The simultaneous activation of surface lattice oxygen and dioxygen is key to transition metal oxide-based catalytic CO oxidation systems. However, the reaction is difficult at room temperature owing to the high metal–oxygen bond energy. This study presents a triboelectric plasma–transition metal oxide catalytic system driven by a triboelectric nanogenerator, which realizes CO oxidation reaction at room temperature and atmospheric pressure. Among the transition metal oxides evaluated, MnO2 nanostructures exhibited an optimal CO oxidation activity of 0.24 mmol·g–1·h–1 and a low energy consumption converted per mole CO of 6.0 × 103 kJ. For the activation of both surface lattice oxygen and dioxygen, multiple reaction pathways with barriers ranging from 0.37 to 2.43 eV have been revealed by X-ray photoelectron spectroscopy, electron paramagnetic resonance, and density functional theory simulation. These catalytic reaction phenomena have been explained by an extended Mars–van Krevelen mechanism, in which multiple pathways with various barriers were overcome by the electrons in the plasma with a uniform and broad distribution probability. This work provides an efficient strategy for the conversion and utilization of mechanical energy for chemical synthesis.
The development of novel catalysts with high-activity to improve the thermal-induced pyrolysis of energetic molecular perovskite is of great importance. In this work, flower-like MnO 2 nanostructure was fabricated by a facile hydrothermal method with KMnO 4 as only precursor, and its thermal-induced pyrolysis performance of energetic molecular perovskite DAP-4 was studied. Results showed the catalysis thermal-induced pyrolysis peak temperature of DAP-4 had reduced by 50 °C from 386 °C (raw DAP-4) to 336 °C (DAP-4/10 wt% MnO 2 ) by the flower-like MnO 2 nanostructure , with rich oxygen vacancy added. The heat release of DAP-4 thermal-induced pyrolysis processes had a trend of increasing from 3423 J/g to 3563 J/g first and then decreasing to 2223 J/g. The apparent activation energy of DAP-4 had been reduced to 144 kJ/mol with addition of 10 wt% MnO 2 . The catalysis mechanism of MnO 2 with flower-like nanostructure on thermal-induced pyrolysis of DAP-4 was provided.
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