Covalent-Organic Frameworks Composed of Rhenium Bipyridine and Metal Porphyrins: Designing Heterobimetallic Frameworks with Two Distinct Metal Sites

Johnson, Eric M.; Haiges, Ralf; Marinescu, Smaranda C.

doi:10.1021/acsami.8b07795

Title: Covalent-Organic Frameworks Composed of Rhenium Bipyridine and Metal Porphyrins: Designing Heterobimetallic Frameworks with Two Distinct Metal Sites

Journal Article · 10 October 2018 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.8b07795 · OSTI ID:1614860

Johnson, Eric M. ^[1];

^[2];

^[2]

Univ. of Southern California, Los Angeles, CA (United States). Dept. of Chemistry; University of Minnesota
Univ. of Southern California, Los Angeles, CA (United States). Dept. of Chemistry

The incorporation of homogeneous catalysts for CO₂ reduction into extended frameworks has been a successful strategy for increasing catalyst lifetime and activity, but the effects of the linkers on catalysis are underexplored. In this work, a novel rhenium bipyridine complex was synthesized for the purpose of designing a covalent-organic framework (COF) with both metalloporphyrin and metal bipyridine moieties. Investigation of the rhenium complex as a homogeneous catalyst shows a faradaic efficiency of 81(8)% for the electrocatalytic conversion of CO₂ to CO upon the addition of methanol as the proton source. Treatment of the rhenium complex with tetra(4-aminophenyl)porphyrin under Schiff base conditions produces the desired COF, as indicated by powder X-ray diffraction (PXRD) studies. Metalation of the porphyrins was accomplished through postsynthetic modification with CoCl₂ and FeCl₃ metal precursors. The retention of the PXRD peaks and appearance of new Co and Fe peaks in the corresponding X-ray photoelectron spectroscopy spectra suggest the successful incorporation of a secondary metal site into the framework. Cyclic voltammetry measurements display increases in current densities when the atmosphere is changed from N₂ to CO₂. Finally, controlled potential electrolyses show that the cobalt-postmetalated COF has the highest activity toward CO₂ reduction, reaching a faradaic efficiency of 18(2)%.

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Research Organization:: Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0008688

OSTI ID:: 1614860

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 44 Vol. 10; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Covalent-Organic Frameworks Composed of Rhenium Bipyridine and Metal Porphyrins: Designing Heterobimetallic Frameworks with Two Distinct Metal Sites

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