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Synthesis of carbon-supported sub-2 nanometer bimetallic catalysts by strong metal-sulfur interaction.

ABSTRACT: Small-sized bimetallic nanoparticles that integrate the advantages of efficient exposure of the active metal surface and optimal geometric/electronic effects are of immense interest in the field of catalysis, yet there are few universal strategies for synthesizing such unique structures. Here, we report a novel method to synthesize sub-2 nm bimetallic nanoparticles (Pt-Co, Rh-Co, and Ir-Co) on mesoporous sulfur-doped carbon (S-C) supports. The approach is based on the strong chemical interaction between metals and sulfur atoms that are doped in the carbon matrix, which suppresses the metal aggregation at high temperature and thus ensures the formation of small-sized and well alloyed bimetallic nanoparticles. We also demonstrate the enhanced catalytic performance of the small-sized bimetallic Pt-Co nanoparticle catalysts for the selective hydrogenation of nitroarenes.

SUBMITTER: Xu SL

PROVIDER: S-EPMC8163286 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Biodiesel is of high interest due to increased demand for energy with the concern regarding more sustainable production processes. However, an inevitable by-product is glycerol. Hence, the conversion of this by-product to higher-value chemicals, especially 1,3-propanediol (1,3-PDO) via glycerol hydrogenolysis reaction, is one of the most effective pathways towards a profitable process. In general, this process is catalyzed by a highly active Pt-based catalyst supported on γ-Al2O3. However, its low 1,3-PDO selectivity and stability due to surface deactivation of such catalysts remained. This led to the surface modification by WOx to improve both the selectivity by means of the increased Brønsted acidity and the stability in terms of Pt leaching-resistance. Hence, we applied experimental and density functional theory (DFT)-based techniques to study the fundamentals of how WOx modified the catalytic performance in the Pt/γ-Al2O3 catalyst and provided design guidelines. The effects of WOx promoter on improved activity were due to the shifting of the total density of states towards the antibonding region evident by the total density of states (TDOS) profile. On the improved 1,3-PDO selectivity, the main reason was the increasing number of Brønsted acid sites due to the added WOx promoter. Interestingly, the stability improvement was due to the strong metal-support interaction (SMSI) that occurred in the catalyst, like typical high leaching-resistant catalysts. Also, the observed strong metal-support-promoter interaction (SMSPI) is an additional effect preventing leaching. The SMSPI stemmed from additional bonding between the WOx species and the Pt active site, which significantly strengthened Pt adsorption to support and a high electron transfer from both Pt and Al2O3 to WOx promoter. This suggested that the promising promoter for our reaction performed in the liquid phase would improve the stability if SMSI occurred, where the special case of the WOx promoter would even highly improve the stability through SMSPI. Nevertheless, various promoters that can promote SMSPI need investigations.

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Synthesis of carbon-supported sub-2 nanometer bimetallic catalysts by strong metal-sulfur interaction.

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