Vladimir Paunovic ́+, Ronghe Lin+, Matthias Scharfe, Amol P. Amrute, Sharon Mitchell,
Roland Hauert, and Javier Pérez-Ramírez*
Angew. Chem. Int. Ed. 2017, 56, 9791-9795
http://onlinelibrary.wiley.com/doi/10.1002/anie.201704406/abstract
Abstract:
The industrialization of bromine-mediated natural
gas upgrading is contingent on the ability to fully recycle
hydrogen bromide (HBr), which is the end form of the halogen
after the activation and coupling of the alkanes. Europium
oxybromide (EuOBr) is introduced as a unique catalytic
material to close the bromine loop via HBr oxidation,
permitting low-temperature operation and long lifetimes with
a stoichiometric feed (O2:HBr=0.25)—conditions at which
any catalyst reported to date severely deactivates because of
excessive bromination. Besides, EuOBr exhibits unparalleled
selectivity to methyl bromide in methane oxybromination,
which is an alternative route for bromine looping. This novel
active phase is finely dispersed on appropriate carriers and
scaled up to technical extrudates, enhancing the utilization of
the europium phase while preserving the performance. This
catalytic system paves the way for sustainable valorization of
stranded natural gas via bromine chemistry.
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