The Role of Water in Carbon Dioxide Adsorption in Porphyrinic Metal-Organic Frameworks

Bettina Baumgartner; P. Tim Prins; Jaap N. Louwen; Matteo Monai; Bert M. Weckhuysen

doi:10.1002/cctc.202300722

The Role of Water in Carbon Dioxide Adsorption in Porphyrinic Metal-Organic Frameworks

Bettina Baumgartner, P. Tim Prins, Jaap N. Louwen, Matteo Monai, Bert M. Weckhuysen^*

^*Corresponding author for this work

Sub Inorganic Chemistry and Catalysis

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Capturing and converting CO₂ through artificial photosynthesis using photoactive, porous materials is a promising approach for addressing increasing CO₂ concentrations. Porphyrinic Zr-based metal-organic frameworks (MOFs) are of particular interest as they incorporate a photosensitizer in the porous structure. Herein, the initial step of the artificial photosynthesis is studied: CO₂ sorption and activation in the presence of water. A combined vibrational and visible spectroscopic approach was used to monitor the adsorption of CO₂ into PCN-222 and PCN-223 MOFs, and the photophysical changes of the porphyrinic linker as a function of water concentration. A shift in CO₂ sorption site and bending of the porphyrin macrocycle in response to humidity was observed, and CO₂/H₂O competition experiments revealed that the exchange of CO₂ with H₂O is pore-size dependent. Therefore, humidity and pore-size can be used to tune CO₂ sorption, CO₂ capacity, and light harvesting in porphyrinic MOFs, which are key factors for CO₂ photoreduction.

Original language	English
Article number	e202300722
Journal	ChemCatChem
Volume	15
Issue number	19
DOIs	https://doi.org/10.1002/cctc.202300722
Publication status	Published - 6 Oct 2023

Bibliographical note

Funding Information:
. This work was financially supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation program funded by the Ministry of Education, Culture and Science (OC&W), of the government of the Netherlands, and by the ARC‐CBBC (Advanced Research Center–Chemical Building Blocks Consortium). The authors thank Joren Dorresteijn (Utrecht University) for SEM imaging. B.B. acknowledges additional funding by the Austrian Science Fund (FWF) under the project number J4607‐N and by the Dutch Research Council (NWO) under the grant number OCENW.XS22.4.067. The experimental setup was manufactured at the scientific instrumentation domain at the Faculty of Sciences of Utrecht University. We thank SURF (www.surf.nl) for the support in using the National Supercomputer Snellius

Publisher Copyright:
© 2023 The Authors. ChemCatChem published by Wiley-VCH GmbH.

Funding

This work was financially supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation program funded by the Ministry of Education, Culture and Science (OC&W), of the government of the Netherlands, and by the ARC-CBBC (Advanced Research Center–Chemical Building Blocks Consortium). The authors thank Joren Dorresteijn (Utrecht University) for SEM imaging. B.B. acknowledges additional funding by the Austrian Science Fund (FWF) under the project number J4607-N and by the Dutch Research Council (NWO) under the grant number OCENW.XS22.4.067. The experimental setup was manufactured at the scientific instrumentation domain at the Faculty of Sciences of Utrecht University. We thank SURF (www.surf.nl) for the support in using the National Supercomputer Snellius. . This work was financially supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation program funded by the Ministry of Education, Culture and Science (OC&W), of the government of the Netherlands, and by the ARC‐CBBC (Advanced Research Center–Chemical Building Blocks Consortium). The authors thank Joren Dorresteijn (Utrecht University) for SEM imaging. B.B. acknowledges additional funding by the Austrian Science Fund (FWF) under the project number J4607‐N and by the Dutch Research Council (NWO) under the grant number OCENW.XS22.4.067. The experimental setup was manufactured at the scientific instrumentation domain at the Faculty of Sciences of Utrecht University. We thank SURF (www.surf.nl) for the support in using the National Supercomputer Snellius

Funders	Funder number
ARC-CBBC
ARC‐CBBC
Advanced Research Center
Chemical Building Blocks Consortium
Joren Dorresteijn
MCEC
Netherlands Center for Multiscale Catalytic Energy Conversion
SURF
Universiteit Utrecht
Austrian Science Fund	J4607‐N
Ministerie van onderwijs, cultuur en wetenschap
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	OCENW.XS22.4.067

Keywords

Adsorption
artificial photosynthesis
CO capture
metal-organic framework
spectroscopy

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ChemCatChem - 2023 - Baumgartner - The Role of Water in Carbon Dioxide Adsorption in Porphyrinic Metal‐Organic FrameworksFinal published version, 4.32 MBLicence: CC BY

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abstract = "Capturing and converting CO2 through artificial photosynthesis using photoactive, porous materials is a promising approach for addressing increasing CO2 concentrations. Porphyrinic Zr-based metal-organic frameworks (MOFs) are of particular interest as they incorporate a photosensitizer in the porous structure. Herein, the initial step of the artificial photosynthesis is studied: CO2 sorption and activation in the presence of water. A combined vibrational and visible spectroscopic approach was used to monitor the adsorption of CO2 into PCN-222 and PCN-223 MOFs, and the photophysical changes of the porphyrinic linker as a function of water concentration. A shift in CO2 sorption site and bending of the porphyrin macrocycle in response to humidity was observed, and CO2/H2O competition experiments revealed that the exchange of CO2 with H2O is pore-size dependent. Therefore, humidity and pore-size can be used to tune CO2 sorption, CO2 capacity, and light harvesting in porphyrinic MOFs, which are key factors for CO2 photoreduction.",

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The Role of Water in Carbon Dioxide Adsorption in Porphyrinic Metal-Organic Frameworks

Abstract

Bibliographical note

Funding

Keywords

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