Electrochemical and Photochemical Reduction of CO2 Catalyzed by Re(I) Complexes Carrying Local Proton Sources

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F19%3A00505698" target="_blank" >RIV/61388955:_____/19:00505698 - isvavai.cz</a>

Výsledek na webu

<a href="http://hdl.handle.net/11104/0297110" target="_blank" >http://hdl.handle.net/11104/0297110</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.organomet.8b00588" target="_blank" >10.1021/acs.organomet.8b00588</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Electrochemical and Photochemical Reduction of CO2 Catalyzed by Re(I) Complexes Carrying Local Proton Sources

Popis výsledku v původním jazyce

The novel rhenium complexes fac-Re(pdbpy)(CO)(3)Cl (pdbpy = 4-phenyl-6-(phenyl-2,6-diol)-2,2'-bipyridine), 1, and fac-Re(ptbpy)(CO)(3)Cl (ptbpy = 4-phenyl-6-(phenyl-3,4,5-triol)-2,2'-bipyridine), 2, have been synthesized, and the single crystal X-ray diffraction (SC-XRD) structure of 1 was solved. The electrochemical behaviors of the complexes in acetonitrile under Ar and their catalytic performances for CO2 reduction with added water and MeOH are discussed. A detailed IR spectroelectrochemical study under Ar and CO2 atmospheres coupled with DFT calculations allows the identification of reduced species and the interpretation of the reduction mechanisms. Comparison between the rhenium complexes and the corresponding Mn derivatives Mn(pdbpy)(CO)(3)Br, 3, and Mn(ptbpy)(CO)(3)Br, 4, has been also considered. Finally, photostimulated conversion of the CO2 was investigated with catalysts (1, 3, and 4) under visible light irradiation (lambda > 420 nm) in acetonitrile as solvent. Remarkably, 1 and 3 catalysts were active toward CO2, producing formate with good selectivity and turnover number (TON). For example, 3 gives 62% selectivity for HCOO- and a TON of 80, and Re compound 1 gives 74% selectivity for HCOO- and a TON of 86.

Název v anglickém jazyce

Electrochemical and Photochemical Reduction of CO2 Catalyzed by Re(I) Complexes Carrying Local Proton Sources

Popis výsledku anglicky

The novel rhenium complexes fac-Re(pdbpy)(CO)(3)Cl (pdbpy = 4-phenyl-6-(phenyl-2,6-diol)-2,2'-bipyridine), 1, and fac-Re(ptbpy)(CO)(3)Cl (ptbpy = 4-phenyl-6-(phenyl-3,4,5-triol)-2,2'-bipyridine), 2, have been synthesized, and the single crystal X-ray diffraction (SC-XRD) structure of 1 was solved. The electrochemical behaviors of the complexes in acetonitrile under Ar and their catalytic performances for CO2 reduction with added water and MeOH are discussed. A detailed IR spectroelectrochemical study under Ar and CO2 atmospheres coupled with DFT calculations allows the identification of reduced species and the interpretation of the reduction mechanisms. Comparison between the rhenium complexes and the corresponding Mn derivatives Mn(pdbpy)(CO)(3)Br, 3, and Mn(ptbpy)(CO)(3)Br, 4, has been also considered. Finally, photostimulated conversion of the CO2 was investigated with catalysts (1, 3, and 4) under visible light irradiation (lambda > 420 nm) in acetonitrile as solvent. Remarkably, 1 and 3 catalysts were active toward CO2, producing formate with good selectivity and turnover number (TON). For example, 3 gives 62% selectivity for HCOO- and a TON of 80, and Re compound 1 gives 74% selectivity for HCOO- and a TON of 86.

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/GA18-09848S" target="_blank" >GA18-09848S: Fotoelektrochemická redukce oxidu uhličitého na měděných pěnových elektrodách modifikovaných oxidy mědi</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2019

Kód důvěrnosti údajů

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

Název periodika

Organometallics

ISSN

0276-7333

e-ISSN

—

Svazek periodika

38

Číslo periodika v rámci svazku

6

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

1351-1360

Kód UT WoS článku

000462944200023

EID výsledku v databázi Scopus

2-s2.0-85060550124