1 research outputs found
Hydrogenation of Nitroarenes by Onsite-Generated Surface Hydroxyl from Water
Directly using water as a hydrogen source for hydrogenation
of
nitroarenes to anilines (HNA) without using H2 is an ideal
reduction reaction route but is limited by unfavorable thermodynamics.
Herein, we report a high-efficiency and durable H2O-based
HNA process achieved by using in situ-generated hydroxyl species from
water as a hydrogen donor and low-cost CO as an oxygen acceptor over
a molybdenum carbide-supported gold catalyst (Au/α-MoC1–x). It affords nitroarene conversion of over 99% with
aniline selectivity of over 99% and excellent functional group tolerance
at 25 °C and remains stable after 10 cycles, outperforming the
traditional H2-involved route. Spectroscopic and theoretical
studies reveal the key role of Au/α-MoC1–x boundaries, at which not only hydroxyl species are
generated as a soft reductant on α-MoC1–x but also the nitro group is selectively hydrogenated
to anilines with other unsaturated groups intact, and residual O*
is removed by adsorbed CO on the atomically thin Au layer. This process
provides a durable H2O-based route for aniline production
at room temperature