Coordination of few-atomic Pt clusters with Mo to boost the hydrogenation reduction of bromate

SEPARATION AND PURIFICATION TECHNOLOGY(2024)

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摘要
Here, we prepared microporous carbon (PC) supported Pt catalysts with different isolated Pt atoms and designed pathways to introduce Mo into the catalysts. Bromate (BrO3- ) was applied as the model oxyanion to evaluate the hydrogenation decontamination efficiency and catalyst activity. At a catalyst dosage of 0.05 g l- 1, BrO3- was reduced by 98.3 % after reaction for 30 min over Pt2-PC with Pt atomic clusters, much higher than that of single atom (Pt0.5-PC, 5.1 %) and nanoparticle (Ptn-PC, 43.2 %) counterparts. H2 was dissociated in a heterolytical manner on the highly isolated Pt active sites and the formed active H+/H- pairs dominated the removal of BrO3supported by the experimental data and density functional theory (DFT) calculation. High-valent Mo in the solution could be reduced to lower valent by consecutive active H, which further joined BrO3- reduction directly. In comparison, Mo atoms anchored on PC substrate scrambled N ligands with Pt, favoring the enrichment of BrO3- anions on the catalyst surface, thus the generated active H could react with the nearby BrO3- instantly. This study highlights the role of few-atomic Pt clusters for H2 activation and provides a strategy to boost the liquid phase catalytic hydrogenation reaction.
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关键词
Bromate,Hydrogenation reduction,Pt-PC,Mo species,Pt cluster
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