Seeking a simple and moderate route to generate reactive oxygen species (ROS) for antibiosis is of great interest and challenge. This work demonstrates that molecule transition and electron rearrangement processes can directly occur only through chemisorption interaction between the adsorbed O and high-energy {111} facet-exposed MgO with abundant surface oxygen vacancies (SOVs), hence producing singlet oxygen and superoxide anion radicals without light irradiation. These ROS were confirmed by electron paramagnetic resonance, in situ Raman, and scavenger experiments. Furthermore, heat plays a crucial role for the electron transfer process to accelerate the formation of ·O, which is verified by temperature kinetic experiments of nitro blue tetrazolium reduction in the dark. Therefore, the presence of oxygen vacancy can be considered as an intensification of the activation process. The designed MgO is acquired in one step via constructing a reduction atmosphere during the combustion reaction process, which has an ability similar to that of noble metal Pd to activate molecular oxygen and can be used as an effective bacteriocide in the dark.
Methane is a greenhouse
gas that contributes to global warming.
Hence, effectively removing the low concentration (<1000 ppm) of
methane in the environment is an issue that deserves research in the
field of catalysis. In this study, oxygen–magnesium bivacancies
are simultaneously imbedded into MgO by designing an in situ reduction
combustion atmosphere for oxygen release and substituting magnesium
with carbon to induce the formation of magnesium vacancies. The DFT
calculations reveal that the surface electron density of MgO is improved
by the oxygen vacancy structure and the substitution of Mg by C in
bulk; this accelerates migration of the charge from the material surface
to the adsorbed oxygen species, which leads to abundant surface peroxide
species that enable activation and oxidation of methane at a low temperature
(below 200 °C). This work could provide a concept for developing
non-noble or transition metal oxides for low-temperature activation
and conversion of alkanes in the thermocatalytic field through reactive
oxygen species.
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