Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(L...Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(LMBs).Despite this,the application of GPEs is still hindered by inadequate ionic conductivity,low Li^(+)transference number,and subpar physicochemical properties.Herein,Ti O_(2-x)nanofibers(NF)with oxygen vacancy defects were synthesized by a one-step process as inorganic fillers to enhance the thermal/mechanical/ionic-transportation performances of composite GPEs.Various characterizations and theoretical calculations reveal that the oxygen vacancies on the surface of Ti O_(2-x)NF accelerate the dissociation of Li PF_6,promote the rapid transfer of free Li^(+),and influence the formation of Li F-enriched solid electrolyte interphase.Consequently,the composite GPEs demonstrate enhanced ionic conductivity(1.90m S cm^(-1)at room temperature),higher lithium-ion transference number(0.70),wider electrochemical stability window(5.50 V),superior mechanical strength,excellent thermal stability(210℃),and improved compatibility with lithium,resulting in superior cycling stability and rate performance in both Li||Li,Li||Li Fe PO_(4),and Li||Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2)cells.Overall,the synergistic influence of nanofiber morphology and enriched oxygen vacancy structure of fillers on electrochemical properties of composite GPEs is comprehensively investigated,thus,it is anticipated to shed new light on designing high-performance GPEs LMBs.展开更多
Exploring highly foldable batteries with no safety hazard is a crucial task for the realization of portable,wearable,and implantable electric devices.Given these concerns,developing solid-state batteries is one of the...Exploring highly foldable batteries with no safety hazard is a crucial task for the realization of portable,wearable,and implantable electric devices.Given these concerns,developing solid-state batteries is one of the most promising routes to achieve this aspiration.Because of the excellent flexibility and processability,polyvinylidene fluoride(PVDF) based electrolytes possess great potential to pack high energy density flexible batteries,however,suffers the various intrinsic shortcomings such as inferior ionic conductivity,a high degree of crystallinity,and lack of reactive groups.Clearing the progress of the present state and concluding the specific challenges faced by PVDF based electrolytes will help to develop PVDF based polymer batteries.In this review,we summarize the recent progress of gel polymer electrolytes and all solid polymer electrolytes based on PVDF.The ion transport mechanisms and preparation methods of PVDF based electrolytes are briefly introduced.Meanwhile,the current design principle and properties of electrolytes are highlighted and systematically discussed.Some peculiar modified strategies performed in lithium-sulfur batteries and lithium-oxygen batteries are also included.Finally,this review describes the challenges and prospects of some solid-state electrolytes to provide strategies for manufacturing high-performance PVDF electrolytes aimed at practical application with flexible requirements.展开更多
Objective and Impact Statement.Real-time monitoring of the temperatures of regional tissue microenvironments can serve as the diagnostic basis for treating various health conditions and diseases.Introduction.Tradition...Objective and Impact Statement.Real-time monitoring of the temperatures of regional tissue microenvironments can serve as the diagnostic basis for treating various health conditions and diseases.Introduction.Traditional thermal sensors allow measurements at surfaces or at near-surface regions of the skin or of certain body cavities.Evaluations at depth require implanted devices connected to external readout electronics via physical interfaces that lead to risks for infection and movement constraints for the patient.Also,surgical extraction procedures after a period of need can introduce additional risks and costs.Methods.Here,we report a wireless,bioresorbable class of temperature sensor that exploits multilayer photonic cavities,for continuous optical measurements of regional,deep-tissue microenvironments over a timeframe of interest followed by complete clearance via natural body processes.Results.The designs decouple the influence of detection angle from temperature on the reflection spectra,to enable high accuracy in sensing,as supported by in vitro experiments and optical simulations.Studies with devices implanted into subcutaneous tissues of both awake,freely moving and asleep animal models illustrate the applicability of this technology for in vivo measurements.Conclusion.The results demonstrate the use of bioresorbable materials in advanced photonic structures with unique capabilities in tracking of thermal signatures of tissue microenvironments,with potential relevance to human healthcare.展开更多
As a resonator-based optical hardware in analog optical computing, a microring synapse can be straightforwardly configured to simulate the connection weights between neurons, but it faces challenges in precision and s...As a resonator-based optical hardware in analog optical computing, a microring synapse can be straightforwardly configured to simulate the connection weights between neurons, but it faces challenges in precision and stability due to cross talk and environmental perturbations. Here, we propose and demonstrate a self-calibration scheme with dual-wavelength synchronization to monitor and calibrate the synaptic weights without interrupting the computation tasks. We design and fabricate an integrated 4 × 4 microring synapse and deploy our self-calibration scheme to validate its effectiveness. The precision and robustness are evaluated in the experiments with favorable performance, achieving 2-bit precision improvement and excellent robustness to environmental temperature fluctuations(the weights can be corrected within 1 s after temperature changes 0.5°C). Moreover, we demonstrate matrix inversion tasks based on Newton iterations beyond 7-bit precision using this microring synapse. Our scheme provides an accurate and real-time weight calibration independently parallel from computations and opens up new perspectives for precision boost solutions to large-scale analog optical computing.展开更多
Background The outbreak of the severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)has greatly threatened public health.Recent studies have revealed that the spike receptor-binding domain(RBD)of SARS-CoV-2 is a...Background The outbreak of the severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)has greatly threatened public health.Recent studies have revealed that the spike receptor-binding domain(RBD)of SARS-CoV-2 is a potent target for vaccine development.However,adjuvants are usually required to strengthen the immunogenicity of recombinant antigens.Different types of adjuvants can elicit different immune responses.Methods We developed an RBD recombinant protein vaccine with a polyriboinosinic acid–polyribocytidylic acid[poly(I:C)]adjuvant to evoke a strong immune response.The delivery of poly(I:C)was optimized in two steps.First,poly(I:C)was complexed with a cationic polymer,poly-l-lysine(PLL),to form poly(I:C)–PLL,a polyplex core.Thereafter,it was loaded into five different lipid shells(group II,III-1,2-distearoyl-sn-glycero-3-phosphocholine[DSPC],III-1,2-dioleoyl-sn-glycero-3-phosphoethanolamine[DOPE],IV-DOPE,and IV-DSPC).We performed an enzyme-linked immunosorbent assay and enzyme-linked immunosorbent spot assay to compare the ability of the five lipopolyplex adjuvants to enhance the immunogenicity of the SARS-CoV-2 RBD protein,including humoral and cellular immune responses.Finally,the adjuvant with the highest immunogenicity was selected to verify the protective immunity of the vaccine through animal challenge experiments.Results Recombinant RBD protein has low immunogenicity.The different adjuvants we developed enhanced the immunogenicity of the RBD protein in different ways.Among the lipopolyplexes,those containing DOPE(III-DOPE and IV-DOPE)elicited RBD-specific immunoglobulin G antibody responses,and adjuvants with four components elicited better RBD-specific immunoglobulin G antibody responses than those containing three components(P<0.05).The IC50 and IC90 titers indicated that the IV-DOPE lipopolyplex had the greatest neutralization ability,with IC50 titers of 1/117,490.Furthermore,in the challenge study,IV-DOPE lipopolyplex protected mice from SARS-CoV-2 infection.On the fourth day after infection,the average animal body weights were reduced by 18.56%(24.164±0.665 g vs.19.678±0.455 g)and 0.06%(24.249±0.683 g vs.24.235±0.681 g)in the MOCK and vaccine groups,respectively.In addition,the relative expression of viral RNA in the vaccinated group was significantly lower than that in the MOCK group(P<0.05).Interstitial inflammatory cell infiltration was observed in the MOCK group,whereas no obvious damage was observed in the vaccinated group.Conclusions The IV-DOPE–adjuvanted SARS-CoV-2 recombinant RBD protein vaccine efficiently protected mice from SARS-CoV-2 in the animal challenge study.Therefore,IV-DOPE is considered an exceptional adjuvant for SARS-CoV-2 recombinant RBD protein-based vaccines and has the potential to be further developed into a SARS-CoV-2 recombinant RBD protein-based vaccine.展开更多
Flowrate control in flexible bioelectronics with targeted drug delivery capabilities is essential to ensure timely and safe delivery.For neuroscience and pharmacogenetics studies in small animals,these flexible bioele...Flowrate control in flexible bioelectronics with targeted drug delivery capabilities is essential to ensure timely and safe delivery.For neuroscience and pharmacogenetics studies in small animals,these flexible bioelectronic systems can be tailored to deliver small drug volumes on a controlled fashion without damaging surrounding tissues from stresses induced by excessively high flowrates.The drug delivery process is realized by an electrochemical reaction that pressurizes the internal bioelectronic chambers to deform a flexible polymer membrane that pumps the drug through a network of microchannels implanted in the small animal.The flowrate temporal profile and global maximum are governed and can be modeled by the ideal gas law.Here,we obtain an analytical solution that groups the relevant mechanical,fluidic,environmental,and electrochemical terms involved in the drug delivery process into a set of three nondimensional parameters.The unique combinations of these three nondimensional parameters(related to the initial pressure,initial gas volume,and microfluidic resistance)can be used to model the flowrate and scale up the flexible bioelectronic design for experiments in medium and large animal models.The analytical solution is divided into(1)a fast variable that controls the maximum flowrate and(2)a slow variable that models the temporal profile.Together,the two variables detail the complete drug delivery process and control using the three nondimensional parameters.Comparison of the analytical model with alternative numerical models shows excellent agreement and validates the analytic modeling approach.These findings serve as a theoretical framework to design and optimize future flexible bioelectronic systems used in biomedical research,or related medical fields,and analytically control the flowrate and its global maximum for successful drug delivery.展开更多
基金supported by the National Natural Science Foundation of China(52122702,52277215)the Natural Science Foundation of Heilongjiang Province of China(JQ2021E005)。
文摘Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(LMBs).Despite this,the application of GPEs is still hindered by inadequate ionic conductivity,low Li^(+)transference number,and subpar physicochemical properties.Herein,Ti O_(2-x)nanofibers(NF)with oxygen vacancy defects were synthesized by a one-step process as inorganic fillers to enhance the thermal/mechanical/ionic-transportation performances of composite GPEs.Various characterizations and theoretical calculations reveal that the oxygen vacancies on the surface of Ti O_(2-x)NF accelerate the dissociation of Li PF_6,promote the rapid transfer of free Li^(+),and influence the formation of Li F-enriched solid electrolyte interphase.Consequently,the composite GPEs demonstrate enhanced ionic conductivity(1.90m S cm^(-1)at room temperature),higher lithium-ion transference number(0.70),wider electrochemical stability window(5.50 V),superior mechanical strength,excellent thermal stability(210℃),and improved compatibility with lithium,resulting in superior cycling stability and rate performance in both Li||Li,Li||Li Fe PO_(4),and Li||Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2)cells.Overall,the synergistic influence of nanofiber morphology and enriched oxygen vacancy structure of fillers on electrochemical properties of composite GPEs is comprehensively investigated,thus,it is anticipated to shed new light on designing high-performance GPEs LMBs.
基金supported by the National Natural Science Foundation of China(Grant No.51502063)the Project for guiding local Science and Technology Development by Central Government of Chin(ZY18C04)+1 种基金the Fundamental Research Foundation for Universities of Heilongjiang Province(LGYC2018JQ006)the Science Funds for Young Innovative Talents of HUST(No.201505).
文摘Exploring highly foldable batteries with no safety hazard is a crucial task for the realization of portable,wearable,and implantable electric devices.Given these concerns,developing solid-state batteries is one of the most promising routes to achieve this aspiration.Because of the excellent flexibility and processability,polyvinylidene fluoride(PVDF) based electrolytes possess great potential to pack high energy density flexible batteries,however,suffers the various intrinsic shortcomings such as inferior ionic conductivity,a high degree of crystallinity,and lack of reactive groups.Clearing the progress of the present state and concluding the specific challenges faced by PVDF based electrolytes will help to develop PVDF based polymer batteries.In this review,we summarize the recent progress of gel polymer electrolytes and all solid polymer electrolytes based on PVDF.The ion transport mechanisms and preparation methods of PVDF based electrolytes are briefly introduced.Meanwhile,the current design principle and properties of electrolytes are highlighted and systematically discussed.Some peculiar modified strategies performed in lithium-sulfur batteries and lithium-oxygen batteries are also included.Finally,this review describes the challenges and prospects of some solid-state electrolytes to provide strategies for manufacturing high-performance PVDF electrolytes aimed at practical application with flexible requirements.
基金This work utilized Northwestern University Micro/Nano Fabrication Facility(NUFAB)which is partially supported by Soft and Hybrid Nanotechnology Experimental(SHyNE)Resource(NSF ECCS-1542205)+3 种基金the Materials Research Science and Engineering Center(DMR-1720139)the State of Illinois,and Northwestern University.Y.H.acknowledges the support from the National Science Foundation,USA(grant no.CMMI1635443)supported by Querrey Simpson Institute for Bioelectronicssupported by Cancer Center Support Grant P30 CA060553 from the National Cancer Institute awarded to the Robert H.Lurie Comprehensive Cancer Center.
文摘Objective and Impact Statement.Real-time monitoring of the temperatures of regional tissue microenvironments can serve as the diagnostic basis for treating various health conditions and diseases.Introduction.Traditional thermal sensors allow measurements at surfaces or at near-surface regions of the skin or of certain body cavities.Evaluations at depth require implanted devices connected to external readout electronics via physical interfaces that lead to risks for infection and movement constraints for the patient.Also,surgical extraction procedures after a period of need can introduce additional risks and costs.Methods.Here,we report a wireless,bioresorbable class of temperature sensor that exploits multilayer photonic cavities,for continuous optical measurements of regional,deep-tissue microenvironments over a timeframe of interest followed by complete clearance via natural body processes.Results.The designs decouple the influence of detection angle from temperature on the reflection spectra,to enable high accuracy in sensing,as supported by in vitro experiments and optical simulations.Studies with devices implanted into subcutaneous tissues of both awake,freely moving and asleep animal models illustrate the applicability of this technology for in vivo measurements.Conclusion.The results demonstrate the use of bioresorbable materials in advanced photonic structures with unique capabilities in tracking of thermal signatures of tissue microenvironments,with potential relevance to human healthcare.
基金National Key Research and Development Program of China(2021YFB2801900,2021YFB2801903)National Natural Science Foundation of China(62075075,62275088,U21A20511)Innovation Project of Optics Valley Laboratory(OVL2021BG001)
文摘As a resonator-based optical hardware in analog optical computing, a microring synapse can be straightforwardly configured to simulate the connection weights between neurons, but it faces challenges in precision and stability due to cross talk and environmental perturbations. Here, we propose and demonstrate a self-calibration scheme with dual-wavelength synchronization to monitor and calibrate the synaptic weights without interrupting the computation tasks. We design and fabricate an integrated 4 × 4 microring synapse and deploy our self-calibration scheme to validate its effectiveness. The precision and robustness are evaluated in the experiments with favorable performance, achieving 2-bit precision improvement and excellent robustness to environmental temperature fluctuations(the weights can be corrected within 1 s after temperature changes 0.5°C). Moreover, we demonstrate matrix inversion tasks based on Newton iterations beyond 7-bit precision using this microring synapse. Our scheme provides an accurate and real-time weight calibration independently parallel from computations and opens up new perspectives for precision boost solutions to large-scale analog optical computing.
文摘Background The outbreak of the severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)has greatly threatened public health.Recent studies have revealed that the spike receptor-binding domain(RBD)of SARS-CoV-2 is a potent target for vaccine development.However,adjuvants are usually required to strengthen the immunogenicity of recombinant antigens.Different types of adjuvants can elicit different immune responses.Methods We developed an RBD recombinant protein vaccine with a polyriboinosinic acid–polyribocytidylic acid[poly(I:C)]adjuvant to evoke a strong immune response.The delivery of poly(I:C)was optimized in two steps.First,poly(I:C)was complexed with a cationic polymer,poly-l-lysine(PLL),to form poly(I:C)–PLL,a polyplex core.Thereafter,it was loaded into five different lipid shells(group II,III-1,2-distearoyl-sn-glycero-3-phosphocholine[DSPC],III-1,2-dioleoyl-sn-glycero-3-phosphoethanolamine[DOPE],IV-DOPE,and IV-DSPC).We performed an enzyme-linked immunosorbent assay and enzyme-linked immunosorbent spot assay to compare the ability of the five lipopolyplex adjuvants to enhance the immunogenicity of the SARS-CoV-2 RBD protein,including humoral and cellular immune responses.Finally,the adjuvant with the highest immunogenicity was selected to verify the protective immunity of the vaccine through animal challenge experiments.Results Recombinant RBD protein has low immunogenicity.The different adjuvants we developed enhanced the immunogenicity of the RBD protein in different ways.Among the lipopolyplexes,those containing DOPE(III-DOPE and IV-DOPE)elicited RBD-specific immunoglobulin G antibody responses,and adjuvants with four components elicited better RBD-specific immunoglobulin G antibody responses than those containing three components(P<0.05).The IC50 and IC90 titers indicated that the IV-DOPE lipopolyplex had the greatest neutralization ability,with IC50 titers of 1/117,490.Furthermore,in the challenge study,IV-DOPE lipopolyplex protected mice from SARS-CoV-2 infection.On the fourth day after infection,the average animal body weights were reduced by 18.56%(24.164±0.665 g vs.19.678±0.455 g)and 0.06%(24.249±0.683 g vs.24.235±0.681 g)in the MOCK and vaccine groups,respectively.In addition,the relative expression of viral RNA in the vaccinated group was significantly lower than that in the MOCK group(P<0.05).Interstitial inflammatory cell infiltration was observed in the MOCK group,whereas no obvious damage was observed in the vaccinated group.Conclusions The IV-DOPE–adjuvanted SARS-CoV-2 recombinant RBD protein vaccine efficiently protected mice from SARS-CoV-2 in the animal challenge study.Therefore,IV-DOPE is considered an exceptional adjuvant for SARS-CoV-2 recombinant RBD protein-based vaccines and has the potential to be further developed into a SARS-CoV-2 recombinant RBD protein-based vaccine.
基金R.A.acknowledges support from the National Science Foundation Graduate Research Fellowship(NSF grant number DGE-1842165)and from the Ford Foundation Predoctoral Fellowship。
文摘Flowrate control in flexible bioelectronics with targeted drug delivery capabilities is essential to ensure timely and safe delivery.For neuroscience and pharmacogenetics studies in small animals,these flexible bioelectronic systems can be tailored to deliver small drug volumes on a controlled fashion without damaging surrounding tissues from stresses induced by excessively high flowrates.The drug delivery process is realized by an electrochemical reaction that pressurizes the internal bioelectronic chambers to deform a flexible polymer membrane that pumps the drug through a network of microchannels implanted in the small animal.The flowrate temporal profile and global maximum are governed and can be modeled by the ideal gas law.Here,we obtain an analytical solution that groups the relevant mechanical,fluidic,environmental,and electrochemical terms involved in the drug delivery process into a set of three nondimensional parameters.The unique combinations of these three nondimensional parameters(related to the initial pressure,initial gas volume,and microfluidic resistance)can be used to model the flowrate and scale up the flexible bioelectronic design for experiments in medium and large animal models.The analytical solution is divided into(1)a fast variable that controls the maximum flowrate and(2)a slow variable that models the temporal profile.Together,the two variables detail the complete drug delivery process and control using the three nondimensional parameters.Comparison of the analytical model with alternative numerical models shows excellent agreement and validates the analytic modeling approach.These findings serve as a theoretical framework to design and optimize future flexible bioelectronic systems used in biomedical research,or related medical fields,and analytically control the flowrate and its global maximum for successful drug delivery.