Photocatalytic Aqueous CO2 Reduction to CO and CH4 Sensitized by Ullazine Supramolecular Polymers

Dumele, Oliver; Đorđević, Luka; Sai, Hiroaki; Cotey, Thomas J.; Sangji, M. Hussain; Sato, Kohei; Dannenhoffer, Adam J.; Stupp, Samuel I.

doi:10.1021/jacs.1c12155

Title: Photocatalytic Aqueous CO₂ Reduction to CO and CH₄ Sensitized by Ullazine Supramolecular Polymers

Journal Article · 10 February 2022 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.1c12155 · OSTI ID:1846590

Dumele, Oliver ^[1];

^[2];

^[3]; Cotey, Thomas J. ^[3];

^[3];

^[4]; Dannenhoffer, Adam J. ^[3];

^[2]

Northwestern Univ., Evanston, IL (United States); Center for Bio-Inspired Energy Science
Northwestern Univ., Evanston, IL (United States); Northwestern Univ., Chicago, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Chicago, IL (United States)

There has been rapid progress on the chemistry of supramolecular scaffolds that harness sunlight for aqueous photocatalytic production of hydrogen. However, great efforts are still needed to develop similar photosynthetic systems for the great challenge of CO₂ reduction especially if they avoid the use of nonabundant metals. This work investigates the synthesis of supramolecular polymers capable of sensitizing catalysts that require more negative potentials than proton reduction. The monomers are chromophore amphiphiles based on a diareno-fused ullazine core that undergo supramolecular polymerization in water to create entangled nanoscale fibers. Under 450 nm visible light these fibers sensitize a dinuclear cobalt catalyst for CO₂ photoreduction to generate carbon monoxide and methane using a sacrificial electron donor. The supramolecular photocatalytic system can generate amounts of CH₄ comparable to those obtained with a precious metal-based [Ru(phen)₃](PF₆)₂ sensitizer and, in contrast to Ru-based catalysts, retains photocatalytic activity in all aqueous media over 6 days. Furthermore, the present study demonstrates the potential of tailored supramolecular polymers as renewable energy and sustainability materials.

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Research Organization:: Northwestern Univ., Evanston, IL (United States). Center for Bio-Inspired Energy Science

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0000989

OSTI ID:: 1846590

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 7 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
99 GENERAL AND MISCELLANEOUS
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CCDC 1878608: Experimental Crystal Structure Determination Oliver, Dumele∞,; Luka, Đorđević∞,; Hiroaki, Sai, https://doi.org/10.5517/ccdc.csd.cc211v87 The current record is supplemented by this dataset	dataset	January 2022
CCDC 1878609: Experimental Crystal Structure Determination Oliver, Dumele∞,; Luka, Đorđević∞,; Hiroaki, Sai, https://doi.org/10.5517/ccdc.csd.cc211v98 The current record is supplemented by this dataset	dataset	January 2022
CCDC 1878614: Experimental Crystal Structure Determination Oliver, Dumele∞,; Luka, Đorđević∞,; Hiroaki, Sai, https://doi.org/10.5517/ccdc.csd.cc211vgf The current record is supplemented by this dataset	dataset	January 2022
CCDC 1878616: Experimental Crystal Structure Determination Oliver, Dumele∞,; Luka, Đorđević∞,; Hiroaki, Sai, https://doi.org/10.5517/ccdc.csd.cc211vjh The current record is supplemented by this dataset	dataset	January 2022

Title: Photocatalytic Aqueous CO2 Reduction to CO and CH4 Sensitized by Ullazine Supramolecular Polymers

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Title: Photocatalytic Aqueous CO₂ Reduction to CO and CH₄ Sensitized by Ullazine Supramolecular Polymers