compounds njenge-methanol ne-formic acid (HCOOH). Ukuze kukhiqizwe lokhu kokugcina, kudingeka umthombo wama-hydride ions (H-), alingana ne-proton eyodwa nama-electron amabili. Isibonelo, i-reduction-oxidation pair ye-nicotinamide adenine dinucleotide (NAD+/NADH) iyi-generator kanye ne-reservoir ye-hydride (H-) ezinhlelweni zezinto eziphilayo.
Ngenxa yalesi simo, ithimba labacwaningi eliholwa nguSolwazi uHitoshi Tamiaki waseRitsumeikan University, eJapane, lasungula indlela entsha yamakhemikhali besebenzisa ama-complexes e-NAD+/NADH afana ne-ruthenium ukuze kuncishiswe i-CO2 ibe yi-HCOOH. Imiphumela yocwaningo lwabo yanyatheliswa kumagazini i-ChemSusChem ngoJanuwari 13, 2023.
USolwazi Tamiaki uchaza isisusa socwaningo lwakhe. “Muva nje kuboniswe ukuthi i-ruthenium complex enemodeli ye-NAD+, [Ru(bpy)2(pbn)](PF6)2, incishiswa ngama-electron amabili nge-photochemical. Lokhu kwabangela i-NADH type complex efanayo [Ru (bpy) )2 (pbnHH)](PF6)2 lapho kukhona i-triethanolamine ku-acetonitrile (CH3CN) ngaphansi kokukhanya okubonakalayo,” kusho yena.
"Ngaphezu kwalokho, ukubilisa i-CO2 ibe yisisombululo se-[Ru(bpy)2(pbnHH)]2+ kuvuselela i-[Ru(bpy)2(pbn)]2+ futhi kukhiqize ama-ion e-formate (HCOO-). Kodwa-ke, isivinini sayo sokukhiqiza siphansi impela. Sifushane. Ngakho-ke, ukuguqula i-H- ibe yi-CO2 kudinga uhlelo oluthuthukisiwe lwe-catalytic."
Ngakho-ke, abacwaningi bahlole ama-reagent ahlukahlukene kanye nezimo zokusabela ezisiza ekunciphiseni ukukhishwa kwe-carbon dioxide. Ngokusekelwe kulezi zivivinyo, baphakamise ukunciphisa ama-electron amabili okubangelwa ukukhanya kwe-redox pair [Ru(bpy)2(pbn)]2+/[Ru(bpy)2(pbnHH)]2+ phambi kwe-1, 3-. Dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH). Ngaphezu kwalokho, amanzi (H2O) ku-CH3CN esikhundleni se-triethanolamine athuthukise kakhulu isivuno.

Ngaphezu kwalokho, abacwaningi baphinde bahlola izindlela zokusabela ezingaba khona besebenzisa amasu afana ne-nuclear magnetic resonance, i-cyclic voltammetry kanye ne-UV-visible spectrophotometry. Ngokusekelwe kulokhu, bacabangele lokhu: Okokuqala, lapho kuphuma i-photoexcitation ye-[Ru(bpy)2(pbn)]2+, kwakheka i-free radical [RuIII(bpy)2(pbn•-)]2+*, edlula kulokhu kuncipha okulandelayo: I-BIH Get [RuII(bpy)2(pbn•-)]2+ kanye ne-BIH•+. Ngemva kwalokho, i-H2O iphrothotha i-ruthenium complex ukuze yakhe i-[Ru(bpy)2(pbnH•)]2+ kanye ne-BI•. Umkhiqizo ophumayo uyahlukaniswa ukuze wakhe i-[Ru(bpy)2(pbnHH)]2+ bese ubuyela ku-[Ru(bpy)2(pbn)]2+. Owokuqala ube usuncishiswa yi-BI• ukuze kukhiqizwe i-[Ru(bpy)(bpy•−)(pbnHH)]+. Le nhlanganisela iyisikhuthazi esisebenzayo esiguqula i-H- ibe yi-CO2, esikhiqiza i-HCOO- kanye ne-formic acid.
Abacwaningi bakhombisile ukuthi ukusabela okuhlongozwayo kunenombolo ephezulu yokuguqulwa (inani lama-moles e-carbon dioxide aguqulwa yi-moles eyodwa ye-catalyst) - 63.
Abacwaningi bajabule kakhulu ngalezi zinto ezitholakele futhi banethemba lokuthuthukisa indlela entsha yokuguqula amandla (ukukhanya kwelanga kube amandla amakhemikhali) ukuze kukhiqizwe izinto ezintsha ezivuselelekayo.
“Indlela yethu izonciphisa nenani eliphelele le-carbon dioxide eMhlabeni futhi isize ekugcineni umjikelezo we-carbon. Ngakho-ke, inganciphisa ukufudumala komhlaba esikhathini esizayo,” kusho uSolwazi Tamiaki. “Ngaphezu kwalokho, ubuchwepheshe obusha bokuthutha i-hydride ephilayo buzosinika amakhemikhali ayigugu.”
Ulwazi olwengeziwe: Yusuke Kinoshita et al., Ukudluliselwa kwe-hydride ephilayo ebangelwa ukukhanya ku-CO2** okuqondiswa yi-ruthenium complexes njengamamodeli emibhangqwana ye-redox ye-NAD+/NADH, ChemSusChem (2023). I-DOI: 10.1002/cssc.202300032

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