Recently,
Zn
x
Zr1–x
O2–x
catalysts
have attracted attention as next-generation CO2-to-methanol
hydrogenation catalysts. In this study, we examined the effect of
the Zn content on CO2-to-methanol hydrogenation over Zn
x
Zr1–x
O2–x
catalysts and determined the active-site
structure through both calculations and experiments. When the Zn content
was low, Zn
x
Zr1–x
O2–x
contained Zn clusters
(isolated [ZnO
a
] clusters and [Zn
b
O
c
] oligomers).
The presence of clusters indicates the formation of Zn–O–Zr
sites. Interestingly, our calculations revealed that the Zn species
in the clusters are easily exposed on the Zn
x
Zr1–x
O2–x
surface. This result is in line with the experimental
results, suggesting that Zn species were unevenly distributed on the
Zn
x
Zr1–x
O2–x
surface and deposited near
the surface. The addition of excess Zn to ZrO2 led to the
formation of both Zn-containing clusters and ZnO nanoparticles. During
the reactions, the Zn–O–Zr sites derived from the clusters
showed specific activity for CO2-to-methanol hydrogenation.
Understanding the active-site structure will lead to the future development
of Zn
x
Zr1–x
O2–x
catalysts.
Highly monodisperse particles composed of a magnetic silica core and fluorescent polymer shell were synthesized with a combined technique of heterocoagulation and soap-free emulsion polymerization. Prior to heterocoagulation, monodisperse, submicrometer-sized silica particles were prepared with the Stober method, and magnetic nanoparticles were prepared with a modified Massart method in which a cationic silane coupling agent of N-trimethoxysilylpropyl- N, N, N-trimethylammonium chloride was added just after coprecipitation of Fe (2+) and Fe (3+). The silica particles with negative surface potential were heterocoagulated with the magnetic nanoparticles with positive surface potential. The magnetic silica particles obtained with the heterocoagulation were treated with sodium silicate to modify their surfaces with silica. In the formation of a fluorescent polymer shell onto the silica-coated magnetic silica cores, an amphoteric initiator of 2,2'-azobis[ N-(2-carboxyethyl)-2-2-methylpropionamidine] (VA-057) was used to control the colloidal stability of the magnetic cores during the polymer coating. The polymerization of St in the presence of a hydrophobic fluorophore of pyrene could coat the cores with fluorescent polymer shells, resulting in monodisperse particles with a magnetic silica core and fluorescent polymer shell. Measurements of zeta potential for the composite particles in different pH values indicated that the composite particles had an amphoteric property originating from VA-057 initiator.
Hereditary dentatorubral-pallidoluysian atrophy (DRPLA) is an autosomal dominant neurodegenerative disease with variable clinical phenotypes. Progressive ataxia, choreoathetosis, and dementia are the main clinical features of adult-onset cases, whereas the main feature in juvenile-onset DRPLA is progressive myoclonus epilepsy. Earlier onset is apparent in successive generations (anticipation). The molecular abnormality underlying DRPLA is an expanded, unstable CAG trinucleotide repeat on chromosome 12p. We analyzed 71 DNA samples obtained from 12 Japanese DRPLA pedigrees that included 38 affected individuals. Normal alleles had 7 to 23 repeats, DRPLA alleles 53 to 88 repeats. DRPLA alleles also were detected in five asymptomatic family members. Patients with juvenile onset had significantly larger repeats than did those with adult onset, and there was a significant negative correlation between CAG repeat length and age at onset. In 80% of the paternal transmissions, there was an increase of more than five repeats, whereas all the maternal transmissions showed either a decrease or an increase of fewer than five repeats. There was a significant correlation between father-child differences in repeat length and differences in age at onset. The analysis of CAG repeat length is a reliable diagnostic test for DRPLA and is of value for the presymptomatic detection of individuals at risk. The expansion of CAG repeats is important in phenotypic variation and anticipation. In addition, the sex of the transmitting parent has a significant effect on the molecular mechanism of anticipation.
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