Local Proton Source in Electrocatalytic CO2 Reduction with [Mn(bpy-R)(CO)(3)Br] Complexes

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F17%3A00473905" target="_blank" >RIV/61388955:_____/17:00473905 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1002/chem.201605546" target="_blank" >http://dx.doi.org/10.1002/chem.201605546</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/chem.201605546" target="_blank" >10.1002/chem.201605546</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Local Proton Source in Electrocatalytic CO2 Reduction with [Mn(bpy-R)(CO)(3)Br] Complexes

Popis výsledku v původním jazyce

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.

Název v anglickém jazyce

Local Proton Source in Electrocatalytic CO2 Reduction with [Mn(bpy-R)(CO)(3)Br] Complexes

Popis výsledku anglicky

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.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10405 - Electrochemistry (dry cells, batteries, fuel cells, corrosion metals, electrolysis)

Projekt

<a href="/cs/project/GA14-05180S" target="_blank" >GA14-05180S: Přenos elektronu v nanoměřítku. Od redoxního mechanismu k molekulární vodivosti.</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2017

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Chemistry A European Journal

ISSN

1521-3765

e-ISSN

—

Svazek periodika

23

Číslo periodika v rámci svazku

20

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

12

Strana od-do

4782-4793

Kód UT WoS článku

000399327100010

EID výsledku v databázi Scopus

2-s2.0-85013678071