Great enthusiasm in single-atom catalysts for various catalytic reactions continues to heat up. However, the poor activity of the existing single/dual-metal-atom catalysts does not meet the actual requirement. In this scenario, the precise design of triple-metal-atom catalysts is vital but still challenging. Here, a triple-atom site catalyst of FeCoZn catalyst coordinated with S and N, which is doped in the carbon matrix (named FeCoZn-TAC/SNC), is designed. The FeCoZn catalyst can mimic the activity of oxidase by activating O 2 into • O 2 − radicals by virtue of its atomically dispersed metal active sites. Employing this characteristic, triple-atom catalysts can become a great driving force for the development of novel biosensors featuring adequate sensitivity. First, the property of FeCoZn catalyst as an oxidase-like nanozyme was explored. The obtained FeCoZn-TAC/SNC shows remarkably enhanced catalytic performance than that of FeCoZn-TAC/NC and single/dual-atom site catalysts (FeZn, CoZn, FeCo-DAC/NC and Fe, Zn, Co-SAC/NC) because of trimetallic sites, demonstrating the synergistic effect. Further, the utility of the oxidase-like FeCoZn-TAC/SNC in biosensor field is evaluated by the colorimetric sensing of ascorbic acid. The nanozyme sensor shows a wide concentration range from 0.01 to 90 μM and an excellent detection limit of 6.24 nM. The applicability of the nanozyme sensor in biologically relevant detection was further proved in serum. The implementation of TAC in colorimetric detection holds vast promise for further development of biomedical research and clinical diagnosis.
Air pollution is a serious problem. Refractory thiophene sulfides, which cause air pollution, bring great challenges to their rapid and accurate identification. In this work, we propose a fluorescent sensor array based on two perovskite nanocrystals (CsPbBr 3 NCs and CsPbBr 3 /SiO 2 NCs) to distinguish different thiophene sulfides. The hydrogen bonding force between the thiophenics of thiophene sulfides and the amino groups of the perovskite NCs results in the weakening of the fluorescence signals of the perovskite NCs. The diverse interactions between thiophene sulfides and two perovskite NCs provide rich information, which can be obtained on the sensor array and identified by linear discriminant analysis. Five thiophene sulfides (i.e., benzothiophene, dibenzothiophene, 2-methylbenzothiophene, 3-methylthiophene, and thiophene) were discriminated by the sensor array at concentrations of 10−50 ppm. The effectiveness of the sensor array was further verified in the discrimination of blinded samples, in which all 10 samples were correctly identified. In addition, it is gratifying that even binary mixtures of thiophene sulfides could be distinguished by the proposed sensor array.
Recently, single-atom catalysts are attracting much attention in sensor field due to their remarkable peroxidase-or oxidase-like activities. Herein, peroxidase-like FeCoZn triple-atom catalyst supported on S-and N-doped carbon derived from ZIF-8 (FeCoZn-TAC/SNC) serves as a proof-of-concept nanozyme. In this paper, a dual-channel nanozyme-based colorimetric sensor array is presented for identifying seven preservatives in food. Further experiments reveal that the peroxidase-like activity of the FeCoZn TAzyme enables it to catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) and o-phenylenediamine (OPD) in the presence of H 2 O 2 , yielding the blue oxTMB and yellow oxOPD, respectively. However, food preservatives are adsorbed on the nanozyme surface through π-π stacking interaction and hydrogen bond, and the reduction in catalytic activity of FeCoZn TAzyme causes differential colorimetric signal variations, which provide unique "fingerprints" for each food preservative.
Although great achievements have been made in the study of artificial enzymes, the design of nanozymes with high catalytic activities of natural enzymes and the further establishment of sensitive biosensors still remain challenging. Here, two nanozymes, i.e., ZnCoFe three-atom nanozyme (TAzyme) and Sn single-atom nanozyme (SAzyme)/Ti3C2T x , are developed, which show peroxidase-like catalytic activities by catalyzing the reaction of hydrogen peroxide (H2O2), 4-aminoantipyrine (4-AAP), and phenolic acids to generate colorimetric reactions. The involvement of different phenolic acids leads to the generation of different color products. These subtle color-variation profiles between these phenolic acids prompt us to exploit an electronic tongue based on the two nanozymes to distinguish phenolic acids. Data interpretation by the pattern recognition method, such as linear discriminant analysis (LDA), displays good clustering separation of six different phenolic acids at concentrations of 0.1 μM to 1 mM, validating the effectiveness of the colorimetric nanozyme sensor array.
The effective recognition of antioxidants is considered to have far-reaching significance in medical diagnosis. Here, an efficient visual sensing strategy is developed to identify multiple antioxidants, which takes advantage of the etching of two gold nanomaterials (i.e., Au nanorods (Au NRs) and Au nanobipyramids (Au NBPs)) by the oxidation product (TMB2+) of tetramethylbenzidine (TMB). TMB is oxidized to TMB2+, catalyzed by horseradish peroxidase (HRP), and TMB2+ can etch Au NRs and Au NBPs, resulting in the changes in the wavelength and color of the solution. Various antioxidants react with TMB2+ to varying degrees, resulting in different amounts of remaining TMB2+ and causing different degrees of Au etching, which realized the discrimination and determination of the eight antioxidants with a limit of detection of 100 nM. Importantly, our sensor array also showed excellent practical application capability in human serum samples.
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