Enhanced Light\nAlkane Oxidation under Impurity-Containing\nConditions by Low-Coordinated Co–O Structures Boosting C–H\nBond Activation

Anthropogenic light alkanes pose significant environmental\nand\nhealth hazards; however, achieving their efficient catalytic oxidation,\nparticularly under industrial conditions with impurities, remains\na huge challenge. Tuning the coordinated structure of metal atoms\nis a promising strategy for improving their low-temperature efficiency\nfor stable C–H bond activation. Herein, we propose a one-step\nmethod for precisely modulating the coordination structures of Co\natoms in a Co<sub>3</sub>O<sub>4</sub> catalyst by controlling the\ndiverse nucleation rates of Co(OH)<sub>x</sub> species. The Co<sub>3</sub>O<sub>4</sub>-L catalyst with the lowest Co–O bonding\nexhibits exceptional catalytic performance, achieving complete oxidation\nof 1000 ppm propane and methane at just 179 and 290 °C, respectively.\nThis performance is far superior to that of known catalysts, which\ntypically require over 250 and 350 °C for 90% conversion of propane\nand methane, respectively. Additionally, Co<sub>3</sub>O<sub>4</sub>-L demonstrates excellent activity and stability in the presence\nof multiple organic components, as well as SO<sub>2</sub> and H<sub>2</sub>O. The promoted electron-pair interactions between σ/σ*\nC–H orbitals and <i>d</i> orbitals of low-coordinated\nCo<sup>2+</sup> species by sufficient low saturation sites strengthens\nthe adsorption and activation of light alkanes and facilitates the\ncleavage of the C–H bond, ultimately reducing the reaction\nenergy barrier. The high stability and antitoxicity are due to the\nabundant surface dangling bond-induced structural stability and rapid\noxygen replenishment, which is facilitated by high electron transport\ncapacity. This study establishes a solid foundation for further exploration\nof effective catalytic platforms for light alkanes under impurity-containing\nconditions.