The landscape of breast cancer treatment has undergone a transformative shift with the integration of immunotherapy.Historically considered a“cold”tumor with limited immunogenicity,breast cancer management was domin...The landscape of breast cancer treatment has undergone a transformative shift with the integration of immunotherapy.Historically considered a“cold”tumor with limited immunogenicity,breast cancer management was dominated by surgery,chemotherapy,radiotherapy,and targeted therapies1.However,the advent of immune checkpoint inhibitors(ICIs)has challenged this paradigm,opening a new frontier.The initial breakthrough in triple-negative breast cancer(TNBC)demonstrated that a subset of patients could derive profound and durable clinical benefit from pembrolizumab and atezolizumab2,3.Today,precision immunotherapy aims to identify the patients most likely to respond,to convert immunologically silent tumors into responsive tumors,and to strategically combine immunotherapies with other modalities to overcome resistance.This evolution from empirical application to biomarker-driven strategies marks the critical juncture at which we stand,transitioning promising clinical trial data into refined,effective,and accessible clinical practice4.Recent key clinical studies on breast cancer immunotherapy are summarized in Table 1.展开更多
Hydrogen has emerged as a promising clean energy source,leading to numerous recent efforts to integrate hydrogen into turbine engine applications[1].This integration has the potential to significantly enhance engine e...Hydrogen has emerged as a promising clean energy source,leading to numerous recent efforts to integrate hydrogen into turbine engine applications[1].This integration has the potential to significantly enhance engine efficiency while reducing carbon dioxide emissions[2].However,the degradation of nickel alloys induced by hydrogen has been well documented[3-7].Consequently,hydrogen-assisted failure of nickel alloys poses a critical concern for the design and safe operation of hydrogen-powered turbine engines.展开更多
High-performance lithium metal batteries benefit from the construction of composite polymer electrolytes(CPEs)which are synthesized by incorporating inorganic fillers into polymer matrices[1].However,the random distri...High-performance lithium metal batteries benefit from the construction of composite polymer electrolytes(CPEs)which are synthesized by incorporating inorganic fillers into polymer matrices[1].However,the random distribution of added fillers within the polymer matrix can lead to tortuous ion pathways and longer transmission distances(Fig.1).As a result,the ion transport capability of CPEs may decrease,while interface contact may deteriorate.Therefore,the organized arrangement of fillers emerges as a crucial consideration in constructing electrolyte membranes.One highly effective approach is the adoption of a vertically aligned filler configuration,where ceramic fillers are constructed to be perpendicular to the electrolyte membrane.If so,the filler/electrolyte interface impedance can be significantly reduced,while continuous ion transport channels along the specified direction are formed,thus significantly enhancing the ion conduction(Fig.1(a))[1].展开更多
The unique wave-manipulation capabilities of zero-index metamaterials(ZIMs)offer a new opportunity for realizing bound states in the continuum(BICs).However,the relationship between anomalous scattering and BICs remai...The unique wave-manipulation capabilities of zero-index metamaterials(ZIMs)offer a new opportunity for realizing bound states in the continuum(BICs).However,the relationship between anomalous scattering and BICs remains underexplored when parity–time(PT)symmetry is introduced.In this work,we demonstrate that a BIC splits into a pair of lasing modes carrying opposite topological charges by introducing PT symmetry through gain-loss cylinders embedded in ZIM layers.Theoretical analysis and numerical simulations reveal that lasing and unidirectional transparency phenomena result from the singularities and exceptional points of the scattering matrix.Moreover,exceptional points can be tuned via propagation phase modulation in the air gap,and their coalescence produces quasi-BICs with symmetric responses.This work provides a framework for manipulating BICs and topological lasing modes in non-Hermitian systems,offering new insights for designing non-Hermitian photonic devices.展开更多
The introduction of iron significantly enhances the catalytic activity of a catalytic system for the oxygen evolution reaction(OER).However,the high dissolution tendency of iron components may lead to irreversible los...The introduction of iron significantly enhances the catalytic activity of a catalytic system for the oxygen evolution reaction(OER).However,the high dissolution tendency of iron components may lead to irreversible loss of active sites,thereby compromising the long-term stability of the catalytic system.Herein,we constructed a heterostructure of FeOOH decorated Ce-Ni_(3)S_(2)/NiS(FeOOH,Ce-Ni_(3)S_(2)/NiS)on a nickel foam substrate through a combined approach of hydrothermal sulfidation and electrochemical activation.By establishing a dynamic dissolution-adsorption equilibrium between Fe^(3+)in the electrolyte and the surface FeOOH layer,the loss of active sites was effectively mitigated.Simultaneously,the Fe(3d)-Ce(4f)orbital coupling effectively modulates the electronic structure of metal active centers,constructing a highly stable Ni_(3)S_(2)/NiS electrocatalytic system.OER performance tests show that the catalyst delivers 266 mV overpotential to achieve 100 mA cm^(-2),while demonstrating exceptional durability by maintaining stability for 100 h at an ultrahigh current density of 2.0 A cm^(-2).In addition,an anion-exchange membrane(AEM)electrolyzer(FeOOH,Ce-Ni_(3)S_(2)/NiS//Pt)maintains operation continuously for 100 hours at 1000 mA cm^(-2).This study proposes an electrolyte-mediated dynamic interface regulation strategy,providing new design principles for developing industrial water electrolysis catalysts with both high activity and exceptional stability.展开更多
The self-reconstruction of Ni-based electrodes and the in situ generation of oxy-hydroxides are widely investigated as crucial prerequisites for efficient oxygen evolution reaction(OER).However,the transformation is u...The self-reconstruction of Ni-based electrodes and the in situ generation of oxy-hydroxides are widely investigated as crucial prerequisites for efficient oxygen evolution reaction(OER).However,the transformation is usually time-consuming and surface-limited,resulting in insufficient active sites with unsatisfactory intrinsic activity.Herein,we provide a NH_(3)-treated Fe-doped NiMoO_(4) hydrate as a highly active OER pre-catalyst,with an overpotential of only 240 mV at 100 mA cm^(−2) and 270 mV at 300 mA cm^(−2).By combination of multiple quasi-situ and in situ techniques,the enhanced performance is ascribed to the lattice distortion in the pre-catalyst induced by the NH_(3) treatment.Firstly,the lattice defects with tensile strain and voids accelerate the selective dissolution of MoO_(4)^(2−)and ensure the rapid and bulk reconstruction of the pre-catalyst with enriched active sites.Moreover,it could modulate the electronic structure and optimize the synergism between Ni and Fe,facilitating the dynamic evolution of Fe-doped γ-NiOOH(γ-Ni(Fe)OOH).The intimately interacted Ni–Fe dual-sites from γ-Ni(Fe)OOH and the resultant distorted structure facilitate the formation and adsorption of active oxygen species,accounting for the improved intrinsic activity for OER.展开更多
Linker conformation engineering provides opportunities for the structural diversity of coordination polymers(CPs);however,the approaches for modulating the synthesis solvents to influence linker conformation are very ...Linker conformation engineering provides opportunities for the structural diversity of coordination polymers(CPs);however,the approaches for modulating the synthesis solvents to influence linker conformation are very limited,and they are facing unpredictable challenges to date.Herein,through strategies of solvent-oriented structural self-assembly and solvent-induced single-crystal to single-crystal transformation,eight structurally distinct Cd-CPs were controllably synthesized with the same linkers for the first time.The decisive role of solvents in the self-assembly and transformations in CPs has been demonstrated in depth.Besides,rare reversible CP-based phase transition phenomena at low temperatures were observed.One of these represents the first example of an unprecedented turn-on–off CP-based Fe^(3+)ion sensor.展开更多
Ni-based materials have emerged as promising anode electrocatalysts that can replace noble metals for the methanol oxidation reaction(MOR).However,the potential applications of Ni-based metal–organic gels(Ni-MOGs)in ...Ni-based materials have emerged as promising anode electrocatalysts that can replace noble metals for the methanol oxidation reaction(MOR).However,the potential applications of Ni-based metal–organic gels(Ni-MOGs)in MOR have rarely been recognized.In this study,using the readily prepared Al-MOG(MIL-53(Al))without MOR activity as a template,we fabricated AlNi-MOG and AlNi-based trimetallic MOGs(Cu,Co and Fe)by a simple solvothermal method,which could be directly used as electrocatalysts for the MOR.Among them,the as-obtained AlNiCu-MOG exhibited better MOR activity with an area-specific peak current density of 17.1 mA cm^(−2)than AlNi-MOG(11.46 mA cm^(−2)),which could be attributed to the electron coupling between Ni and Cu.Moreover,the addition of the conductive material acetylene black(AB)could immensely increase the electric conductivity of AlNiCu-MOG,leading to its improved MOR activity with a peak current density of 33.24 mA cm^(−2).These results represent an important first step towards the application of MOGs in the MOR.展开更多
Molybdenum sulfide(MoS_(2))with a high theoretical capacity and large interlayer distance has triggered extensive attention as a promising alternative anode for lithium ion batteries(LIBs)and sodium ion batteries(SIBs...Molybdenum sulfide(MoS_(2))with a high theoretical capacity and large interlayer distance has triggered extensive attention as a promising alternative anode for lithium ion batteries(LIBs)and sodium ion batteries(SIBs).However,the sluggish kinetics and structural collapse induced by its poor conductivity usually lead to unsatisfactory rate capability and poor cycling performance.Herein,few-layered MoS_(2) with abundant S vacancies were anchored on V_(2)C-MXene and embedded in carbon via an in situ assembly and carbonization strategy.The V_(2)C-MXene substrate suppressed the agglomeration and stacking of MoS_(2) nanosheets,facilitated the efficient exposure of MoS_(2) and shortened the diffusion pathways,which favored ion accessibility and induced a strong capacitive-controlled charge storage behavior.Experimental results and theoretical calculations revealed that the electronic coupling between MoS_(2) and V_(2)C-MXene not only induced abundant S vacancies and modulated the charge distribution but also promoted Li/Na adsorption and lowered the ion diffusion energy barrier.Consequently,the V_(2)C-MXene coupled MoS_(2)@C electrode delivered high capacities of 732.8 and 337.3 mA h g^(-1) at 1 A g^(-1) in LIBs and SIBs,respectively.This work provided a new insight into the rational design of stable and advanced electrode materials for energy storage and conversion.展开更多
Photocatalytic two-electron oxygen reduction offers a sustainable method to produce hydrogen peroxide(H_(2)O_(2)).However,the efficiency of carbon nitride(CN)in this process is hindered by serious charge recombination...Photocatalytic two-electron oxygen reduction offers a sustainable method to produce hydrogen peroxide(H_(2)O_(2)).However,the efficiency of carbon nitride(CN)in this process is hindered by serious charge recombination and slow diffusion of oxygen.This work reports the thermal vapor-assisted surface chemical modification of CN by 4-aminobenzoyl groups(PABA/CN),which alters the conjugation system,extends the light absorption range,and enhances charge separation and electron transfer.Besides,it tunes the CN surface to be hydrophobic,which forms a gas/solid/liquid triphase interface in photocatalytic H_(2)O_(2)production,and thus significantly improves O_(2) diffusion and proton supply for photosynthesis of H_(2)O_(2).Photocatalytic experiments revealed that PABA/CN delivered an H_(2)O_(2)yield of up to 745μmol g^(-1)h^(-1)in pure water,8 times that of pristine CN,ranking among the top performances of CNbased photocatalysts.Moreover,its selectivity reached 70%.Mechanism studies identified a two-step one-electron oxygen reduction reaction pathway for H_(2)O_(2)photoproduction.Overall,this work simultaneously addresses the issues of mass transfer of O_(2),light harvesting,and charge separation of CN in photosynthesis of H_(2)O_(2)via surface chemical modification with 4-aminobenzoyl moieties,which extendsπ-conjugation and imparts surface hydrophobicity.展开更多
Ligand engineering is crucial for tailoring the catalytic and fluorescence properties of gold nanoclusters(AuNCs).However,the mechanisms through which ligands synergistically affect these properties remain largely une...Ligand engineering is crucial for tailoring the catalytic and fluorescence properties of gold nanoclusters(AuNCs).However,the mechanisms through which ligands synergistically affect these properties remain largely unexplored.Here we employed single-molecule fluorescence microscopy and ensemble fluorescence spectroscopy to investigate how water-soluble thiol ligands modulate the fluorescence and catalytic activities of AuNCs.Our findings reveal that small ligands,such as 3-mercaptopropionic acid(MPA),provide high catalytic activity,despite lacking fluorescence.Medium-sized ligands,like glutathione(GSH)and the lysine-cysteine-lysine(KCK)peptide,enhance fluorescence and maintain catalytic activity through their stable ligand structures and non-competitive mechanisms.Large protein ligands,such as bovine serum albumin(BSA),significantly increase fluorescence and catalytic activity by controlling their conformation to enhance substrate adsorption but experience reduced catalytic rates due to their competitive binding at high substrate concentrations.Additionally,pH levels influence these properties,with fluorescence intensity increasing under alkaline conditions and catalytic activity peaking in acidic environments for small and medium-sized ligand-AuNCs.For BSA-AuNCs,optimal activity is observed at neutral pH due to favorable protein conformation,where enhanced substrate adsorption has a more significant impact on the catalytic rate than merely exposing gold active sites.These insights into the ligand size and structure-dependent modulation of the catalytic and fluorescence properties of AuNCs lay a foundation for designing efficient fluorescent catalysts.展开更多
Local structure engineering is one of the most useful strategies for tunable down-shifting and upconversion emissions in halide double perovskites(DPs).However,the roles of the local structure,including local symmetry...Local structure engineering is one of the most useful strategies for tunable down-shifting and upconversion emissions in halide double perovskites(DPs).However,the roles of the local structure,including local symmetry,coordination structure,and active sites,in these DPs remain largely unexplored.Herein,we studied the local structure-correlated up/down-conversion luminescence in Yb^(3+)/Er^(3+)/Ho^(3+)co/tridoped Cs_(2)LiInCl_(6) with a unique local structure.展开更多
Small-sized Pt-based intermetallic compounds(IMCs)with unique electronic and geometrical structures are promising candidates as next-generation oxygen-reduction reaction(ORR)catalysts in protonexchange membrane fuel c...Small-sized Pt-based intermetallic compounds(IMCs)with unique electronic and geometrical structures are promising candidates as next-generation oxygen-reduction reaction(ORR)catalysts in protonexchange membrane fuel cells(PEMFCs).However,the synthesis of IMC catalysts remains challenging owing to the trade-off relation between the alloying/ordering degree and particle aggregation/sintering under a high-temperature annealing process.Herein,we demonstrate a cuprous sulfide(Cu_(1.96)S)intermediate-assisted strategy for the scalable synthesis of PtCu_(3) intermetallic electrocatalysts on an S-doped carbon black support.We identify that the Cu_(1.96)S intermediate formed at low temperature gradually releases metallic Cu species at high temperatures to form a small-sized and uniform Pt-Cu alloy with target stoichiometry,which eventually ensures the formation of well-ordered intermetallic PtCu_(3) structures.The prepared intermetallic PtCu_(3) catalysts exhibit enhanced ORR performance with a mass activity of 3.2 A mg_(Pt)^(-1) and retain 72%of the initial activity after durability tests.展开更多
Developing stable and efficient single-atom electrocatalysts for the acidic oxygen evolution reaction(OER)is crucial for advancing proton exchange membrane water electrolysis(PEMWE).However,the lack of precisely tailo...Developing stable and efficient single-atom electrocatalysts for the acidic oxygen evolution reaction(OER)is crucial for advancing proton exchange membrane water electrolysis(PEMWE).However,the lack of precisely tailored coordination environments capable of preventing Ir single-atom dissolution remains a critical barrier.Herein,we construct Ir single-atom catalysts supported on Co_(3)O_(4)(IrSA-Co_(3)O_(4))via the synchronized formation of Co defects and the immobilization of Ir single atoms during precursor pyrolysis.Atomically dispersed Ir atoms are anchored at octahedral Co defect sites,forming a configuration of single atoms confined within the spinel lattice.Benefiting from the oxygen-bridged electronic coupling within the Ir–O–Co configuration,the electronic structure of Ir sites is optimized to enable moderate intermediate adsorption while mitigating dissolution.As a result,IrSA-Co_(3)O_(4)achieves a low overpotential of 199 mV at 10 mA cm^(−2)in 0.5 M H_(2)SO_(4)and operates stably for 150 h at 200 mA cm^(−2)during PEMWE.This work provides new insights into the rational design of stable single-atom catalysts for acidic OER by effectively suppressing active-site dissolution.展开更多
To the Editor:Chinese herbal medicines(CHMs)are critical components of traditional Chinese medicine(TCM),[1]with their cold and hot properties being fundamental for guiding clinical applications and ensuring therapeut...To the Editor:Chinese herbal medicines(CHMs)are critical components of traditional Chinese medicine(TCM),[1]with their cold and hot properties being fundamental for guiding clinical applications and ensuring therapeutic efficacy.[2]However,the traditional method of identifying the cold and hot properties of CHMs relies heavily on the subjective experience of TCM practitioners and clinical practice,often leading to uncertainty and inconsistency.As such,there is a pressing need for more precise,rapid,and objective strategies to accurately identify the cold and hot properties of CHMs and their active ingredients.展开更多
The Realgar-Indigo Naturalis formula(RIF)is a proprietary Chinese medicine,which is one of the important drugs in the treatment of pediatric acute promyelocytic leukemia(APL).However,the dose of RIF in clinical applic...The Realgar-Indigo Naturalis formula(RIF)is a proprietary Chinese medicine,which is one of the important drugs in the treatment of pediatric acute promyelocytic leukemia(APL).However,the dose of RIF in clinical application is not uniform and the long-term effectiveness and safety of combining RIF with all-trans retinoic acid(ATRA)in a larger population of pediatric APL patients remains undocumented.We conducted a multicenter single-arm clinical trial(ChiCTR-OIC-16010014)in China.Individuals newly diagnosed with APL were treated with CCCG-APL-2017 protocol which is based on RIF and ATRA in consolidation.The event-free survival(EFS)and overall survival(OS)outcomes were evaluated.We recruited 200 patients diagnosed with APL.The six-year OS rate was 100%in the low-risk(LR)group and 97.6%in the high-risk(HR)group.The six-year EFS rate was 98.3%in the LR group and 97.6%in the HR group.Plasma levels of arsenic remained stable after the administration of RIF at a dosage of 60 mg/kg/d for seven days and returned to baseline levels within fourteen days after discontinuation of RIF administration,which is consistent with a concentration of 135 mg/d/kg.Furthermore,controlling white blood cells(WBC)to maintain levels at or below 30×10^(9)/L during induction therapy can decrease the incidence of induced differentiation syndrome(DS)or alleviate its symptoms.Our study demonstrated that the CCCG-APL-2017 protocol,which combines RIF with ATRA,is both effective and safe in treating children with APL.展开更多
Chiral metal-organic frameworks(CMOFs),an emerging class of heterogeneous chiral catalysts,show significant potential for application in asymmetric catalysis due to their tunable pore shapes and sizes,large internal s...Chiral metal-organic frameworks(CMOFs),an emerging class of heterogeneous chiral catalysts,show significant potential for application in asymmetric catalysis due to their tunable pore shapes and sizes,large internal surface areas,and rich chiral environments[1-4].Through over 20 years of development,researchers have invested heavily in exploring new CMOFs to enhance asymmetric catalytic performance[5-10].However,the dual pursuit of a substantial specific surface area and robust stability within a single CMOF presents a considerable challenge.Additionally,efficient CMOF catalysts,frequently synthesized from privileged chiral ligands such as proline,2,2'-bis(diphenylphosphino)-1,1'-binaph thyl(BINAP),Salen,and bis(oxazoline)(Box)[11,12],tend to exhibit more complex structures compared to their corresponding privileged chiral counterparts,thereby necessitating higher production costs.Consequently,the development of novel synthetic methodologies for constructing CMOFs as effective chiral catalysts remains a challenging endeavor.展开更多
Introduction:Vaccination stands as the most effective preventive measure against yellow fever(YF).However,the YF vaccination associated Adverse Events following Immunization(AEFI)cases occur occasionally.Methods:The G...Introduction:Vaccination stands as the most effective preventive measure against yellow fever(YF).However,the YF vaccination associated Adverse Events following Immunization(AEFI)cases occur occasionally.Methods:The Guangdong Provincial Center for Disease Control and Prevention utilized Targeted Next-Generation Sequencing(tNGS)to determine whether the imported suspected YF case was infected by the wild-type YF virus strain or experienced an AEFI.Results:tNGS analysis successfully yielded a 10.2 kb viral genomic sequence.Subsequent in-depth analysis revealed high similarity to the YF vaccine strain 17D-213 and classified the sequence within the West Africa II genotype,clustering with the 17D vaccine strain.Conclusions and Implications for Public Health Practice:This case represented YF AEFI.The implementation of tNGS technology enables more precise and expeditious pathogen sequencing,providing critical evidence for accurate disease diagnosis and informed public health interventions.展开更多
Flexible hybrid systems usually combine soft modules(mechanically matched with skin or clothes)and hard modulus(like rigid circuits).However,the risk of interface failure due to modulus mismatch between flexible compo...Flexible hybrid systems usually combine soft modules(mechanically matched with skin or clothes)and hard modulus(like rigid circuits).However,the risk of interface failure due to modulus mismatch between flexible components and rigid circuits limits the system’s complexity and durability.The diverse features of flexible components further complicate the development of a universal interface.In this work,we demonstrated a cocoon-mimetic feature-matched interface(CFI)that offers stable electrical contact with flexible surface.It also matches flexible systems features in stretchability(lower than 0.22Ωcm^(-1)during 900%elongation),durability(stable resistance after 20000 times 100%elongation),breathability(gas permeability 614 mm S^(-1))and self-adhesive(0.18±0.01 N mm^(-1)).We developed a direct spray-on-skin sensor and used CFI to form a hand task recognition system.This system,deployable in seconds,has 97.7%accuracy in recognition of eight hand tasks.This research offers a promising solution for flexible hybrid systems interfacing challenges.展开更多
Transient electronics,comprising of degradable devices that disintegrate and disappear after their operational life,has received considerable interest in recent years because of the concerns related to the rapidly gro...Transient electronics,comprising of degradable devices that disintegrate and disappear after their operational life,has received considerable interest in recent years because of the concerns related to the rapidly growing electronic waste(e-waste).However,the degradability or biodegradability of electronic devices alone is insufficient to ascertain environmental safety.The evaluation of the nature of degradation by-products is also essential to assess the environmental impact of a degradable device.Herein,we investigate systematically the hydrolytic degradation by-products of two different types of devices viz.a capacitive pressure sensor and a photodetector,using liquid chromatograph mass spectrometry.The findings reveal that,despite the inherent degradability of constituent materials used in an electronic device,the released by-products can be toxic or could be complex molecules with unknown chemistry such as carcinogenic or contain almost non-degradable polystyrene derivatives/microplastic(e.g.,from PEDOT:PSS),or have copper complexes resulting from degraded silk fibroin and poly(ethylene oxide)mass fragments.This analysis underlines the need for careful selection and reassessment of materials employed in transient electronics,as an important factor,to mitigate the end-of-life issues associated with electronics and its environmental impact.展开更多
基金supported by the Non-communicable Chronic Diseases National Science and Technology Major Project(Grant No.2025ZD0544003).
文摘The landscape of breast cancer treatment has undergone a transformative shift with the integration of immunotherapy.Historically considered a“cold”tumor with limited immunogenicity,breast cancer management was dominated by surgery,chemotherapy,radiotherapy,and targeted therapies1.However,the advent of immune checkpoint inhibitors(ICIs)has challenged this paradigm,opening a new frontier.The initial breakthrough in triple-negative breast cancer(TNBC)demonstrated that a subset of patients could derive profound and durable clinical benefit from pembrolizumab and atezolizumab2,3.Today,precision immunotherapy aims to identify the patients most likely to respond,to convert immunologically silent tumors into responsive tumors,and to strategically combine immunotherapies with other modalities to overcome resistance.This evolution from empirical application to biomarker-driven strategies marks the critical juncture at which we stand,transitioning promising clinical trial data into refined,effective,and accessible clinical practice4.Recent key clinical studies on breast cancer immunotherapy are summarized in Table 1.
基金supported by the Science Center for Gas Turbine Project(No.P2022-B-IV-009-002).
文摘Hydrogen has emerged as a promising clean energy source,leading to numerous recent efforts to integrate hydrogen into turbine engine applications[1].This integration has the potential to significantly enhance engine efficiency while reducing carbon dioxide emissions[2].However,the degradation of nickel alloys induced by hydrogen has been well documented[3-7].Consequently,hydrogen-assisted failure of nickel alloys poses a critical concern for the design and safe operation of hydrogen-powered turbine engines.
基金supported by the National Natural Science Foundation of China(No.51972293)Hangzhou Key Research Program Project(2023SZD0099)LingYan Project(2024C01090).
文摘High-performance lithium metal batteries benefit from the construction of composite polymer electrolytes(CPEs)which are synthesized by incorporating inorganic fillers into polymer matrices[1].However,the random distribution of added fillers within the polymer matrix can lead to tortuous ion pathways and longer transmission distances(Fig.1).As a result,the ion transport capability of CPEs may decrease,while interface contact may deteriorate.Therefore,the organized arrangement of fillers emerges as a crucial consideration in constructing electrolyte membranes.One highly effective approach is the adoption of a vertically aligned filler configuration,where ceramic fillers are constructed to be perpendicular to the electrolyte membrane.If so,the filler/electrolyte interface impedance can be significantly reduced,while continuous ion transport channels along the specified direction are formed,thus significantly enhancing the ion conduction(Fig.1(a))[1].
基金supported by the National Natural Science Foundation of China(Grant Nos.12504361,12274313,and 62465005)the Natural Science Foundation of Guangxi(Grant No.2025GXNSFBA069179)the Guangxi Colleges and Universities Young and Middle-aged Teachers’Basic Scientific Research Ability Enhancement Project(Grant No.2025KY0093)。
文摘The unique wave-manipulation capabilities of zero-index metamaterials(ZIMs)offer a new opportunity for realizing bound states in the continuum(BICs).However,the relationship between anomalous scattering and BICs remains underexplored when parity–time(PT)symmetry is introduced.In this work,we demonstrate that a BIC splits into a pair of lasing modes carrying opposite topological charges by introducing PT symmetry through gain-loss cylinders embedded in ZIM layers.Theoretical analysis and numerical simulations reveal that lasing and unidirectional transparency phenomena result from the singularities and exceptional points of the scattering matrix.Moreover,exceptional points can be tuned via propagation phase modulation in the air gap,and their coalescence produces quasi-BICs with symmetric responses.This work provides a framework for manipulating BICs and topological lasing modes in non-Hermitian systems,offering new insights for designing non-Hermitian photonic devices.
基金supported by the National Natural Science Foundation of China(22479161 and 52274308)the Research and Application of High-Efficiency Hydrogen Production Technology(2024YQX202)the Fundamental Research Funds for the Central Universities(24CX03012A).
文摘The introduction of iron significantly enhances the catalytic activity of a catalytic system for the oxygen evolution reaction(OER).However,the high dissolution tendency of iron components may lead to irreversible loss of active sites,thereby compromising the long-term stability of the catalytic system.Herein,we constructed a heterostructure of FeOOH decorated Ce-Ni_(3)S_(2)/NiS(FeOOH,Ce-Ni_(3)S_(2)/NiS)on a nickel foam substrate through a combined approach of hydrothermal sulfidation and electrochemical activation.By establishing a dynamic dissolution-adsorption equilibrium between Fe^(3+)in the electrolyte and the surface FeOOH layer,the loss of active sites was effectively mitigated.Simultaneously,the Fe(3d)-Ce(4f)orbital coupling effectively modulates the electronic structure of metal active centers,constructing a highly stable Ni_(3)S_(2)/NiS electrocatalytic system.OER performance tests show that the catalyst delivers 266 mV overpotential to achieve 100 mA cm^(-2),while demonstrating exceptional durability by maintaining stability for 100 h at an ultrahigh current density of 2.0 A cm^(-2).In addition,an anion-exchange membrane(AEM)electrolyzer(FeOOH,Ce-Ni_(3)S_(2)/NiS//Pt)maintains operation continuously for 100 hours at 1000 mA cm^(-2).This study proposes an electrolyte-mediated dynamic interface regulation strategy,providing new design principles for developing industrial water electrolysis catalysts with both high activity and exceptional stability.
基金supported by the National Natural Science Foundation of China(21808035,21901040)the Natural Science Foundation of Fujian Province(2019J05058,2021J05216,2022J01922)+2 种基金the Fujian Provincial Department of Finance(GY-Z220231)the Fujian Fishery Disaster Reduction Centre(GY-H-22146)the College Student Innovation and Entrepreneurship Training Program(x202110388068).
文摘The self-reconstruction of Ni-based electrodes and the in situ generation of oxy-hydroxides are widely investigated as crucial prerequisites for efficient oxygen evolution reaction(OER).However,the transformation is usually time-consuming and surface-limited,resulting in insufficient active sites with unsatisfactory intrinsic activity.Herein,we provide a NH_(3)-treated Fe-doped NiMoO_(4) hydrate as a highly active OER pre-catalyst,with an overpotential of only 240 mV at 100 mA cm^(−2) and 270 mV at 300 mA cm^(−2).By combination of multiple quasi-situ and in situ techniques,the enhanced performance is ascribed to the lattice distortion in the pre-catalyst induced by the NH_(3) treatment.Firstly,the lattice defects with tensile strain and voids accelerate the selective dissolution of MoO_(4)^(2−)and ensure the rapid and bulk reconstruction of the pre-catalyst with enriched active sites.Moreover,it could modulate the electronic structure and optimize the synergism between Ni and Fe,facilitating the dynamic evolution of Fe-doped γ-NiOOH(γ-Ni(Fe)OOH).The intimately interacted Ni–Fe dual-sites from γ-Ni(Fe)OOH and the resultant distorted structure facilitate the formation and adsorption of active oxygen species,accounting for the improved intrinsic activity for OER.
基金support of the National Natural Science Foundation of China(Project No.22061047)Yunnan Fundamental Research Projects(Project No.2016FB023)+1 种基金the Yunnan Provincial Department of Education for funding the research fund project(Project No.2023Y0239)the Advanced Analysis and Measurement Center of Yunnan University for the sample testing service.
文摘Linker conformation engineering provides opportunities for the structural diversity of coordination polymers(CPs);however,the approaches for modulating the synthesis solvents to influence linker conformation are very limited,and they are facing unpredictable challenges to date.Herein,through strategies of solvent-oriented structural self-assembly and solvent-induced single-crystal to single-crystal transformation,eight structurally distinct Cd-CPs were controllably synthesized with the same linkers for the first time.The decisive role of solvents in the self-assembly and transformations in CPs has been demonstrated in depth.Besides,rare reversible CP-based phase transition phenomena at low temperatures were observed.One of these represents the first example of an unprecedented turn-on–off CP-based Fe^(3+)ion sensor.
基金supported by the NSF of China(No.21971143,21805165,21673127 and 21671119)The 111 Project(D20015)ITOYMR in the Higher Education Institutions of Hubei Province(T201904).
文摘Ni-based materials have emerged as promising anode electrocatalysts that can replace noble metals for the methanol oxidation reaction(MOR).However,the potential applications of Ni-based metal–organic gels(Ni-MOGs)in MOR have rarely been recognized.In this study,using the readily prepared Al-MOG(MIL-53(Al))without MOR activity as a template,we fabricated AlNi-MOG and AlNi-based trimetallic MOGs(Cu,Co and Fe)by a simple solvothermal method,which could be directly used as electrocatalysts for the MOR.Among them,the as-obtained AlNiCu-MOG exhibited better MOR activity with an area-specific peak current density of 17.1 mA cm^(−2)than AlNi-MOG(11.46 mA cm^(−2)),which could be attributed to the electron coupling between Ni and Cu.Moreover,the addition of the conductive material acetylene black(AB)could immensely increase the electric conductivity of AlNiCu-MOG,leading to its improved MOR activity with a peak current density of 33.24 mA cm^(−2).These results represent an important first step towards the application of MOGs in the MOR.
基金supported by the Natural Science Foundation of China[Grant Number 51904152 and 42002040]the Program for Science&Technology Innovation Talents in Universities of Henan Province[Grant Number 20HASTIT020]+2 种基金the Young Backbone Teachers Training Plan of Henan Province,the Natural Science Foundation of Henan Province[Grant Number 222300420502]the Key Science and Technology Program of Henan Province[Grant Number 222102240044]the Key Scientific Research Projects in Colleges and Universities of Henan Province[Grant Number 21B610010].
文摘Molybdenum sulfide(MoS_(2))with a high theoretical capacity and large interlayer distance has triggered extensive attention as a promising alternative anode for lithium ion batteries(LIBs)and sodium ion batteries(SIBs).However,the sluggish kinetics and structural collapse induced by its poor conductivity usually lead to unsatisfactory rate capability and poor cycling performance.Herein,few-layered MoS_(2) with abundant S vacancies were anchored on V_(2)C-MXene and embedded in carbon via an in situ assembly and carbonization strategy.The V_(2)C-MXene substrate suppressed the agglomeration and stacking of MoS_(2) nanosheets,facilitated the efficient exposure of MoS_(2) and shortened the diffusion pathways,which favored ion accessibility and induced a strong capacitive-controlled charge storage behavior.Experimental results and theoretical calculations revealed that the electronic coupling between MoS_(2) and V_(2)C-MXene not only induced abundant S vacancies and modulated the charge distribution but also promoted Li/Na adsorption and lowered the ion diffusion energy barrier.Consequently,the V_(2)C-MXene coupled MoS_(2)@C electrode delivered high capacities of 732.8 and 337.3 mA h g^(-1) at 1 A g^(-1) in LIBs and SIBs,respectively.This work provided a new insight into the rational design of stable and advanced electrode materials for energy storage and conversion.
基金supported by the Natural Science Foundation of China(22462012)Natural Science Fund of Jiangxi Province for Distinguished Young Scholars(20224ACB213003)Graduate student research fellowship of Jiangxi Normal University(YJS2023029).
文摘Photocatalytic two-electron oxygen reduction offers a sustainable method to produce hydrogen peroxide(H_(2)O_(2)).However,the efficiency of carbon nitride(CN)in this process is hindered by serious charge recombination and slow diffusion of oxygen.This work reports the thermal vapor-assisted surface chemical modification of CN by 4-aminobenzoyl groups(PABA/CN),which alters the conjugation system,extends the light absorption range,and enhances charge separation and electron transfer.Besides,it tunes the CN surface to be hydrophobic,which forms a gas/solid/liquid triphase interface in photocatalytic H_(2)O_(2)production,and thus significantly improves O_(2) diffusion and proton supply for photosynthesis of H_(2)O_(2).Photocatalytic experiments revealed that PABA/CN delivered an H_(2)O_(2)yield of up to 745μmol g^(-1)h^(-1)in pure water,8 times that of pristine CN,ranking among the top performances of CNbased photocatalysts.Moreover,its selectivity reached 70%.Mechanism studies identified a two-step one-electron oxygen reduction reaction pathway for H_(2)O_(2)photoproduction.Overall,this work simultaneously addresses the issues of mass transfer of O_(2),light harvesting,and charge separation of CN in photosynthesis of H_(2)O_(2)via surface chemical modification with 4-aminobenzoyl moieties,which extendsπ-conjugation and imparts surface hydrophobicity.
基金supported by the Natural Science Foundation of Shandong Province(ZR2023MB010)the National Natural Science Foundation of China(21874154,22177133)the Research Project of General Administration of China Customs(2022HK058).
文摘Ligand engineering is crucial for tailoring the catalytic and fluorescence properties of gold nanoclusters(AuNCs).However,the mechanisms through which ligands synergistically affect these properties remain largely unexplored.Here we employed single-molecule fluorescence microscopy and ensemble fluorescence spectroscopy to investigate how water-soluble thiol ligands modulate the fluorescence and catalytic activities of AuNCs.Our findings reveal that small ligands,such as 3-mercaptopropionic acid(MPA),provide high catalytic activity,despite lacking fluorescence.Medium-sized ligands,like glutathione(GSH)and the lysine-cysteine-lysine(KCK)peptide,enhance fluorescence and maintain catalytic activity through their stable ligand structures and non-competitive mechanisms.Large protein ligands,such as bovine serum albumin(BSA),significantly increase fluorescence and catalytic activity by controlling their conformation to enhance substrate adsorption but experience reduced catalytic rates due to their competitive binding at high substrate concentrations.Additionally,pH levels influence these properties,with fluorescence intensity increasing under alkaline conditions and catalytic activity peaking in acidic environments for small and medium-sized ligand-AuNCs.For BSA-AuNCs,optimal activity is observed at neutral pH due to favorable protein conformation,where enhanced substrate adsorption has a more significant impact on the catalytic rate than merely exposing gold active sites.These insights into the ligand size and structure-dependent modulation of the catalytic and fluorescence properties of AuNCs lay a foundation for designing efficient fluorescent catalysts.
基金supported by the National Natural Science Foundation of China-Yunnan Joint Fund(U1902222)the National Natural Science Foundation of China(12064021 and 51862020)+1 种基金the Foundation of Yunnan Province(202001AT070037,202101AT070104 and 202101AT070097)Yunnan Major Scientific and Technological Projects(grant no.202202AG050016).
文摘Local structure engineering is one of the most useful strategies for tunable down-shifting and upconversion emissions in halide double perovskites(DPs).However,the roles of the local structure,including local symmetry,coordination structure,and active sites,in these DPs remain largely unexplored.Herein,we studied the local structure-correlated up/down-conversion luminescence in Yb^(3+)/Er^(3+)/Ho^(3+)co/tridoped Cs_(2)LiInCl_(6) with a unique local structure.
基金the National Natural Science Foundation of China(Grants 22221003 and 22071225)the Fundamental Research Funds for the Central Universities(Grant WK2060190103)+3 种基金the Joint Funds from Hefei National Synchrotron Radiation Laboratory(Grant KY2060000175)Collaborative Innovation Program of Hefei Science Center of CAS(Grant 2021HSC-CIP015)USTC Research Funds of the Double First-Class Initiative,the fellowship of China Postdoctoral Science Foundation(2022M712179)the Shenzhen Science and Technology Program(Grant JCYJ20200109110416441).
文摘Small-sized Pt-based intermetallic compounds(IMCs)with unique electronic and geometrical structures are promising candidates as next-generation oxygen-reduction reaction(ORR)catalysts in protonexchange membrane fuel cells(PEMFCs).However,the synthesis of IMC catalysts remains challenging owing to the trade-off relation between the alloying/ordering degree and particle aggregation/sintering under a high-temperature annealing process.Herein,we demonstrate a cuprous sulfide(Cu_(1.96)S)intermediate-assisted strategy for the scalable synthesis of PtCu_(3) intermetallic electrocatalysts on an S-doped carbon black support.We identify that the Cu_(1.96)S intermediate formed at low temperature gradually releases metallic Cu species at high temperatures to form a small-sized and uniform Pt-Cu alloy with target stoichiometry,which eventually ensures the formation of well-ordered intermetallic PtCu_(3) structures.The prepared intermetallic PtCu_(3) catalysts exhibit enhanced ORR performance with a mass activity of 3.2 A mg_(Pt)^(-1) and retain 72%of the initial activity after durability tests.
基金supported by the National Natural Science Foundation of China(92472117,22402081,22509085,and 52371226)the Natural Science Foundation of Jiangsu Province(BK20210311,BK20221482,and BK20251369)+2 种基金the China National Postdoctoral Program for Innovative Talents(BX20250441)the China Postdoctoral Science Foundation(2025M774272)the Jiangsu Funding Program for Excellent Postdoctoral Talent.
文摘Developing stable and efficient single-atom electrocatalysts for the acidic oxygen evolution reaction(OER)is crucial for advancing proton exchange membrane water electrolysis(PEMWE).However,the lack of precisely tailored coordination environments capable of preventing Ir single-atom dissolution remains a critical barrier.Herein,we construct Ir single-atom catalysts supported on Co_(3)O_(4)(IrSA-Co_(3)O_(4))via the synchronized formation of Co defects and the immobilization of Ir single atoms during precursor pyrolysis.Atomically dispersed Ir atoms are anchored at octahedral Co defect sites,forming a configuration of single atoms confined within the spinel lattice.Benefiting from the oxygen-bridged electronic coupling within the Ir–O–Co configuration,the electronic structure of Ir sites is optimized to enable moderate intermediate adsorption while mitigating dissolution.As a result,IrSA-Co_(3)O_(4)achieves a low overpotential of 199 mV at 10 mA cm^(−2)in 0.5 M H_(2)SO_(4)and operates stably for 150 h at 200 mA cm^(−2)during PEMWE.This work provides new insights into the rational design of stable single-atom catalysts for acidic OER by effectively suppressing active-site dissolution.
基金supported by the Scientific and Technological Innovation Project of China Academy of Chinese Medical Sciences(CACMS)(No.CI2023C065YLL)Scientific and technological innovation project of CACMS(No.CI2021B003)+1 种基金CACMS Innovation Fund(No.CI2021A01509)National Natural Science Foundation of China(No.61872297).
文摘To the Editor:Chinese herbal medicines(CHMs)are critical components of traditional Chinese medicine(TCM),[1]with their cold and hot properties being fundamental for guiding clinical applications and ensuring therapeutic efficacy.[2]However,the traditional method of identifying the cold and hot properties of CHMs relies heavily on the subjective experience of TCM practitioners and clinical practice,often leading to uncertainty and inconsistency.As such,there is a pressing need for more precise,rapid,and objective strategies to accurately identify the cold and hot properties of CHMs and their active ingredients.
基金supported by National Key Research and Development Program of China(2021YFE0106900)the Chinese Academy of Medical Sciences(CAMS)Innovation Fund for Medical Sciences(2021-I2M-1-041,2021-I2M-1-001)the National Natural Science Foundation of China(82270144).
文摘The Realgar-Indigo Naturalis formula(RIF)is a proprietary Chinese medicine,which is one of the important drugs in the treatment of pediatric acute promyelocytic leukemia(APL).However,the dose of RIF in clinical application is not uniform and the long-term effectiveness and safety of combining RIF with all-trans retinoic acid(ATRA)in a larger population of pediatric APL patients remains undocumented.We conducted a multicenter single-arm clinical trial(ChiCTR-OIC-16010014)in China.Individuals newly diagnosed with APL were treated with CCCG-APL-2017 protocol which is based on RIF and ATRA in consolidation.The event-free survival(EFS)and overall survival(OS)outcomes were evaluated.We recruited 200 patients diagnosed with APL.The six-year OS rate was 100%in the low-risk(LR)group and 97.6%in the high-risk(HR)group.The six-year EFS rate was 98.3%in the LR group and 97.6%in the HR group.Plasma levels of arsenic remained stable after the administration of RIF at a dosage of 60 mg/kg/d for seven days and returned to baseline levels within fourteen days after discontinuation of RIF administration,which is consistent with a concentration of 135 mg/d/kg.Furthermore,controlling white blood cells(WBC)to maintain levels at or below 30×10^(9)/L during induction therapy can decrease the incidence of induced differentiation syndrome(DS)or alleviate its symptoms.Our study demonstrated that the CCCG-APL-2017 protocol,which combines RIF with ATRA,is both effective and safe in treating children with APL.
基金supported by the National Key R&D Program of China(2022YFA1503300)and the National Natural Science Foundation of China(21971241 and 21935010)。
文摘Chiral metal-organic frameworks(CMOFs),an emerging class of heterogeneous chiral catalysts,show significant potential for application in asymmetric catalysis due to their tunable pore shapes and sizes,large internal surface areas,and rich chiral environments[1-4].Through over 20 years of development,researchers have invested heavily in exploring new CMOFs to enhance asymmetric catalytic performance[5-10].However,the dual pursuit of a substantial specific surface area and robust stability within a single CMOF presents a considerable challenge.Additionally,efficient CMOF catalysts,frequently synthesized from privileged chiral ligands such as proline,2,2'-bis(diphenylphosphino)-1,1'-binaph thyl(BINAP),Salen,and bis(oxazoline)(Box)[11,12],tend to exhibit more complex structures compared to their corresponding privileged chiral counterparts,thereby necessitating higher production costs.Consequently,the development of novel synthetic methodologies for constructing CMOFs as effective chiral catalysts remains a challenging endeavor.
基金Supported by the Guangdong Provincial Key Laboratory of Pathogen Detection for Emerging Infectious Disease Response(2023B1212010010).
文摘Introduction:Vaccination stands as the most effective preventive measure against yellow fever(YF).However,the YF vaccination associated Adverse Events following Immunization(AEFI)cases occur occasionally.Methods:The Guangdong Provincial Center for Disease Control and Prevention utilized Targeted Next-Generation Sequencing(tNGS)to determine whether the imported suspected YF case was infected by the wild-type YF virus strain or experienced an AEFI.Results:tNGS analysis successfully yielded a 10.2 kb viral genomic sequence.Subsequent in-depth analysis revealed high similarity to the YF vaccine strain 17D-213 and classified the sequence within the West Africa II genotype,clustering with the 17D vaccine strain.Conclusions and Implications for Public Health Practice:This case represented YF AEFI.The implementation of tNGS technology enables more precise and expeditious pathogen sequencing,providing critical evidence for accurate disease diagnosis and informed public health interventions.
基金supported by the National Key Research and Development Program of China(2021YFC3002200)the National Natural Science Foundation of China(U20A20168)+1 种基金the Scientific and Technological Innovation Project of China Academy of Chinese Medical Sciences(CI2023C002YG,ZN2023A01)a grant from the Guoqiang Institute,Tsinghua University.
文摘Flexible hybrid systems usually combine soft modules(mechanically matched with skin or clothes)and hard modulus(like rigid circuits).However,the risk of interface failure due to modulus mismatch between flexible components and rigid circuits limits the system’s complexity and durability.The diverse features of flexible components further complicate the development of a universal interface.In this work,we demonstrated a cocoon-mimetic feature-matched interface(CFI)that offers stable electrical contact with flexible surface.It also matches flexible systems features in stretchability(lower than 0.22Ωcm^(-1)during 900%elongation),durability(stable resistance after 20000 times 100%elongation),breathability(gas permeability 614 mm S^(-1))and self-adhesive(0.18±0.01 N mm^(-1)).We developed a direct spray-on-skin sensor and used CFI to form a hand task recognition system.This system,deployable in seconds,has 97.7%accuracy in recognition of eight hand tasks.This research offers a promising solution for flexible hybrid systems interfacing challenges.
文摘Transient electronics,comprising of degradable devices that disintegrate and disappear after their operational life,has received considerable interest in recent years because of the concerns related to the rapidly growing electronic waste(e-waste).However,the degradability or biodegradability of electronic devices alone is insufficient to ascertain environmental safety.The evaluation of the nature of degradation by-products is also essential to assess the environmental impact of a degradable device.Herein,we investigate systematically the hydrolytic degradation by-products of two different types of devices viz.a capacitive pressure sensor and a photodetector,using liquid chromatograph mass spectrometry.The findings reveal that,despite the inherent degradability of constituent materials used in an electronic device,the released by-products can be toxic or could be complex molecules with unknown chemistry such as carcinogenic or contain almost non-degradable polystyrene derivatives/microplastic(e.g.,from PEDOT:PSS),or have copper complexes resulting from degraded silk fibroin and poly(ethylene oxide)mass fragments.This analysis underlines the need for careful selection and reassessment of materials employed in transient electronics,as an important factor,to mitigate the end-of-life issues associated with electronics and its environmental impact.
