Incorporating ATP into biomimetic catalysts for realizing exceptional enzymatic performance over a broad temperature range

Abstract

There has been great interest in the development of artificial inorganic nanomaterials that mimic natural peroxidases. Unfortunately, these nanomaterials usually possess relatively low catalytic activity and are generally considered to work effectively only within a narrow temperature range (for example, they are inactive at high temperatures). Intriguingly, adenosine triphosphate (ATP) is not only the ubiquitous energy currency of life, it is also known to form charge transfer complexes with aromatic molecules and to participate in free radical redox chemistry. Inspired by its unique properties, for the first time, we reveal a novel catalytic role for ATP and show that ATP is an ideal boosting agent for markedly improving the catalytic activity of a peroxidase mimic over a broad temperature range and, more significantly, making it possible to achieve exceptionally efficient high-temperature catalytic reactions. These observations pave the way for identifying highly effective modulators that promote the overall performance of artificial enzymes. NPG Asia Materials (2014) 6, e114; doi:10.1038/am.2014.42; published online 18 July 2014 INTRODUCTION Natural enzymes, which are biological molecules of immense catalytic force and high substrate specificity, have attracted considerable attention for use in pharmaceutical processes, agrochemical production, biosensing and food industry applications. 1-3 However, their applications are largely limited by their intrinsic properties, such as the sensitivity of catalytic activity to environmental conditions and low operational stability (owing to denaturation and digestion), as well as by the high costs of preparation and purification. 4,5 To circumvent the aforementioned limitations, tremendous efforts have been made to develop biomimetic catalysts. Among the countless examples of artificial enzymes, the emergence of and recent advances in nanotechnology and biology provide new opportunities for designing functional nanomaterials with enzyme-like characteristics. 4,[6][7][8] These materials might serve as novel and promising artificial enzymes with the advantages of facile preparation, tunability of catalytic activity and high stability under stringent conditions. Owing to the excellent catalytic properties of these nanomaterials, Scrimin and co-workers 7 called them 'nanozymes' in analogy to the nomenclature of catalytically active polymers (synzymes). Magnetic nanoparticles, 4,9 CeO 2 , 6,10-12 V 2 O 5 , 13,14 gold nanoparticles, 7,8,[15][16][17][18] PtPd ÀFe 3 O 4 , 19,20 carbon nanotubes, 21,22 graphene oxide and graphene nanocomposites 23,24 and other types of nanoparticle have been found to exhibit unique enzyme-like catalytic activities and have

A Thermophilic Tetramolecular G‐Quadruplex/Hemin DNAzyme

“…Natural proteinaceous peroxidases possess high catalytic activity but are sensitive to thermal denaturation . Although different nanomaterials have been developed to catalyze peroxidase‐type reactions at elevated temperatures, the improvements of catalytic activity and thermal stability did not meet initial expectations . In this study, a thermally stable and highly competent DNAzyme, so called thermophilic DNAzyme, with efficient peroxidase activity at high temperature is reported through a series of model reactions and the rapid oxidation of hazardous organic pollutants (Figure ).…”

“…Natural proteinaceous peroxidases possess high catalytic activity but are sensitive to thermal denaturation . Although different nanomaterials have been developed to catalyze peroxidase‐type reactions at elevated temperatures, the improvements of catalytic activity and thermal stability did not meet initial expectations .…”

Iron Oxide Nanozyme: A Multifunctional Enzyme Mimetic for Biomedical Applications

“…Like natural enzymes, IONzymes are stimulated or inhibited by some chemicals. Currently, the reported activators include ATP, ADP, AMP 42 , 43 and DNA. Notably, ATP can enhance the peroxidase-like activity at neutral pH by complexation with Fe 3 O 4 nanoparticles to participate in single electron transfer reactions 44 .…”

Guide to Selecting a Biorecognition Element for Biosensors

“…50–55 As an example, nanozymes mimic enzymatic catalytic function by interfacing with a recognition element mimic and an inorganic catalysts. 25,50,56 The nanostructured surface can have high sensitivity but poor specificity, as multiple bioanalytes can be simultaneously catalytically activated. 57–59 Even though progress has been made to improve the selectivity of biorecognition element mimics with nanozymes, this sensor paradigm remains less selective than the other discussed paradigms within this review.…”