Boosting Electrochemical Catalysis and Nonenzymatic Sensing Toward Glucose by Single‐Atom Pt Supported on Cu@CuO Core–Shell Nanowires

Abstract

Diabetes Federation. [3] For quick patient screening and medical monitoring, it is crucial to develop fast and accurate sensors for glucose detection. [4] The commercial glucose sensors are electrochemical enzymatic based, but they have limitations, such as susceptible to deterioration from environmental influence (pH, temperature, and humidity) and poor stability due to inactivation of enzymes. [5] Therefore, electrochemical nonenzymatic glucose sensors have received increasing attention for the next-generation sensing applications. One option is to use noble metals (Pt, Pd, Au, etc.) and their alloys [6][7][8][9][10][11] as modified electrodes toward electrochemical glucose sensing. However, their commercial applications are limited by high cost and scarcity. Therefore, it is critical to develop highly efficient and lowcost electrocatalysts, based on non-noble metals. [12] Previously, Ni, Co, and Cu have been extensively used for electrochemical nonenzymatic glucose sensing. [13][14][15] Especially, the Cu-based catalysts are desirable due to their low-cost, high electrical conductivity, nontoxicity, and great electrocatalytic ability toward glucose. [16] Various Cu or CuO x nanostructures, such as nanoparticles, [17] nanorods, [18] flower-like structure, [19] have shown great potential of being used in electrochemical glucose sensing, attributing to high aspect ratio and high surface area. [20,21] For rational design of new Cu-based nanomaterials for nonenzymatic glucose sensing, fundamental research is needed to understand the catalytic mechanism and its impacts on sensing performance. [22] Single-atom catalysts (SACs) belong to a class of catalysts with specific characteristics of metal single atoms immobilized on supporters, [23][24][25][26] which provide high catalytic activity and selectivity in various catalytic reactions due to their unsaturated coordination environment and unique electronic structure. [27][28][29][30][31] The 100% atom utilization of metal also maximizes atomic economy. [32] Moreover, the identified active centers and structural simplicity could be ideal model for understanding the relationship between the structure and catalytic activity, with which one can use for rational design of atomic-scale catalyst targeting at specified reaction. [33,34] In addition, the use of SACs for electrochemical sensing [35][36][37][38] is still in the early stage of development, with much questions related to the sensing It is critical to develop high-performance electrocatalyst for electrochemical nonenzymatic glucose sensing. In this work, a single-atom Pt supported on Cu@ CuO core-shell nanowires (Pt 1 /Cu@CuO NWs) for electrochemical nonenzymatic glucose sensor is designed. Pt 1 /Cu@CuO NWs exhibit excellent electrocatalytic oxidation toward glucose with 70 mV lower onset potential (0.131 V) and 2.4 times higher response current than Cu NWs. Sensors fabricated using Pt 1 / Cu@CuO NWs also show high sensitivity (852.163 µA mM −1 cm −2 ), low detection limit (3.6 µM), wide linear range (0.01-5.18 µM...

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“…Density functional theory (DFT) calculations were employed to gain further insights into the superior electrocatalytic reactivity of LIG-TiO 2 –Pt toward H 2 O 2 . Previous literature reported that the binding energy of H 2 O 2 (Δ E *) on a catalyst’s surface can be utilized to evaluate its sensing performance toward an H 2 O 2 sensor. , Hereof, the corresponding adsorption sites of H 2 O 2 on LIG-TiO 2 , LIG-Pt, and LIG-TiO 2 –Pt are shown in Figure G, indicating that the active sites are Ti, Pt, and Ti–Pt atoms, respectively. The charge density difference and Bader charge analysis (Figure H,I) point out that the Pt nanoparticle anchored on the TiO 2 surface loses more electrons (0.223 e – ), indicating a strong electronic interaction between the Pt and TiO 2 nanoparticles.…”

“…Pt (14.14 × 10 −4 S cm −1 ) exhibits a faster electron conduction capacity, which highly aligns with the abovementioned CV, EIS, i−t, and ECSA results (Figure2F).Density functional theory (DFT) calculations were employed to gain further insights into the superior electrocatalytic reactivity of LIG-TiO 2 −Pt toward H 2 O 2 . Previous literature reported that the binding energy of H 2 O 2 (ΔE*) on a catalyst's surface can be utilized to evaluate its sensing performance toward an H 2 O 2 sensor 39,40. Hereof, the corresponding adsorption sites ofH 2 O 2 on LIG-TiO 2 , LIG-Pt, and LIG-TiO 2 −Pt are shown in Figure 2G, indicating that the active sites are Ti, Pt, and Ti−Pt atoms, respectively.…”

Fe Single-Atom Carbon Dots Nanozyme Collaborated with Nucleic Acid Exonuclease III-Driven DNA Walker Cascade Amplification Strategy for Circulating Tumor DNA Detection

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“…On the other hand, the noble metal (Ag, Pt, Au, Pd, etc.) functionalization [24,25] can induce electronic and catalytic effects to greatly enhance the sensing properties of ZnO to detect TEA. The noble metals will provide a large number of active sites for the adsorption and dissociation of oxygen molecules.…”