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Surface engineering of earth-abundant Fe catalysts for selective hydrodeoxygenation of phenolics in liquid phase.


ABSTRACT: Development of inexpensive sulfur-free catalysts for selective hydrogenolysis of the C-O bond in phenolics (i.e., selective removal of oxygen without aromatic ring saturation) under liquid-phase conditions is highly challenging. Here, we report an efficient approach to engineer earth-abundant Fe catalysts with a graphene overlayer and alkali metal (i.e., Cs), which produces arenes with 100% selectivity from liquid-phase hydrodeoxygenation (HDO) of phenolics with high durability. In particular, we report that a thin (a few layers) surface graphene overlayer can be engineered on metallic Fe particles (G@Fe) by a controlled surface reaction of a carbonaceous compound, which prevents the iron surface from oxidation by hydroxyls or water produced during HDO reaction. More importantly, further tailoring the surface electronic properties of G@Fe with the addition of cesium, creating a Cs-G@Fe composite catalyst in contrast to a deactivated Cs@Fe one, promotes the selective C-O bond cleavage by inhibiting the tautomerization, a pathway that is very facile under liquid-phase conditions. The current study could open a general approach to rational design of highly efficient catalysts for HDO of phenolics.

SUBMITTER: Zhang J 

PROVIDER: S-EPMC7448371 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Surface engineering of earth-abundant Fe catalysts for selective hydrodeoxygenation of phenolics in liquid phase.

Zhang Jianghao J   Sun Junming J   Kovarik Libor L   Engelhard Mark H MH   Du Lei L   Sudduth Berlin B   Li Houqian H   Wang Yong Y  

Chemical science 20200518 23


Development of inexpensive sulfur-free catalysts for selective hydrogenolysis of the C-O bond in phenolics (<i>i.e.</i>, selective removal of oxygen without aromatic ring saturation) under liquid-phase conditions is highly challenging. Here, we report an efficient approach to engineer earth-abundant Fe catalysts with a graphene overlayer and alkali metal (<i>i.e.</i>, Cs), which produces arenes with 100% selectivity from liquid-phase hydrodeoxygenation (HDO) of phenolics with high durability. In  ...[more]

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