Thov xyuam xim rau kev siv cov kua qaub formic

Tsab xov xwm no tau raug tshuaj xyuas raws li Science X cov txheej txheem kho thiab cov cai. Cov neeg kho tau hais txog cov yam ntxwv hauv qab no thaum ua kom ntseeg tau tias cov ntsiab lus muaj kev ncaj ncees:
Kev hloov pauv huab cua yog ib qho teeb meem thoob ntiaj teb. Qhov ua rau muaj kev hloov pauv huab cua tseem ceeb yog kev hlawv roj av ntau dhau. Lawv tsim cov pa roj carbon dioxide (CO2), uas yog cov pa roj uas ua rau lub ntiaj teb sov. Vim li no, tsoomfwv thoob ntiaj teb tab tom tsim cov cai los txwv cov pa roj carbon no. Txawm li cas los xij, kev txo cov pa roj carbon tej zaum yuav tsis txaus. Cov pa roj carbon dioxide kuj tseem yuav tsum tau tswj hwm. googletag.cmd.push(function() { googletag.display('div-gpt-ad-1449240174198-2′); });
Hauv qhov no, cov kws tshawb fawb pom zoo kom hloov cov pa roj carbon dioxide mus ua cov tshuaj muaj nqis xws li methanol thiab formic acid (HCOOH). Yuav kom tsim tau qhov tom kawg, yuav tsum muaj qhov chaw ntawm hydride ions (H-), uas sib npaug rau ib qho proton thiab ob lub electrons. Piv txwv li, khub txo qis-oxidation ntawm nicotinamide adenine dinucleotide (NAD + / NADH) yog lub tshuab tsim hluav taws xob thiab lub chaw khaws cia ntawm hydride (H-) hauv cov kab ke hauv lub cev.
Nyob rau hauv qhov teeb meem no, ib pab pawg kws tshawb fawb uas coj los ntawm Xibfwb Hitoshi Tamiaki los ntawm Ritsumeikan University, Nyiv Pooj, tau tsim ib txoj kev siv tshuaj tshiab siv cov ruthenium-zoo li NAD+/NADH complexes los txo CO2 rau HCOOH. Cov txiaj ntsig ntawm lawv txoj kev tshawb fawb tau luam tawm hauv phau ntawv xov xwm ChemSusChem rau lub Ib Hlis 13, 2023.
Xibfwb Tamiaki piav qhia txog qhov laj thawj rau nws txoj kev tshawb fawb. "Tsis ntev los no tau pom tias cov ruthenium complex nrog NAD+ qauv, [Ru(bpy)2(pbn)](PF6)2, dhau los ntawm kev txo qis photochemical ob-electron. Nws tau ua rau muaj NADH hom complex [Ru(bpy))2(pbnHH)](PF6)2 nyob rau hauv qhov muaj triethanolamine hauv acetonitrile (CH3CN) nyob rau hauv lub teeb pom kev, "nws hais.
"Ntxiv rau qhov ntawd, kev ua kom CO2 npuas rau hauv [Ru(bpy)2(pbnHH)]2+ kua ua rau [Ru(bpy)2(pbn)]2+ rov tsim dua thiab tsim cov formate ions (HCOO-). Txawm li cas los xij, nws qhov ceev tsim khoom qis heev. Luv. Yog li ntawd, kev hloov H- mus rau CO2 xav tau lub kaw lus catalytic zoo dua."
Yog li ntawd, cov kws tshawb fawb tau tshawb nrhiav ntau yam tshuaj reagents thiab cov xwm txheej tshuaj tiv thaiv uas pab txo cov pa roj carbon dioxide. Raws li cov kev sim no, lawv tau tawm tswv yim los ntawm lub teeb kom txo tau ob-electron ntawm cov khub redox [Ru(bpy)2(pbn)]2+/[Ru(bpy)2(pbnHH)]2+ nyob rau hauv qhov muaj 1, 3-. Dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH). Tsis tas li ntawd, dej (H2O) hauv CH3CN es tsis txhob triethanolamine ua rau cov txiaj ntsig zoo dua.

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Ntxiv rau, cov kws tshawb fawb kuj tau tshawb nrhiav cov txheej txheem ua haujlwm uas siv cov txheej txheem xws li nuclear magnetic resonance, cyclic voltammetry thiab UV-pom spectrophotometry. Raws li qhov no, lawv tau xav tias: Ua ntej, thaum photoexcitation ntawm [Ru(bpy)2(pbn)]2+, cov dawb radical [RuIII(bpy)2(pbn•-)]2+* raug tsim, uas dhau los ntawm cov hauv qab no txo ​​qis: BIH Tau txais [RuII(bpy)2(pbn•-)]2+ thiab BIH•+. Tom qab ntawd, H2O protonates lub ruthenium complex los tsim [Ru(bpy)2(pbnH•)]2+ thiab BI•. Cov khoom tshwm sim yog disproportionated rau tsim [Ru(bpy)2(pbnHH)]2+ thiab rov qab mus rau [Ru(bpy)2(pbn)]2+. Tus thawj coj ces raug txo los ntawm BI• los tsim [Ru(bpy)(bpy•-)(pbnHH)]+. Cov tshuaj no yog ib qho catalyst uas hloov H- mus rau CO2, tsim HCOO- thiab formic acid.
Cov kws tshawb nrhiav tau qhia tias qhov kev tshuaj tiv thaiv uas tau npaj tseg muaj tus lej hloov pauv siab (tus lej ntawm moles ntawm carbon dioxide hloov pauv los ntawm ib mole ntawm catalyst) - 63.
Cov kws tshawb nrhiav zoo siab heev rau cov kev tshawb pom no thiab vam tias yuav tsim tau ib txoj hauv kev tshiab los hloov lub zog (lub hnub ci mus ua lub zog tshuaj lom neeg) los tsim cov khoom siv tshiab uas rov ua dua tshiab tau.
"Peb txoj kev no kuj tseem yuav txo tag nrho cov pa roj carbon dioxide hauv ntiaj teb thiab pab tswj lub voj voog carbon. Yog li ntawd, nws tuaj yeem txo qhov kub ntawm lub ntiaj teb yav tom ntej," Xibfwb Tamiaki hais ntxiv. "Tsis tas li ntawd, cov thev naus laus zis thauj mus los organic hydride tshiab yuav muab cov khoom muaj nqis rau peb."
Cov ntaub ntawv ntxiv: Yusuke Kinoshita et al., Kev hloov pauv organic hydride los ntawm lub teeb mus rau CO2 ** uas tau txais los ntawm ruthenium complexes ua qauv rau NAD + / NADH redox couples, ChemSusChem (2023). DOI: 10.1002 / cssc.202300032

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Yog tias koj ntsib teeb meem sau yuam kev, tsis raug, lossis xav xa daim ntawv thov kom hloov kho cov ntsiab lus ntawm nplooj ntawv no, thov siv daim foos no. Yog tias muaj lus nug dav dav, thov siv peb daim foos tiv tauj. Yog xav tau cov lus taw qhia dav dav, siv ntu lus tawm tswv yim rau pej xeem hauv qab no (ua raws li cov lus qhia).
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Lub sijhawm tshaj tawm: Lub Kaum Ob Hlis-04-2023