Brominated flame retardants(BFRs)are persistent organic pollutants worldwide.However,the effect of BFRs on the development of atherosclerosis is currently unknown.Here we aimed to investigate the effects of three typi...Brominated flame retardants(BFRs)are persistent organic pollutants worldwide.However,the effect of BFRs on the development of atherosclerosis is currently unknown.Here we aimed to investigate the effects of three typical BFRs(BDE-47,BDE-209,and DBDPE)on the development of atherosclerosis and explored the underlying mechanisms using an in vitro cell model and ApoE^(−/−)mice.Our data showed that BFRs significantly inhibited the viability of human aortic endothelial cells(HAECs)and induced the generation of ROS.BFRs significantly enhanced the content of Ox-LDL in THP-1 macrophages,which promoted the formation of foam cells.In an in vivo study,BFRs exposure significantly increased the plaque area and lipid content in the aortic root of mice.BFRs significantly increased the ROS level in plaques and promoted the expression level of adhesion molecule ICAM-1,which enhanced the recruitment of macrophages.Transcriptome analysis showed that differentially expressed genes(DEGs)were significantly enriched in signaling pathways related to oxidative stress and lipid metabolism.In summary,these results indicate that BFRs exposure can promote the development of atherosclerosis by increasing macrophage recruitment and foam cell formation,which elucidates the impact of BFRs on atherosclerosis for the first time,and provide scientific clues for the prevention and treatment of atherosclerosis.展开更多
In fulfillment of the national science-and-technology development agenda, the Department of Chemical Sciences of the National Natural Science Foundation of China (NSFC) convened the Strategic Symposium on the Fifteent...In fulfillment of the national science-and-technology development agenda, the Department of Chemical Sciences of the National Natural Science Foundation of China (NSFC) convened the Strategic Symposium on the Fifteenth FiveYear (20262030) Development Plan for Electrochemistry held in Xiamen on 29 August, 2025-the culminating year of the Fourteenth Five-Year (2021-2025) Development Plan. More than forty leading experts in the field of electrochemistry participated with spanning nine thematic fronts: Interfacial Electrocatalysis, Interfacial Electrochemistry for Energy Storage, Bioelectrochemistry, Electrochemistry of Hydrogen Energy, Electrochemical Micro-/Nano-Manufacturing, Operando Electrochemical Characterization, Electro-Thermal Coupling Catalysis, Theoretical and Computational Electrochemistry,and Electrochemical Synthesis. The forum assembled China's foremost electrochemical expertise to blueprint high-quality disciplinary growth for the coming five-year period, thereby serving overarching national strategic needs and sharpening the international competitiveness of Chinese electrochemistry.This paper is presented to highlight the strategic needs and priority areas for the next five years (2026-2030) based on this symposium. The development status of basic research and applied basic research in China's electrochemistry field is systematically reviewed. The in-depth analyses of the existing problems and key challenges in the research and development of electrochemistry related fields are outlined, and the frontier research areas and development trends in the next 5-10 years by integrating national major strategic needs are discussed, which will further promote the academic community to reach a clearer consensus. The proposed strategic roadmap is intended to accelerate a sharpened community consensus, propel the discipline toward high-quality advancement, and furnish a critical reference for building China into a world-leading science and technology power.展开更多
Lithium metal anodes,with a theoretical capacity of up to 3860 mAh·g−1,are regarded as the cornerstone for developing next-generation high-energy-density batteries.However,several key challenges hinder their prac...Lithium metal anodes,with a theoretical capacity of up to 3860 mAh·g−1,are regarded as the cornerstone for developing next-generation high-energy-density batteries.However,several key challenges hinder their practical applications,includ-ing dendrite formation,unstable solid electrolyte interphase(SEI),side reactions with electrolytes,and associated safety risks.This review systematically explores the mechanisms of lithium nucleation,growth,and stripping in both liquid and solid-state battery systems,analyzing critical theoretical concepts like heterogeneous nucleation thermodynamics,surface diffusion kinetics,space charge effects,and SEI-induced nucleation,which are crucial for understanding the genesis of dendrite growth.Additionally,the review discusses the electrochemical-mechanical coupling failures that lead to SEI degra-dation and the formation of dead lithium.For liquid systems,the review proposes strategies to mitigate dendrite formation and SEI instability,which include electrolyte optimization,artificial SEI design,and electrode framework design.In solid-state batteries,the review offers a granular analysis of the interface challenges associated with polymer,sulfide,and halide electrolytes and summarizes different solutions for different solid-state electrolytes.Meanwhile,the review emphasizes the importance of advanced characterization techniques and computational modeling in understanding and regulating the interface between lithium metal and electrolytes.Looking ahead,the review highlights future research directions that emp-hasize the integration of cross-disciplinary approaches to tackle these interconnected challenges.By addressing these issues,the path will be clear for the rapid commercialization and widespread application of lithium metal batteries,bringing us closer to realizing stable,high-energy-density batteries that can satisfy the escalating demands of modern energy storage applications across various industries.展开更多
In this paper,the third-order nonlinear optical(NLO)properties of covalent organic framework(COF)materials with conjugated amphoteric ion structure are studied for the first time.A highly ordered crystalline ultrathin...In this paper,the third-order nonlinear optical(NLO)properties of covalent organic framework(COF)materials with conjugated amphoteric ion structure are studied for the first time.A highly ordered crystalline ultrathin films of the ionic COF material PySQ-iCOF was successfully fabricated using a solid-liquid interface method,meanwhile the building units extracted to be independent small molecule,1-PySA,were synthesized for comparative studies.Compared to 1-PySA,PySQ-iCOF possesses not only a larger conjugated system but also exhibits enhanced polarization and charge transfer capabilities.The NLO properties of PySQ-iCOF and the small molecule 1-PySA were investigated using Z-scan technique at a wavelength of 532 nm,revealing the PySQ-iCOF thin film exhibits outstanding NLO performance.Specifically,it demonstrates saturable absorption under nanosecond(ns)pulse laser irradiation(β=9.59×10^(-6) m/W),while exhibiting reverse saturable absorption under femtosecond(fs)pulse conditions(β=6.91×10^(-8) m/W).Furthermore,the PySQ-iCOF film exhibits strong negative refractive nonlinearity,−6×10^(-12) m^(2)/W for ns and -3.8×10^(-13) m^(2)/W for fs,respectively.Transient absorption spectroscopy studies indicate that the pulse-width-dependent nonlinear absorption char-acteristics of the PySQ-iCOF film originate from the generation of triplet excited states.Both nonlinear absorption coefficient and nonlinear refractive index of the PySQ-iCOF film surpass those of most reported organic materials measured under comparable conditions,which provides huge potential in all-optical manipulating and switching at the nanoscale as outstanding NLO materials.展开更多
The efficiency of organic semiconductor photocatalysts is typically limited by their capability of photogenerated electron transport.Herein,a photocatalyst is proposed initially through the specific axial coordination...The efficiency of organic semiconductor photocatalysts is typically limited by their capability of photogenerated electron transport.Herein,a photocatalyst is proposed initially through the specific axial coordination interaction between imidazole-C_(60)(ImC_(60))and zinc tetraphenyl porphyrin(ZnTPP)named ImC_(60)-ZnTPP.Subsequently,detailed structural characterizations along with theoretical calculation reveal that the unique ImC_(60)-ZnTPP possesses head-to-tail stacking supra-structures,leading to the formation of a continuous array of C_(60)–C_(60) with ultrashort spacing and ensuring strongπ–πinteractions and homogeneous electronic coupling,which could tremendously promote electron transport along the(−111)crystal facet of ImC_(60)-ZnTPP.Consequently,compared to other fullerene-based photocatalysts,ImC_(60)-ZnTPP shows exceptional photocatalytic hydrogen production activity,with an efficiency of up to 80.95 mmol g^(-1) h^(-1).This study provides a novel strategy to design highly efficient fullerene-based photocatalytic systems for solar-driven energy conversion and extend their artificial photosynthetic use.展开更多
Unstable electrode/electrolyte interfaces and heterogeneous Zn deposition would reduce the Coulombic efficiency and cycle life of Zn metal batteries(ZMBs). Applying water-in-salt(WIS) electrolytes has proven to be an ...Unstable electrode/electrolyte interfaces and heterogeneous Zn deposition would reduce the Coulombic efficiency and cycle life of Zn metal batteries(ZMBs). Applying water-in-salt(WIS) electrolytes has proven to be an effective strategy to address the above issues. However, an understanding of the reaction mechanisms on the Zn anode at nanoscale is still elusive. Here we utilize in situ atomic force microscopy to visualize the solid electrolyte interphase(SEI) formation and Zn deposition/dissolution processes in WIS electrolyte and construct relationships between interfacial behavior and electrochemical performance. The formation processes, chemical properties, and structure of the on-site formed SEI are deeply explored.The SEI with a “plum-pudding” model can guide uniform Zn deposition and reversible dissolution. Mechanistic understanding of the interfacial evolution of the SEI layer and Zn deposition/dissolution has been achieved and will benefit the structural optimization and interfacial engineering of ZMBs.展开更多
Zn metal batteries are highly attractive because of their high theoretical specific capacity,intrinsic safety and resource availability.However,further development is significantly hindered by low Coulomb efficiency,w...Zn metal batteries are highly attractive because of their high theoretical specific capacity,intrinsic safety and resource availability.However,further development is significantly hindered by low Coulomb efficiency,which is closely linked to reaction processes occurring at electrode/electrolyte interfaces.Herein,we have achieved a real-time visualization and comprehensive analysis of the interfacial evolution of Zn metal anode via in situ AFM in organic and aqueous electrolytes,respectively.The processes of uneven nucleation,dendrite growth,the Zn O formation and the dissolution of Zn substrate are directly probed in aqueous electrolyte,which induces interfacial deterioration and ultimately results in battery failure.In organic electrolyte,the in situ observations show that the homogeneous nuclei form on the Zn surface to induce the dendrite-free deposition,however,exhibiting poor Zn plating/stripping reversibility.This work delves into the dynamic evolution and electrochemical behaviors regulated by solvents,which provides in-depth understanding of structure-reactivity correlations and further interfacial engineering.展开更多
The performance of lithium metal batteries(LMBs)is greatly hampered by the unstable solid electrolyte interphase(SEI)and uncontrollable growth of Li dendrites.To address this question,we developed a weak polar additiv...The performance of lithium metal batteries(LMBs)is greatly hampered by the unstable solid electrolyte interphase(SEI)and uncontrollable growth of Li dendrites.To address this question,we developed a weak polar additive strategy to develop stable and dendrite-free electrolyte for LMBs.In this paper,the effects of additives on the Li^(+)solvation kinetics and the electrode-electrolyte interphases(EEI)formation are discussed.The function of synergistically boosting the superior Li^(+)kinetics and alleviating solvent decomposition on the electrodes is confirmed.From the thermodynamic view,the exothermic process of defluorination reaction for 3,5-difluoropyridine(3,5-DFPy)results in the formation of LiF-rich SEI layer for promoting the uniform Li nucleation and deposition.From the dynamic view,the weakened Li^(+)solvation structure induced by weak polar 3,5-DFPy contributes to better Li^(+)kinetics through the easier Li^(+)desolvation.As expected,Li||Li cell with 1.0 wt%3,5-DFPy exhibits 400 cycles at 1.0 mA cm^(-2)with a deposition capacity of 0.5 mAh cm^(-2),and the Li||LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)batteries delivers the highly reversible capacity after 200 cycles.展开更多
In this paper a methodology is proposed to model the stochastic electro-thermal degradation accumulation in cables.The cable life and the reliability are predicted by estimating the accumulated electro-thermal degrada...In this paper a methodology is proposed to model the stochastic electro-thermal degradation accumulation in cables.The cable life and the reliability are predicted by estimating the accumulated electro-thermal degradation during seasonal load cycles.The degradation is considered,in a novel approach,as stochastic in nature due to variations in the manufacturing process of insulation raw material and in operational and environmental conditions.The methodology is based on estimation of life by using combined electro-thermal life model,simulation of degradation accumulation process under electro-thermal stress in each season of the year based on Miner’s cumulative damage theory and reliability prediction from a probabilistic point of view.A case study is demonstrated on 10 k V XLPE cables which are directly buried in the UK and China.Results show that,the electro-thermal life of the cable is 56 and 69 years in China and the UK,respectively at 50%failure probability,or the life of the cable in the UK would be 13 years longer than in China,when other stresses such as mechanical and environmental are also considered and assumed to be the same.展开更多
Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we ...Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we report a new synthetic poly-dioxolane (PDOL) approach to constructing an artificial 'elastic' SEI to stabilize the Li/electrolyte interface and the Li deposition/dissolution behavior in a variety of electrolytes. By coating PDOL with optimized molecular weights and synthetic routes on Li metal anode, the 'elastic' SEI layer could be maintained on top of the Li metal anode to accommodate the Li deposition/dissolution. No dendrite formation was observed during the cycling process, and the interfacial side reactions were reduced significantly. Consequently, we successfully achieved 330 cycles with a CE of 98.4% in ether electrolytes and 90 cycles with a CE of 94.3% in carbonate electrolytes. Simultaneously, the Li-metal batteries with LiFePO_(4) as cathodes also exhibited improved cycling performance. This strategy could promote the development of dendrite-free metal anodes toward high-performance Li-metal batteries.展开更多
Gel polymer electrolytes(GPEs)are one of the promising candidates for high-energy-density quasi-solid-state lithium metal batteries(QSSLMBs),for their high ionic conductivity and excellent interfacial compatibility.Th...Gel polymer electrolytes(GPEs)are one of the promising candidates for high-energy-density quasi-solid-state lithium metal batteries(QSSLMBs),for their high ionic conductivity and excellent interfacial compatibility.The comprehension of dynamic evolution and structure-reactivity correlation at the GPE/Li interface becomes significant.Here,in situ electrochemical atomic force microscopy(EC-AFM)provides insights into the LiNO_(3)-regulated micromechanism of the Li plating/stripping processes upon cycles in GPE-based LMBs at nanoscale.The additive LiNO_(3)induces the formation of amorphous nitride SEI film and facilitates Li^(+) ion diffusion.It stabilizes a compatible interface and regulates the Li nucleation/growth at steady kinetics.The deposited Li is in the shape of chunks and tightly compact.The Li dissolution shows favorable reversibility,which guarantees the cycling performance of LMBs.In situ AFM monitoring provides a deep understanding into the dynamic evolution of Li deposition/dissolution and the interphasial properties of tunable SEI film,regulating the rational design of electrolyte and optimizing interfacial establishment for GPE-based QSSLMBs.展开更多
The solid electrolyte interphase(SEI),a passivation film covering the electrode surface,is crucial to the lifetime and efficiency of the lithium-ion(Li-ion)battery.Understanding the Li-ion diffusion mechanism within p...The solid electrolyte interphase(SEI),a passivation film covering the electrode surface,is crucial to the lifetime and efficiency of the lithium-ion(Li-ion)battery.Understanding the Li-ion diffusion mechanism within possible components in the mosaic-structured SEI is an essential step to improve the Li-ion conductivity and thus the battery performance.Here,we investigate the Li-ion diffusion mechanism within three amorphous SEI components(i.e.,the inorganic inner layer,organic outer layer,and their mixture with 1:1 molar ratio)via ab initio molecular dynamic(AIMD)simulations.Our simulations show that the Li-ion diffusion coefficient in the inorganic layer is two orders of magnitude faster than that in the organic layer.Therefore,the inorganic layer makes a major contribution to the Li-ion diffusion.Furthermore,we find that the Li-ion diffusivity in the organic layer decreases slightly with the increase of the carbon chain from the methyl to ethyl owing to the steric hindrance induced by large groups.Overall,our current work unravels the Li-ion diffusion mechanism,and provides an atomic-scale insight for the understanding of the Li-ion transport in the SEI components.展开更多
BACKGROUND Ferroptosis has recently been associated with multiple degenerative diseases.Ferroptosis induction in cancer cells is a feasible method for treating neoplastic diseases.However,the association of iron proli...BACKGROUND Ferroptosis has recently been associated with multiple degenerative diseases.Ferroptosis induction in cancer cells is a feasible method for treating neoplastic diseases.However,the association of iron proliferation-related genes with prognosis in HER2+breast cancer(BC)patients is unclear.AIM To identify and evaluate fresh ferroptosis-related biomarkers for HER2+BC.METHODS First,we obtained the mRNA expression profiles and clinical information of HER2+BC patients from the TCGA and METABRIC public databases.A four gene prediction model comprising PROM2,SLC7A11,FANCD2,and FH was subsequently developed in the TCGA cohort and confirmed in the METABRIC cohort.Patients were stratified into high-risk and low-risk groups based on their median risk score,an independent predictor of overall survival(OS).Based on these findings,immune infiltration,mutations,and medication sensitivity were analyzed in various risk groupings.Additionally,we assessed patient prognosis by combining the tumor mutation burden(TMB)with risk score.Finally,we evaluated the expression of critical genes by analyzing single-cell RNA sequencing(scRNA-seq)data from malignant vs normal epithelial cells.RESULTS We found that the higher the risk score was,the worse the prognosis was(P<0.05).We also found that the immune cell infiltration,mutation,and drug sensitivity were different between the different risk groups.The highrisk subgroup was associated with lower immune scores and high TMB.Moreover,we found that the combination of the TMB and risk score could stratify patients into three groups with distinct prognoses.HRisk-HTMB patients had the worst prognosis,whereas LRisk-LTMB patients had the best prognosis(P<0.0001).Analysis of the scRNAseq data showed that PROM2,SLC7A11,and FANCD2 were significantly differentially expressed,whereas FH was not,suggesting that these genes are expressed mainly in cancer epithelial cells(P<0.01).CONCLUSION Our model helps guide the prognosis of HER2+breast cancer patients,and its combination with the TMB can aid in more accurate assessment of patient prognosis and provide new ideas for further diagnosis and treatment.展开更多
In recent years,with the rise of video media such as YouTube and Tik Tok,the short video creation industry has emerged.How to spread China's excellent culture and how to“tell a good Chinese story”have become a h...In recent years,with the rise of video media such as YouTube and Tik Tok,the short video creation industry has emerged.How to spread China's excellent culture and how to“tell a good Chinese story”have become a hot concern.Using the 5W Model of Communication as a framework for analysis,this paper selects Chinese short videos with high popularity on YouTube as the object of the study.Studies found that the success of these videos was associated with five factors in the process of communication,which are communication main forces,communication content,communication channels,communication audience,and audience effects.Through theoretical and data analysis,the study concluded five strategies in video production to help promote Intercultural communication.展开更多
基金supported by the grants from Natural Science Foundation of Guangdong Province(NO.2023A1515010198)Shenzhen Basic Research Project(JCYJ20240813142717023)the Sanming Project of Medicine in Shenzhen(NO.SZSM202311019).
文摘Brominated flame retardants(BFRs)are persistent organic pollutants worldwide.However,the effect of BFRs on the development of atherosclerosis is currently unknown.Here we aimed to investigate the effects of three typical BFRs(BDE-47,BDE-209,and DBDPE)on the development of atherosclerosis and explored the underlying mechanisms using an in vitro cell model and ApoE^(−/−)mice.Our data showed that BFRs significantly inhibited the viability of human aortic endothelial cells(HAECs)and induced the generation of ROS.BFRs significantly enhanced the content of Ox-LDL in THP-1 macrophages,which promoted the formation of foam cells.In an in vivo study,BFRs exposure significantly increased the plaque area and lipid content in the aortic root of mice.BFRs significantly increased the ROS level in plaques and promoted the expression level of adhesion molecule ICAM-1,which enhanced the recruitment of macrophages.Transcriptome analysis showed that differentially expressed genes(DEGs)were significantly enriched in signaling pathways related to oxidative stress and lipid metabolism.In summary,these results indicate that BFRs exposure can promote the development of atherosclerosis by increasing macrophage recruitment and foam cell formation,which elucidates the impact of BFRs on atherosclerosis for the first time,and provide scientific clues for the prevention and treatment of atherosclerosis.
文摘In fulfillment of the national science-and-technology development agenda, the Department of Chemical Sciences of the National Natural Science Foundation of China (NSFC) convened the Strategic Symposium on the Fifteenth FiveYear (20262030) Development Plan for Electrochemistry held in Xiamen on 29 August, 2025-the culminating year of the Fourteenth Five-Year (2021-2025) Development Plan. More than forty leading experts in the field of electrochemistry participated with spanning nine thematic fronts: Interfacial Electrocatalysis, Interfacial Electrochemistry for Energy Storage, Bioelectrochemistry, Electrochemistry of Hydrogen Energy, Electrochemical Micro-/Nano-Manufacturing, Operando Electrochemical Characterization, Electro-Thermal Coupling Catalysis, Theoretical and Computational Electrochemistry,and Electrochemical Synthesis. The forum assembled China's foremost electrochemical expertise to blueprint high-quality disciplinary growth for the coming five-year period, thereby serving overarching national strategic needs and sharpening the international competitiveness of Chinese electrochemistry.This paper is presented to highlight the strategic needs and priority areas for the next five years (2026-2030) based on this symposium. The development status of basic research and applied basic research in China's electrochemistry field is systematically reviewed. The in-depth analyses of the existing problems and key challenges in the research and development of electrochemistry related fields are outlined, and the frontier research areas and development trends in the next 5-10 years by integrating national major strategic needs are discussed, which will further promote the academic community to reach a clearer consensus. The proposed strategic roadmap is intended to accelerate a sharpened community consensus, propel the discipline toward high-quality advancement, and furnish a critical reference for building China into a world-leading science and technology power.
基金supported by grants from the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant Nos.XDB1040100 and XDB1040300)the National Natural Science Foundation of China(Grant Nos.22379108,52202279,52225105,22279127,22425403,92372125,22421001,22205241,22425403,92372125,22421001,22205241,92472207,52472223,52102280,22393900 and 22209010)+1 种基金the National Key Research and Development Program of China(Grant Nos.2021YFF0500600 and 2021YFB2500300)the Fundamental Research Funds for the Central Univer-sities(Grant No.WK9990000170)。
文摘Lithium metal anodes,with a theoretical capacity of up to 3860 mAh·g−1,are regarded as the cornerstone for developing next-generation high-energy-density batteries.However,several key challenges hinder their practical applications,includ-ing dendrite formation,unstable solid electrolyte interphase(SEI),side reactions with electrolytes,and associated safety risks.This review systematically explores the mechanisms of lithium nucleation,growth,and stripping in both liquid and solid-state battery systems,analyzing critical theoretical concepts like heterogeneous nucleation thermodynamics,surface diffusion kinetics,space charge effects,and SEI-induced nucleation,which are crucial for understanding the genesis of dendrite growth.Additionally,the review discusses the electrochemical-mechanical coupling failures that lead to SEI degra-dation and the formation of dead lithium.For liquid systems,the review proposes strategies to mitigate dendrite formation and SEI instability,which include electrolyte optimization,artificial SEI design,and electrode framework design.In solid-state batteries,the review offers a granular analysis of the interface challenges associated with polymer,sulfide,and halide electrolytes and summarizes different solutions for different solid-state electrolytes.Meanwhile,the review emphasizes the importance of advanced characterization techniques and computational modeling in understanding and regulating the interface between lithium metal and electrolytes.Looking ahead,the review highlights future research directions that emp-hasize the integration of cross-disciplinary approaches to tackle these interconnected challenges.By addressing these issues,the path will be clear for the rapid commercialization and widespread application of lithium metal batteries,bringing us closer to realizing stable,high-energy-density batteries that can satisfy the escalating demands of modern energy storage applications across various industries.
基金the National Natural Science Foundation of China(22171076)Jing Li at the Technical Institute of Physics and Chemistry,Chinese Academy of Sciences(CAS),for his measurement of dynamic processes.
文摘In this paper,the third-order nonlinear optical(NLO)properties of covalent organic framework(COF)materials with conjugated amphoteric ion structure are studied for the first time.A highly ordered crystalline ultrathin films of the ionic COF material PySQ-iCOF was successfully fabricated using a solid-liquid interface method,meanwhile the building units extracted to be independent small molecule,1-PySA,were synthesized for comparative studies.Compared to 1-PySA,PySQ-iCOF possesses not only a larger conjugated system but also exhibits enhanced polarization and charge transfer capabilities.The NLO properties of PySQ-iCOF and the small molecule 1-PySA were investigated using Z-scan technique at a wavelength of 532 nm,revealing the PySQ-iCOF thin film exhibits outstanding NLO performance.Specifically,it demonstrates saturable absorption under nanosecond(ns)pulse laser irradiation(β=9.59×10^(-6) m/W),while exhibiting reverse saturable absorption under femtosecond(fs)pulse conditions(β=6.91×10^(-8) m/W).Furthermore,the PySQ-iCOF film exhibits strong negative refractive nonlinearity,−6×10^(-12) m^(2)/W for ns and -3.8×10^(-13) m^(2)/W for fs,respectively.Transient absorption spectroscopy studies indicate that the pulse-width-dependent nonlinear absorption char-acteristics of the PySQ-iCOF film originate from the generation of triplet excited states.Both nonlinear absorption coefficient and nonlinear refractive index of the PySQ-iCOF film surpass those of most reported organic materials measured under comparable conditions,which provides huge potential in all-optical manipulating and switching at the nanoscale as outstanding NLO materials.
基金supported by the National Natural Science Foundation of China(52322204,52072374,52272052)the National Key R&D Program of China(Grant No.2022YFA1205900)the Youth Innovation Promotion Association of CAS(Y2022015).
文摘The efficiency of organic semiconductor photocatalysts is typically limited by their capability of photogenerated electron transport.Herein,a photocatalyst is proposed initially through the specific axial coordination interaction between imidazole-C_(60)(ImC_(60))and zinc tetraphenyl porphyrin(ZnTPP)named ImC_(60)-ZnTPP.Subsequently,detailed structural characterizations along with theoretical calculation reveal that the unique ImC_(60)-ZnTPP possesses head-to-tail stacking supra-structures,leading to the formation of a continuous array of C_(60)–C_(60) with ultrashort spacing and ensuring strongπ–πinteractions and homogeneous electronic coupling,which could tremendously promote electron transport along the(−111)crystal facet of ImC_(60)-ZnTPP.Consequently,compared to other fullerene-based photocatalysts,ImC_(60)-ZnTPP shows exceptional photocatalytic hydrogen production activity,with an efficiency of up to 80.95 mmol g^(-1) h^(-1).This study provides a novel strategy to design highly efficient fullerene-based photocatalytic systems for solar-driven energy conversion and extend their artificial photosynthetic use.
基金financially supported by the National Key R&D Program of China (No. 2021YFB2500300)the CAS Project for Young Scientists in Basic Research (No. YSBR-058)+1 种基金the National Science Foundation of China (No. 22205241)the National Postdoctoral Program for Innovative Talents (No. BX20220306) of the Chinese Postdoctoral Science Foundation。
文摘Unstable electrode/electrolyte interfaces and heterogeneous Zn deposition would reduce the Coulombic efficiency and cycle life of Zn metal batteries(ZMBs). Applying water-in-salt(WIS) electrolytes has proven to be an effective strategy to address the above issues. However, an understanding of the reaction mechanisms on the Zn anode at nanoscale is still elusive. Here we utilize in situ atomic force microscopy to visualize the solid electrolyte interphase(SEI) formation and Zn deposition/dissolution processes in WIS electrolyte and construct relationships between interfacial behavior and electrochemical performance. The formation processes, chemical properties, and structure of the on-site formed SEI are deeply explored.The SEI with a “plum-pudding” model can guide uniform Zn deposition and reversible dissolution. Mechanistic understanding of the interfacial evolution of the SEI layer and Zn deposition/dissolution has been achieved and will benefit the structural optimization and interfacial engineering of ZMBs.
基金financially supported by the CAS Project for Young Scientists in Basic Research(No.YSBR-058)the National Key R&D Program of China(No.2021YFB2500300)+1 种基金the National Natural Science Foundation of China(Nos.92372125,22205241)the National Postdoctoral Program for Innovative Talents(No.BX20220306)of the Chinese Postdoctoral Science Foundation。
文摘Zn metal batteries are highly attractive because of their high theoretical specific capacity,intrinsic safety and resource availability.However,further development is significantly hindered by low Coulomb efficiency,which is closely linked to reaction processes occurring at electrode/electrolyte interfaces.Herein,we have achieved a real-time visualization and comprehensive analysis of the interfacial evolution of Zn metal anode via in situ AFM in organic and aqueous electrolytes,respectively.The processes of uneven nucleation,dendrite growth,the Zn O formation and the dissolution of Zn substrate are directly probed in aqueous electrolyte,which induces interfacial deterioration and ultimately results in battery failure.In organic electrolyte,the in situ observations show that the homogeneous nuclei form on the Zn surface to induce the dendrite-free deposition,however,exhibiting poor Zn plating/stripping reversibility.This work delves into the dynamic evolution and electrochemical behaviors regulated by solvents,which provides in-depth understanding of structure-reactivity correlations and further interfacial engineering.
基金supported by the National Natural Science Foundation of China(U21A20311)Researchers Supporting Project Number(RSP2025R304),King Saud University,Riyadh,Saudi Arabia。
文摘The performance of lithium metal batteries(LMBs)is greatly hampered by the unstable solid electrolyte interphase(SEI)and uncontrollable growth of Li dendrites.To address this question,we developed a weak polar additive strategy to develop stable and dendrite-free electrolyte for LMBs.In this paper,the effects of additives on the Li^(+)solvation kinetics and the electrode-electrolyte interphases(EEI)formation are discussed.The function of synergistically boosting the superior Li^(+)kinetics and alleviating solvent decomposition on the electrodes is confirmed.From the thermodynamic view,the exothermic process of defluorination reaction for 3,5-difluoropyridine(3,5-DFPy)results in the formation of LiF-rich SEI layer for promoting the uniform Li nucleation and deposition.From the dynamic view,the weakened Li^(+)solvation structure induced by weak polar 3,5-DFPy contributes to better Li^(+)kinetics through the easier Li^(+)desolvation.As expected,Li||Li cell with 1.0 wt%3,5-DFPy exhibits 400 cycles at 1.0 mA cm^(-2)with a deposition capacity of 0.5 mAh cm^(-2),and the Li||LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)batteries delivers the highly reversible capacity after 200 cycles.
文摘In this paper a methodology is proposed to model the stochastic electro-thermal degradation accumulation in cables.The cable life and the reliability are predicted by estimating the accumulated electro-thermal degradation during seasonal load cycles.The degradation is considered,in a novel approach,as stochastic in nature due to variations in the manufacturing process of insulation raw material and in operational and environmental conditions.The methodology is based on estimation of life by using combined electro-thermal life model,simulation of degradation accumulation process under electro-thermal stress in each season of the year based on Miner’s cumulative damage theory and reliability prediction from a probabilistic point of view.A case study is demonstrated on 10 k V XLPE cables which are directly buried in the UK and China.Results show that,the electro-thermal life of the cable is 56 and 69 years in China and the UK,respectively at 50%failure probability,or the life of the cable in the UK would be 13 years longer than in China,when other stresses such as mechanical and environmental are also considered and assumed to be the same.
基金This research was supported financially by the Major Program of the National Natural Science Foundation of China(21890731).
文摘Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we report a new synthetic poly-dioxolane (PDOL) approach to constructing an artificial 'elastic' SEI to stabilize the Li/electrolyte interface and the Li deposition/dissolution behavior in a variety of electrolytes. By coating PDOL with optimized molecular weights and synthetic routes on Li metal anode, the 'elastic' SEI layer could be maintained on top of the Li metal anode to accommodate the Li deposition/dissolution. No dendrite formation was observed during the cycling process, and the interfacial side reactions were reduced significantly. Consequently, we successfully achieved 330 cycles with a CE of 98.4% in ether electrolytes and 90 cycles with a CE of 94.3% in carbonate electrolytes. Simultaneously, the Li-metal batteries with LiFePO_(4) as cathodes also exhibited improved cycling performance. This strategy could promote the development of dendrite-free metal anodes toward high-performance Li-metal batteries.
基金financially supported by the National Key R&D Program of China(Grant No.2016YFA0202500)the National Natural Science Fund for Excellent Young Scholars(Grant No.21722508)。
文摘Gel polymer electrolytes(GPEs)are one of the promising candidates for high-energy-density quasi-solid-state lithium metal batteries(QSSLMBs),for their high ionic conductivity and excellent interfacial compatibility.The comprehension of dynamic evolution and structure-reactivity correlation at the GPE/Li interface becomes significant.Here,in situ electrochemical atomic force microscopy(EC-AFM)provides insights into the LiNO_(3)-regulated micromechanism of the Li plating/stripping processes upon cycles in GPE-based LMBs at nanoscale.The additive LiNO_(3)induces the formation of amorphous nitride SEI film and facilitates Li^(+) ion diffusion.It stabilizes a compatible interface and regulates the Li nucleation/growth at steady kinetics.The deposited Li is in the shape of chunks and tightly compact.The Li dissolution shows favorable reversibility,which guarantees the cycling performance of LMBs.In situ AFM monitoring provides a deep understanding into the dynamic evolution of Li deposition/dissolution and the interphasial properties of tunable SEI film,regulating the rational design of electrolyte and optimizing interfacial establishment for GPE-based QSSLMBs.
基金R.Wen acknowledges the financial support from the National Key R&D Program of China(No.2021YFB2500300)the CAS Project for Young Scientists in Basic Research(No.YSBR-058)+2 种基金S.Xu acknowledges funding support from the Chinese Ministry of Science and Technology(No.2021YFB3800303)DP Technology Corporation(No.2021110016001141)the School of Materials Science and Engineering at Peking University.
文摘The solid electrolyte interphase(SEI),a passivation film covering the electrode surface,is crucial to the lifetime and efficiency of the lithium-ion(Li-ion)battery.Understanding the Li-ion diffusion mechanism within possible components in the mosaic-structured SEI is an essential step to improve the Li-ion conductivity and thus the battery performance.Here,we investigate the Li-ion diffusion mechanism within three amorphous SEI components(i.e.,the inorganic inner layer,organic outer layer,and their mixture with 1:1 molar ratio)via ab initio molecular dynamic(AIMD)simulations.Our simulations show that the Li-ion diffusion coefficient in the inorganic layer is two orders of magnitude faster than that in the organic layer.Therefore,the inorganic layer makes a major contribution to the Li-ion diffusion.Furthermore,we find that the Li-ion diffusivity in the organic layer decreases slightly with the increase of the carbon chain from the methyl to ethyl owing to the steric hindrance induced by large groups.Overall,our current work unravels the Li-ion diffusion mechanism,and provides an atomic-scale insight for the understanding of the Li-ion transport in the SEI components.
基金The Science and Technology Commission of Shanxi province,No.201901D111428.
文摘BACKGROUND Ferroptosis has recently been associated with multiple degenerative diseases.Ferroptosis induction in cancer cells is a feasible method for treating neoplastic diseases.However,the association of iron proliferation-related genes with prognosis in HER2+breast cancer(BC)patients is unclear.AIM To identify and evaluate fresh ferroptosis-related biomarkers for HER2+BC.METHODS First,we obtained the mRNA expression profiles and clinical information of HER2+BC patients from the TCGA and METABRIC public databases.A four gene prediction model comprising PROM2,SLC7A11,FANCD2,and FH was subsequently developed in the TCGA cohort and confirmed in the METABRIC cohort.Patients were stratified into high-risk and low-risk groups based on their median risk score,an independent predictor of overall survival(OS).Based on these findings,immune infiltration,mutations,and medication sensitivity were analyzed in various risk groupings.Additionally,we assessed patient prognosis by combining the tumor mutation burden(TMB)with risk score.Finally,we evaluated the expression of critical genes by analyzing single-cell RNA sequencing(scRNA-seq)data from malignant vs normal epithelial cells.RESULTS We found that the higher the risk score was,the worse the prognosis was(P<0.05).We also found that the immune cell infiltration,mutation,and drug sensitivity were different between the different risk groups.The highrisk subgroup was associated with lower immune scores and high TMB.Moreover,we found that the combination of the TMB and risk score could stratify patients into three groups with distinct prognoses.HRisk-HTMB patients had the worst prognosis,whereas LRisk-LTMB patients had the best prognosis(P<0.0001).Analysis of the scRNAseq data showed that PROM2,SLC7A11,and FANCD2 were significantly differentially expressed,whereas FH was not,suggesting that these genes are expressed mainly in cancer epithelial cells(P<0.01).CONCLUSION Our model helps guide the prognosis of HER2+breast cancer patients,and its combination with the TMB can aid in more accurate assessment of patient prognosis and provide new ideas for further diagnosis and treatment.
基金supported by 2023 Wenzhou Philosophy and Social Science Planning Annual Project(2023年温州市社科联项目)(23WSK131YBM)Student Science Research Project of Wenzhou University(2023kx038)+2 种基金Student Innovation and Entrepreneurship Training Program Project of WZU(JWXC2023075)Zhejiang Foreign Language Society Project(ZWYB2023023)Zhejiang University Student Science and Technology Innovation Activity Plan(XMS2206006).
文摘In recent years,with the rise of video media such as YouTube and Tik Tok,the short video creation industry has emerged.How to spread China's excellent culture and how to“tell a good Chinese story”have become a hot concern.Using the 5W Model of Communication as a framework for analysis,this paper selects Chinese short videos with high popularity on YouTube as the object of the study.Studies found that the success of these videos was associated with five factors in the process of communication,which are communication main forces,communication content,communication channels,communication audience,and audience effects.Through theoretical and data analysis,the study concluded five strategies in video production to help promote Intercultural communication.