Abstract
The performance of heteronuclear clusters [AlXO3 ]+ (X=Al, AlO4 , AlMg2 O2 , AlZnO, AlAu2 , Mg, Y, VO, NbO, TaO) in activating methane has been explored by a combination of high-level quantum calculations with reported and supplementary gas-phase experiments. With different dopants in [AlXO3 ]+ , the mechanism, reactivity and selectivity towards methane activation varies accordingly. The classic HAT competes with PCET, depending on the composition of intramolecular interactions. Although the existence of terminal oxygen radical is beneficial for classic HAT, the Alt -C interaction in the [AlXO3 ]+ clusters as enhanced by the strongly electronegative doping groups (X=Al, AlZnO, Mg, Zn, VO, NbO, TaO) favors the PCET process, facilitating C-H bond breaking. In addition, with different dopants, the destiny of the split methyl group varies accordingly. While strong interaction between Alt and CH3 results in the formation of the Alt -C bond, dopants with variable valance may promote the formation of deep-oxidation products like formaldehyde. It has been discussed in detail how to regulate the activity and selectivity of the active center of the catalyst via rational doping.
Published Version
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