The selective oxidation of methane under mild conditions remains the “Holy Grail of Catalysis”. The key to activating methane and inhibiting over-oxidation of target oxygenates lies in designing active centers. Copper nanoparticles were loaded onto TiO2 nanofibers using the photo-deposition method. The resulting catalysts were found to effectively convert methane into C1 oxygenated products under mild conditions. Compared with previously reported catalysts, it delivers a superior performance of up to 2510.7 mmol·gCu−1·h−1 productivity with a selectivity of around 100% at 80 °C for 5 min. Microstructure characterizations and density functional theory (DFT) calculations indicate that TiO2 in the mixed phase of anatase and rutile significantly increases the Cu+/Cu0 ratio of the supported Cu species, and this ratio is linearly related to the formation rate of oxygen-containing species. The CuI site promotes the generation of active O species from H2O2 dissociation on Cu2O (111). These active O species reduce the energy barrier for breaking the C–H bond of CH4, thus boosting the catalytic activity. The methane conversion mechanism was proposed as a methyl radical pathway to form CH3OH and CH3OOH, and then the generated CH3OH is further oxidized to HOCH2OOH.

Yolk-shell SiO2 particles (YP) with center-radial meso-channels were fabricated through a simple and effective method. Al-containing YP-supported NiMo catalysts with different Al amounts (NiMo/AYP-x, x = Si/Al molar proportion) were prepared and dibenzothiophene (DBT) and 4,6-dimethyl-dibenzothiophene (4,6-DMDBT) were employed as the probes to evaluate the hydrodesulfurization (HDS) catalytic performance. The as-prepared AYP-x carriers and corresponding catalysts were characterized by some advanced characterizations to obtain deeper correlations between physicochemical properties and the HDS performance. The average pore sizes of series AYP-x supports are above 6.0 nm, which favors the mass transfer of organic sulfides. The cavity between the yolk and the shell is beneficial for the enrichment of S-containing compounds and the accessibility between reactants and active metals. Aluminum embedded into the silica framework could facilitate the formation of Lewis (L) and Brønsted (B) acid sites and adjust the metal-support interaction (MSI). Among all the as-synthesized catalysts, NiMo/AYP-20 catalyst shows the highest HDS activities. The improved HDS activity of NiMo/AYP-20 catalyst is attributed to the perfect combination of excellent structural properties of the yolk-shell mesoporous silica, enhanced acidity, moderate MSI, and good accessibility/dispersion of active components.
Air pollution from particulate matter produced by incomplete combustion of diesel fuel has become a serious environmental pollution problem, which can be addressed by catalytic combustion. In this work, a series of K-modified MnOδ catalysts with different microstructures were synthesized by the hydrothermal method, and the relationship between structure of the catalysts and their catalytic performance for soot combustion was studied by characterization techniques and density functional theory (DFT) calculations. Results showed that the prepared catalysts had good catalytic performance for soot combustion and could completely oxidize soot at temperatures below 400 °C. The cryptomelane-type K2−xMn8O16 (K-OMS-2) with tunnel structure had excellent NO oxidation capacity and abundance of Mn4+ ions (Mn4+/Mn3+ = 1.24) with good redox ability, and it demonstrated better soot combustion performance than layered birnessite-type K2Mn4O8 (K-OL-1). The T10, T50, and T90 temperatures of K-OMS-2 were 269, 314, and 346 °C, respectively. The K-OMS-2 catalyst also showed excellent stability after five catalytic cycles, with T10, T50, and T90 values holding in the ranges of 270 ± 2, 316 ± 2, and 348 ± 3 °C, respectively.