Pickering Emulsion Interfacial Engineering Synergized with Bimetallic Electronic Modulation for Selective...

Area of Science:

• Heterogeneous catalysis
• Supramolecular chemistry
• Materials science

Background:

• Achieving high activity and selectivity in heterogeneous hydrogenation of multifunctional substrates is challenging.
• Developing efficient catalytic systems for selective chemical transformations is crucial.

Purpose of the Study:

• To present a strategy for selective hydrogenation of p-chloronitrobenzene (p-CNB) by modulating the interfacial microenvironment and electronic structure of active sites.
• To investigate a synergistic catalytic mechanism involving Pickering emulsion interfaces and bimetallic catalysts.

Main Methods:

• Design and synthesis of a functionalized quaternary ammonium polyether surfactant for Pickering emulsion formation.
• In situ anchoring of PdCu bimetallic catalysts onto the self-assembled interface.
• Systematic experiments and density functional theory (DFT) calculations to elucidate the catalytic mechanism.

Main Results:

• The Pickering emulsion interface acted as a microreactor, stabilizing intermediates and reducing activation barriers.
• PdCu bimetallic catalysts exhibited synergistic effects, with Cu incorporation suppressing dehalogenation.
• Achieved ≥99.9% conversion and 95.4% selectivity for p-chloroaniline under mild conditions with excellent recyclability.

Conclusions:

• The integrated approach of Pickering emulsion interfacial engineering and bimetallic electronic modulation provides new insights for constructing efficient interfacial catalytic systems.
• This strategy effectively addresses the selective transformation challenges of complex substrates, breaking the activity-selectivity trade-off.