Developing highly efficient photocatalysts
to utilize solar radiation
for converting CO2 into solar fuels is of great importance
for energy sustainability and carbon neutralization. Herein, through
an alkali-etching-introduced interface reconstruction strategy, a
nanowire photocatalyst denoted as V–Bi19Br3S27, with rich Br and S dual-vacancies and surface Bi–O
bonding introduced significant near-infrared (NIR) light response,
has been developed. The as-obtained V–Bi19Br3S27 nanowires exhibit a highly efficient metallic
photocatalytic reduction property for converting CO2 into
CH3OH when excited solely under NIR light irradiation.
Free of any cocatalyst and sacrificial agent, metallic defective V–Bi19Br3S27 shows 2.3-fold higher CH3OH generation than Bi19Br3S27 nanowires. The detailed interfacial structure evolution and reaction
mechanism have been carefully illustrated down to the atomic scale.
This work provides a unique interfacial engineering strategy for developing
high-performance sulfur-based NIR photocatalysts for photon reducing
CO2 into alcohol for achieving high-value solar fuel chemicals,
which paves the way for efficiently using the solar radiation energy
extending to the NIR range to achieve the carbon neutralization goal.
A series of 61 imines with various typical structures were synthesized, and the thermodynamic affinities (defined as enthalpy changes or redox potentials in this work) of the imines to abstract hydride anions, hydrogen atoms, and electrons, the thermodynamic affinities of the radical anions of the imines to abstract hydrogen atoms and protons, and the thermodynamic affinities of the hydrogen adducts of the imines to abstract electrons in acetonitrile were determined by using titration calorimetry and electrochemical methods. The pure heterolytic and homolytic dissociation energies of the C=N pi-bond in the imines were estimated. The polarity of the C=N double bond in the imines was examined using a linear free-energy relationship. The idea of a thermodynamic characteristic graph (TCG) of imines as an efficient "Molecule ID Card" was introduced. The TCG can be used to quantitatively diagnose and predict the characteristic chemical properties of imines and their various reaction intermediates as well as the reduction mechanism of the imines. The information disclosed in this work could not only supply a gap of thermodynamics for the chemistry of imines but also strongly promote the fast development of the applications of imines.
The selective transformation of furfural to 1,4-pentanediol has been achieved with up to 90% yield in a CO2/H2/H2O system over Ru catalytic species supported on a mesoporous carbon.
Conclusions:
In prelingually deaf children with cochlear implants, tone perception and production performance are highly correlated. This result is consistent with the hypothesis that tone perception is the prerequisite for good tone production.
Objectives:
Previous research has shown remarkable deficits in tone perception and production in native tone languagespeaking, prelingually deafened children with cochlear implants. The purpose of the present study was to investigate the relationship between tone perception and production in those children.
Methods:
Twenty-five prelingually deaf children with cochlear implants participated in the study. All subjects were Advanced Bionics CII/90K users with various lengths of implant use. To evaluate tone perception performance, subjects completed a computerized tone contrast test. For tone production performance, an artificial neural network was used to evaluate the accuracy of tones recorded from each of the 25 subjects.
Results:
Large individual differences in tone perception and production performance were observed in these subjects. Tone perception accuracy ranged from 50.0 to 96.9% correct (chance performance = 50% correct; mean = 71.0% correct). Tone production performance ranged from 19.4 to 97.2% correct (mean = 52.0% correct). A strong correlation was found between tone perception and production performance in this group of subjects (r = 0.805).
A new
dual catalyst system composed of choline-derived ionic liquids
(ILs) and Pd/C was developed for the selective hydrogenolysis of Kraft
lignin to monophenols. Among a series of investigated choline-derived
ILs, [Ch][MeSO3] displayed a strong acidity, good thermal
stability, and excellent lignin solubility. Under the reaction conditions
of the mass ratio of [Ch][MeSO3] to Pd/C being 1, the Pd/C
loading of 3.5 wt %, H2 pressure of 2.0 MPa, reaction time
of 5 h, and temperature of 200 °C, the conversion of Kraft lignin
and the selectivity to phenol (PL) and catechol (COL) reached 20.3%,
18.4%, and 18.1%, respectively. In order to rationalize the formation
of PL and COL in our [Ch][MeSO3]-Pd/C system, the hydrogenolysis
of a suitable lignin model compound (guaiacylglycerol-β-guaiacyl
ether) was studied under the same condition for Kraft lignin. The
results suggested that the mechanism involved fragmentation of lignin
catalyzed by both acid and Pd/C, followed by acid-catalyzed C–O
and C–C cleavage of the fragmented compounds resulting in the
formation of PL and COL.
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