Mechanism of pH-switchable peroxidase and catalase-like activities of gold, silver, platinum and palladium

Abstract Despite being increasingly used as artificial enzymes, little has been known for the origin of the pH-switchable peroxidase-like and catalase-like activities of metals. Using calculations and experiments, we report the mechanisms for both activities and their pH-switchability for metals Au,...

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Bibliographic Details
Published in:Biomaterials 2015-04, Vol.48, p.37-44
Main Authors: Li, Junnan, Liu, Wenqi, Wu, Xiaochun, Gao, Xingfa
Format: Article
Language:English
Subjects:
Adsorption
Advanced Basic Science
Catalase - chemistry
Catalysts
Density-functional calc
Dentistry
Enzymes
Gold
Gold - chemistry
Hydrogen Peroxide - chemistry
Hydrogen-Ion Concentration
Mathematical analysis
Metals
Palladium
Palladium - chemistry
Peroxidase - chemistry
Platinum
Platinum - chemistry
Reaction mechanisms
Silver
Silver - chemistry
Surface
Surface chemistry
Surface Properties
Surgical implants
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Summary:Abstract Despite being increasingly used as artificial enzymes, little has been known for the origin of the pH-switchable peroxidase-like and catalase-like activities of metals. Using calculations and experiments, we report the mechanisms for both activities and their pH-switchability for metals Au, Ag, Pd and Pt. The calculations suggest that both activities are intrinsic properties of metals, regardless of the surfaces and intersections of facets exposed to environments. The pre-adsorbed OH groups on the surfaces, which are only favorably formed in basic conditions, trigger the switch between both activities and render the pH-switchability. The adsorption energies between H2 O2 and metals can be used as convenient descriptors to predict the relative enzyme-like activities of the metals with similar surface morphologies. The results agree with the enzyme-mimic activities that have been experimentally reported for Au, Ag, Pt and predict that Pd should have the similar properties. The prediction, as well as the predicted activity order for the four metals, has been verified by the experimental tests. The results thus provide an in-depth insight into the peroxidase-like and catalase-like activities of the metals and will guide the de novo design, synthesis and application of artificial enzymes based on inorganic materials.
ISSN:0142-9612
1878-5905
DOI:10.1016/j.biomaterials.2015.01.012