Catalytic
ozonation of methyl mercaptan (CH3SH) can
effectively control this unbearable odorous sulfur-containing volatile
organic compound (S-VOC). The construction of an electronic metal–support
interaction (EMSI) coordination structure to maximize the number of
active sites and increase the intrinsic activity of active sites is
an effective means to improve catalytic performance. In this work,
the abundant Si–OH groups on PSBA-15 (SBA-15 before calcination)
were used to anchor Mn to form a Si–O–Mn-based EMSI
coordination structure. Detailed characterizations and theoretical
simulations reveal that the strong EMSI effect significantly adjusts
and stabilizes the electronic structure of Mn 3d states, resulting
in an electron-rich center on the Si–O–Mn bond to promote
the specific adsorption/activation of ozone (O3) and an
electron-poor center on the (Si–O−)Mn–O bond
to adsorb a large amount of CH3SH accompanied by its own
oxidative degradation. In situ Raman and in situ Fourier transform infrared (FTIR) analyses identify
that catalytic ozonation over 3.0Mn-PSBA generates atomic oxygen species
(AOS/*O) and reactive oxygen species (ROS/•O2
–) to achieve efficient decomposition of
CH3SH into CO2/SO4
2–. Furthermore, the electrons obtained from CH3SH in electron-poor
centers are transferred to maintain the redox cycle of Mn2+/3+ → Mn4+ → Mn2+/3+ through the
internal bond bridge, thus accomplishing the efficient and stable
degradation of CH3SH prolonged to 180 min. Therefore, the
rational design of catalysts with abundant active sites and optimized
inherent activity via the EMSI effect can provide
significant potential to improve catalytic performance and eliminate
odorous gases.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.