19 research outputs found
Emerging advanced oxidation processes for the elimination of micro-pollutants
Emerging advanced oxidation processes for the elimination of micro-pollutant
Spontaneous Iodide Activation at the Air–Water Interface of Aqueous Droplets
We present experimental evidence that atomic and molecular
iodine,
I and I2, are produced spontaneously in the dark at the
air–water interface of iodide-containing droplets without any
added catalysts, oxidants, or irradiation. Specifically, we observe
I3– formation within droplets, and I2 emission into the gas phase from NaI-containing droplets
over a range of droplet sizes. The formation of both products is enhanced
in the presence of electron scavengers, either in the gas phase or
in solution, and it clearly follows a Langmuir–Hinshelwood
mechanism, suggesting an interfacial process. These observations are
consistent with iodide oxidation at the interface, possibly initiated
by the strong intrinsic electric field present there, followed by
well-known solution-phase reactions of the iodine atom. This interfacial
chemistry could be important in many contexts, including atmospheric
aerosols
Can Silica Particles Reduce Air Pollution by Facilitating the Reactions of Aliphatic Aldehyde and NO<sub>2</sub>?
This
study investigated the heterogeneous atmospheric reactions
of acetaldehyde, propanal, and butanal with NO<sub>2</sub> onto silica
(SiO<sub>2</sub>) clusters using a theoretical approach. By analyzing
spectral features and adsorption parameters, the formation of hydrogen
bonds and negative adsorption energies provide evidence that an efficient
spontaneous uptake of aliphatic aldehydes onto SiO<sub>2</sub> could
occur. The atmospheric reaction mechanisms show that when aldehydes
and NO<sub>2</sub> react on the surface model, the H atom abstraction
reaction from the aldehydic molecule by NO<sub>2</sub> is an exclusive
channel, forming nitrous acid and acyl radicals. This study included
kinetics exploring the reaction of aldehydes with NO<sub>2</sub> using
a canonical variational transition state theory. The reaction rate
constants are increased in the presence of SiO<sub>2</sub> between
the temperatures 217 and 298 K. This may explain how aldehydes can
temporarily stay on mineral particles without chemical reactions.
The results suggest that silica can depress the rate at which the
studied aldehydes react with NO<sub>2</sub> and possibly reduce air
pollution generated by these atmospheric reactions
Kinetics and Mechanism of <sup>•</sup>OH Mediated Degradation of Dimethyl Phthalate in Aqueous Solution: Experimental and Theoretical Studies
The hydroxyl radical (<sup>•</sup>OH) is one of the main
oxidative species in aqueous phase advanced oxidation processes, and
its initial reactions with organic pollutants are important to understand
the transformation and fate of organics in water environments. Insights
into the kinetics and mechanism of <sup>•</sup>OH mediated
degradation of the model environmental endocrine disruptor, dimethyl
phthalate (DMP), have been obtained using radiolysis experiments and
computational methods. The bimolecular rate constant for the <sup>•</sup>OH reaction with DMP was determined to be (3.2 ±
0.1) × 10<sup>9</sup> M<sup>–1</sup>s<sup>–1</sup>. The possible reaction mechanisms of radical adduct formation (RAF),
hydrogen atom transfer (HAT), and single electron transfer (SET) were
considered. By comparing the experimental absorption spectra with
the computational results, it was concluded that the RAF and HAT were
the dominant reaction pathways, and OH-adducts (<sup>•</sup>DMPOH<sub>1</sub>, <sup>•</sup>DMPOH<sub>2</sub>) and methyl
type radicals <sup>•</sup>DMPÂ(-H)Âα were identified as
dominated intermediates. Computational results confirmed the identification
of transient species with maximum absorption around 260 nm as <sup>•</sup>DMPOH<sub>1</sub> and <sup>•</sup>DMPÂ(-H)Âα,
and these radical intermediates then converted to monohydroxylated
dimethyl phthalates and monomethyl phthalates. Experimental and computational
analyses which elucidated the mechanism of <sup>•</sup>OH-mediated
degradation of DMP are discussed in detail
Relationship between the mutagenic ratio on TA98 without S9 activation and IR by SOS/<i>umu</i> test without S9 activation.
<p>Relationship between the mutagenic ratio on TA98 without S9 activation and IR by SOS/<i>umu</i> test without S9 activation.</p
Genotoxic activity of organic extracts in water samples detected by SOS/<i>umu</i> test from six sampling locations in Guangzhou drinking water source.
<p>Lower-case letters indicated pair-wise comparison in the dry season in different sampling regions at the same water level and upper-case letters indicated pair-wise comparison in the wet season in different sampling regions at the same water level. *indicated the significant difference from the wet season.</p
Synthesis and Characterization of Novel Plasmonic Ag/AgX-CNTs (X = Cl, Br, I) Nanocomposite Photocatalysts and Synergetic Degradation of Organic Pollutant under Visible Light
A series of novel well-defined Ag/AgX
(X = Cl, Br, I) loaded carbon nanotubes (CNTs) composite photocatalysts
(Ag/AgX-CNTs) were fabricated for the first time via a facile ultrasonic
assistant deposition–precipitation method at the room temperature
(25 ± 1 °C). X-ray diffraction, X-ray photoelectron spectroscopy,
nitrogen adsorption–desorption analysis, scanning electron
microscopy, and ultraviolet–visible light absorption spectra
analysis were used to characterize the structure, morphology, and
optical properties of the as-prepared photocatalysts. Results confirmed
the existence of the direct interfacial contact between Ag/AgX nanoparticles
and CNTs, and Ag/AgX-CNTs nanocomposites exhibit superior absorbance
in the visible light (VL) region owing to the surface plasmon resonance
(SPR) of Ag nanoparticles. The fabricated composite photocatalysts
were employed to remove 2,4,6-tribromophenol (TBP) in aqueous phase.
A remarkably enhanced VL photocatalytic degradation efficiency of
Ag/AgX-CNTs nanocomposites was observed when compared to that of pure
AgX or CNTs. The photocatalytic activity enhancement of Ag/AgX-CNTs
was due to the effective electron transfer from photoexcited AgX and
plasmon-excited Ag(0) nanoparticles to CNTs. This can effectively
decrease the recombination of electron–hole pairs, lead to
a prolonged lifetime of the photoholes that promotes the degradation
efficiency
Synthesis of Carbon Nanotube–Anatase TiO<sub>2</sub> Sub-micrometer-sized Sphere Composite Photocatalyst for Synergistic Degradation of Gaseous Styrene
The carbon nanotube (CNT)–sub-micrometer-sized
anatase TiO<sub>2</sub> sphere composite photocatalysts were synthesized
by a facile
one-step hydrothermal method using titanium tetrafluoride as titanium
source and CNTs as structure regulator. Various technologies including
X-ray diffraction, UV–visible absorption spectra, N<sub>2</sub> adsorption–desorption, scanning electron microscopy, and
transmission electron microscopy were employed to characterize the
structure properties of the prepared composite photocatalysts. The
results indicated that the composite photocatalysts consisted of CNTs
wrapping around the sub-micrometer-sized anatase TiO<sub>2</sub> spheres
with controllable crystal facets and that the aggregated particles
with average diameter ranged from 200 to 600 nm. The fabricated composite
photocatalysts were used to degrade gaseous styrene in this work.
As expected, a synergistic effect that remarkably enhancing the photocatalytic
degradation efficiency of gaseous styrene by the prepared composite
photocatalysts was observed in comparison with that the degradation
efficiency using pure anatase TiO<sub>2</sub> and the adsorption of
CNTs. Similar results were also confirmed in the decolorization of
liquid methyl orange. Further investigation demonstrated that the
synergistic effect in the photocatalytic activity was related to the
structure of the sub-micrometer-sized anatase TiO<sub>2</sub> spheres
and the significant roles of CNTs in the composite photocatalysts.
By controlling the content of CNTs, the content of TiO<sub>2</sub> or the temperature during the hydrothermal synthesis process, anatase
TiO<sub>2</sub> spheres with controllable crystallite size and dominant
crystal facets such as {001}, {101}, or polycrystalline could be obtained,
which was beneficial for the increase in the synergistic effect and
further enhancement of the photocatalytic efficiencies