We herein report a visible-light photoredox-catalyzed regioselective sulfonylation of alkenes with sulfonyl hydrazides assisted by oximes at room temperature, which affords a variety of sulfones in good yields. The initial mechanistic experiments demonstrate that the hydroxyl group within oximes plays a crucial role in this sulfonylation.
The O2 preadsorption properties prior to the application
for nanomaterials have rarely attracted attention; however, they greatly
affect the surface nature between gas and nanomaterials. Here, a hierarchically
ZnO nest-like architecture (ZnO NAs) with nanosheets was synthesized
by a facile hydrothermal method without structure-directing agents
and templates. The percentage of exposed (001) facet for ZnO NAs is
∼95% according to its micromorphology. A gas sensor fabricated
by ZnO NAs exhibits high sensitivity, low detection limit, fast response,
and good selectivity to acetone at the low working temperature (105
°C). The distinct gas-sensing properties of ZnO NAs are mainly
attributed to the specific surface area (63.46 m2/g) and
high active (001) facet for the nanosheets. Note that a preadsorption
of O2 from air on ZnO NAs and the gas reaction mechanism
are put forward based on the preadsorbed behavior and target gas response.
Moreover, by the aid of first-principles on the analysis of its surface
adsorption energy and adsorption structure at (001) facet of ZnO NAs,
it is identified that an oxygen preadsorption step on the facet occurs
once it makes contact with air due to a lowest surface adsorption
energy (−3.149 eV) for oxygen molecule. After the O2 preadsorption onto the surface, acetone is with the lowest surface
adsorption energy of −0.687 eV, assigned to a chemical adsorption
compared with the other gases. It benefits the acetone adsorption
on the (001) facet for ZnO NAs, as well as following electron transfer
and gas response. The sensitivity and selectivity for gas sensor based
on ZnO NAs are well certified by both gas-resistance response and
computational simulation.
An iron(ii)-catalyzed radical cyclization of oximes with hypervalent iodine reagents was developed, which enabled the construction of the isoxazoline backbone.
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