Knitting Nitrogen Patterns into Carbocatalysts for Strong Bond Activation (2022-02-18)
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Knitting Nitrogen Patterns into Carbocatalysts for Strong Bond Activation (2022-02-18)
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2022
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Abstract
Catalytic cleavage of strong bonds including H-H, C-O, and C-H bonds is a
highly desired fundamental transformation for the production of chemicals and
fuels. Transition metal-containing catalysts are employed although
accompanied with poor selectivity in hydrotreatment; metal-free catalysts have
been reported primarily for hydrogenation and oxidative dehydrogenation. We
report the nitrogen-assembly carbons (NACs) with closely-spaced graphitic
nitrogen as active sites, as the first metal-free catalyst achieving room
temperature dihydrogen dissociation and subsequent application in the
transformation of bio-derived oxygenates (Nat. Commun. 2020, 11, 4091). NACs
exhibit high selectivity towards alkylarenes for hydrogenolysis of aryl ethers as
model bio-oxygenates without over-hydrogeneration of arenes. Various kinetic
and mechanistic experiments were carried out to demonstrate the assemblies of
graphitic N are the active sites supported by DFT calculations. Isotope labeling
studies further reveal the cleavage of C-OH is achieved by the formation of
reversible C-Nsurf bond as in the chemisorbed species. Moreover, we further
show that NAC catalysts are versatile for activating heterocycles as liquid
organic hydrogen carriers (LOHCs) to release hydrogen (Sci. Adv. 2022, 8,
eabl9478). The discovery of nitrogen assembly as active sites can open up
broad opportunities for rational design of new metal-free catalysts for
challenging chemical reactions to meet the challenges for a carbon-neutral
future.
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Friday, February 18, 2022, 3:00 p.m.; Chem 200; Dr. Long Qi, Associate Scientist, U.S. DOE Ames Laboratory, Ames, Iowa
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Spring 2022 Seminar Series
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Qi, Long; University of Minnesota Duluth. Department of Chemistry and Biochemistry. (2022). Knitting Nitrogen Patterns into Carbocatalysts for Strong Bond Activation (2022-02-18). Retrieved from the University Digital Conservancy, https://hdl.handle.net/11299/227537.
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