Tuning Internal Strain in Metal-Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction.
Angew Chem Int Ed Engl
; 59(11): 4572-4580, 2020 Mar 09.
Article
em En
| MEDLINE
| ID: mdl-31914215
ABSTRACT
A gas-phase approach to form Zn coordination sites on metal-organic frameworks (MOFs) by vapor-phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution-phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO2 to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200-300â
mV. Using element-specific X-ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square-pyramidal geometry with four Zn-N bonds in the equatorial plane and one Zn-OH2 bond in the axial plane. The fine-tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials.
Texto completo:
1
Base de dados:
MEDLINE
Idioma:
En
Ano de publicação:
2020
Tipo de documento:
Article
País de afiliação:
Estados Unidos