Detection of target analytes at low concentrations is significant in various fields,including pharmaceuticals,healthcare,and environmental protection.Theophylline(TP),a natural alkaloid used as a bronchodilator to tre...Detection of target analytes at low concentrations is significant in various fields,including pharmaceuticals,healthcare,and environmental protection.Theophylline(TP),a natural alkaloid used as a bronchodilator to treat respiratory disorders such as asthma,bronchitis,and emphysema,has a narrow therapeutic window with a safe plasma concentration ranging from 55.5-111.0μmol·L^(-1)in adults.Accurate monitoring of TP levels is essential because too low or too high can cause se-rious side effects.In this regard,non-enzymatic electrochemical sensors offer a practical solution with rapidity,portability,and high sensitivity.This article aims to provide a comprehensive review of the recent developments of non-enzymatic electrochemical sensors for TP detection,highlighting the basic principles,electro-oxidation mechanisms,catalytic effects,and the role of modifying materials on electrode performance.Carbon-based electrodes such as glassy carbon electrodes(GCEs),carbon paste electrodes(CPEs),and carbon screen-printed electrodes(SPCEs)have become the primary choices for non-enzymatic sensors due to their chemical stability,low cost,and flexibility in modification.This article identifies the sig-nificant contribution of various modifying materials,including nanomaterials such as carbon nanotubes(CNTs),graphene,metal oxides,and multi-element nanocomposites.These modifications enhance sensors’electron transfer,sensitivity,and selectivity in detecting TP at low concentrations in complex media such as blood plasma and pharmaceutical samples.The electro-oxidation mechanism of TP is also discussed in depth,emphasizing the hydroxyl and carbonyl reaction pathways strongly influenced by pH and electrode materials.These mechanisms guide the selection of the appropriate electrode ma-terial for a particular application.The main contribution of this article is to identify superior modifying materials that can improve the performance of non-enzymatic electrochemical sensors.In a recent study,the combination of multi-element nanocomposites based on titanium dioxide(TiO_(2)),CNTs,and gold nanoparticles(AuNPs)resulted in the lowest detection limit of 3×10^(-5)μmol·L^(-1),reflecting the great potential of these materials for developing high-performance electrochemical sensors.The main conclusion of this article is the importance of a multidisciplinary approach in electrode material design to support the sensitivity and selectivity of TP detection.In addition,there is still a research gap in understanding TP’s more detailed oxidation mechanism,especially under pH variations and complex environments.Therefore,further research on electrode modification and analysis of the TP oxidation mechanism are urgently needed to improve the accuracy and sta-bility of the sensor while expanding its applications in pharmaceutical monitoring and medical diagnostics.By integrating various innovative materials and technical approaches,this review is expected to be an essential reference for developing efficient and affordable non-enzymatic electrochemical sensors.展开更多
In this work,a novel bifunctional zirconium dioxide@zeolitic imidazolate framework-90(ZrO_(2)@ZIF-90)nanozyme was successfully developed for the catalytic degradation and electrochemical detection of methyl parathion(...In this work,a novel bifunctional zirconium dioxide@zeolitic imidazolate framework-90(ZrO_(2)@ZIF-90)nanozyme was successfully developed for the catalytic degradation and electrochemical detection of methyl parathion(MP).The ZrO_(2)@ZIF-90 nanozyme with phosphatase hydrolysis activity can convert MP into p-nitrophenol(p-NP).The addition of ZrO_(2)riched in Lewis acid Zr(IV)sites significantly enhanced the phosphatase hydrolysis activity of ZIF-90.ZrO_(2)@ZIF-90 also displayed satisfactory electrocatalytic performance on account of the high surface area,high porosity and powerful enrichment ability of the ZIF-90 and the excellent ion transfer capacity of ZrO_(2).A ZrO_(2)@ZIF-90 nanozyme modified glassy carbon electrode(ZrO_(2)@ZIF-90/GCE)was then fabricated to analyze p-NP formed through MP degradation.Under the optimized conditions,the developed sensor displayed satisfactory analytical performance with a low limit of detection of 0.53μmol/L and two wide linear ranges(3-10 and 10-200μmol/L).ZrO_(2)@ZIF-90 nanozyme accomplished to the degradation and electrochemical detection of MP in river water and spiked fruits.This study identifies a promising new strategy for the design of bifunctional nanozymes for the detection of environmental hazards.展开更多
We report the design of a sensitive,electrochemical aptasensor for detection of ochratoxin A(OTA)with an extraordinary tunable dynamic sensing range.This electrochemical aptasensor is constructed based on the target i...We report the design of a sensitive,electrochemical aptasensor for detection of ochratoxin A(OTA)with an extraordinary tunable dynamic sensing range.This electrochemical aptasensor is constructed based on the target induced aptamer-folding detection mechanism and the recognition between OTA and its aptamers results in the conformational change of the aptamer probe and thus signal changes for measurement.The dynamic sensing range of the electrochemical aptasensor is successfully tuned by introduction of free assistant aptamer probes in the sensing system.Our electrochemical aptasensor shows an extraordinary dynamic sensing range of 11-order magnitude of OTA concentration from 10^−8 to 10^2 ng/g.Of great significance,the signal response in all OTA concentration ranges is at the same current scale,demonstrating that our sensing protocol in this research could be applied for accurate detections of OTA in a broad range without using any complicated treatment of signal amplification.Finally,OTA spiked red wine and maize samples in different dynamic sensing ranges are determined with the electrochemical aptasensor under optimized sensing conditions.This tuning strategy of dynamic sensing range may offer a promising platform for electrochemical aptasensor optimizations in practical applications.展开更多
In this study, integrated multi-wall carbon nanotube （MWCNT） electrodes were prepared in the holes of glass directly by microwave plasma chemical vapour deposition （MWPCVD）. The electrochemical behaviour of catech...In this study, integrated multi-wall carbon nanotube （MWCNT） electrodes were prepared in the holes of glass directly by microwave plasma chemical vapour deposition （MWPCVD）. The electrochemical behaviour of catechol at the integrated MWCNT electrodes was investigated. The oxygen plasma treated CNT electrodes had better electrochemical performance for the analysis of catechol than that of as-synthesized CNT electrodes. Both the as-synthesized CNTs and plasma treated CNTs were characterized by TEM（transmission electron microscopy, XPS（X-ray photoelectron spectroscopy） and Raman spectroscopy. The results revealed that the oxygen plasma activation is an effective method to enhance the electrochemical properties of CNT electrodes.展开更多
Electronic waste(e-waste)and diabetes are global challenges to modern societies.However,solving these two challenges together has been challenging until now.Herein,we propose a laser-induced transfer method to fabrica...Electronic waste(e-waste)and diabetes are global challenges to modern societies.However,solving these two challenges together has been challenging until now.Herein,we propose a laser-induced transfer method to fabricate portable glucose sensors by recycling copper from e-waste.We bring up a laser-induced full-automatic fabrication method for synthesizing continuous heterogeneous Cu_(x)O(h-Cu_(x)O)nano-skeletons electrode for glucose sensing,offering rapid(<1 min),clean,air-compatible,and continuous fabrication,applicable to a wide range of Cu-containing substrates.Leveraging this approach,h-Cu_(x)O nanoskeletons,with an inner core predominantly composed of Cu_(2)O with lower oxygen content,juxtaposed with an outer layer rich in amorphous Cu_(x)O(a-Cu_(x)O)with higher oxygen content,are derived from discarded printed circuit boards.When employed in glucose detection,the h-Cu_(x)O nano-skeletons undergo a structural evolution process,transitioning into rigid Cu_(2)O@CuO nano-skeletons prompted by electrochemical activation.This transformation yields exceptional glucose-sensing performance(sensitivity:9.893 mA mM^(-1) cm^(-2);detection limit:0.34μM),outperforming most previously reported glucose sensors.Density functional theory analysis elucidates that the heterogeneous structure facilitates gluconolactone desorption.This glucose detection device has also been downsized to optimize its scalability and portability for convenient integration into people’s everyday lives.展开更多
Effect of electrode insulation on the electric field and the flow field of the machining gap during electrochemical drilling（ECD） is numerically studied. Electric field simulation shows that the current density alon...Effect of electrode insulation on the electric field and the flow field of the machining gap during electrochemical drilling（ECD） is numerically studied. Electric field simulation shows that the current density along the side gap decreases with increasing the thickness of electrode insulation. And the analysis of the electrolyte flow in the frontal gap shows that the insulation thickness has a remarkable influence on the pressure distributions. Ex- periments investigate the influence of the insulation thickness on the main characteristics of the machined hole, i.e. , radial overcut, entrance conicity, and current stability. The poor hole is observed and identified as most likely to occur with a combination of the low tool feed rate and the low insulation thickness. The appropriate thickness of the insulating layer leads to an improvement on hole accuracy and machining stability.展开更多
In this paper, a novel method for selectively detection of dopamine(DA) in the interference of ascorbic acid(AA) is described. A nanometer-sized gold flower microelectrode(NGFME) is prepared by flame-etching and elect...In this paper, a novel method for selectively detection of dopamine(DA) in the interference of ascorbic acid(AA) is described. A nanometer-sized gold flower microelectrode(NGFME) is prepared by flame-etching and electrochemical deposition. The electrode tip was characterized by scanning electron microscope(SEM). The NGFME is sized at about 100 μm and dimensions of thorns of the electrode were in nanometers. By modifying with DA aptamer on the surface, the prepared aptasensor can selectively detect DA even in the presence of high concentration AA. Experimental results show that this NGFME has no response to AA. As a comparison, the carbon fiber electrode without DA aptamer modification is unable to effectively detect DA in the presence of AA. The NGFME is easy-to-prepare, selective and sensitive for DA detection down to 25 μM. The electrode can be expected to detect DA in vivo and in real biological samples.展开更多
基金the funding from Lembaga Penelitian dan Pengabdian Masyarakat(LPPM)Universitas Indonesia,by Riset Kolaborasi Indonesia(RKI)-World Class University(WCU)Program with grant number NKB-1067/UN2-RST/HKP.05.00/2023 and NKB-781/UN2.RST/HKP.05.00/2024.
文摘Detection of target analytes at low concentrations is significant in various fields,including pharmaceuticals,healthcare,and environmental protection.Theophylline(TP),a natural alkaloid used as a bronchodilator to treat respiratory disorders such as asthma,bronchitis,and emphysema,has a narrow therapeutic window with a safe plasma concentration ranging from 55.5-111.0μmol·L^(-1)in adults.Accurate monitoring of TP levels is essential because too low or too high can cause se-rious side effects.In this regard,non-enzymatic electrochemical sensors offer a practical solution with rapidity,portability,and high sensitivity.This article aims to provide a comprehensive review of the recent developments of non-enzymatic electrochemical sensors for TP detection,highlighting the basic principles,electro-oxidation mechanisms,catalytic effects,and the role of modifying materials on electrode performance.Carbon-based electrodes such as glassy carbon electrodes(GCEs),carbon paste electrodes(CPEs),and carbon screen-printed electrodes(SPCEs)have become the primary choices for non-enzymatic sensors due to their chemical stability,low cost,and flexibility in modification.This article identifies the sig-nificant contribution of various modifying materials,including nanomaterials such as carbon nanotubes(CNTs),graphene,metal oxides,and multi-element nanocomposites.These modifications enhance sensors’electron transfer,sensitivity,and selectivity in detecting TP at low concentrations in complex media such as blood plasma and pharmaceutical samples.The electro-oxidation mechanism of TP is also discussed in depth,emphasizing the hydroxyl and carbonyl reaction pathways strongly influenced by pH and electrode materials.These mechanisms guide the selection of the appropriate electrode ma-terial for a particular application.The main contribution of this article is to identify superior modifying materials that can improve the performance of non-enzymatic electrochemical sensors.In a recent study,the combination of multi-element nanocomposites based on titanium dioxide(TiO_(2)),CNTs,and gold nanoparticles(AuNPs)resulted in the lowest detection limit of 3×10^(-5)μmol·L^(-1),reflecting the great potential of these materials for developing high-performance electrochemical sensors.The main conclusion of this article is the importance of a multidisciplinary approach in electrode material design to support the sensitivity and selectivity of TP detection.In addition,there is still a research gap in understanding TP’s more detailed oxidation mechanism,especially under pH variations and complex environments.Therefore,further research on electrode modification and analysis of the TP oxidation mechanism are urgently needed to improve the accuracy and sta-bility of the sensor while expanding its applications in pharmaceutical monitoring and medical diagnostics.By integrating various innovative materials and technical approaches,this review is expected to be an essential reference for developing efficient and affordable non-enzymatic electrochemical sensors.
基金financially supported by the National Natural Science Foundation of China(No.31972149)Innovation Capability Improvement Project of Scientific and Technological Small and Medium-sized Enterprises in Shandong Province(No.2022TSGC2409)the Mac Diarmid Institute for Advanced Materials and Nanotechnology and the Dodd-Walls Centre for Photonic and Quantum Technologies。
文摘In this work,a novel bifunctional zirconium dioxide@zeolitic imidazolate framework-90(ZrO_(2)@ZIF-90)nanozyme was successfully developed for the catalytic degradation and electrochemical detection of methyl parathion(MP).The ZrO_(2)@ZIF-90 nanozyme with phosphatase hydrolysis activity can convert MP into p-nitrophenol(p-NP).The addition of ZrO_(2)riched in Lewis acid Zr(IV)sites significantly enhanced the phosphatase hydrolysis activity of ZIF-90.ZrO_(2)@ZIF-90 also displayed satisfactory electrocatalytic performance on account of the high surface area,high porosity and powerful enrichment ability of the ZIF-90 and the excellent ion transfer capacity of ZrO_(2).A ZrO_(2)@ZIF-90 nanozyme modified glassy carbon electrode(ZrO_(2)@ZIF-90/GCE)was then fabricated to analyze p-NP formed through MP degradation.Under the optimized conditions,the developed sensor displayed satisfactory analytical performance with a low limit of detection of 0.53μmol/L and two wide linear ranges(3-10 and 10-200μmol/L).ZrO_(2)@ZIF-90 nanozyme accomplished to the degradation and electrochemical detection of MP in river water and spiked fruits.This study identifies a promising new strategy for the design of bifunctional nanozymes for the detection of environmental hazards.
基金This work is financially supported by the NSFC grant of 21475030the S&T Research Project of Anhui Province15czz03109the National 10000 Talents-Youth Top-notch Talent Program.
文摘We report the design of a sensitive,electrochemical aptasensor for detection of ochratoxin A(OTA)with an extraordinary tunable dynamic sensing range.This electrochemical aptasensor is constructed based on the target induced aptamer-folding detection mechanism and the recognition between OTA and its aptamers results in the conformational change of the aptamer probe and thus signal changes for measurement.The dynamic sensing range of the electrochemical aptasensor is successfully tuned by introduction of free assistant aptamer probes in the sensing system.Our electrochemical aptasensor shows an extraordinary dynamic sensing range of 11-order magnitude of OTA concentration from 10^−8 to 10^2 ng/g.Of great significance,the signal response in all OTA concentration ranges is at the same current scale,demonstrating that our sensing protocol in this research could be applied for accurate detections of OTA in a broad range without using any complicated treatment of signal amplification.Finally,OTA spiked red wine and maize samples in different dynamic sensing ranges are determined with the electrochemical aptasensor under optimized sensing conditions.This tuning strategy of dynamic sensing range may offer a promising platform for electrochemical aptasensor optimizations in practical applications.
基金the Natural Science Foundation of China(No.50572075,50302007)the Key Project of Chinese Ministry of Education(206098)the Youth Sunshine Project of Wuhan City China(No.20045006071-39)
文摘In this study, integrated multi-wall carbon nanotube （MWCNT） electrodes were prepared in the holes of glass directly by microwave plasma chemical vapour deposition （MWPCVD）. The electrochemical behaviour of catechol at the integrated MWCNT electrodes was investigated. The oxygen plasma treated CNT electrodes had better electrochemical performance for the analysis of catechol than that of as-synthesized CNT electrodes. Both the as-synthesized CNTs and plasma treated CNTs were characterized by TEM（transmission electron microscopy, XPS（X-ray photoelectron spectroscopy） and Raman spectroscopy. The results revealed that the oxygen plasma activation is an effective method to enhance the electrochemical properties of CNT electrodes.
基金funded by the Hong Kong Research Grants Council(25201620/C6001-22Y)the Hong Kong Innovation Technology Commission(ITC)under project No.MHP/060/21support of the State Key Laboratory of Advanced Displays and Optoelectronics Technologies at HKUST.
文摘Electronic waste(e-waste)and diabetes are global challenges to modern societies.However,solving these two challenges together has been challenging until now.Herein,we propose a laser-induced transfer method to fabricate portable glucose sensors by recycling copper from e-waste.We bring up a laser-induced full-automatic fabrication method for synthesizing continuous heterogeneous Cu_(x)O(h-Cu_(x)O)nano-skeletons electrode for glucose sensing,offering rapid(<1 min),clean,air-compatible,and continuous fabrication,applicable to a wide range of Cu-containing substrates.Leveraging this approach,h-Cu_(x)O nanoskeletons,with an inner core predominantly composed of Cu_(2)O with lower oxygen content,juxtaposed with an outer layer rich in amorphous Cu_(x)O(a-Cu_(x)O)with higher oxygen content,are derived from discarded printed circuit boards.When employed in glucose detection,the h-Cu_(x)O nano-skeletons undergo a structural evolution process,transitioning into rigid Cu_(2)O@CuO nano-skeletons prompted by electrochemical activation.This transformation yields exceptional glucose-sensing performance(sensitivity:9.893 mA mM^(-1) cm^(-2);detection limit:0.34μM),outperforming most previously reported glucose sensors.Density functional theory analysis elucidates that the heterogeneous structure facilitates gluconolactone desorption.This glucose detection device has also been downsized to optimize its scalability and portability for convenient integration into people’s everyday lives.
基金Supported by the National Natural Science Foundation of China(50635040)the National High Technology Research and Development Program of China("863"Program)(2006AA04Z321)the Natural Science Foundation of Jiangsu Province(BK2008043)~~
文摘Effect of electrode insulation on the electric field and the flow field of the machining gap during electrochemical drilling（ECD） is numerically studied. Electric field simulation shows that the current density along the side gap decreases with increasing the thickness of electrode insulation. And the analysis of the electrolyte flow in the frontal gap shows that the insulation thickness has a remarkable influence on the pressure distributions. Ex- periments investigate the influence of the insulation thickness on the main characteristics of the machined hole, i.e. , radial overcut, entrance conicity, and current stability. The poor hole is observed and identified as most likely to occur with a combination of the low tool feed rate and the low insulation thickness. The appropriate thickness of the insulating layer leads to an improvement on hole accuracy and machining stability.
基金Supported by the National Natural Science Foundation of China(Nos.31470960 and 21422508)
文摘In this paper, a novel method for selectively detection of dopamine(DA) in the interference of ascorbic acid(AA) is described. A nanometer-sized gold flower microelectrode(NGFME) is prepared by flame-etching and electrochemical deposition. The electrode tip was characterized by scanning electron microscope(SEM). The NGFME is sized at about 100 μm and dimensions of thorns of the electrode were in nanometers. By modifying with DA aptamer on the surface, the prepared aptasensor can selectively detect DA even in the presence of high concentration AA. Experimental results show that this NGFME has no response to AA. As a comparison, the carbon fiber electrode without DA aptamer modification is unable to effectively detect DA in the presence of AA. The NGFME is easy-to-prepare, selective and sensitive for DA detection down to 25 μM. The electrode can be expected to detect DA in vivo and in real biological samples.
