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Insights into CO2 adsorption and chemical fixation properties of VPI-100 metal–organic frameworks

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/C8TA06383D· OSTI ID:1493738
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  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
+ Show Author Affiliations
Here, metal–organic frameworks (MOFs) have shown great promise as efficient CO2 adsorbents, as well as an emerging class of heterogeneous catalysts for conversion of CO2 to other useful chemicals. In this work, we synthesized and characterized two isostructural hafnium-based MOFs, denoted as Hf-VPI-100 (Cu) and Hf-VPI-100 (Ni). Both frameworks demonstrated high catalytic efficiency for cycloaddition of CO2 to epoxides under ambient pressure. In situ PXRD, QCM and DRIFTs have been used to probe the interaction between the guest molecules (CO2/epoxide) and Hf-VPI-100. The crystal structures of these frameworks were preserved during the exposure to CO2 atmosphere up to 20 bar. The epoxide uptake per unit cell of VPI-100 and diffusion coefficients have been calculated by QCM analysis. Comparison of catalytic efficiency between Hf-VPI-100 and the previously reported Zr-based VPI-100, aided by electronic structure calculations revealed that the open metal centers in the metallocyclam act as the primary Lewis acid sites to facilitate the catalytic conversion of CO2.
Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357; SC0012445; SC0012704
OSTI ID:
1493738
Alternate ID(s):
OSTI ID: 1469235
OSTI ID: 1498866
Report Number(s):
BNL--211361-2019-JAAM; 146984
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 44 Vol. 6; ISSN JMCAET; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (1)

Carbon capture and conversion using metal–organic frameworks and MOF-based materials journal January 2019

Figures / Tables (9)

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