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1.
ACS Appl Mater Interfaces ; 16(13): 16106-16119, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38427537

RESUMO

Catalysis involving gold supported on metal oxides has undergone extensive examination. However, the nature of the catalytic site under actual reaction conditions and the role of the support continue to be vigorously debated. This study addresses these issues through experimental investigations and theoretical simulations. We explore a novel catalytic mechanism that employs dynamic single-atom catalysis for the hydrochlorination of acetylene. This catalytic mechanism occurs in defective ZrO2-supported Au-Zr single-atom alloys. Specifically, the dynamic single-atom catalysis is a result of the mobility of the gold cation, which is accelerated by Cl radicals and strongly couples with the abundant unsaturated surface sites of ZrO2 in a synergistic manner. As a result, the Au electronic structure dynamically evolves, leading to a decrease in the addition reaction energy barrier. Notably, the Au cation can detach from the Au-Zr alloy structure to catalyze the hydrochlorination of acetylene near the Zr-Ov-Zr sites and then reintegrate back into the Au-Zr alloy structure upon completion of the reaction. This study underscores the significance of dynamic active sites under reaction conditions and their pivotal role in catalysis.

2.
Commun Chem ; 5(1): 2, 2022 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-36697741

RESUMO

Vinyl chloride, the monomer of polyvinyl chloride (PVC), is industrially synthesized via acetylene hydrochlorination. Thereby, easy to sublimate but toxic mercury chloride catalysts are widely used. It is imperative to find environmentally friendly non-mercury catalysts to promote the green production of PVC. Low-cost copper-based catalysts are promising candidates. In this study, phosphorus-doped Cu-based catalysts are prepared. It is shown that the type of phosphorus configuration and the distribution on the surface of the carrier can be adjusted by changing the calcination temperature. Among the different phosphorus species, the formed P-C bond plays a key role. The coordination structure formed by the interaction between P-C bonds and atomically dispersed Cu2+ species results in effective and stable active sites. Insights on how P-C bonds activate the substrate may provide ideas for the design and optimization of phosphorus-doped catalysts for acetylene hydrochlorination.

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