I-atikili le ibuyekezwe ngokuya kweenkambiso nemigomo yokuhlela ye-Science X. Abahleli bagandelele iimfanelo ezilandelako ngesikhathi baqinisekisa ukuthembeka kokuqukethwe:
Ukutjhuguluka kobujamo bezulu mraro wephasi loke. Into ebangela ukutjhuguluka kobujamo bezulu kukutjhiswa khulu kweembaseli. Zikhiqiza i-carbon dioxide (CO2), irhasi ye-greenhouse efaka isandla ekufuthumeleni kwephasi. Ngokuya ngalokhu, urhulumende ephasini loke wenza imigomo yokunciphisa ukukhutjhwa kwekhabhoni. Kodwana, ukwehlisa ukukhutjhwa kwekhabhoni kwaphela kungenzeka kungabi ngokwaneleko. Ukukhutjhwa kwe-carbon dioxide nakho kufuze kulawulwe. googletag.cmd.push(function() { googletag.display('div-gpt-ad-1449240174198-2′); });
Mayelana nalokhu, abososayensi bahlongoza ukutjhugululwa kwamakhemikhali we-carbon dioxide ibe ziinhlanganisela ezingezelelweko ezifana ne-methanol ne-formic acid (HCOOH). Ukukhiqiza lokhu kokugcina, umthombo wama-ayoni we-hydride (H-), olingana neprothoni yinye nama-elektroni amabili, uyatlhogeka. Ukwenza isibonelo, i-reduction-oxidation pair ye-nicotinamide adenine dinucleotide (NAD+/NADH) yi-generator ne-reservoir ye-hydride (H-) eenhlelweni zezinto eziphilako.
Ngaphandle kwalokhu, isiqhema sabarhubhululi esidoswa phambili nguProfesa Hitoshi Tamiaki we-Ritsumeikan University, e-Japan, sakha indlela etja yamakhemikhali ngokusebenzisa ama-NAD+/NADH afana ne-ruthenium ukwehlisa i-CO2 ibe yi-HCOOH. Imiphumela yocwaningo lwabo yavezwa kujenali i-ChemSusChem mhlana ali-13 kuTjhirhweni wee-2023.
UProfesa Tamiaki uhlathulula umnqopho wokwenza irhubhululo lakhe. “Kusanda kutjengiswa bona i-ruthenium complex enemodeli ye-NAD+, [Ru(bpy)2(pbn)](PF6)2, yenza ukwehliswa kwama-elekthroni amabili nge-photochemical. Kwabangela i-NADH type complex [Ru (bpy) )2 (pbnHH)](PF6) (CH3CN) ngaphasi kokukhanya okubonakalako,” watjho.
"Ngaphezu kwalokho, ukububula i-CO2 ibe yisisombululo se-[Ru(bpy)2(pbnHH)]2+ kuvuselela i-[Ru(bpy)2(pbn)]2+ begodu kukhiqize ama-ayoni we-formate (HCOO-). Nanyana kunjalo, ijubane lokukhiqiza layo liphasi khulu. Mfitjhani. Ngalokho-ke, ukutjhugulula i-H- ibe yi-CO2 kutlhoga ihlelo elithuthukisiweko le-catalytic."
Ngalokho-ke, abarhubhululi baphenye ama-reagents ahlukahlukeneko kanye nobujamo bokuphendula obusiza ekwehliseni ukukhutjhwa kwekhabhoni dioxide. Ngokuya ngalokhu kuhlola, baphakamisa ukunciphisa ama-elekthroni amabili okubangelwa kukhanya kwe-redox pair [Ru(bpy)2(pbn)]2+/[Ru(bpy)2(pbnHH)]2+ phambi kwe-1, 3-. I-Dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH). Ukungezelela, amanzi (H2O) ku-CH3CN esikhundleni se-triethanolamine enza ngcono isivuno.

Ukungezelela, abarhubhululi baphinde baphenya iindlela zokuphendula ezingaba khona ngokusebenzisa amaqhinga afana ne-nuclear magnetic resonance, i-cyclic voltammetry kanye ne-UV-visible spectrophotometry. Ngokuya ngalokhu, bacabanga: Kokuthoma, ngemva kokuvuselelwa kwe-[Ru(bpy)2(pbn)]2+, i-free radical [RuIII(bpy)2(pbn•-)]2+* iyabunjwa, eyenza ukwehliswa okulandelako: BIH Thola i-[RuII(bpy)2(pbn)-2++++. Ngemva kwalokho, i-H2O yenza bona kube ne-ruthenium complex ukwakha [Ru(bpy)2(pbnH•)]2+ kanye ne-BI•. Umkhiqizo ophumelako awulinganiswa ukwenza i-[Ru(bpy)2(pbnHH)]2+ bese ubuyela ku-[Ru(bpy)2(pbn)]2+. Eyokuqala yehliswa yi-BI• ukukhiqiza i-[Ru(bpy)(bpy•−)(pbnHH)]+. I-complex le yi-catalyst esebenzako etjhugulula i-H- ibe yi-CO2, ikhiqize i-HCOO- ne-formic acid.
Abarhubhululi batjengisa bona ukusabela okuphakanyisiweko kunenomboro ephezulu yokutjhuguluka (inani lama-mole wekhabhoni dayokisayidi atjhugululwe yi-mole eyodwa ye-catalyst) – 63.
Abarhubhululi bathabile ngokutholakala lokhu begodu banethemba lokuthuthukisa indlela etja yokutjhugulula amandla (ukukhanya kwelanga kube mamandla wamakhemikhali) ukukhiqiza izinto ezitjha ezivuselelekako.
"Indlela yethu izokwehlisa inani elipheleleko le-carbon dioxide ephasini begodu isize ukugcina umjikelezo we-carbon. Ngalokho-ke, ingehlisa ukufuthumala kwephasi esikhathini esizako," kungezelela uPhrofesa Tamiaki. "Ngaphezu kwalokho, amathekhnoloji amatjha wokuthutha ama-hydride azosinikela amakhompawundi aqakathekileko."
Ilwazi elinabileko: U-Yusuke Kinoshita et al., Ukudluliselwa kwe-organic hydride okubangelwa kukhanya ku-CO2** okulawulwa ziinhlanganisela ze-ruthenium njengeemodeli ze-NAD+/NADH redox couples, ChemSusChem (2023). DOI: 10.1002/cssc.202300032

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