We report the first use of polymeric carbon nitride (CN) for the catalytic selective oxidation of HS. The as-prepared CN with unique ultrathin "nanomeshes" structure exhibits excellent HS conversion and high S selectivity. In particular, the CN nanomesh also displays better durability in the desulfurization reaction than traditional catalysts, such as carbon- and iron-based materials.
CeO2-based
catalysts are potentially suitable for H2S-selective oxidation,
but their practical application is
limited due to the problem of sulfate formation. Herein, we report
a facile citric acid-assisted hydrothermal process for the fabrication
of porous Fe-doped CeO2 with flower-like morphology that
can drastically promote the catalytic activities of CeO2 with high durability. Among the synthesized catalysts, the one with
well-defined (110) and (100) planes is highly active for H2S-selective oxidation with H2S conversion and sulfur selectivity
of almost 100% at 220 °C, superior to most of the reported Ce-based
catalysts. Meanwhile, outstanding catalytic stability is achieved
because the presence of Fe ions alleviates ceria deactivation due
to sulfation. The results of systematic investigation prove that the
doping of Fe not only raises the density of oxygen vacancies but also
promotes the redox ability and oxygen activity of the catalyst. We
conducted in situ DRIFTS (diffuse reflection infrared
Fourier transform spectroscopy) experiments and density functional
theory (DFT) calculations to disclose the reaction mechanism of H2S oxidation. The derived insights are important for the design
of efficient ceria-related catalysts for practical applications.
A series of graphitic
carbon nitride (CN) in the form of nanosheets
with porous structure have been prepared through thermal treatment
of bulk CN in air. Compared with the bulk counterpart, the as-generated
holey CN nanosheets are larger in specific surface area. Endowed with
more active sites and enhanced mass transport ability, the latter
display catalytic performance substantially superior to the former,
exhibiting higher H2S conversion and S selectivity in the
oxidation of H2S to S. Moreover, the CN nanosheets show
much better durability than traditional catalysts. It is envisaged
that the strategy is a general technique that can be extended to produce
porous CN nanosheets from other nitrogen-rich precursors, as well
as to prepare other 2D carbon-based materials for potential applications.
Developing NH 3 separation technology with high efficiency is very meaningful for the advancement of the NH 3 synthesis process. In this work, a new class of deep eutectic solvents (DESs) were designed by pairing N,N,N′,N′-tetramethyl-1,3-propanediamine dihydrochloride ([TMPDA]Cl 2 ) with phenol (PhOH) at the molar ratios of 1:3∼7. [TMPDA]Cl 2 + PhOH DESs have multiple weak-acidic groups and viscosities of as low as 48.1 cP at 298.2 K. They also exhibit excellent performance for the separation of NH 3 , showing not only efficient and selective but also reversible absorption of NH 3 . Especially, the solubilities of NH 3 in [TMPDA]Cl 2 + PhOH DESs at low pressures can reach 4.49 mol/kg of NH 3 at 298.2 K and 13.3 kPa, being superior to those of most of the DESs and ILs reported in the literature. The mechanism of NH 3 absorption was further elucidated by quantum chemistry calculations and 1 H NMR spectra. It is validated that the efficient absorption of NH 3 in DESs origins from the strong interaction of multiple weak-acidic groups of DESs with NH 3 .
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