Exploring the interaction between two neighbouring monomers has great potential to significantly raise the performance and deepen the mechanistic understanding of heterogeneous catalysis. Herein, we demonstrate that the synergetic interaction between neighbouring Pt monomers on MoS greatly enhanced the CO hydrogenation catalytic activity and reduced the activation energy relative to isolated monomers. Neighbouring Pt monomers were achieved by increasing the Pt mass loading up to 7.5% while maintaining the atomic dispersion of Pt. Mechanistic studies reveal that neighbouring Pt monomers not only worked in synergy to vary the reaction barrier, but also underwent distinct reaction paths compared with isolated monomers. Isolated Pt monomers favour the conversion of CO into methanol without the formation of formic acid, whereas CO is hydrogenated stepwise into formic acid and methanol for neighbouring Pt monomers. The discovery of the synergetic interaction between neighbouring monomers may create a new path for manipulating catalytic properties.
Exploring how hydrophilicity regulates catalytic properties at the molecular level remains a grand challenge, although it has great potential to offer guidelines for developing highly efficient catalysts and deepen the mechanistic understanding of heterogeneous catalysis. Here, we provide molecular-level insight into the influence of surface hydroxyl groups on hydrophilic SiC quantum dots (QDs) on CO 2 hydrogenation. In CO 2 hydrogenation into methanol, SiC QDs exhibited higher catalytic activity and lower activation energy than commercial SiC. Mechanistic studies revealed that the surface hydroxyl species on SiC QDs was directly involved in CO 2 hydrogenation through the addition of H atoms in hydroxyl groups into CO 2 to form HCOO* as the intermediate. The unique reaction path decreased the energy barrier for the formation of HCOO*, facilitating the activation of CO 2 . Our understanding of surface hydrophilicity directly instructs the development of efficient catalysts toward CO 2 hydrogenation.
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