Interactions between deoxyribonucleic acid(DNA) and metal ions are vital for maintaining life functions, however,there are still unsolved questions about its mechanisms. It is of great practical significance to study ...Interactions between deoxyribonucleic acid(DNA) and metal ions are vital for maintaining life functions, however,there are still unsolved questions about its mechanisms. It is of great practical significance to study these issues for medical chip design, drug development, health care, etc. In this investigation, the conductivity properties of λ-DNA solutions with mono-/divalent metal ions(Na+, K^(+), Mg^(2+), and Ca^(2+)) are experimentally studied as they are electrically driven through a 5 μm microfluidic channel. Experimental data indicate that the conductivities of λ-DNA solutions with metal ions(M+/M2+) basically tend to reduce firstly and then increase as the voltage increases, of which the turning points varied with the metal ions. When the voltage surpasses turning points, the conductivity of λ-DNA-M+solutions increases with the concentration of metal ions, while that of λ-DNA-M^(2+)solutions decrease. Moreover, the conductivity of λ-DNA-M^(2+)solutions is always smaller than that of λ-DNA-M+solutions, and with high-concentration M^(2+), it is even smaller than that of the λ-DNA solution. The main reasons for the above findings could be attributed to the polarization of electrodes and different mechanisms of interactions between metal ions and λ-DNA molecules. This investigation is helpful for the precise manipulation of single DNA molecules in micro-/nanofluidic space and the design of new biomedical micro-/nanofluidic sensors.展开更多
Carbon-free electrochemical nitrogen reduction reaction(NRR)is an appealing strategy for green ammonia synthesis,but there is still a significant performance bottleneck.Conventional working electrode is usually floode...Carbon-free electrochemical nitrogen reduction reaction(NRR)is an appealing strategy for green ammonia synthesis,but there is still a significant performance bottleneck.Conventional working electrode is usually flooded by the electrolyte during the NRR test,and only the surface material could get access to the nitrogen,which inevitably gives rise to sluggish reaction rate.Herein,an asymmetric electrode design is proposed to tackle this challenge.An aerophilic layer is constructed on one face of the electrocatalyst-loaded electrode,while the other side maintains its original structure,aiming to achieve facilitated nitrogen transfer and electrolyte permeation within the conductive skeleton simultaneously.This asymmetric architecture affords extensive threephase reaction region within the electrode as demonstrated by the combination of theoretical simulations and experimental measurements,which gives full play to the loaded electrocatalyst.As expected,the proofof-concept asymmetric electrode delivers an NH_(3)yield rate of 40.81μg h^(−1)mg^(−1)and a Faradaic efficiency of 71.71%at−0.3 V versus the reversible hydrogen electrode,which are more than 4 and 7 times that of conventional electrode,respectively.This work presents a versatile strategy for enhancing the interfacial reaction kinetics and is instructive to electrode design for gas-involved electrochemical reactions.展开更多
Planar micro-supercapacitors show great potential as the energy storage unit in miniaturized electronic devices. Asymmetric structures have been widely inves- tigated in micro-supercapacitors, and carbon-based materia...Planar micro-supercapacitors show great potential as the energy storage unit in miniaturized electronic devices. Asymmetric structures have been widely inves- tigated in micro-supercapacitors, and carbon-based materials are commonly applied in the electrodes. To integrate different metal oxides in both electrodes in micro-supercapacitors, the critical challenge is the pairing of different faradic metal oxides. Herein, we propose a strategy of matching the voltage and capadtance of two faradic materials that are fully integrated into one high-performance asymmetric micro-supercapacitor by a facile and controllable fabrication process. The fabricated micro-supercapacitors employ MnO2 as the positive active material and Fe203 as the negative active material, respectively. The planar asymmetric micro-supercapacitors possess a high capacitance of 60 F-cm-3, a high energy density of 12 mW.h.cm-3, and a broad operation voltage range up to 1.2 V.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 62275216 and 61775181)the Innovation Capability Support Program of Shaanxi Province of China (Grant Nos. S2018-ZC-TD-0061 and TZ0393)the National Key Scientific Instrument and Equipment Development Projects of China (Grant No. 51927804)。
文摘Interactions between deoxyribonucleic acid(DNA) and metal ions are vital for maintaining life functions, however,there are still unsolved questions about its mechanisms. It is of great practical significance to study these issues for medical chip design, drug development, health care, etc. In this investigation, the conductivity properties of λ-DNA solutions with mono-/divalent metal ions(Na+, K^(+), Mg^(2+), and Ca^(2+)) are experimentally studied as they are electrically driven through a 5 μm microfluidic channel. Experimental data indicate that the conductivities of λ-DNA solutions with metal ions(M+/M2+) basically tend to reduce firstly and then increase as the voltage increases, of which the turning points varied with the metal ions. When the voltage surpasses turning points, the conductivity of λ-DNA-M+solutions increases with the concentration of metal ions, while that of λ-DNA-M^(2+)solutions decrease. Moreover, the conductivity of λ-DNA-M^(2+)solutions is always smaller than that of λ-DNA-M+solutions, and with high-concentration M^(2+), it is even smaller than that of the λ-DNA solution. The main reasons for the above findings could be attributed to the polarization of electrodes and different mechanisms of interactions between metal ions and λ-DNA molecules. This investigation is helpful for the precise manipulation of single DNA molecules in micro-/nanofluidic space and the design of new biomedical micro-/nanofluidic sensors.
基金National Natural Science Foundation of China,Grant/Award Numbers:U21A20332,52103226,52202275,52203314,12204253Distinguished Young Scholars Fund of Jiangsu Province,Grant/Award Number:BK20220061+1 种基金Fellowship of China Postdoctoral Science Foundation,Grant/Award Number:2021M702382Suzhou Foreign Academician Workstation,Grant/Award Number:SWY2022001。
文摘Carbon-free electrochemical nitrogen reduction reaction(NRR)is an appealing strategy for green ammonia synthesis,but there is still a significant performance bottleneck.Conventional working electrode is usually flooded by the electrolyte during the NRR test,and only the surface material could get access to the nitrogen,which inevitably gives rise to sluggish reaction rate.Herein,an asymmetric electrode design is proposed to tackle this challenge.An aerophilic layer is constructed on one face of the electrocatalyst-loaded electrode,while the other side maintains its original structure,aiming to achieve facilitated nitrogen transfer and electrolyte permeation within the conductive skeleton simultaneously.This asymmetric architecture affords extensive threephase reaction region within the electrode as demonstrated by the combination of theoretical simulations and experimental measurements,which gives full play to the loaded electrocatalyst.As expected,the proofof-concept asymmetric electrode delivers an NH_(3)yield rate of 40.81μg h^(−1)mg^(−1)and a Faradaic efficiency of 71.71%at−0.3 V versus the reversible hydrogen electrode,which are more than 4 and 7 times that of conventional electrode,respectively.This work presents a versatile strategy for enhancing the interfacial reaction kinetics and is instructive to electrode design for gas-involved electrochemical reactions.
基金This work was supported by the National Key Research and Development Program of China (No. 2016YFA0202603), the National Basic Research Program of China (No. 2013CB934103), the Programme of Introducing Talents of Discipline to Universities (No. B17034), the National Natural Science Foundation of China (Nos. 51521001, 51502227, 51579198, and 51302203), the National Natural Science Fund for Distinguished Young Scholars (No. 51425204), and the Fundamental Research Funds for the Central Universities (WUT: 2016III001, 2016III005, 2016III006).
文摘Planar micro-supercapacitors show great potential as the energy storage unit in miniaturized electronic devices. Asymmetric structures have been widely inves- tigated in micro-supercapacitors, and carbon-based materials are commonly applied in the electrodes. To integrate different metal oxides in both electrodes in micro-supercapacitors, the critical challenge is the pairing of different faradic metal oxides. Herein, we propose a strategy of matching the voltage and capadtance of two faradic materials that are fully integrated into one high-performance asymmetric micro-supercapacitor by a facile and controllable fabrication process. The fabricated micro-supercapacitors employ MnO2 as the positive active material and Fe203 as the negative active material, respectively. The planar asymmetric micro-supercapacitors possess a high capacitance of 60 F-cm-3, a high energy density of 12 mW.h.cm-3, and a broad operation voltage range up to 1.2 V.