Prussian blue analogs(PBAs)have emerged as environmentally friendly and structurally tunable cathode materials for aqueous ammonium-ion batteries(AIBs).However,the fundamental role of crystalline H_(2)O in regulating ...Prussian blue analogs(PBAs)have emerged as environmentally friendly and structurally tunable cathode materials for aqueous ammonium-ion batteries(AIBs).However,the fundamental role of crystalline H_(2)O in regulating ammonium-ion storage and transport remains poorly understood.In this study,we present a comprehensive comparison between hydrated NH_(4)NiHCF-H_(2)O and its anhydrous counterpart NH_(4)NiHCF,revealing the critical contribution of interstitial water to electrochemical performance.Structural and spectroscopic analyses confirm that interstitial water forms robust hydrogen bonds with NH_(4)+ions,stabilizing the PBA framework and mitigating structural degradation during cycling.Electrochemical measurements show that NH_(4)NiHCF-H_(2)O delivers a significantly higher specific capacity of 61 mA h g^(−1)at 0.2 C and markedly improved rate performance compared to NH_(4)NiHCF(48 mA h g^(−1)at 0.2 C).Kinetic analysis reveals that interstitial water enhances NH_(4)+diffusion,as evidenced by higher diffusion coefficients.Furthermore,density functional theory(DFT)calculations demonstrate that crystal water acts as a hydrogen bond acceptor,preferentially interacting with NH_(4)+and reducing the migration energy barrier,thereby facilitating fast ion transport.This work provides fundamental insights into the role of crystal water in PBAs and offers a rational design strategy for improving the kinetics,structural stability of PBAs cathodes for AIBs.展开更多
As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term...As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.展开更多
The principal challenge in optimizing biomass-derived hard carbon(HC)is the concurrent enhancement of specific capacity,cycling durability,and rate performance,as these properties are closely related to the disordered...The principal challenge in optimizing biomass-derived hard carbon(HC)is the concurrent enhancement of specific capacity,cycling durability,and rate performance,as these properties are closely related to the disordered carbon network and abundant pore structure.However,inadequate controllability of morphology,insufficiently regulated pore structures,and the complexity of post-processing modifications hinders the practical application of HC.In this work,a high-temperature and high-pressure expansion pretreatment technique is proposed to regulate the structure of starch precursors,enabling the precise design of ordered graphitic-like microcrystals and closed pores within HC.The optimized starch-based HC displayed remarkable electrochemical efficiency,with a reversible capacity of 332.0 mAh g^(-1),an initial Coulombic efficiency of 90.4%,and stable cycling over 3000 cycles.Meanwhile,advanced full-cell utilizing Na4Fe3(PO_(4))_(2)P_(2)O_(7) cathode achieve stable cycling performance exceeding 1000 cycles,demonstrating outstanding performance.This research innovatively employs a green expansion process to achieve structural regulation of HC,thereby providing an environmentally friendly and economically viable technical pathway for its large-scale production.展开更多
Alzheimer’s disease is initially thought to be caused by age-associated accumulation of plaques,in recent years,research has increasingly associated Alzheimer’s disease with lysosomal storage and metabolic disorders...Alzheimer’s disease is initially thought to be caused by age-associated accumulation of plaques,in recent years,research has increasingly associated Alzheimer’s disease with lysosomal storage and metabolic disorders,and the explanation of its pathogenesis has shifted from amyloid and tau accumulation to oxidative stress and impaired lipid and glucose metabolism aggravated by hypoxic conditions.However,the underlying mechanisms linking those cellular processes and conditions to disease progression have yet to be defined.Here,we applied a disease similarity approach to identify unknown molecular targets of Alzheimer’s disease by using transcriptomic data from congenital diseases known to increase Alzheimer’s disease risk,namely Down syndrome,Niemann-Pick type C disease,and mucopolysaccharidoses I.We uncovered common pathways,hub genes,and miRNAs across in vitro and in vivo models of these diseases as potential molecular targets for neuroprotection and amelioration of Alzheimer’s disease pathology,many of which have never been associated with Alzheimer’s disease.We then investigated common molecular alterations in brain samples from a Niemann-Pick type C disease mouse model by juxtaposing them with brain samples of both human and mouse models of Alzheimer’s disease.Detailed phenotypic,molecular,chronological,and biological aging analyses revealed that the Npc1tm(I1061T)Dso mouse model can serve as a potential short-lived in vivo model for brain aging and Alzheimer’s disease research.This research represents the first comprehensive approach to congenital disease association with neurodegeneration and a new perspective on Alzheimer’s disease research while highlighting shortcomings and lack of correlation in diverse in vitro models.Considering the lack of an Alzheimer’s disease mouse model that recapitulates the physiological hallmarks of brain aging,the short-lived Npc1^(tm(I1061T)Dso) mouse model can further accelerate the research in these fields and offer a unique model for understanding the molecular mechanisms of Alzheimer’s disease from a perspective of accelerated brain aging.展开更多
Objective Cerebral venous outflow disorders(CVOD)can impair cerebral perfusion and produce diverse,often debilitating symptoms,substantially reducing quality of life.Intermittent hypoxiahyperoxia training(IHHT)has dem...Objective Cerebral venous outflow disorders(CVOD)can impair cerebral perfusion and produce diverse,often debilitating symptoms,substantially reducing quality of life.Intermittent hypoxiahyperoxia training(IHHT)has demonstrated therapeutic potential across various pathologies and may represent a promising non-pharmacological approach for CVOD management.Methods Patients with imaging-confirmed CVOD underwent 14 IHHT sessions,each comprising four cycles of 10-minute hypoxia(11%O_(2))stimulation and 20-minute hyperoxia(38%O_(2)).Physiological parameters and adverse events were monitored throughout the intervention.Clinical scales,24-hour ambulatory blood pressure,blood tests,jugular ultrasound,and perfusion imaging were assessed preand post-intervention.Results No participants experienced intolerable discomfort or severe adverse events;vital signs remained within normal ranges.No significant changes were observed in 24-hour blood pressure,blood cell counts,lipid profiles,or other blood markers.Notably,60%of patients(n=12)reported overall symptom improvement on the Patient Global Impression of Change scale.Headache severity,as measured by the visual analogue scale,significantly decreased(6.33±1.22 vs.4.89±2.03,P=0.016).In patients with internal jugular vein(IJV)stenosis,significant improvements were observed in regional cerebral blood flow(including the insula,occipital lobe,internal capsule,and lenticula)and left J3-segment IJV flow volume(107.27[47.50,160.00]vs.140.83[55.00,210.00]mL/min,P=0.011).Conclusion The current IHHT protocol is safe and well-tolerated in patients with CVOD.IHHT may alleviate CVOD-related symptoms by improving oxygen saturation,cerebral perfusion,and venous outflow pattern,supporting its potential as a non-invasive therapeutic strategy.展开更多
Charge-transfer complexes(CTCs)have emerged as promising n-type organic thermoelectric(TE)materials due to their inherent high electrical conductivity and tunable transport polarities.In this study,we performed a comp...Charge-transfer complexes(CTCs)have emerged as promising n-type organic thermoelectric(TE)materials due to their inherent high electrical conductivity and tunable transport polarities.In this study,we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes(CnBTBT,n=4,8,12)as donors and fluorinated derivatives of tetracyanoquinodimethane(F_(m)TCNQ,m=0,2,4)as acceptors,aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure-property relationships.Our calculation results,based on the Boltzmann transport equation and deformation potential theory,reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties.Notably,the CnBTBT-F_(m)TCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics,particularly C4BTBT-F4TCNQ,which achieves an excellent power factor of 671µW cm^(-1) K^(-2) at an optimal charge carrier concentration.Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.展开更多
Melanoma Differentiation-Associated gene 5(MDA5)serves as a pattern recognition receptor(PRR)that identifies pathogen-associated molecular patterns(PAMPs),making it instrumental in antiviral defense.However,its non-ca...Melanoma Differentiation-Associated gene 5(MDA5)serves as a pattern recognition receptor(PRR)that identifies pathogen-associated molecular patterns(PAMPs),making it instrumental in antiviral defense.However,its non-canonical role in adaptive immunity,particularly in regulating B-cell immune functions,is poorly characterized.Here,we demonstrate that MDA5 is critical for the marginal zone(MZ)B-cell differentiation,B-cell receptor(BCR)signal transduction,and cytoskeletal dynamics.We determined that the MDA5-NF-κB-DNM1 axis governs actin polymerization and that this impairment in Mda5 knockout(KO)B cells can be rescued by the treatment with the dynamin1(DNM1)activator Bis-T-23.Furthermore,MDA5 deficiency induces metabolic perturbations in B cells,characterized by a reduced extracellular acidification rate(ECAR)and oxygen consumption rate(OCR),excessive reactive oxygen species(ROS)accumulation,and increased mitochondrial fission.Notably,taurine levels are decreased in Mda5 KO B cells,and in vitro taurine supplementation rescues impaired BCR signaling.Finally,MDA5-deficient mice exhibit a blunted humoral immune response.Overall,this study reveals the key functions and molecular mechanisms of MDA5 in B-cell differentiation,BCR signaling,and the humoral immune response.展开更多
基金supported by the National Natural Science Foundation of China (52172227)the Natural Science Foundation of Hubei Province (2023AFA114)+2 种基金the Guizhou Provincial Key Technology R&D Program (ZD[2025]019)provided by the Startup Fund (20QD80 and 22QD28)support from the Science&Technology Top Talents Program of Guizhou Province ([2024]349)
文摘Prussian blue analogs(PBAs)have emerged as environmentally friendly and structurally tunable cathode materials for aqueous ammonium-ion batteries(AIBs).However,the fundamental role of crystalline H_(2)O in regulating ammonium-ion storage and transport remains poorly understood.In this study,we present a comprehensive comparison between hydrated NH_(4)NiHCF-H_(2)O and its anhydrous counterpart NH_(4)NiHCF,revealing the critical contribution of interstitial water to electrochemical performance.Structural and spectroscopic analyses confirm that interstitial water forms robust hydrogen bonds with NH_(4)+ions,stabilizing the PBA framework and mitigating structural degradation during cycling.Electrochemical measurements show that NH_(4)NiHCF-H_(2)O delivers a significantly higher specific capacity of 61 mA h g^(−1)at 0.2 C and markedly improved rate performance compared to NH_(4)NiHCF(48 mA h g^(−1)at 0.2 C).Kinetic analysis reveals that interstitial water enhances NH_(4)+diffusion,as evidenced by higher diffusion coefficients.Furthermore,density functional theory(DFT)calculations demonstrate that crystal water acts as a hydrogen bond acceptor,preferentially interacting with NH_(4)+and reducing the migration energy barrier,thereby facilitating fast ion transport.This work provides fundamental insights into the role of crystal water in PBAs and offers a rational design strategy for improving the kinetics,structural stability of PBAs cathodes for AIBs.
基金the Young Elite Scientists Sponsorship Program by JXAST(2024QT11)the National Natural Science Foundation of China(22465001,22309003)the Jiangxi Provincial Natural Science Foundation(20232BAB203042,20242BAB22002).
文摘As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.
基金supported by the National Natural Science Foundation of China(5257043994)the Natural Science Foundation of Yunnan Province(202501AS070125,202501CF070129)+1 种基金the Innovation Capacity Construction and Enhancement Projects of Engineering Research Center of Yunnan Province(2023-XMDJ-00617107)the Scientific and Technological Project of Yunnan Precious Metals Laboratory(YPML-20240502015).
文摘The principal challenge in optimizing biomass-derived hard carbon(HC)is the concurrent enhancement of specific capacity,cycling durability,and rate performance,as these properties are closely related to the disordered carbon network and abundant pore structure.However,inadequate controllability of morphology,insufficiently regulated pore structures,and the complexity of post-processing modifications hinders the practical application of HC.In this work,a high-temperature and high-pressure expansion pretreatment technique is proposed to regulate the structure of starch precursors,enabling the precise design of ordered graphitic-like microcrystals and closed pores within HC.The optimized starch-based HC displayed remarkable electrochemical efficiency,with a reversible capacity of 332.0 mAh g^(-1),an initial Coulombic efficiency of 90.4%,and stable cycling over 3000 cycles.Meanwhile,advanced full-cell utilizing Na4Fe3(PO_(4))_(2)P_(2)O_(7) cathode achieve stable cycling performance exceeding 1000 cycles,demonstrating outstanding performance.This research innovatively employs a green expansion process to achieve structural regulation of HC,thereby providing an environmentally friendly and economically viable technical pathway for its large-scale production.
基金supported by the NIA/NIH(1K01AG060040).Studies performed by JN were funded by the NICHD/NIH(5R00HD096117)Microscopy Core Facility supported,in part,with funding from NIH-NCI Cancer Center Support Grant P30 CA016059.
文摘Alzheimer’s disease is initially thought to be caused by age-associated accumulation of plaques,in recent years,research has increasingly associated Alzheimer’s disease with lysosomal storage and metabolic disorders,and the explanation of its pathogenesis has shifted from amyloid and tau accumulation to oxidative stress and impaired lipid and glucose metabolism aggravated by hypoxic conditions.However,the underlying mechanisms linking those cellular processes and conditions to disease progression have yet to be defined.Here,we applied a disease similarity approach to identify unknown molecular targets of Alzheimer’s disease by using transcriptomic data from congenital diseases known to increase Alzheimer’s disease risk,namely Down syndrome,Niemann-Pick type C disease,and mucopolysaccharidoses I.We uncovered common pathways,hub genes,and miRNAs across in vitro and in vivo models of these diseases as potential molecular targets for neuroprotection and amelioration of Alzheimer’s disease pathology,many of which have never been associated with Alzheimer’s disease.We then investigated common molecular alterations in brain samples from a Niemann-Pick type C disease mouse model by juxtaposing them with brain samples of both human and mouse models of Alzheimer’s disease.Detailed phenotypic,molecular,chronological,and biological aging analyses revealed that the Npc1tm(I1061T)Dso mouse model can serve as a potential short-lived in vivo model for brain aging and Alzheimer’s disease research.This research represents the first comprehensive approach to congenital disease association with neurodegeneration and a new perspective on Alzheimer’s disease research while highlighting shortcomings and lack of correlation in diverse in vitro models.Considering the lack of an Alzheimer’s disease mouse model that recapitulates the physiological hallmarks of brain aging,the short-lived Npc1^(tm(I1061T)Dso) mouse model can further accelerate the research in these fields and offer a unique model for understanding the molecular mechanisms of Alzheimer’s disease from a perspective of accelerated brain aging.
基金sponsored by the National Natural Science Foundation of China(Nos.82027802,82101389,82274401,and 81971114)Beijing Nova Program(No.20230484286)+1 种基金Beijing Natural Science Foundation(7254366)the General Project of Science and Technology of Beijing Municipal Education Commission(No.KM202110025018).
文摘Objective Cerebral venous outflow disorders(CVOD)can impair cerebral perfusion and produce diverse,often debilitating symptoms,substantially reducing quality of life.Intermittent hypoxiahyperoxia training(IHHT)has demonstrated therapeutic potential across various pathologies and may represent a promising non-pharmacological approach for CVOD management.Methods Patients with imaging-confirmed CVOD underwent 14 IHHT sessions,each comprising four cycles of 10-minute hypoxia(11%O_(2))stimulation and 20-minute hyperoxia(38%O_(2)).Physiological parameters and adverse events were monitored throughout the intervention.Clinical scales,24-hour ambulatory blood pressure,blood tests,jugular ultrasound,and perfusion imaging were assessed preand post-intervention.Results No participants experienced intolerable discomfort or severe adverse events;vital signs remained within normal ranges.No significant changes were observed in 24-hour blood pressure,blood cell counts,lipid profiles,or other blood markers.Notably,60%of patients(n=12)reported overall symptom improvement on the Patient Global Impression of Change scale.Headache severity,as measured by the visual analogue scale,significantly decreased(6.33±1.22 vs.4.89±2.03,P=0.016).In patients with internal jugular vein(IJV)stenosis,significant improvements were observed in regional cerebral blood flow(including the insula,occipital lobe,internal capsule,and lenticula)and left J3-segment IJV flow volume(107.27[47.50,160.00]vs.140.83[55.00,210.00]mL/min,P=0.011).Conclusion The current IHHT protocol is safe and well-tolerated in patients with CVOD.IHHT may alleviate CVOD-related symptoms by improving oxygen saturation,cerebral perfusion,and venous outflow pattern,supporting its potential as a non-invasive therapeutic strategy.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Science(No.XDB0520000)the National Natural Science Foundation of China(Nos.52273170 and 52394271)the National Key R&D Program of China(No.2022YFA1203200).
文摘Charge-transfer complexes(CTCs)have emerged as promising n-type organic thermoelectric(TE)materials due to their inherent high electrical conductivity and tunable transport polarities.In this study,we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes(CnBTBT,n=4,8,12)as donors and fluorinated derivatives of tetracyanoquinodimethane(F_(m)TCNQ,m=0,2,4)as acceptors,aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure-property relationships.Our calculation results,based on the Boltzmann transport equation and deformation potential theory,reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties.Notably,the CnBTBT-F_(m)TCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics,particularly C4BTBT-F4TCNQ,which achieves an excellent power factor of 671µW cm^(-1) K^(-2) at an optimal charge carrier concentration.Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.
基金supported by the National Natural Science Foundation of China(82371784,32311530061)the National Key Research and Development Program of China(2023YFC2507900,2023YFC2706300)+2 种基金R&D Program of Guangzhou Laboratory(SRPG22-006)State Key Laboratory for Diagnosis and Treatment of Severe Zoonotic Infectious Diseases(2024ZZ10014)the Hubei Provincial Natural Science Foundation of China(Grant number:2024AFB634).
文摘Melanoma Differentiation-Associated gene 5(MDA5)serves as a pattern recognition receptor(PRR)that identifies pathogen-associated molecular patterns(PAMPs),making it instrumental in antiviral defense.However,its non-canonical role in adaptive immunity,particularly in regulating B-cell immune functions,is poorly characterized.Here,we demonstrate that MDA5 is critical for the marginal zone(MZ)B-cell differentiation,B-cell receptor(BCR)signal transduction,and cytoskeletal dynamics.We determined that the MDA5-NF-κB-DNM1 axis governs actin polymerization and that this impairment in Mda5 knockout(KO)B cells can be rescued by the treatment with the dynamin1(DNM1)activator Bis-T-23.Furthermore,MDA5 deficiency induces metabolic perturbations in B cells,characterized by a reduced extracellular acidification rate(ECAR)and oxygen consumption rate(OCR),excessive reactive oxygen species(ROS)accumulation,and increased mitochondrial fission.Notably,taurine levels are decreased in Mda5 KO B cells,and in vitro taurine supplementation rescues impaired BCR signaling.Finally,MDA5-deficient mice exhibit a blunted humoral immune response.Overall,this study reveals the key functions and molecular mechanisms of MDA5 in B-cell differentiation,BCR signaling,and the humoral immune response.
