Noble-metal alloys are widely used as heterogeneous catalysts. However, due to the existence of scaling properties of adsorption energies on transition metal surfaces, the enhancement of catalytic activity is frequently accompanied by side reactions leading to a reduction in selectivity for the target product. Herein, we describe an approach to breaking the scaling relationship for propane dehydrogenation, an industrially important reaction, by assembling single atom alloys (SAAs), to achieve simultaneous enhancement of propylene selectivity and propane conversion. We synthesize γ-alumina-supported platinum/copper SAA catalysts by incipient wetness co-impregnation method with a high copper to platinum ratio. Single platinum atoms dispersed on copper nanoparticles dramatically enhance the desorption of surface-bounded propylene and prohibit its further dehydrogenation, resulting in high propylene selectivity (~90%). Unlike previous reported SAA applications at low temperatures (<400 °C), Pt/Cu SAA shows excellent stability of more than 120 h of operation under atmospheric pressure at 520 °C.
This review describes recent advances in the propane dehydrogenation process in terms of emerging technologies, catalyst development and new chemistry.
The concept of aggregation-induced emission (AIE) has been exploited to render non-luminescent Cu(I) SR complexes strongly luminescent. The Cu(I) SR complexes underwent controlled aggregation with Au(0) . Unlike previous AIE methods, our strategy does not require insoluble solutions or cations. X-ray crystallography validated the structure of this highly fluorescent nanocluster: Six thiolated Cu atoms are aggregated by two Au atoms (Au2 Cu6 nanoclusters). The quantum yield of this nanocluster is 11.7 %. DFT calculations imply that the fluorescence originates from ligand (aryl groups on the phosphine) to metal (Cu(I) ) charge transfer (LMCT). Furthermore, the aggregation is affected by the restriction of intramolecular rotation (RIR), and the high rigidity of the outer ligands enhances the fluorescence of the Au2 Cu6 nanoclusters. This study thus presents a novel strategy for enhancing the luminescence of metal nanoclusters (by the aggregation of active metal complexes with inert metal atoms), and also provides fundamental insights into the controllable synthesis of highly luminescent metal nanoclusters.
A probability-based computational screening study has successfully identified an optimal bimetallic alloy (Pt3In) for the propane dehydrogenation reaction.
Tailoring the nanocluster at an atomic level leads to a tetrahedron-shaped FCC Pt1Ag28(S-Adm)18(PPh3)4 nanocluster and a large enhancement in photoluminescence.
Supported vanadium oxides are one of the most promising alternative catalysts for propane dehydrogenation (PDH) and efforts have been made to improve its catalytic performance. However, unlike Pt-based catalysts, the nature of the active site and surface structure of the supported vanadium catalysts under reductive reaction conditions still remain elusive. This paper describes the surface structure and the important role of surface-bound hydroxyl groups on VO / γ-Al O catalysts under reaction conditions employing in situ DRIFTS experiments and DFT calculations. It is shown that hydroxyl groups on the VO /Al O catalyst (V-OH) are produced under H pre-reduction, and the catalytic performance for PDH is closely connected to the concentration of V-OH species on the catalyst. The hydroxyl groups are found to improve the catalyst that leads to better stability by suppressing the coke deposition.
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