Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silic...Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.展开更多
Over the past few years,the flexible quasi-solid-state zinc-ion hybrid supercapacitors(FQSS ZHSCs)have been found to be ideal for wearable electronics applications due to their high areal capacitance and energy densit...Over the past few years,the flexible quasi-solid-state zinc-ion hybrid supercapacitors(FQSS ZHSCs)have been found to be ideal for wearable electronics applications due to their high areal capacitance and energy density.The assembly of desirable ZHSCs devices that have promising practical applications is of high importance,whereas it is still challenging to assemble ZHSCs devices.In this study,a ZHSC that exhibited ultrahigh areal capacitance and high stability was developed by using an active carbon cloth(ACC)cathode,which could improve ionic adsorption.The as-obtained ACC cathode had an energy storage mechanism due to the electrical double-layer capacitive behavior of Zn^(2+),which was accompanied by the dissolution/deposition of Zn_(4)SO_(4)(OH)6·5H2O.The ACC//Zn@ACC ZHSC device exhibited an areal capacitance of 2437 mF cm^(−2)(81 F cm^(−3),203 F g^(-1) under the mass of ACC with∼12 mg cm^(−2))at 1 mA cm^(−2),an areal energy density of 1.354 mWh cm^(−2) at 1 mW cm^(−2),as well as high stability(with an insignificant capacitance decline after 20000 cycles),which was demonstrated to outperform the existing ZHSCs.Furthermore,the assembled flexible device still had competitive capacitance,energy density and service life when integrated into a FQSS ZHSC.When applied in practice,the device could achieve high mechanical flexibility,wearable stability and output.This study can inspire the development of the FQSS ZHSC device to satisfy the demands for wearable energy storage devices with high performance.展开更多
Spider-capture-silk(SCS)can directionally capture and transport water from humid air relying on the unique geometrical structure.Although there have been adequate reports on the fabrication of artificial SCSs from pet...Spider-capture-silk(SCS)can directionally capture and transport water from humid air relying on the unique geometrical structure.Although there have been adequate reports on the fabrication of artificial SCSs from petroleum-based materials,it remains a big challenge to innovate bio-based SCS mimicking fibers with high-performance fog collection ability and efficiency simultaneously.Herein,we report an eco-friendly and economical fiber system for water collection by coating gelatin on degummed silk.Compared to the previously reported fibers with the best fog collection ability(~13.10μL),Gelatin on silk fiber 10(GSF10)can collect larger water droplet(~16.70μL in 330 s)with~98%less mass.Meanwhile,the water collection efficiency of GSF10 demonstrates~72%and~48%enhancement to the existing best water collection polymer coated SCS fibers and spidroin eMaSp2 coated degummed silk respectively in terms of volume-to-TCL(vapor-liquid-solid three-phase contact line)index.The simultaneous function of superhydro-philicity,surface energy gradient,and~65%water-induced volume swelling of the gelatin knots are the key factors in advancing the water collection performance.Abundant availability of feedstocks and~75%improved space utiliza-tion guarantee the scalability and practical application of such bio-based fiber.展开更多
Recently,ammonium-ion(NH_(4)^(+))storage is in a booming stage in aqueous energy storage systems due to its multitudinous merits.To seek suitable electrode materials with excellent NH_(4)^(+)-storage is still in the e...Recently,ammonium-ion(NH_(4)^(+))storage is in a booming stage in aqueous energy storage systems due to its multitudinous merits.To seek suitable electrode materials with excellent NH_(4)^(+)-storage is still in the exploratory stage and full of challenge.Herein,an inorganic-polymer hybrid,poly(3,4-ethylenedioxithiophene)(PEDOT)intercalated hydrated vanadium oxide(VOH),named as VOH/PEDOT,is developed to tune the structure of VOH for boosting NH_(4)^(+)storage.By the intercalation of PEDOT,the interlayer space of VOH is increased from 11.5Åto 14.2Å,which notably facilitates the rapid transport of electrons and charges between layers and improves the electrochemical properties for NH_(4)^(+)storage.The achieved performances are much better than progressive NH_(4)^(+)hosting materials.In addition,the concentration of polyvinyl alcohol/ammonium chloride(PVA/NH_(4)Cl)electrolyte exerts a great impact on the NH_(4)^(+)storage in VOH/PEDOT.The VOH/PEDOT electrode delivers specific capacitance of 327 F g^(-1)in 1 M PVA/NH_(4)Cl electrolyte at-0.2–1 V.Furthermore,the quasi-solid-state VOH/PEDOT//active carbon hybrid supercapacitor(QSS VOH/PEDOT//AC HSC)device is assembled for NH_(4)^(+)storage,and it exhibits the capacitance of 328 mF cm^(-2)at 1 mA cm^(-2).The energy density of QSS VOH/PEDOT//AC NH4 t-HSC can reach 2.9 Wh m^(-2)(2.6 mWh cm^(-3),10.4 Wh kg^(-1))at 1 Wm^(-2)(0.9 mWh cm-3,35.7 W kg^(-1)).This work not only proves that the PEDOT intercalation can boost the NH_(4)^(+)storage capacity of vanadium oxides,but also provides a novel direction for the development of NH_(4)^(+)storage materials.展开更多
Interplay between macrophages and dendritic cells in the processing and presentation of bacterial antigens for T-cell immune responses remains poorly understood. Using a Listeria monocytogenes （Lm） infection model, ...Interplay between macrophages and dendritic cells in the processing and presentation of bacterial antigens for T-cell immune responses remains poorly understood. Using a Listeria monocytogenes （Lm） infection model, we demonstrate that dendritic cells （DCs） require the support of macrophages to elicit protective immunity against Lm infection. DCs themselves were inefficient at taking up Lm but capable of taking up microparticles （MPs） released by Lm-infected macrophages. These MPs transferred Lm antigens to DCs, allowing DCs to present Lm antigen to effector T cells. MP-mediated Lm antigen transfer required M HC class I participation, since M HC class I deficiency in macrophages resulted in a significant reduction of T-cell activation. Moreover, the vaccination of mice with MPs from Lm-infected macrophages produced strong protective immunity against Lm infection. We here identify an intrinsic antigen transfer program between macrophages and DCs during Lm infection, and emphasize that macrophages also play an essential role in DC-elicited Lm-specific T-cell responses.展开更多
The long-term immunity and functional recovery after SARS-CoV-2 infection have implications in preventive measures and patient quality of life.Here we analyzed a prospective cohort of 121 recovered COVID-19 patients f...The long-term immunity and functional recovery after SARS-CoV-2 infection have implications in preventive measures and patient quality of life.Here we analyzed a prospective cohort of 121 recovered COVID-19 patients from Xiangyang,China at 1-year after diagnosis.Among them,chemiluminescence immunoassay-based screening showed 99%(95%CI,98–100%)seroprevalence 10–12 months after infection,comparing to 0.8%(95%CI,0.7–0.9%)in the general population.Total anti-receptor-binding domain(RBD)antibodies remained stable since discharge,while anti-RBD IgG and neutralization levels decreased over time.A predictive model estimates 17%(95%CI,11–24%)and 87%(95%CI,80–92%)participants were still 50%protected against detectable and severe re-infection of WT SARS-CoV-2,respectively,while neutralization levels against B.1.1.7 and B.1.351 variants were significantly reduced.All non-severe patients showed normal chest CT and 21%reported COVID-19-related symptoms.In contrast,53%severe patients had abnormal chest CT,decreased pulmonary function or cardiac involvement and 79%were still symptomatic.Our findings suggest long-lasting immune protection after SARS-CoV-2 infection,while also highlight the risk of immune evasive variants and long-term consequences for COVID-19 survivors.展开更多
Synthetic glucocorticoid dexamethasone is the first trial-proven drug that reduces COVID-19 mortality by suppressing immune system.In contrast,interferons are a crucial component of host antiviral immunity and can be ...Synthetic glucocorticoid dexamethasone is the first trial-proven drug that reduces COVID-19 mortality by suppressing immune system.In contrast,interferons are a crucial component of host antiviral immunity and can be directly suppressed by glucocorticoids.To investigate whether therapeutic interferons can compensate glucocorticoids-induced loss of antiviral immunity,we retrospectively analyzed a cohort of 387 PCR-confirmed COVID-19 patients with quasi-random exposure to interferons and conditional exposure to glucocorticoids.Among patients receiving glucocorticoids,early interferon therapy was associated with earlier hospital discharge(adjusted HR 1.68,95%Cl 1.19-2.37)and symptom relief(adjusted HR 1.48;95%Cl 1.06-2.08),while these associations were insignificant among glucocorticoids nonusers.Early interferon therapy was also associated with lower prevalence of prolonged viral shedding(adjusted OR 0.24,95%Cl 0.10-0.57)only among glucocorticoids users.Additionally,these associations were glucocorticoid cumulative dose-and timing-dependent.These findings reveal potential therapeutic synergy between interferons and glucocorticoids in COVID-19 that warrants further investigation.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(DUT21LK34)Natural Science Foundation of Liaoning Province(2020-MS-113).
文摘Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.
基金supported the National Natural Science Foundation of China (21771030)Fundamental Research Funds for the Central Universities (DUT21LK34)Natural Science Foundation of Liaoning Province (2020-MS-113).
文摘Over the past few years,the flexible quasi-solid-state zinc-ion hybrid supercapacitors(FQSS ZHSCs)have been found to be ideal for wearable electronics applications due to their high areal capacitance and energy density.The assembly of desirable ZHSCs devices that have promising practical applications is of high importance,whereas it is still challenging to assemble ZHSCs devices.In this study,a ZHSC that exhibited ultrahigh areal capacitance and high stability was developed by using an active carbon cloth(ACC)cathode,which could improve ionic adsorption.The as-obtained ACC cathode had an energy storage mechanism due to the electrical double-layer capacitive behavior of Zn^(2+),which was accompanied by the dissolution/deposition of Zn_(4)SO_(4)(OH)6·5H2O.The ACC//Zn@ACC ZHSC device exhibited an areal capacitance of 2437 mF cm^(−2)(81 F cm^(−3),203 F g^(-1) under the mass of ACC with∼12 mg cm^(−2))at 1 mA cm^(−2),an areal energy density of 1.354 mWh cm^(−2) at 1 mW cm^(−2),as well as high stability(with an insignificant capacitance decline after 20000 cycles),which was demonstrated to outperform the existing ZHSCs.Furthermore,the assembled flexible device still had competitive capacitance,energy density and service life when integrated into a FQSS ZHSC.When applied in practice,the device could achieve high mechanical flexibility,wearable stability and output.This study can inspire the development of the FQSS ZHSC device to satisfy the demands for wearable energy storage devices with high performance.
基金The National Natural Science Foundation of China(Nos.52073186,52073241)State Key Laboratory of Polymer Materials Engineering(sklpme2021-3-01)+2 种基金Funding of Engineering Characteristic Team,Sichuan University(2020SCUNG122)Hong Kong General Research Fund(15201719)the Guangdong Basic and Applied Basic Research Foundation,Shenzhen Joint Fund,Youth Fund Project 2019(2019A1515111207).
文摘Spider-capture-silk(SCS)can directionally capture and transport water from humid air relying on the unique geometrical structure.Although there have been adequate reports on the fabrication of artificial SCSs from petroleum-based materials,it remains a big challenge to innovate bio-based SCS mimicking fibers with high-performance fog collection ability and efficiency simultaneously.Herein,we report an eco-friendly and economical fiber system for water collection by coating gelatin on degummed silk.Compared to the previously reported fibers with the best fog collection ability(~13.10μL),Gelatin on silk fiber 10(GSF10)can collect larger water droplet(~16.70μL in 330 s)with~98%less mass.Meanwhile,the water collection efficiency of GSF10 demonstrates~72%and~48%enhancement to the existing best water collection polymer coated SCS fibers and spidroin eMaSp2 coated degummed silk respectively in terms of volume-to-TCL(vapor-liquid-solid three-phase contact line)index.The simultaneous function of superhydro-philicity,surface energy gradient,and~65%water-induced volume swelling of the gelatin knots are the key factors in advancing the water collection performance.Abundant availability of feedstocks and~75%improved space utiliza-tion guarantee the scalability and practical application of such bio-based fiber.
基金supported by the Fundamental Research Funds for the Central Universities(DUT21LK34)Natural Science Foundation of Liaoning Province(2020-MS-113).
文摘Recently,ammonium-ion(NH_(4)^(+))storage is in a booming stage in aqueous energy storage systems due to its multitudinous merits.To seek suitable electrode materials with excellent NH_(4)^(+)-storage is still in the exploratory stage and full of challenge.Herein,an inorganic-polymer hybrid,poly(3,4-ethylenedioxithiophene)(PEDOT)intercalated hydrated vanadium oxide(VOH),named as VOH/PEDOT,is developed to tune the structure of VOH for boosting NH_(4)^(+)storage.By the intercalation of PEDOT,the interlayer space of VOH is increased from 11.5Åto 14.2Å,which notably facilitates the rapid transport of electrons and charges between layers and improves the electrochemical properties for NH_(4)^(+)storage.The achieved performances are much better than progressive NH_(4)^(+)hosting materials.In addition,the concentration of polyvinyl alcohol/ammonium chloride(PVA/NH_(4)Cl)electrolyte exerts a great impact on the NH_(4)^(+)storage in VOH/PEDOT.The VOH/PEDOT electrode delivers specific capacitance of 327 F g^(-1)in 1 M PVA/NH_(4)Cl electrolyte at-0.2–1 V.Furthermore,the quasi-solid-state VOH/PEDOT//active carbon hybrid supercapacitor(QSS VOH/PEDOT//AC HSC)device is assembled for NH_(4)^(+)storage,and it exhibits the capacitance of 328 mF cm^(-2)at 1 mA cm^(-2).The energy density of QSS VOH/PEDOT//AC NH4 t-HSC can reach 2.9 Wh m^(-2)(2.6 mWh cm^(-3),10.4 Wh kg^(-1))at 1 Wm^(-2)(0.9 mWh cm-3,35.7 W kg^(-1)).This work not only proves that the PEDOT intercalation can boost the NH_(4)^(+)storage capacity of vanadium oxides,but also provides a novel direction for the development of NH_(4)^(+)storage materials.
基金This work was supported by the National Basic Research Program of China （2012CB932500）, Funds for International Cooperation and Exchange of the National Natural Science Foundation of China （30911120482）, the Program for New Century Excellent Talents in University （NCET-08-0219） and the Fundamental Research Funds for the Central Universities （HUST-2010JC024, HUST-2011TS027）.
文摘Interplay between macrophages and dendritic cells in the processing and presentation of bacterial antigens for T-cell immune responses remains poorly understood. Using a Listeria monocytogenes （Lm） infection model, we demonstrate that dendritic cells （DCs） require the support of macrophages to elicit protective immunity against Lm infection. DCs themselves were inefficient at taking up Lm but capable of taking up microparticles （MPs） released by Lm-infected macrophages. These MPs transferred Lm antigens to DCs, allowing DCs to present Lm antigen to effector T cells. MP-mediated Lm antigen transfer required M HC class I participation, since M HC class I deficiency in macrophages resulted in a significant reduction of T-cell activation. Moreover, the vaccination of mice with MPs from Lm-infected macrophages produced strong protective immunity against Lm infection. We here identify an intrinsic antigen transfer program between macrophages and DCs during Lm infection, and emphasize that macrophages also play an essential role in DC-elicited Lm-specific T-cell responses.
基金This work was supported by Xiangyang Science and Technology Bureau(2020YL10,2020YL14,2020YL17,and 2020YL39)National Natural Science Foundation of China(31501116)+2 种基金Shenzhen Science and Technology Innovation Commission(JCYJ20190809100005672)Shenzhen Sanming Project of Medicine(SZSM201911013)US Department of Veterans Affairs(5I01BX001353).
文摘The long-term immunity and functional recovery after SARS-CoV-2 infection have implications in preventive measures and patient quality of life.Here we analyzed a prospective cohort of 121 recovered COVID-19 patients from Xiangyang,China at 1-year after diagnosis.Among them,chemiluminescence immunoassay-based screening showed 99%(95%CI,98–100%)seroprevalence 10–12 months after infection,comparing to 0.8%(95%CI,0.7–0.9%)in the general population.Total anti-receptor-binding domain(RBD)antibodies remained stable since discharge,while anti-RBD IgG and neutralization levels decreased over time.A predictive model estimates 17%(95%CI,11–24%)and 87%(95%CI,80–92%)participants were still 50%protected against detectable and severe re-infection of WT SARS-CoV-2,respectively,while neutralization levels against B.1.1.7 and B.1.351 variants were significantly reduced.All non-severe patients showed normal chest CT and 21%reported COVID-19-related symptoms.In contrast,53%severe patients had abnormal chest CT,decreased pulmonary function or cardiac involvement and 79%were still symptomatic.Our findings suggest long-lasting immune protection after SARS-CoV-2 infection,while also highlight the risk of immune evasive variants and long-term consequences for COVID-19 survivors.
基金This study was supported by US Department of Veterans Affairs(5101BX001353)National Natural Science Foundation of China(31501116)+1 种基金Shenzhen Sanming Project of Medicine(SZSM201911013)Shenzhen Science and Technology Innovation Commission(JCYJ20190809100005672).
文摘Synthetic glucocorticoid dexamethasone is the first trial-proven drug that reduces COVID-19 mortality by suppressing immune system.In contrast,interferons are a crucial component of host antiviral immunity and can be directly suppressed by glucocorticoids.To investigate whether therapeutic interferons can compensate glucocorticoids-induced loss of antiviral immunity,we retrospectively analyzed a cohort of 387 PCR-confirmed COVID-19 patients with quasi-random exposure to interferons and conditional exposure to glucocorticoids.Among patients receiving glucocorticoids,early interferon therapy was associated with earlier hospital discharge(adjusted HR 1.68,95%Cl 1.19-2.37)and symptom relief(adjusted HR 1.48;95%Cl 1.06-2.08),while these associations were insignificant among glucocorticoids nonusers.Early interferon therapy was also associated with lower prevalence of prolonged viral shedding(adjusted OR 0.24,95%Cl 0.10-0.57)only among glucocorticoids users.Additionally,these associations were glucocorticoid cumulative dose-and timing-dependent.These findings reveal potential therapeutic synergy between interferons and glucocorticoids in COVID-19 that warrants further investigation.
