56 research outputs found
Structural Distortion Controlled Spin-Crossover Behavior
Two
mononuclear isomorphous complexes FeÂ(<b>L1</b>)<sub>2</sub>(SCN)<sub>2</sub> (<b>1</b>) and FeÂ(<b>L2</b>)<sub>2</sub>(SCN)<sub>2</sub> (<b>2</b>) [<b>L1</b> = 2-(pyridin-3-yl)-1<i>H</i>-imidazoÂ[4,5-<i>f</i>]Â1,10-phenanthroline; <b>L2</b> = 2-(pyridin-4-yl)-1<i>H</i>-imidazoÂ[4,5-<i>f</i>]Â1,10-phenanthroline] were obtained based on 1,10-phenanthroline
derivatives. Due to the different structural distortion in the coordination
geometries, <b>1</b> exhibits gradual spin transition around
room temperature (<i>T</i><sub>1/2</sub> = 315 K), while <b>2</b> displays a stable high-spin state
Rationally Designed Porous MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> Nanoneedles for Low-Temperature Selective Catalytic Reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub>
In this work, a novel
porous nanoneedlelike MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> catalyst (MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> nanoneedles) was developed
for the first time by rationally heat-treating metal–organic
frameworks including MnFe precursor synthesized by hydrothermal method.
A counterpart catalyst (MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> nanoparticles) without porous nanoneedle
structure was also prepared by a similar procedure for comparison.
The two catalysts were systematically characterized by scanning and
transmission electron microscopy, X-ray diffraction, thermogravimetric
analysis, X-ray photoelectron spectroscopy, hydrogen temperature-programmed
reduction, ammonia temperature-programmed desorption, and in situ
diffuse reflectance infrared Fourier transform spectroscopy (in situ
DRIFT), and their catalytic activities were evaluated by selective
catalytic reduction (SCR) of NO<sub><i>x</i></sub> by NH<sub>3</sub>. The results showed that the rationally designed MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> nanoneedles
presented outstanding low-temperature NH<sub>3</sub>-SCR activity
(100% NO<sub><i>x</i></sub> conversion in a wide temperature
window from 120 to 240 °C), high selectivity for N<sub>2</sub> (nearly 100% N<sub>2</sub> selectivity from 60 to 240 °C),
and excellent water resistance and stability in comparison with the
counterpart MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> nanoparticles. The reasons can be attributed not
only to the unique porous nanoneedle structure but also to the uniform
distribution of MnO<sub><i>x</i></sub> and FeO<sub><i>x</i></sub>. More importantly, the desired Mn<sup>4+</sup>/Mn<sup><i>n</i>+</sup> and O<sub>α</sub>/(O<sub>α</sub> + O<sub>β</sub>) ratios, as well as rich redox sites and abundant
strong acid sites on the surface of the porous MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> nanoneedles, also
contribute to these excellent performances. In situ DRIFT suggested
that the NH<sub>3</sub>-SCR of NO over MnO<sub><i>x</i></sub>–FeO<sub><i>x</i></sub> nanoneedles follows both
Eley–Rideal and Langmuir–Hinshelwood mechanisms
Hydrothermal Synthesis of CaIn<sub>2</sub>S<sub>4</sub>‑Reduced Graphene Oxide Nanocomposites with Increased Photocatalytic Performance
A series
of CaIn<sub>2</sub>S<sub>4</sub>-reduced graphene oxide
(RGO) nanocomposites with different RGO contents were fabricated using
a facile hydrothermal approach. During the hydrothermal process, the
reduction of graphene oxide to RGO, in situ deposition of synthesized
CaIn<sub>2</sub>S<sub>4</sub> nanoparticles on RGO nanosheets and
formation of chemical-bonding CaIn<sub>2</sub>S<sub>4</sub>-RGO nanocomposites
were performed simultaneously. Under visible light irradiation, the
as-prepared CaIn<sub>2</sub>S<sub>4</sub>-RGO nanocomposites showed
enhanced photocatalytic performance for rhodamine B degradation and
phenol oxidation. The sample with 5 wt % RGO hybridized CaIn<sub>2</sub>S<sub>4</sub> exhibited the highest photocatalytic activity. The
enhancement of photocatalytic performance may be related to the increased
adsorption/reaction sites, positive shift of the valence band potential,
and high separation efficiency of photogenerated charge carriers due
to the electronic interaction between CaIn<sub>2</sub>S<sub>4</sub> and RGO. We hope that this work can not only provide an in-depth
study on the photocatalytic mechanism of RGO-enhanced activity, but
also provide some insights for fabricating efficient and stable RGO-based
photocatalysts in the potential applications of purifying polluted
water resources
Two Magnetic Switching Complexes Based on the Fe<sup>II</sup> Ion
Two neutral mononuclear
ironÂ(II) complexes with different spin-crossover (SCO) properties,
FeÂ(<b>L1</b>)<sub>2</sub>(SCN)<sub>2</sub> (<b>1</b>)
and FeÂ(<b>L2</b>)<sub>2</sub>(SCN)<sub>2</sub> (<b>2</b>) (<b>L1</b> = 2-(thiophen-3-yl)-1<i>H</i>-imidazoÂ[4,5-<i>f</i>]Â[1,10]Âphenanthroline and <b>L2</b> = 2-(thiophen-2-yl)-1<i>H</i>-imidazoÂ[4,5-<i>f</i>]Â[1,10]Âphenanthroline),
were solvothermally synthesized. With the different substituted position
in 1,10-phenanthroline derivatives, <b>1</b> exhibits gradual
SCO around room temperature with <i>T</i><sub>1/2</sub> =
280 K, while <b>2</b> displays abrupt SCO with 10 K hysteresis
at <i>T</i><sub>1/2</sub>↓ = 210 K and <i>T</i><sub>1/2</sub>↑ = 220 K
A Series of Weakley-type Polyoxomolybdates: Synthesis, Characterization, and Magnetic Properties by a Combined Experimental and Theoretical Approach
Using DCC as the
dehydrating agent, a series of Weakley-type polyoxomolybdates [Bu<sub>4</sub>N]<sub>3</sub>{LnÂ[Mo<sub>5</sub>O<sub>13</sub>(OMe)<sub>4</sub>(NO)]<sub>2</sub>} (Ln = Tb, Dy, Ho, Er) were synthesized in a one-pot
reaction and structurally characterized by elemental, IR, UV–vis
analysis, PXRD, and single-crystal X-ray diffraction. Furthermore,
the static and dynamic measurements were utilized to investigate their
magnetic performances. Typically, slow relaxation of magnetization
was observed for Dy analogues with an energy barrier for the reversal
of the magnetization of 50 K, which is the highest barrier height
observed on the polyoxomolybdates-based single-molecule magnets (SMMs).
For a deep understanding of the appearance of the SMM behavior on
Weakley-type polyoxomolybdates series, <i>ab initio</i> calculations
on {DyÂ[Mo<sub>5</sub>O<sub>13</sub>(OMe)<sub>4</sub>(NO)]<sub>2</sub>}<sup>3–</sup> have been conducted
A Family of Co<sup>II</sup>Co<sup>III</sup><sub>3</sub> Single-Ion Magnets with Zero-Field Slow Magnetic Relaxation: Fine Tuning of Energy Barrier by Remote Substituent and Counter Cation
The synthesis, structures, and magnetic
properties of a family
of air-stable star-shaped Co<sup>II</sup>Co<sup>III</sup><sub>3</sub> complexes were investigated. These complexes contain only one paramagnetic
CoÂ(II) ion with the approximate <i>D</i><sub>3</sub> coordination
environment in the center and three diamagnetic CoÂ(III) ions in the
peripheral. Magnetic studies show their slow magnetic relaxation in
the absence of an applied dc field, which is characteristic behavior
of single-molecule magnets (SMMs), caused by the individual CoÂ(II)
ion with approximate <i>D</i><sub>3</sub> symmetry in the
center. Most importantly, it was demonstrated that the anisotropy
energy barrier can be finely tuned by the periphery substituent of
the ligand and the countercation. The anisotropy energy barrier can
be increased significantly from 38 K to 147 K
Table_1_Valsa mali Pathogenic Effector VmPxE1 Contributes to Full Virulence and Interacts With the Host Peroxidase MdAPX1 as a Potential Target.DOCX
<p>The Valsa canker, caused by Valsa mali (V. mali), is a destructive disease of apple in Eastern Asia. Effector proteins are important for fungal pathogenicity. We studied a candidate effector VmPxE1 isolated based on the genome information of V. mali. By using the yeast invertase secretion assay system, VmPxE1 was shown to contain a signal peptide with secretory functions. VmPxE1 can suppress BCL-2-associated X protein (BAX)-induced cell death with a high efficacy of 92% in Nicotiana benthamiana. The expression of VmPxE1 was upregulated during the early infection stage and deletion of VmPxE1 led to significant reductions in virulence on both apple twigs and leaves. VmPxE1 was also shown to target an apple ascorbate peroxidase (MdAPX1) by the yeast two-hybrid screening, bimolecular fluorescence complementation and in vivo co-immunoprecipitation. Sequence phylogenetic analysis suggested that MdAPX1 was an ascorbate peroxidase belonging to a subgroup of heme-dependent peroxidases of the plant superfamily. The ectopic expression of MdAPX1 in the mutant of VmPxE1 significantly enhanced resistance to H<sub>2</sub>O<sub>2</sub>, while the presence of VmPxE1 seems to disturb MdAPX1 function. The present results provide insights into the functions of VmPxE1 as a candidate effector of V. mali in causing apple canker.</p
Image_3_Valsa mali Pathogenic Effector VmPxE1 Contributes to Full Virulence and Interacts With the Host Peroxidase MdAPX1 as a Potential Target.TIF
<p>The Valsa canker, caused by Valsa mali (V. mali), is a destructive disease of apple in Eastern Asia. Effector proteins are important for fungal pathogenicity. We studied a candidate effector VmPxE1 isolated based on the genome information of V. mali. By using the yeast invertase secretion assay system, VmPxE1 was shown to contain a signal peptide with secretory functions. VmPxE1 can suppress BCL-2-associated X protein (BAX)-induced cell death with a high efficacy of 92% in Nicotiana benthamiana. The expression of VmPxE1 was upregulated during the early infection stage and deletion of VmPxE1 led to significant reductions in virulence on both apple twigs and leaves. VmPxE1 was also shown to target an apple ascorbate peroxidase (MdAPX1) by the yeast two-hybrid screening, bimolecular fluorescence complementation and in vivo co-immunoprecipitation. Sequence phylogenetic analysis suggested that MdAPX1 was an ascorbate peroxidase belonging to a subgroup of heme-dependent peroxidases of the plant superfamily. The ectopic expression of MdAPX1 in the mutant of VmPxE1 significantly enhanced resistance to H<sub>2</sub>O<sub>2</sub>, while the presence of VmPxE1 seems to disturb MdAPX1 function. The present results provide insights into the functions of VmPxE1 as a candidate effector of V. mali in causing apple canker.</p
CaIn<sub>2</sub>O<sub>4</sub>/Fe-TiO<sub>2</sub> Composite Photocatalysts with Enhanced Visible Light Performance for Hydrogen Production
A series
of CaIn<sub>2</sub>O<sub>4</sub>/Fe-TiO<sub>2</sub> composite photocatalysts
with tunable Fe-TiO<sub>2</sub> contents were prepared in which Fe-TiO<sub>2</sub> nanoparticles were uniformly deposited onto the surface of
CaIn<sub>2</sub>O<sub>4</sub> nanorods. The photocatalytic activities
of Pt-loaded CaIn<sub>2</sub>O<sub>4</sub>/Fe-TiO<sub>2</sub> composites
were evaluated for H<sub>2</sub> evolution from aqueous KI solution
under visible light irradiation. It was found that the composites
showed higher H<sub>2</sub> evolution rates in comparison with pure
CaIn<sub>2</sub>O<sub>4</sub> or Fe-TiO<sub>2</sub>, which could be
attributed to the increased surface area and enhanced visible light
absorption. A high H<sub>2</sub> evolution rate of 280 ÎĽmol
h<sup>–1</sup> g<sup>–1</sup> was achieved when the
mass ratio of Fe-TiO<sub>2</sub> to CaIn<sub>2</sub>O<sub>4</sub> was
0.5, which was 12.3 and 2.2 times higher than that of pure CaIn<sub>2</sub>O<sub>4</sub> and Fe-TiO<sub>2</sub>, respectively. Furthermore,
the interfaces between CaIn<sub>2</sub>O<sub>4</sub> nanorods and
Fe-TiO<sub>2</sub> nanoparticles facilitated efficient charge separation
that also led to the improved photocatalytic activity. This study
may provide some inspiration for the fabrication of visible-light-driven
photocatalysts with efficient and stable performance
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