The controlled assembly of nanomaterials has demon-strated significant potential in advancing technological devices.However,achieving highly efficient and low-loss assembly technique for nanomate-rials,enabling the cr...The controlled assembly of nanomaterials has demon-strated significant potential in advancing technological devices.However,achieving highly efficient and low-loss assembly technique for nanomate-rials,enabling the creation of hierarchical structures with distinctive func-tionalities,remains a formidable challenge.Here,we present a method for nanomaterial assembly enhanced by ionic liquids,which enables the fabrication of highly stable,flexible,and transparent electrodes featuring an organized layered structure.The utilization of hydrophobic and non-volatile ionic liquids facilitates the production of stable interfaces with water,effectively preventing the sedimentation of 1D/2D nanomaterials assembled at the interface.Furthermore,the interfacially assembled nanomaterial monolayer exhibits an alternate self-climbing behavior,enabling layer-by-layer transfer and the formation of a well-ordered MXene-wrapped silver nanowire network film.The resulting composite film not only demonstrates exceptional photoelectric performance with a sheet resistance of 9.4Ωsq^(-1) and 93%transmittance,but also showcases remarkable environmental stability and mechanical flexibility.Particularly noteworthy is its application in transparent electromagnetic interference shielding materials and triboelectric nanogenerator devices.This research introduces an innovative approach to manufacture and tailor functional devices based on ordered nanomaterials.展开更多
We propose a process of quantum-confined ion superfluid (QISF),which is enthalpy-driven confined ordered fluid,to explain the transmission of nerve signals.The ultrafast Na^+ and K^+ ions transportation through all so...We propose a process of quantum-confined ion superfluid (QISF),which is enthalpy-driven confined ordered fluid,to explain the transmission of nerve signals.The ultrafast Na^+ and K^+ ions transportation through all sodium-potassium pump nanochannels simultaneously in the membrane is without energy loss,and leads to QISF wave along the neuronal axon,which acts as an information medium in the ultrafast nerve signal transmission.The QISF process will not only provide a new view point for a reasonable explanation of ultrafast signal transmission in the nerves and brain,but also challenge the theory of matter wave for ions,molecules and particles.展开更多
Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined su...Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined superfluid" (QSF). This ordered ultrafast flow in the confined channel can be considered as "quantum tunneling fluid effect" with a "tunneling distance", which is corresponding to the period of QSF. Recent research demonstrated that artificial biomimetic nanochannels also showed the phenomenon of QSF, such as ion and water channels. The introduction of QSF concept in the fields of chemistry and biology may create significant impact. As for chemistry, the QSF effect provides new ideas for accurate synthesis in organic, inorganic, polymer, etc. We believe the implementation of the idea of QSF will promote the development of QSF biochemistry, biophysics, bioinformatics and biomedical science.展开更多
In the neural system,a large number of neurons con-tinuously produce and transmit electrophysiological sig-nals,which communicate between neurons and brain regions.Naturally,bioinformation transformation de-pends on c...In the neural system,a large number of neurons con-tinuously produce and transmit electrophysiological sig-nals,which communicate between neurons and brain regions.Naturally,bioinformation transformation de-pends on conversion from ionics to electronics,and electronics-based neural recording technologies(Fig.1)have been extensively developed since the primitive vol-tage clamp in 1949[1].展开更多
Multiphase catalysis is used in many industrial processes;however,the reaction rate can be restricted by the low accessibility of gaseous reactants to the catalysts in water,especially for oxygen-dependent biocatalyti...Multiphase catalysis is used in many industrial processes;however,the reaction rate can be restricted by the low accessibility of gaseous reactants to the catalysts in water,especially for oxygen-dependent biocatalytic reactions.Despite the fact that solubility and diffusion rates of oxygen in many liquids(such as perfluorocarbon)are much higher than in water,multiphase reactions with a second liquid phase are still difficult to conduct,because the interaction efficiency between immiscible phases is extremely low.Herein,we report an efficient triphase biocatalytic system using oil core-silica shell oxygen nanocarriers.Such design offers the biocatalytic system an extremely large water-solid-oil triphase interfacial area and a short path required for oxygen diffusion.Moreover,the silica shell stabilizes the oil nanodroplets in water and prevents their aggregation.Using oxygen-dependent oxidase enzymatic reaction as an example,we demonstrate this efficient biocatalytic system for the oxidation of glucose,choline,lactate,and sucrose by substituting their corresponding oxidase counterparts.A rate enhancement by a factor of 10-30 is observed when the oxygen nanocarriers are introduced into reaction system.This strategy offers the opportunity to enhance the efficiency of other gaseous reactants involved in multiphase catalytic reactions.展开更多
Ordered-and high-flux flow of molecules and ions in biological channels is considered as a quantumconfined superfluid,which is highly important in chemical reactions and bioinformation transmission.However,the driving...Ordered-and high-flux flow of molecules and ions in biological channels is considered as a quantumconfined superfluid,which is highly important in chemical reactions and bioinformation transmission.However,the driving forces for these ordered arrangements of molecules and ions in confined spaces have not been discussed.Herein,we demonstrate that the driving force of molecular/ionic superfluid formation is the attraction-repulsion balance of particles under the effect of interfacial confinement.展开更多
Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion e...Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.展开更多
Developing photoelectrochemical(PEC)bioassays based on the principle of a photocathodic measurement of enzymatic product H_(2)O_(2) is highly attractive because it can naturally avoid interfering signals arising from ...Developing photoelectrochemical(PEC)bioassays based on the principle of a photocathodic measurement of enzymatic product H_(2)O_(2) is highly attractive because it can naturally avoid interfering signals arising from reductive species inherent to biofluids.However,fluctuant oxygen levels in the analyte solution can compromise the accuracy of photocathodic bioanalysis and restrict its application because oxygen reduction potential is similar to H_(2)O_(2).Herein,we addressed this restriction by constructing a triphase biophotocathode with air–liquid–solid joint interfaces by immobilizing an oxidase enzyme film on the tip part of superhydrophobic p-type semiconductor nanowire arrays.Such a triphase biophotocathode has a reaction zone with steady and air phasedependent oxygen concentration which stabilizes and increases the oxidase kinetics,and enables the photocathodic measurement principle in reliable PEC bioassay development with high selectivity,good accuracy,and a wide linear detection range.Moreover,the biophotocathode shows good stability during repeated testing under light illumination.This reliable PEC bioassay system has broad potential in the fields of disease diagnosis,medical research,and environmental monitoring.展开更多
Mechanosensory elastomers attract intense interests in the academic and industrial fields.However,molecular insight of macroscopic properties remains a significant challenge.Herein,we build up a correlation between th...Mechanosensory elastomers attract intense interests in the academic and industrial fields.However,molecular insight of macroscopic properties remains a significant challenge.Herein,we build up a correlation between the microscopic and macroscopic level by designing a mechanosensory elastomer with aggregation-induced emission luminogens(AIEgens)that monitors chain deformation in situ.The key constituents are the mechanosensory units,which are dynamic dimers bonded by ureidopyrimidinone(UPy)groups and tetraphenylethylene(TPE)for the fluorescence signal output.The photoluminescence(PL)technique successfully monitors elastomer chain deformation under external forces.The PL intensity increases linearly at low elongation,in excellent agreement with Hooke’s law for ideal chains.Strong deviation from linear PL intensity is measured at high elongation,which can be theoretically described by the Langevin function.A correlation between the microscopic and the macroscopic level is then built.展开更多
Silver nanowire(AgNW)networks hold great promises as next-generation flex-ible transparent electrodes(FTEs)for high-performance flexible optoelectronic devices.However,achieving large-area flexible AgNW network electr...Silver nanowire(AgNW)networks hold great promises as next-generation flex-ible transparent electrodes(FTEs)for high-performance flexible optoelectronic devices.However,achieving large-area flexible AgNW network electrodes with low sheet resistance,high optical transmittance,and a smooth surface remains a grand challenge.Here,we report a straightforward and cost-effective roll-to-roll method that includes interface assembly/wetting-induced climbing transfer,nanowelding,and washing processess to fabricate flexible ordered lay-ered AgNW electrodes with high network uniformity.By manipulating the stacking number of the interfacially assembled AgNW monolayer,we can pre-cisely tailor and balance the transparency and the conductivity of the elec-trodes,achieving an exceptional Figure of Merit(FoM)value of 862.Moreover,the ordered layered structure enhances surface smoothness,compared with randomly arranged structures.To highlight the potential of these ordered lay-ered AgNW network electrodes in flexible optoelectronic devices,we success-fully employ them as highly sensitive strain sensors,large-area flexible touch screens,and flexible smart windows.Overall,this work represents a substantial advance toward high-performance FTEs over large areas,opening up exciting opportunities for the development of advanced optoelectronic devices.展开更多
基金This work was supported by the National Natural Science Foundation of China(nos.21988102,and 22305026)the China Postdoctoral Science Foundation(2019M650433).
文摘The controlled assembly of nanomaterials has demon-strated significant potential in advancing technological devices.However,achieving highly efficient and low-loss assembly technique for nanomate-rials,enabling the creation of hierarchical structures with distinctive func-tionalities,remains a formidable challenge.Here,we present a method for nanomaterial assembly enhanced by ionic liquids,which enables the fabrication of highly stable,flexible,and transparent electrodes featuring an organized layered structure.The utilization of hydrophobic and non-volatile ionic liquids facilitates the production of stable interfaces with water,effectively preventing the sedimentation of 1D/2D nanomaterials assembled at the interface.Furthermore,the interfacially assembled nanomaterial monolayer exhibits an alternate self-climbing behavior,enabling layer-by-layer transfer and the formation of a well-ordered MXene-wrapped silver nanowire network film.The resulting composite film not only demonstrates exceptional photoelectric performance with a sheet resistance of 9.4Ωsq^(-1) and 93%transmittance,but also showcases remarkable environmental stability and mechanical flexibility.Particularly noteworthy is its application in transparent electromagnetic interference shielding materials and triboelectric nanogenerator devices.This research introduces an innovative approach to manufacture and tailor functional devices based on ordered nanomaterials.
基金the National Natural Science Foundation of China (Nos.51603211 and 51673107)the National Key R&D Program of China (No.2016YFA0200803)the 111 Project (No.B1 4009).
文摘We propose a process of quantum-confined ion superfluid (QISF),which is enthalpy-driven confined ordered fluid,to explain the transmission of nerve signals.The ultrafast Na^+ and K^+ ions transportation through all sodium-potassium pump nanochannels simultaneously in the membrane is without energy loss,and leads to QISF wave along the neuronal axon,which acts as an information medium in the ultrafast nerve signal transmission.The QISF process will not only provide a new view point for a reasonable explanation of ultrafast signal transmission in the nerves and brain,but also challenge the theory of matter wave for ions,molecules and particles.
基金supported by the National Key R&D Program of China(2017YFA0206900)the National Natural Science Foundation of China(21625303)
文摘Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined superfluid" (QSF). This ordered ultrafast flow in the confined channel can be considered as "quantum tunneling fluid effect" with a "tunneling distance", which is corresponding to the period of QSF. Recent research demonstrated that artificial biomimetic nanochannels also showed the phenomenon of QSF, such as ion and water channels. The introduction of QSF concept in the fields of chemistry and biology may create significant impact. As for chemistry, the QSF effect provides new ideas for accurate synthesis in organic, inorganic, polymer, etc. We believe the implementation of the idea of QSF will promote the development of QSF biochemistry, biophysics, bioinformatics and biomedical science.
基金supported by the National Key R&D program of China (2016YFA0200803)the National Natural Science Foundation (51973227 and 51603211)
文摘In the neural system,a large number of neurons con-tinuously produce and transmit electrophysiological sig-nals,which communicate between neurons and brain regions.Naturally,bioinformation transformation de-pends on conversion from ionics to electronics,and electronics-based neural recording technologies(Fig.1)have been extensively developed since the primitive vol-tage clamp in 1949[1].
基金the National Key R&D Program of China(No.2019YFA0709200)the National Natural Science Foundation of China(Nos.21988102,51772198,21975171).
文摘Multiphase catalysis is used in many industrial processes;however,the reaction rate can be restricted by the low accessibility of gaseous reactants to the catalysts in water,especially for oxygen-dependent biocatalytic reactions.Despite the fact that solubility and diffusion rates of oxygen in many liquids(such as perfluorocarbon)are much higher than in water,multiphase reactions with a second liquid phase are still difficult to conduct,because the interaction efficiency between immiscible phases is extremely low.Herein,we report an efficient triphase biocatalytic system using oil core-silica shell oxygen nanocarriers.Such design offers the biocatalytic system an extremely large water-solid-oil triphase interfacial area and a short path required for oxygen diffusion.Moreover,the silica shell stabilizes the oil nanodroplets in water and prevents their aggregation.Using oxygen-dependent oxidase enzymatic reaction as an example,we demonstrate this efficient biocatalytic system for the oxidation of glucose,choline,lactate,and sucrose by substituting their corresponding oxidase counterparts.A rate enhancement by a factor of 10-30 is observed when the oxygen nanocarriers are introduced into reaction system.This strategy offers the opportunity to enhance the efficiency of other gaseous reactants involved in multiphase catalytic reactions.
基金supported by the National Key R&D program of China(nos.2016YFA0200803 and 2018YFA0208502)the National Natural Science Foundation of China(nos.51973227 and 21988102)the Youth Innovation Promotion Association CAS(no.2020028).
文摘Ordered-and high-flux flow of molecules and ions in biological channels is considered as a quantumconfined superfluid,which is highly important in chemical reactions and bioinformation transmission.However,the driving forces for these ordered arrangements of molecules and ions in confined spaces have not been discussed.Herein,we demonstrate that the driving force of molecular/ionic superfluid formation is the attraction-repulsion balance of particles under the effect of interfacial confinement.
基金supported by the National Key R&D Program of China(2019YFA0709200)the National Natural Science Foundation of China(21988102,51772198 and 21975171)。
文摘Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.
基金supported by the National Key R&D Program of China(no.2019YFA0709200)National Natural Science Foundation of China(nos.21988102,51772198,and 22002101).
文摘Developing photoelectrochemical(PEC)bioassays based on the principle of a photocathodic measurement of enzymatic product H_(2)O_(2) is highly attractive because it can naturally avoid interfering signals arising from reductive species inherent to biofluids.However,fluctuant oxygen levels in the analyte solution can compromise the accuracy of photocathodic bioanalysis and restrict its application because oxygen reduction potential is similar to H_(2)O_(2).Herein,we addressed this restriction by constructing a triphase biophotocathode with air–liquid–solid joint interfaces by immobilizing an oxidase enzyme film on the tip part of superhydrophobic p-type semiconductor nanowire arrays.Such a triphase biophotocathode has a reaction zone with steady and air phasedependent oxygen concentration which stabilizes and increases the oxidase kinetics,and enables the photocathodic measurement principle in reliable PEC bioassay development with high selectivity,good accuracy,and a wide linear detection range.Moreover,the biophotocathode shows good stability during repeated testing under light illumination.This reliable PEC bioassay system has broad potential in the fields of disease diagnosis,medical research,and environmental monitoring.
基金supported by the National Natural Science Foundation of China(nos.21875009 and 51973227)the National Key Research and Development Program of China(nos.2017YFA0206904 and 2017YFA0206900)+1 种基金the Youth Innovation Promotion Association CAS(no.2020028)the Fundamental Research Funds for the Central Universities。
文摘Mechanosensory elastomers attract intense interests in the academic and industrial fields.However,molecular insight of macroscopic properties remains a significant challenge.Herein,we build up a correlation between the microscopic and macroscopic level by designing a mechanosensory elastomer with aggregation-induced emission luminogens(AIEgens)that monitors chain deformation in situ.The key constituents are the mechanosensory units,which are dynamic dimers bonded by ureidopyrimidinone(UPy)groups and tetraphenylethylene(TPE)for the fluorescence signal output.The photoluminescence(PL)technique successfully monitors elastomer chain deformation under external forces.The PL intensity increases linearly at low elongation,in excellent agreement with Hooke’s law for ideal chains.Strong deviation from linear PL intensity is measured at high elongation,which can be theoretically described by the Langevin function.A correlation between the microscopic and the macroscopic level is then built.
基金supported by the National Natural Science Foundation of China(nos.21988102 and 22305026)the China Postdoctoral Science Foundation(2019M650433).
文摘Silver nanowire(AgNW)networks hold great promises as next-generation flex-ible transparent electrodes(FTEs)for high-performance flexible optoelectronic devices.However,achieving large-area flexible AgNW network electrodes with low sheet resistance,high optical transmittance,and a smooth surface remains a grand challenge.Here,we report a straightforward and cost-effective roll-to-roll method that includes interface assembly/wetting-induced climbing transfer,nanowelding,and washing processess to fabricate flexible ordered lay-ered AgNW electrodes with high network uniformity.By manipulating the stacking number of the interfacially assembled AgNW monolayer,we can pre-cisely tailor and balance the transparency and the conductivity of the elec-trodes,achieving an exceptional Figure of Merit(FoM)value of 862.Moreover,the ordered layered structure enhances surface smoothness,compared with randomly arranged structures.To highlight the potential of these ordered lay-ered AgNW network electrodes in flexible optoelectronic devices,we success-fully employ them as highly sensitive strain sensors,large-area flexible touch screens,and flexible smart windows.Overall,this work represents a substantial advance toward high-performance FTEs over large areas,opening up exciting opportunities for the development of advanced optoelectronic devices.