Solid Migration to Assemble a Flower-like Nanozyme with Highly Dense Single Copper Sites for Specific Phenol Oxidation

Abstract

Nanozymes with high catalytic stability and sustainability have emerged as powerful competitors to natural enzymes for diverse biocatalytic applications. However, constructing a nanozyme with high specificity is one of their biggest challenges. Herein, we develop a facile solid migration strategy to access a flower-like single copper site nanozyme (Cu SSN) via direct transformation of copper foam activated by 2-methylimidazole. With highly clustered CuN3 sites whose local structure is similar to that of natural polyphenol oxidase, the Cu SSN exhibits excellent activity and specificity to oxidize phenols without peroxidase-like activity. Furthermore, the Cu SSN shows high sensitivity in the colorimetric detection of epinephrine with a low detection limit of 0.10 μg mL–1, exceeding that of most previously reported enzyme-mimicking catalysts. This work not only provides a simple method for the large-scale preparation of high-performance nanozymes but also offers an inspiration for the design of highly specific nanozymes by mimicking the synergy among sites in natural enzymes.

Chiral CuxCoyS‐CuzS Nanoflowers with Bioinspired Enantioselective Catalytic Performances

“…The catalytic ability of L / D ‐Pen‐NFs is evaluated by the catalytic conversion of 4‐AP (4‐amino antipyrine) and 2,4‐DP (2,4‐dichlorophenol). [ 40 ] In the presence of O 2 , 2,4‐DP, and 4‐AP can generate a red product with a characteristic peak at 510 nm under the catalysis of L ‐Pen‐NF or laccase ( Figures a,b). The products catalyzed by L ‐Pen‐NFs display a deeper red color than those catalyzed by laccase (Figure S5a, Supporting Information), consistent with a higher absorption at 510 nm (Figure S5b,c, Supporting Information).…”

A comprehensive exploration of the latest innovations for advancements in enhancing selectivity of nanozymes for theranostic nanoplatforms

“…For instance, Chen et al developed a flower-like single copper site (CuN 3 ) nanozyme (Cu SSN) with exceptional activity and specificity to oxidize phenols using solid migration. 114 When abundant CuN 3 was engaged, the specific activity of Cu SSN was found to be nine times greater than that of laccase, and it demonstrated remarkable stability even in challenging environmental conditions. Yang's group developed Cu SAs/CN nanozyme with active Cu-N 4 moieties, which exhibited comparable ascorbate POD (APX) mimetic activity and fast kinetic to natural APXs.…”

Nanozymes: powerful catalytic materials for environmental pollutant detection and degradation

“…Such laccase mimic-based assays have also been developed for phenol sensing. [107][108][109][110][111][112][113][114][115][116][117][118][119][120][121][124][125][126][127][128] In a representative study, Liu's group synthesized a guanosine monophosphate (GMP) chelated Cu-based material and found that the material exhibited excellent laccase-mimicking activity. 121 They employed epinephrine as a laccase substrate and found that a colored oxidation product was formed (Fig.…”

“…[225][226][227] Recently, a lot of nanozyme catalytic systems have been developed to degrade phenolic pollutants. 107,[109][110][111][117][118][119]121,124,[228][229][230][231][232][233][234][235][236][237][238][239] In a representative example, Sun et al studied the degradation process of 17β-estradiol (E2) driven by enzyme-like MnO 2 particles in detail. 236 With the presence of humic acid (HA), four pathways of E2 transformation were revealed, including decomposition, homo-coupling, dehydrogenation, and hetero-coupling (Fig.…”

“…225–227 Recently, a lot of nanozyme catalytic systems have been developed to degrade phenolic pollutants. 107,109–111,117–119,121,124,228–239…”