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The Positional Effect of an Immobilized Re Tricarbonyl Catalyst for CO2 Reduction.
Choate, Jeremiah C; Silva, Israel; Hsu, Po Ching; Tran, Kaylyn; Marinescu, Smaranda C.
Afiliación
  • Choate JC; Department of Chemistry, University of Southern California, California, Los Angeles 90089, United States.
  • Silva I; Department of Chemistry, University of Southern California, California, Los Angeles 90089, United States.
  • Hsu PC; Department of Chemistry, University of Southern California, California, Los Angeles 90089, United States.
  • Tran K; Department of Chemistry, University of Southern California, California, Los Angeles 90089, United States.
  • Marinescu SC; Department of Chemistry, University of Southern California, California, Los Angeles 90089, United States.
ACS Appl Mater Interfaces ; 2024 Sep 10.
Article en En | MEDLINE | ID: mdl-39255361
ABSTRACT
The storage of renewable energy through the conversion of CO2 to CO provides a viable solution for the intermittent nature of these energy sources. The immobilization of rhenium(I) tricarbonyl molecular complexes is presented through the reductive coupling of bis(diazonium) aryl substituents. The heterogenized complex was characterized through ultra-visible, attenuated total reflectance, infrared reflection absorption spectroscopy, and X-ray photoelectron spectroscopy to probe the electronic structure of the immobilized complex. In addition, studies of cyclic voltammetry, controlled potential electrolysis, and electrochemical impedance spectroscopy were conducted to examine the CO2 reduction activity. The structure and CO2 reduction performance were compared with a previously reported immobilized rhenium(I) tricarbonyl molecular complex to probe the effect of varying the tethering of the aryl substituent from the 5,5'-position to the 4,4'-position of the 2,2'-bipyridine backbone. The immobilized complex on carbon cloth at the 4,4'-position provided excellent selectivity (FECO > 99%) and maximum TONCO and TOFCO values of 3359 and 0.9 s-1, respectively, without the addition of a BroÌ·nsted acid source. A nonaqueous flow cell demonstrated the stability of this complex during a 5 h electrolysis. Tethering at the 4,4'-position, compared to the 5,5'-position, yielded lower overall activity for CO2 reduction and was attributed to the difference in growth morphology and formation of aggregations, due to Re-Re dimer formation and π-π stacking interactions within the metallopolymer matrix. For carbon cloth substrates, an optimized catalyst loading was determined to be 44.6 ± 11 nmol/cm2.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos