Tiantong Zhang, Bao Wang, Yao Nian, Menghui Liu, Yiming Jia, Jinli Zhang* and You Han*,
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引用次数: 4
Abstract
Active sites on ligand-enhanced Cu-based catalysts for acetylene hydrochlorination have not been clearly identified yet due to their complex nature and dynamic evolution under working conditions. Herein, we correlate experimental measurements with theoretical simulations to show that the indirect ligand-coordinated sites induced by excess copper chloride are superior. The catalyst experimentally exhibits a unique dual nature that the catalytic activity could be inhibited or boosted by changing the ratio of copper chloride and ligand. By adopting molecular dynamics simulation to obtain the dynamic evolution of active sites, coupled with density functional theory calculations, we show that excess copper chloride molecules spontaneously assemble into chain structures, thus inducing indirect ligand-coordinated sites which together with the electron transfer along the copper chloride chain are crucial for the high catalytic activity. This knowledge provides fundamental insights into the origin of activity in Cu-ligand catalysts for acetylene hydrochlorination and the identification of active sites in complex catalytic systems.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.