Herein, we report commercially available carbon-supported-palladium
(Pd/C)-catalyzed N-methylation of nitroarenes and
amines using MeOH as both a C1 and a H2 source. This transformation
proceeds with high atom-economy and in an environmentally friendly
way via borrowing hydrogen mechanism. A total of >30 structurally
diverse N-methylamines, including bioactive compounds,
were selectively synthesized with isolated yields of up to 95%. Furthermore,
selective N-methylation and deuteration of nimesulide,
a nonsteroidal anti-inflammatory drug, were realized through the late-stage
functionalization.
Designing new materials for selective Fischer–Tropsch
synthesis
(FTS) is an elegant way to enhance local feedstock utilization like
biomass and waste. In this approach, we have designed a thermally
and chemically stable bimetallic PtCo/NC hybrid nanocomposite catalyst
derived from a zeolitic imidazolate framework (ZIF-67, which contains
cobalt as a metal center) through carbonization for low-temperature
(413–473 K) aqueous-phase Fischer–Tropsch synthesis
(AFTS). The selectivity of the desired range of hydrocarbons is adjusted
using a highly dispersed PtCo bimetallic alloy, which facilitates
extraordinary reduction of a metal oxide to active species by the
synergic effect under the AFTS reaction conditions. The ZIF-derived
catalyst tested in this study exhibited the highest activity to date
for very low temperatures (433 K) in aqueous-phase Fischer–Tropsch
synthesis with CO conversion rates between 0.61 and 1.20 molCO·molCo
–1·h–1. Insights of the remarkable catalyst activity were examined by in situ X-ray photoelectron spectroscopy (XPS) studies corroborated
by density functional theory (DFT) calculation. The bimetallic Co3Pt (111) surface was found to be highly active for the C–C
coupling reaction between surface-adsorbed C and CO, forming a CCO
intermediate with a very low activation barrier (E
a = 0.37 eV), in comparison to the C–C coupling
activation barrier obtained over the Co (111) surface (E
a = 0.87 eV). This unique approach and observations create
a new path for developing next-generation advanced catalyst systems
and processes for selective low-temperature FTS.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.