An ultrasensitive electrochemical sensor based on polydopamine/carboxylic multi-walled carbon nanotubes(MWCNTs à COOH) nanocomposites modified glassy carbon electrode(GCE) was presented in this work, which has be...An ultrasensitive electrochemical sensor based on polydopamine/carboxylic multi-walled carbon nanotubes(MWCNTs à COOH) nanocomposites modified glassy carbon electrode(GCE) was presented in this work, which has been developed for highly selective and highly sensitive determination of an antimicrobial drug, metronidazole. The preparation of polydopamine/MWCNTs–COOH nanocomposites/GCE sensor is simple and possesses high reproducible, where polydopamine can be coated on the surface of MWCNTs–COOH via a simple electropolymerization process. Under optimized conditions, the proposed sensor showed ultrasensitive determination for metronidazole with a wide linear detection range from5 to 5000 mmol/dm^3 and a low detection limit of 0.25 mmol/dm^3(S/N=3). Moreover, the proposed sensor has been successfully applied for the quantitative determination of metronidazole in real drug samples. This work may provide a novel and effective analytical platform for determination of metronidazole in application of real pharmaceutical and biological samples analysis.展开更多
The electrochemical behavior of a carboxyl-modified carbon nanotube films was investigated to explore its possibility in electroanalytical applicaton. Cyclic voltammetry of quinone was conducted in 1mol/L Na2SO4, whic...The electrochemical behavior of a carboxyl-modified carbon nanotube films was investigated to explore its possibility in electroanalytical applicaton. Cyclic voltammetry of quinone was conducted in 1mol/L Na2SO4, which showed a stable, quasi-reversible voltammetric response for quinone / hydroquinone, and the anodic and the cathodic peak potentials were 0.657V and -0.029V (vs. SCE) at a scan rate of 0.1V.s-1, respectively. Both anodic and cathodic peak currents depended linearly on the square root of the scan rate over the range of 0.01-0.5V.s-1, which suggested that the process of the electrode reactions was diffusion-controlled. Carboxyl-modified carbon nanotube electrodes made it possible to determine low level of dopamine selectively in the presence of a large excess of ascorbic acid in acidic media using derivative voltammetry. The results obtained were discussed in details. This work demonstrates the potential of carboxyl-modified carbon nanotube electrodes for electroanalytical applications.展开更多
Due to its properties of mutagenic,teratogenic,and carcinogenic,the detection of furazolidone(FZD)in aquaculture is of great importance for food safety and human health.In this study,molecularly imprinted fi lms modif...Due to its properties of mutagenic,teratogenic,and carcinogenic,the detection of furazolidone(FZD)in aquaculture is of great importance for food safety and human health.In this study,molecularly imprinted fi lms modifi ed with carboxylated multi-walled carbon nanotube-phosphomolybdic acid composite were used to fabricate an electrochemical sensor for the determination of FZD.The nanocomposites were characterized using infrared spectroscopy,scanning electron microscopy,energy-dispersive X-ray spectroscopy,and X-ray diff raction.The electrochemical characteristics of the modifi ed electrodes were examined using electrochemical impedance spectroscopy,cyclic voltammetry,and diff erential pulse voltammetry.The sensor exhibited exceptional catalytic performance.The calibration curves were acquired in the concentration range of 6 nmol·L^(−1)to 0.6μmol·L^(−1),with a limit of detection of 3.38 nmol·L^(−1).Additionally,the sensor proved successful in recognizing FZD in shrimp samples with satisfactory recoveries and precision.The method provides a strategy to construct a molecularly imprinted electrochemical sensing platform using nanomaterials,which has great promise in the field of food safety.展开更多
Ozone treatment is a common way to functionalize commercial multi-walled carbon nanotubes （CNTs） with various oxygen functionalities like carboxyl, phenol and lactone groups, in order to enhance their textural prope...Ozone treatment is a common way to functionalize commercial multi-walled carbon nanotubes （CNTs） with various oxygen functionalities like carboxyl, phenol and lactone groups, in order to enhance their textural properties and chemical activity. In order to detail the effect of each functional group, we correlated the activity with the surface density of each group, and found that the carboxyl groups play a pivotal role in two important catalytic reactions, namely the electrochemical oxygen reduction reaction （ORR） and agar conversion to 5-hydroxymethylfurfural （HMF）. During the processes, the hydrophilic surface provides a strong affinity for reaction substrates while the improved porosity allows the efficient diffusion of reactants and products. Furthermore, the activity of functionalized CNTs for agar conversion remained almost unchanged during nine cycles of reaction. This work highlights a strategy for improving the activity of CNTs for electrochemical ORR and agar conversion reactions, as well a promising application of carboxyl-rich CNTs as a solid acid catalyst to produce high-purity HMF--an important chemical intermediate.展开更多
A novel type of carboxylated multiwalled carbon nanotube modified electrode（c-MWCNTs/GCE） was constructed and the electrochemical properties of phenacetin（PHE） at it were studied. In a buffer solution of 0.1 mol/L...A novel type of carboxylated multiwalled carbon nanotube modified electrode（c-MWCNTs/GCE） was constructed and the electrochemical properties of phenacetin（PHE） at it were studied. In a buffer solution of 0.1 mol/L HAc-NaAc（pH=5.3）, PHE exhibited a couple of quasi-reversible redox peaks and an anodic peak in the poten- tial range of 0.2--1.2 V at c-MWCNTs/GCE. The peak current was proportional to the concentration of PHE in the range of 4.0× 10^-6_ 1.0 × 10^-4 mol/L with a detection limit of 1.0× 10^-6 mol/L（S/N=3）. The c-MWCNTs/GCE showed excellent repeatability and stability and the electrochemical reaction mechanism of PHE was proposed. This method was used to determine the content of PHE in medical tablets and the recovery was determined to be 96.5%--104.2% by means of a standard addition method.展开更多
Since most electrocatalysts for oxygen evolution reaction(OER),except for precious metal oxides RuO_(2) and IrO_(2),are unstable in harsh acidic solutions,it is highly desirable to develop high-performance OER electro...Since most electrocatalysts for oxygen evolution reaction(OER),except for precious metal oxides RuO_(2) and IrO_(2),are unstable in harsh acidic solutions,it is highly desirable to develop high-performance OER electrocatalysts for acidic media,though it is still a big challenge.Herein,we report a simple strategy to produce carboxyl-enriched multiwalled carbon nanotubes(COOH-MWNTs)that exhibit stable and high electrocatalytic activities for OER in acidic solutions,showing an overpotential at a current density of 10 mA cm^(–2) and a Tafel slope as low as of 265 mV and 82 mV dec^(–1),respectively.As far as we are aware,these results represent the best OER performance for metal-free electrocatalysts,even comparable to those of RuO_(2) and IrO_(2).We have further revealed the catalytic mechanism,which involves one electron lose from the COOH-MWNTs catalyst at the beginning of the OER process to trigger H_(2)O molecule oxidation by forming peralcohol,followed by the recapture of one electron from water molecule to oxidize water and to recover the initial state for the COOH-MWNTs catalyst.The unravel of this new OER mechanism is important as it provides new insights into the crucial role of organic functional groups in electrocatalytic processes.Also,the mechanistic understanding can be used to guide the design and development of novel metalfree catalysts for acidic OER electrocatalysis and beyond.展开更多
A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage system...A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage systems.Herein,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical performance.Experiments and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at interfaces.This device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as seawater.In particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal display.This work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant Nos.21475046,21427809)
文摘An ultrasensitive electrochemical sensor based on polydopamine/carboxylic multi-walled carbon nanotubes(MWCNTs à COOH) nanocomposites modified glassy carbon electrode(GCE) was presented in this work, which has been developed for highly selective and highly sensitive determination of an antimicrobial drug, metronidazole. The preparation of polydopamine/MWCNTs–COOH nanocomposites/GCE sensor is simple and possesses high reproducible, where polydopamine can be coated on the surface of MWCNTs–COOH via a simple electropolymerization process. Under optimized conditions, the proposed sensor showed ultrasensitive determination for metronidazole with a wide linear detection range from5 to 5000 mmol/dm^3 and a low detection limit of 0.25 mmol/dm^3(S/N=3). Moreover, the proposed sensor has been successfully applied for the quantitative determination of metronidazole in real drug samples. This work may provide a novel and effective analytical platform for determination of metronidazole in application of real pharmaceutical and biological samples analysis.
文摘The electrochemical behavior of a carboxyl-modified carbon nanotube films was investigated to explore its possibility in electroanalytical applicaton. Cyclic voltammetry of quinone was conducted in 1mol/L Na2SO4, which showed a stable, quasi-reversible voltammetric response for quinone / hydroquinone, and the anodic and the cathodic peak potentials were 0.657V and -0.029V (vs. SCE) at a scan rate of 0.1V.s-1, respectively. Both anodic and cathodic peak currents depended linearly on the square root of the scan rate over the range of 0.01-0.5V.s-1, which suggested that the process of the electrode reactions was diffusion-controlled. Carboxyl-modified carbon nanotube electrodes made it possible to determine low level of dopamine selectively in the presence of a large excess of ascorbic acid in acidic media using derivative voltammetry. The results obtained were discussed in details. This work demonstrates the potential of carboxyl-modified carbon nanotube electrodes for electroanalytical applications.
基金Supported by the National Natural Science Foundation of China(Grant No.22271119).
文摘Due to its properties of mutagenic,teratogenic,and carcinogenic,the detection of furazolidone(FZD)in aquaculture is of great importance for food safety and human health.In this study,molecularly imprinted fi lms modifi ed with carboxylated multi-walled carbon nanotube-phosphomolybdic acid composite were used to fabricate an electrochemical sensor for the determination of FZD.The nanocomposites were characterized using infrared spectroscopy,scanning electron microscopy,energy-dispersive X-ray spectroscopy,and X-ray diff raction.The electrochemical characteristics of the modifi ed electrodes were examined using electrochemical impedance spectroscopy,cyclic voltammetry,and diff erential pulse voltammetry.The sensor exhibited exceptional catalytic performance.The calibration curves were acquired in the concentration range of 6 nmol·L^(−1)to 0.6μmol·L^(−1),with a limit of detection of 3.38 nmol·L^(−1).Additionally,the sensor proved successful in recognizing FZD in shrimp samples with satisfactory recoveries and precision.The method provides a strategy to construct a molecularly imprinted electrochemical sensing platform using nanomaterials,which has great promise in the field of food safety.
文摘Ozone treatment is a common way to functionalize commercial multi-walled carbon nanotubes （CNTs） with various oxygen functionalities like carboxyl, phenol and lactone groups, in order to enhance their textural properties and chemical activity. In order to detail the effect of each functional group, we correlated the activity with the surface density of each group, and found that the carboxyl groups play a pivotal role in two important catalytic reactions, namely the electrochemical oxygen reduction reaction （ORR） and agar conversion to 5-hydroxymethylfurfural （HMF）. During the processes, the hydrophilic surface provides a strong affinity for reaction substrates while the improved porosity allows the efficient diffusion of reactants and products. Furthermore, the activity of functionalized CNTs for agar conversion remained almost unchanged during nine cycles of reaction. This work highlights a strategy for improving the activity of CNTs for electrochemical ORR and agar conversion reactions, as well a promising application of carboxyl-rich CNTs as a solid acid catalyst to produce high-purity HMF--an important chemical intermediate.
基金Supported by the National Natural Science Foundation of China（Nos.41063007, 21365004）, the Natural Science Foundation of Guangxi Zhuang Autonomous Region, China（Nos.2010GXNSFB013001, 2013GXNSFDA019006） and the Project of the Edu- cation Department of Guangxi Zhuang Autonomous Region, China（No.201103YB130）.
文摘A novel type of carboxylated multiwalled carbon nanotube modified electrode（c-MWCNTs/GCE） was constructed and the electrochemical properties of phenacetin（PHE） at it were studied. In a buffer solution of 0.1 mol/L HAc-NaAc（pH=5.3）, PHE exhibited a couple of quasi-reversible redox peaks and an anodic peak in the poten- tial range of 0.2--1.2 V at c-MWCNTs/GCE. The peak current was proportional to the concentration of PHE in the range of 4.0× 10^-6_ 1.0 × 10^-4 mol/L with a detection limit of 1.0× 10^-6 mol/L（S/N=3）. The c-MWCNTs/GCE showed excellent repeatability and stability and the electrochemical reaction mechanism of PHE was proposed. This method was used to determine the content of PHE in medical tablets and the recovery was determined to be 96.5%--104.2% by means of a standard addition method.
基金support from the Hydrogeological Survey Project of Huangshui River(No.DD20190331)We are also grateful for the partial support by Australian Research Council(DP 190103881 and FL 190100126).
文摘Since most electrocatalysts for oxygen evolution reaction(OER),except for precious metal oxides RuO_(2) and IrO_(2),are unstable in harsh acidic solutions,it is highly desirable to develop high-performance OER electrocatalysts for acidic media,though it is still a big challenge.Herein,we report a simple strategy to produce carboxyl-enriched multiwalled carbon nanotubes(COOH-MWNTs)that exhibit stable and high electrocatalytic activities for OER in acidic solutions,showing an overpotential at a current density of 10 mA cm^(–2) and a Tafel slope as low as of 265 mV and 82 mV dec^(–1),respectively.As far as we are aware,these results represent the best OER performance for metal-free electrocatalysts,even comparable to those of RuO_(2) and IrO_(2).We have further revealed the catalytic mechanism,which involves one electron lose from the COOH-MWNTs catalyst at the beginning of the OER process to trigger H_(2)O molecule oxidation by forming peralcohol,followed by the recapture of one electron from water molecule to oxidize water and to recover the initial state for the COOH-MWNTs catalyst.The unravel of this new OER mechanism is important as it provides new insights into the crucial role of organic functional groups in electrocatalytic processes.Also,the mechanistic understanding can be used to guide the design and development of novel metalfree catalysts for acidic OER electrocatalysis and beyond.
基金the financial support from the National Natural Science Foundation of China(Nos.52172038 and 22179017).
文摘A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage systems.Herein,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical performance.Experiments and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at interfaces.This device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as seawater.In particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal display.This work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.
