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Finely Composition-Tunable Synthesis of Ultrafine Wavy PtRu Nanowires as Effective Electrochemical Sensors for Dopamine Detection Weiyue Zhao, Bing Ni, Qiang Yuan, Ye Wang, Qinghong Zhang, and Xun Wang Langmuir, Just Accepted Manuscript • DOI: 10.1021/acs.langmuir.7b01274 • Publication Date (Web): 28 Jul 2017 Downloaded from http://pubs.acs.org on July 30, 2017
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Finely Composition-Tunable Synthesis of Ultrafine Wavy PtRu Nanowires as Effective Electrochemical Sensors for Dopamine Detection Weiyue Zhaoa, Bing Nib, Qiang Yuan*a, Ye Wangc, Qinghong Zhangc, and Xun Wang*b a
Department of Chemistry, College of Chemistry and Chemical Engineering, Guizhou University, Guiyang, Guizhou province 550025, P. R. China. b Department of Chemistry, Tsinghua University, Beijing 100084, P.R. China. c State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China. Supporting Information
ABSTRACT: Preparing Pt–based one-dimensional (1D) ultrafine nanowires with abundant structural defects/grain boundaries and exploring their novel applications have attracted great interest in real-world applications. Here we introduce an environmentally friendly, facile aqueous solution approach to directly prepare a series of sub-3.0 nm PtRu ultrafine wavy nanowires. Characterizations show that the PtRu nanowires are alloy polycrystalline structures with abundant structural defects/grain boundaries. We firstly introduce the as-synthesized PtRu nanowires into electrochemical biosensors for the detection of DA and find that the Pt7Ru3 nanowires exhibit excellent electrocatalytic activity to DA with fast response, ultralow limit of detection and excellent selectivity at a potential of 0.3 V in 0.1 M phosphate buffered solution (pH=7.2). This study shows an effective approach to the development of ultrafine PtRu nanowires as electrocatalysts for electrochemical nonenzymatic dopamine biosensors.
INTRODUCTION Today, the synthesis of Pt-based one-dimensional (1D) nanowires has been paid great attention because their inherent anisotropic nature can result in many impressive performances.1-6 In addition, 1D nanowires have many other merits such as improving electron-transport and mass-transport characteristics and being self-supporting electrocatalysts that avoids support corrosion.7-9 Meanwhile, the size and composition also intrinsically determine the catalytic performance of catalysts because size reduction can help increase unit mass utilization of Pt,10-12and Pt alloying with other transition metal (Pd, Au, Ag, Ni, Cu, Zn, Co, Rh and Ru) can help to dramatically improve the catalytic activity due to the synergic effect and electronic effect.13-26 Moreover, pioneer researches have shown that the structural defects/grain boundaries have crucial effect on the catalytic performance of metal nanostructures.27-33 Therefore, rational design and synthesis of Pt-based ultrafine 1D alloy nanowires with abundant structural defects/grain boundaries are really desirable and of great importance in nanoscale science and technology. Bimetallic PtRu alloy nanostructures are widely used as catalysts in hydrogenation reactions,34, 35 fuel cells36-39 and electrochemical glucose biosensors40, 41. To the best of our knowledge, however, there is no report for PtRu nanostructures to be utilized in electrochemical biosensors for the detection of dopamine (DA) thus far. DA (3, 4-dihydroxyphenyl ethylamine) serves as significant catecholamine neurotransmitter was discovered to exist in the mammalian brain in the 1950s.42 And the concentration of DA is between 0.01µM and 1µM in serum samples. A variety of diseases, such as epilepsy, Parkinsonism, schizophrenia, Alzheimer’s disease and pleasurable feelings and euphoria,43-45 will be induced when the concentration of DA is abnormal in biological fluids. Currently, the electrochemical method that would exhibit many con-
veniences and advantages to avoid the drawbacks of surfaceenhanced Raman scattering,46 colorimetry,47 chemiluminescence48 and conventional enzymatic sensors,49 is commonly used to recognize DA because DA can be easily oxidized by the catalyst-modified glassy carbon electrode (GCE).50-52 However, the sensitivity, limit of detection (LOD), selectivity and anti-poisoning performance greatly impede commercial applications in electrochemical DA sensors. Therefore, the development of new type of high-performance electrode catalyst material for electrochemical DA sensors is of tremendous importance in clinical diagnosis, biological medicine and antidoping field. In this paper, we introduce an environmentally friendly, facile aqueous solution approach to directly prepare high-yield, sub-3.0 nm PtRu ultrafine wavy nanowires with abundant structural defects/grain boundaries. The composition of these PtRu ultrafine wavy nanowires can be finely tailored in a wide range from Pt10Ru0 to Pt4Ru6, which allows to investigate the correlation among composition and catalytic performance. This is the first report on the quantitative synthesis of ultrafine PtRu bimetallic nanowires according to feeding metal ratio of Pt to Ru in a relatively wide range. Furthermore, we also synthesized the pure Pt ultrafine wavy nanowires under the same conditions, and the size was similar to that of PtRu. We firstly introduced the as-synthesized PtRu ultrafine wavy nanowires into electrochemical biosensors for the detection of DA and found that the PtRu nanowires exhibited excellent electrocatalytic activity to DA with fast response, ultralow limit of detection (LOD) and excellent selectivity. Meanwhile, the PtRu nanowires displayed a composition-dependent catalytic property towards DA oxidation and had much higher sensitivity compared to pure Pt nanowires.
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5b. The current changes are in a good linear relationship with the successive additions of DA on all of the nanowires. The slope on all of PtRu nanowires was steeper than that on Pt nanowires and the slope on Pt7Ru3 was the steepest, which corresponded to the highest sensitivity of Pt7Ru3 nanowires for the detection of DA among all of catalysts. The linear regression equation on Pt7Ru3 was IDA = 0.1086 + 0.1998CDA (R=0.99385) and that on Pt nanwires was IDA = 0.01536+ 0.0482CDA (R=0.99872), (where IDA and CDA stand for the current density (µAµg-1Ptcm-2) and the concentration (µM) of DA, respectively), which clearly show that the Pt7Ru3 nanowires displayed tremendously enhanced sensitivity compared to Pt nanowires (Figure S5). Moreover, after DA test, the Pt7Ru3 nanowires can still maintain the wire structure (Figure S6).
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also in a good linear relationship (Figure 5d). The linear regression equation was IDA = 0.03524 + 0.2069CDA with a correlation coefficient of R = 0.98775. Because glucose (Glu), uric acid (UA) and ascorbic acid (AA) often coexist with DA in human metabolism and can lead to serious interference for electrochemical DA biosensor. In order to investigate the capacity of resisting disturbance of the Pt7Ru3 nanowires, we firstly chose relatively high concentrations of biomolecules (namely, 4.0 µM Glu, 4.0 µM UA, 4.0 µM AA and 4.0 µM DA). In addition to the above biomolecules, the interference of inorganic salts such as Na2SO4 and NaNO3 was also tested. The amperometric current response was carried out through continuously adding interference factors one by one. As shown in Figure 5e, the amperometric current response of DA was much stronger than these interference factors, the addition of interference factors (Na2SO4, NaNO3, Glu, UA and AA) did not result in any interference in the detection of DA, which showed an excellent selectivity to DA on Pt7Ru3 nanowires. Furthermore, we also checked the capacity of resisting disturbance of the Pt7Ru3 nanowires at low DA concentration of 0.2 µM and the concentration of Glu, UA and AA is respectively 1.0µM that was 5.0-times concentration of DA. It can be seen that the Pt7Ru3 nanowires still exhibited excellent selectivity to DA under such test condition (Figure 5f).
CONCLUSIONS
Figure 5. Current densities versus time curve for different concentrations of DA at 0.3V (a, c) and the corresponding calibration curve of the current density versus the DA concentration (b, d). (e) Current response to the injection of 4.0 µM DA (1st), 4.0 µM SO42-, 4.0 µM NO3-, 4.0 µM Glu, 4.0 µM UA, 4.0 µM AA and 4.0 µM DA(2nd). (f) Current response to the injection of 0.2 µM DA, 1.0 µM Glu, 1.0 µM AA, 1.0 µM UA and 0.4 µM DA.
Besides sensitivity and linear range, the limit of detection (LOD) and selectivity also have crucial effect on the actual commercial application of electrochemical DA biosensor. Figure 5c showed the amperometric current response of low concentration of DA from 0.05 to 2.0 µM on Pt7Ru3 nanowires. It can be seen there was an obvious amperometric current response even though the concentration of DA decreased down to 0.05µM, which indicated that there was an ultralow LOD on Pt7Ru3 nanowires for DA. To the best of our knowledge, this study on DA biosensor exhibit the ultralow LOD compared to previous reported DA biosensor (Table S2). Furthermore, within this concentration range of DA, the current changes are
In conclusion, we have developed ultrafine 1D PtRu wavy nanowires with abundant structural defects/grain boundaries. The composition of PtRu nanowires can be finely controlled in a wide range under current synthesis approach. The study on formation mechanism shows the nanowires grow from primary nanoparticles through oriented attachment. For the first time, we introduce the PtRu nanowires as electrocatalysts into electrochemical DA biosensor. The as-synthesized PtRu nanowires have displayed a composition-dependent catalytic activity towards DA oxidation. The Pt7Ru3 nanowires exhibit the best catalytic performance. The impressive limit of detection can be down to 50 nM with high current sensitivity up to 29.0µAmg-1Ptcm-2. Moreover, The Pt7Ru3 nanowires show an excellent selectivity to DA with a fast response. Thus, this work provides not only a facile approach to finely composition-controllable synthesis of ultrafine PtRu bimetallic nanowires but also a new type of electrocatalyst materials for electrochemical DA biosensor.
ASSOCIATED CONTENT Supporting Information. Experimental details, EDX profiles, TEM, HRTEM, i-t and tables.
AUTHOR INFORMATION Corresponding Author *E-mail:
[email protected];
[email protected] Notes The authors declare no competing financial interest.
ACKNOWLEDGMENT This work was supported by the National Natural Science Foundation of China (21361005, 21571038, 21433008, 91545203, 91127040 and 21221062).
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we have developed ultrafine 1D PtRu wavy nanowires with abundant structural defects/grain boundaries for the detection of dopamine.
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