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.
Highlights
Styrene is one of the most important industrial monomers and is traditionally synthesized via the dehydrogenation of ethylbenzene
After the treatment of fluorination, the texture of ND and functionalized nanodiamonds (F-ND) catalysts were explored by scanning electron microscopy (SEM)
The ND catalyst was covered with a small amount of amorphous graphite (Fig. 1b) and a core-shell structure covered with few graphitic layers was formed after the fluorination strategy (Fig. 1c)
Summary
Styrene is one of the most important industrial monomers and is traditionally synthesized via the dehydrogenation of ethylbenzene. Experimental characterizations and density functional theory calculations reveal that the fluorine functionalization promotes the conversion of sp[3] to sp[2] carbon to generate graphitic layers and stimulates and increases the active sites (ketonic C=O) Considerable research efforts have focused on improving the ODH performance based on ND catalysts by identifying and exposing active sites[14], as well as nanostructuring[15], surface engineering[16], and hybridization[17] Among these approaches, surface engineering seems to be an efficient, simple, and costeffective strategy[18]. This work reveals an important strategy for a new avenue for fluorination and property modification of carbon-based catalysts and presents a wide range of possibilities for the further development of ODH reactions
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