Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO2 Reduction**
Abstract
Abstract We present a supramolecular approach to catalyzing photochemical CO 2 reduction through second‐sphere porosity and charge effects. An iron porphyrin box ( PB ) bearing 24 cationic groups, FePB‐2(P) , was made via post‐synthetic modification of an alkyne‐functionalized supramolecular synthon. FePB‐2(P) promotes the photochemical CO 2 reduction reaction (CO 2 RR) with 97 % selectivity for CO product, achieving turnover numbers (TON) exceeding 7000 and initial turnover frequencies (TOF max ) reaching 1400 min −1 . The cooperativity between porosity and charge results in a 41‐fold increase in activity relative to the parent Fe tetraphenylporphyrin ( FeTPP ) catalyst, which is far greater than analogs that augment catalysis through porosity ( FePB‐3(N ), 4‐fold increase) or charge (Fe p ‐tetramethylanilinium porphyrin ( Fe‐ p ‐TMA ), 6‐fold increase) alone. This work establishes that synergistic pendants in the secondary coordination sphere can be leveraged as a design element to augment catalysis at primary active sites within confined spaces.
- Authors:
-
[1];
[1];
[1];
[1]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR); National Institutes of Health (NIH)
- OSTI Identifier:
- 2246868
- Alternate Identifier(s):
- OSTI ID: 1905941
- Grant/Contract Number:
- AC02-05CH11231; S10OD024998
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 62; Journal Issue: 5; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Carbon Dioxide Reduction; Electrocatalysis; Photocatalysis; Porous Cage; Second-Sphere
Citation Formats
An, Lun, De La Torre, Patricia, Smith, Peter T., Narouz, Mina R., and Chang, Christopher J. Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO2 Reduction**. United States: N. p., 2022.
Web. doi:10.1002/anie.202209396.
An, Lun, De La Torre, Patricia, Smith, Peter T., Narouz, Mina R., & Chang, Christopher J. Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO2 Reduction**. United States. https://doi.org/10.1002/anie.202209396
An, Lun, De La Torre, Patricia, Smith, Peter T., Narouz, Mina R., and Chang, Christopher J. Tue .
"Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO2 Reduction**". United States. https://doi.org/10.1002/anie.202209396. https://www.osti.gov/servlets/purl/2246868.
@article{osti_2246868,
title = {Synergistic Porosity and Charge Effects in a Supramolecular Porphyrin Cage Promote Efficient Photocatalytic CO2 Reduction**},
author = {An, Lun and De La Torre, Patricia and Smith, Peter T. and Narouz, Mina R. and Chang, Christopher J.},
abstractNote = {Abstract We present a supramolecular approach to catalyzing photochemical CO 2 reduction through second‐sphere porosity and charge effects. An iron porphyrin box ( PB ) bearing 24 cationic groups, FePB‐2(P) , was made via post‐synthetic modification of an alkyne‐functionalized supramolecular synthon. FePB‐2(P) promotes the photochemical CO 2 reduction reaction (CO 2 RR) with 97 % selectivity for CO product, achieving turnover numbers (TON) exceeding 7000 and initial turnover frequencies (TOF max ) reaching 1400 min −1 . The cooperativity between porosity and charge results in a 41‐fold increase in activity relative to the parent Fe tetraphenylporphyrin ( FeTPP ) catalyst, which is far greater than analogs that augment catalysis through porosity ( FePB‐3(N ), 4‐fold increase) or charge (Fe p ‐tetramethylanilinium porphyrin ( Fe‐ p ‐TMA ), 6‐fold increase) alone. This work establishes that synergistic pendants in the secondary coordination sphere can be leveraged as a design element to augment catalysis at primary active sites within confined spaces.},
doi = {10.1002/anie.202209396},
journal = {Angewandte Chemie (International Edition)},
number = 5,
volume = 62,
place = {United States},
year = {Tue Dec 20 00:00:00 EST 2022},
month = {Tue Dec 20 00:00:00 EST 2022}
}
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