Single-Atom Metal Oxide Sites as Traps for Charge Separation in the Zirconium-Based Metal–Organic Framework NDC–NU-1000
Abstract
Solvothermal deposition in metal–organic frameworks (MOFs) can be utilized to mount single-metal-atom catalytic species at chemically reactive sites on hexa-Zr(IV)-oxy(oxo,hydroxo,aqua) nodes in nanoscale crystallites of the MOF NDC-NU-1000 in a self-limiting fashion. Upon photoexcitation of the 1,3,6,8-tetrakis(p-benzoato)pyrene chromophores of the parent framework, charge transfer may occur between the chromophores and the installed heterometal sites. Extended X-ray absorption fine structure studies revealed the single-atom nature of the installed species. A combination of steady-state and ultrafast optical spectroscopy was utilized to uncover evidence of a charge-separated (CS) state arising in the metalated samples. The relevant dynamics were characterized with transient photoluminescence and femtosecond transient absorption spectroscopy. Here, we find that a titanium-oxy single atom site gives rise to the longest-lived CS species compared to cobalt and nickel in a similar arrangement. This study provides guidance in designing MOF-based catalytic systems for photocatalysis and solar-fuel production.
- Authors:
-
[2];
[2];
[2];
[2];
[1];
[3];
[1];
[1];
[3]
- Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1878492
- Grant/Contract Number:
- AC02-06CH11357; FG02-87ER13808; N00014-20-1-2517; CHE-1048773; DMR-0521267; ECCS-2025633; DMR-1720139
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy and Fuels
- Additional Journal Information:
- Journal Volume: 35; Journal Issue: 23; Journal ID: ISSN 0887-0624
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; charge separation; metal-organic frameworks; single site metal oxides; charge transfer; kinetics; metals; oxides
Citation Formats
Kramar, Boris V., Phelan, Brian T., Sprague-Klein, Emily A., Diroll, Benjamin T., Lee, Sungsik, Otake, Ken-ichi, Palmer, Rebecca, Mara, Michael W., Farha, Omar K., Hupp, Joseph T., and Chen, Lin X. Single-Atom Metal Oxide Sites as Traps for Charge Separation in the Zirconium-Based Metal–Organic Framework NDC–NU-1000. United States: N. p., 2021.
Web. doi:10.1021/acs.energyfuels.1c02623.
Kramar, Boris V., Phelan, Brian T., Sprague-Klein, Emily A., Diroll, Benjamin T., Lee, Sungsik, Otake, Ken-ichi, Palmer, Rebecca, Mara, Michael W., Farha, Omar K., Hupp, Joseph T., & Chen, Lin X. Single-Atom Metal Oxide Sites as Traps for Charge Separation in the Zirconium-Based Metal–Organic Framework NDC–NU-1000. United States. https://doi.org/10.1021/acs.energyfuels.1c02623
Kramar, Boris V., Phelan, Brian T., Sprague-Klein, Emily A., Diroll, Benjamin T., Lee, Sungsik, Otake, Ken-ichi, Palmer, Rebecca, Mara, Michael W., Farha, Omar K., Hupp, Joseph T., and Chen, Lin X. Tue .
"Single-Atom Metal Oxide Sites as Traps for Charge Separation in the Zirconium-Based Metal–Organic Framework NDC–NU-1000". United States. https://doi.org/10.1021/acs.energyfuels.1c02623. https://www.osti.gov/servlets/purl/1878492.
@article{osti_1878492,
title = {Single-Atom Metal Oxide Sites as Traps for Charge Separation in the Zirconium-Based Metal–Organic Framework NDC–NU-1000},
author = {Kramar, Boris V. and Phelan, Brian T. and Sprague-Klein, Emily A. and Diroll, Benjamin T. and Lee, Sungsik and Otake, Ken-ichi and Palmer, Rebecca and Mara, Michael W. and Farha, Omar K. and Hupp, Joseph T. and Chen, Lin X.},
abstractNote = {Solvothermal deposition in metal–organic frameworks (MOFs) can be utilized to mount single-metal-atom catalytic species at chemically reactive sites on hexa-Zr(IV)-oxy(oxo,hydroxo,aqua) nodes in nanoscale crystallites of the MOF NDC-NU-1000 in a self-limiting fashion. Upon photoexcitation of the 1,3,6,8-tetrakis(p-benzoato)pyrene chromophores of the parent framework, charge transfer may occur between the chromophores and the installed heterometal sites. Extended X-ray absorption fine structure studies revealed the single-atom nature of the installed species. A combination of steady-state and ultrafast optical spectroscopy was utilized to uncover evidence of a charge-separated (CS) state arising in the metalated samples. The relevant dynamics were characterized with transient photoluminescence and femtosecond transient absorption spectroscopy. Here, we find that a titanium-oxy single atom site gives rise to the longest-lived CS species compared to cobalt and nickel in a similar arrangement. This study provides guidance in designing MOF-based catalytic systems for photocatalysis and solar-fuel production.},
doi = {10.1021/acs.energyfuels.1c02623},
journal = {Energy and Fuels},
number = 23,
volume = 35,
place = {United States},
year = {Tue Sep 21 00:00:00 EDT 2021},
month = {Tue Sep 21 00:00:00 EDT 2021}
}
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