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Local Proton Source in Electrocatalytic CO2 Reduction with [Mn(bpy-R)(CO)(3)Br] Complexes
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SYSNO ASEP 0473905 Druh ASEP J - Článek v odborném periodiku Zařazení RIV J - Článek v odborném periodiku Poddruh J Článek ve WOS Název Local Proton Source in Electrocatalytic CO2 Reduction with [Mn(bpy-R)(CO)(3)Br] Complexes Tvůrce(i) Franco, F. (IT)
Cometto, C. (IT)
Nencini, L. (IT)
Barolo, C. (IT)
Sordello, F. (IT)
Minero, C. (IT)
Fiedler, Jan (UFCH-W) RID, ORCID
Robert, M. (FR)
Gobetto, R. (IT)
Nervi, C. (IT)Zdroj.dok. Chemistry - A European Journal. - : Wiley - ISSN 0947-6539
Roč. 23, č. 20 (2017), s. 4782-4793Poč.str. 12 s. Jazyk dok. eng - angličtina Země vyd. DE - Německo Klíč. slova electrochemistry ; electrocatalysis ; [Mn(pdbpy)(CO)(3)Br] Complexes Vědní obor RIV CG - Elektrochemie Obor OECD Electrochemistry (dry cells, batteries, fuel cells, corrosion metals, electrolysis) CEP GA14-05180S GA ČR - Grantová agentura ČR Institucionální podpora UFCH-W - RVO:61388955 UT WOS 000399327100010 EID SCOPUS 85013678071 DOI https://doi.org/10.1002/chem.201605546 Anotace The electrochemical behavior of fac-[Mn(pdbpy)(CO)(3)Br] (pdbpy=4-phenyl-6-(phenyl-2,6-diol)-2,2-bipyridine) (1) in acetonitrile under Ar, and its catalytic performances for CO2 reduction with added water, 2,2,2-trifluoroethanol (TFE), and phenol are discussed in detail. Preparative-scale electrolysis experiments, carried out at -1.5V versus the standard calomel electrode (SCE) in CO2-saturated acetonitrile, reveal that the process selectivity is extremely sensitive to the acid strength, producing CO and formate in different faradaic yields. A detailed spectroelectrochemical (IR and UV/Vis) study under Ar and CO2 atmospheres shows that 1 undergoes fast solvolysis, however, dimer formation in acetonitrile is suppressed, resulting in an atypical reduction mechanism in comparison with other reported Mn-I catalysts. Spectroscopic evidence of Mn hydride formation supports the existence of different electrocatalytic CO2 reduction pathways. Furthermore, a comparative investigation performed on the new fac-[Mn(ptbpy)(CO)(3)Br] (ptbpy=4-phenyl-6-(phenyl-3,4,5-triol)-2,2-bipyridine) catalyst (2), bearing a bipyridyl derivative with OH groups in different positions to those in 1, provides complementary information about the role that the local proton source plays during the electrochemical reduction of CO2. Pracoviště Ústav fyzikální chemie J.Heyrovského Kontakt Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Rok sběru 2018
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