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Cooperative catalysis by a single-atom enzyme-metal complex

Xiaoyang Li, Yufei Cao, Kai Luo, Lin Zhang, Yunxiu Bai, Jiarong Xiong, Richard N. Zare, Jun Ge

2022Nature Communications46 citationsDOIOpen Access PDF

Abstract

Abstract Anchoring single metal atoms on enzymes has great potential to generate hybrid catalysts with high activity and selectivity for reactions that cannot be driven by traditional metal catalysts. Herein, we develop a photochemical method to construct a stable single-atom enzyme-metal complex by binding single metal atoms to the carbon radicals generated on an enzyme-polymer conjugate. The metal mass loading of Pd-anchored enzyme is up to 4.0% while maintaining the atomic dispersion of Pd. The cooperative catalysis between lipase-active site and single Pd atom accelerates alkyl-alkyl cross-coupling reaction between 1-bromohexane and B -n-hexyl-9-BBN with high efficiency (TOF is 540 h −1 ), exceeding that of the traditional catalyst Pd(OAc) 2 by a factor of 300 under ambient conditions.

Topics & Concepts

CatalysisMetalAlkylLipaseChemistryConjugateAtom (system on chip)RadicalSelectivityCombinatorial chemistryPhotochemistryEnzymeOrganic chemistryMathematicsEmbedded systemComputer scienceMathematical analysisNanocluster Synthesis and ApplicationsCO2 Reduction Techniques and CatalystsElectrochemical sensors and biosensors