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Heterogeneous Metal-Free Hydrogenation over Defect-Laden Hexagonal Boron Nitride. | LitMetric

Heterogeneous Metal-Free Hydrogenation over Defect-Laden Hexagonal Boron Nitride.

ACS Omega

Department of Physics, Cluster for the Rational Design of Catalysts for Energy Applications and Propulsion, and Center for Advanced Turbomachinery and Energy Research, University of Central Florida, 4000 Central Florida Blvd., PSB 430, Orlando, Florida 32816, United States.

Published: December 2016

AI Article Synopsis

Article Abstract

Catalytic hydrogenation is an important process used for the production of everything from foods to fuels. Current heterogeneous implementations of this process utilize metals as the active species. Until recently, catalytic heterogeneous hydrogenation over a metal-free solid was unknown; implementation of such a system would eliminate the health, environmental, and economic concerns associated with metal-based catalysts. Here, we report good hydrogenation rates and yields for a metal-free heterogeneous hydrogenation catalyst as well as its unique hydrogenation mechanism. Catalytic hydrogenation of olefins was achieved over defect-laden BN (-BN) in a reactor designed to maximize the defects in BN sheets. Good yields (>90%) and turnover frequencies (6 × 10-4 × 10) were obtained for the hydrogenation of propene, cyclohexene, 1,1-diphenylethene, ()- and ()-1,2-diphenylethene, octadecene, and benzylideneacetophenone. Temperature-programmed desorption of ethene over processed -BN indicates the formation of a highly defective structure. Solid-state NMR (SSNMR) measurements of -BN with high and low propene surface coverages show four different binding modes. The introduction of defects into BN creates regions of electronic deficiency and excess. Density functional theory calculations show that both the alkene and hydrogen-bond order are reduced over four specific defects: boron substitution for nitrogen (B), vacancies (V and V), and Stone-Wales defects. SSNMR and binding-energy calculations show that V are most likely the catalytically active sites. This work shows that catalytic sites can be introduced into a material previously thought to be catalytically inactive through the production of defects.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6640807PMC
http://dx.doi.org/10.1021/acsomega.6b00315DOI Listing

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