Photo-fluorination of nanodiamonds catalyzing oxidative dehydrogenation reaction of ethylbenzene

Abstract

Styrene is one of the most important industrial monomers and is traditionally synthesized via the dehydrogenation of ethylbenzene. Here, we report a photo-induced fluorination technique to generate an oxidative dehydrogenation catalyst through the controlled grafting of fluorine atoms on nanodiamonds. The obtained catalyst has a fabulous performance with ethylbenzene conversion reaching 70% as well as styrene yields of 63% and selectivity over 90% on a stream of 400 °C, which outperforms other equivalent benchmarks as well as the industrial K−Fe catalysts (with a styrene yield of 50% even at a much higher temperature of ca. 600 °C). Moreover, the yield of styrene remains above 50% after a 500 h test. Experimental characterizations and density functional theory calculations reveal that the fluorine functionalization not only promotes the conversion of sp3 to sp2 carbon to generate graphitic layers but also stimulates and increases the active sites (ketonic C=O). This photo-induced surface fluorination strategy facilitates innovative breakthroughs on the carbocatalysis for the oxidative dehydrogenation of other arenes.

Dendrimer-Functionalized Nanodiamonds as Safe and Efficient Drug Carriers for Cancer Therapy: Nucleus Penetrating Nanoparticles

“…A lattice fringe spacing of ca. 0.202 nm was attributed to the interplanar distance of the (111) plane of the nanodiamond …”

Metal‐Free Catalytic Reduction of 4‐Nitrophenol to 4‐Aminophenol by sp3@sp2‐Hybridized Bucky Nanodiamond

“…For the versatile structural and electronic properties of the characteristic core/shell architecture, the partially graphitized carbon family has been widely used in oxidative dehydrogenation reactions and other oxidative reactions. [7][8][9][10][11] Generally, the surface chemistry as well as the synergistic effect of the graphitic shell and ND core play a key role in their excellent catalytic performance. However, the sp 3 @sp 2 core-shell structures were rarely used in the reduction reactions.…”

Ferric Single‐Site Catalyst Confined in a Zeolite Framework for Propane Dehydrogenation

“…Fe is the fourth most abundant element in the earth's crust and Fe-based catalysts have been employed commercially for ethylbenzene dehydrogenation, [40] but it still has limited application in propane dehydrogenation. Although ferric zeolites performed the best among various supported ferric catalysts, they have always suffered from low activity or selectivity and deactivation.…”