Eli nqaku liphononongwe ngokweenkqubo kunye nemigaqo-nkqubo yokuhlela yeSayensi X. Abahleli bagxininise ezi mpawu zilandelayo ngelixa beqinisekisa ukuthembeka komxholo:
Utshintsho lwemozulu yingxaki yehlabathi jikelele yokusingqongileyo. Eyona nto ibangela utshintsho lwemozulu kukutshiswa kakhulu kwamafutha efosili. Bavelisa i-carbon dioxide (CO2), igesi ebangela ukufudumala komhlaba enegalelo ekufudumaleni kwehlabathi. Ngenxa yesi sizathu, oorhulumente kwihlabathi liphela baphuhlisa imigaqo-nkqubo yokunciphisa ukukhutshwa kwekhabhoni. Nangona kunjalo, ukunciphisa nje ukukhutshwa kwekhabhoni kusenokunganelanga. Ukukhutshwa kwekhabhoni dioxide nako kufuneka kulawulwe. googletag.cmd.push(function() { googletag.display('div-gpt-ad-1449240174198-2′); });
Kule meko, izazinzulu zicebisa ukuguqulwa kweekhemikhali zekhabhoni diokside zibe ziikhompawundi ezongeziweyo ezifana ne-methanol kunye ne-formic acid (HCOOH). Ukuze kuveliswe le yokugqibela, kufuneka umthombo wee-hydride ions (H-), ezilingana neproton enye kunye nee-electron ezimbini. Umzekelo, isibini se-reduction-oxidation se-nicotinamide adenine dinucleotide (NAD+/NADH) sisixhobo sokuvelisa kunye nokugcina i-hydride (H-) kwiinkqubo zebhayoloji.
Ngenxa yesi sizathu, iqela labaphandi elikhokelwa nguNjingalwazi uHitoshi Tamiaki kwiYunivesithi yaseRitsumeikan, eJapan, liphuhlise indlela entsha yekhemikhali esebenzisa ii-complexes ze-NAD+/NADH ezifana ne-ruthenium ukunciphisa i-CO2 ibe yi-HCOOH. Iziphumo zophando lwabo zapapashwa kwijenali iChemSusChem ngoJanuwari 13, 2023.
UNjingalwazi Tamiaki ucacisa isizathu sophando lwakhe. “Kutshanje kuboniswe ukuba i-ruthenium complex enemodeli ye-NAD+, [Ru(bpy)2(pbn)](PF6)2, incitshiswa yi-photochemical two-electron. Oku kubangele ukuba kubekho i-NADH type complex efanayo [Ru (bpy) )2 (pbnHH)](PF6)2 xa kukho i-triethanolamine kwi-acetonitrile (CH3CN) phantsi kokukhanya okubonakalayo,” utshilo.
"Ukongeza, ukubilisa i-CO2 kwisisombululo se-[Ru(bpy)2(pbnHH)]2+ kuphinda kuvelise i-[Ru(bpy)2(pbn)]2+ kwaye kuvelise ii-ion ze-formate (HCOO-). Nangona kunjalo, isantya sayo semveliso siphantsi kakhulu. Sifutshane. Ke ngoko, ukuguqula i-H- ibe yi-CO2 kufuna inkqubo ephuculweyo ye-catalytic."
Ngoko ke, abaphandi baphande ngee-reagents ezahlukeneyo kunye neemeko zokusabela ezinceda ekunciphiseni ukukhutshwa kwe-carbon dioxide. Ngokusekelwe kolu vavanyo, bacebise ukunciphisa i-redox pair nge-light-induced two-electron [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). Ukongeza, amanzi (H2O) kwi-CH3CN endaweni ye-triethanolamine aphucule ngakumbi isivuno.

Ukongeza, abaphandi baphande neendlela zokusabela ezinokubakho besebenzisa iindlela ezifana ne-nuclear magnetic resonance, i-cyclic voltammetry kunye ne-UV-visible spectrophotometry. Ngokusekelwe koku, bacinge ukuba: Okokuqala, emva kokuvezwa kwe-[Ru(bpy)2(pbn)]2+, i-free radical [RuIII(bpy)2(pbn•-)]2+* iyakhiwa, edlula kule nciphiso ilandelayo: BIH Fumana [RuII(bpy)2(pbn•-)]2+ kunye ne-BIH•+. Emva koko, i-H2O iprototenates i-ruthenium complex ukwenza i-[Ru(bpy)2(pbnH•)]2+ kunye ne-BI•. Imveliso ephumayo iyahlulwahlulwa ukwenza i-[Ru(bpy)2(pbnHH)]2+ kwaye ibuyela kwi-[Ru(bpy)2(pbn)]2+. Eyokuqala emva koko incitshiswa yi-BI• ukuvelisa i-[Ru(bpy)(bpy•−)(pbnHH)]+. Le complex sisincedisi esisebenzayo esiguqula i-H- ibe yi-CO2, esivelisa i-HCOO- kunye ne-formic acid.
Abaphandi babonise ukuba impendulo ecetywayo inenani eliphezulu lokuguqulwa (inani lee-moles ze-carbon dioxide eziguqulwe yi-mole enye ye-catalyst) - 63.
Abaphandi bachulumancile zezi zinto zifunyenweyo kwaye banethemba lokuphuhlisa indlela entsha yokuguqula amandla (ukukhanya kwelanga kube ngamandla eekhemikhali) ukuvelisa izinto ezintsha ezivuselelekayo.
“Indlela yethu iya kunciphisa isixa siphela sekhabhoni dayokhsayidi eMhlabeni kwaye incede ekugcineni umjikelo wekhabhoni. Ke ngoko, inokunciphisa ukufudumala kwehlabathi kwixesha elizayo,” wongezelela uNjingalwazi Tamiaki. “Ukongeza, ubuchwepheshe obutsha bokuthutha i-hydride yendalo buya kusinika iikhompawundi ezixabisekileyo.”
Ulwazi oluthe kratya: Yusuke Kinoshita et al., Ukudluliselwa kwe-hydride ye-organic ebangelwa kukukhanya kwi-CO2** okubangelwa zii-ruthenium complexes njengeemodeli ze-NAD+/NADH redox couples, ChemSusChem (2023). DOI: 10.1002/cssc.202300032

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