Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving...Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.展开更多
Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundame...Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.展开更多
All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional l...All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.展开更多
With the rapid advancement of portable energy devices and sensor technologies,enhancing their catalytic performance,sensing capabilities,and application reliability has become a critical challenge in the fields of mat...With the rapid advancement of portable energy devices and sensor technologies,enhancing their catalytic performance,sensing capabilities,and application reliability has become a critical challenge in the fields of materials and energy science.Single-atom catalysts(SACs),owing to their high atomic utilization,outstanding catalytic activity,and precisely engineered structures enabled by density functional theory and enhanced by artificial intelligence,have shown tremendous potential in advancing portable energy and sensing technologies.While existing reviews predominantly focus on the application of SACs in individual portable devices,systematic discussions on their overall development prospects and challenges within portable energy and sensor fields remain scarce.Therefore,this review comprehensively explores the application potential and recent advancements of SACs in portable zinc-air batteries,proton exchange membrane fuel cells,and sensor technologies.The article highlights the influence of key factors such as material design,structural optimization,and packaging integration on device performance,while also addressing the primary bottlenecks and challenges encountered in current practical applications.Furthermore,it suggests possible future development directions,aiming to offer theoretical insights and engineering guidance for the large-scale deployment of SACs in wearable electronic devices,portable energy systems,and smart sensing technologies.展开更多
The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supp...The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.展开更多
Chronic hepatitis B(CHB)infection remains a serious public health problem worldwide;however,the relationship between cholesterol levels and CHB remains unclear.We isolated peripheral blood mononuclear cells from healt...Chronic hepatitis B(CHB)infection remains a serious public health problem worldwide;however,the relationship between cholesterol levels and CHB remains unclear.We isolated peripheral blood mononuclear cells from healthy blood donors and CHB patients to analyze free cholesterol levels,lipid raft formation,and cholesterol metabolism-related pathways.Hepatitis B virus(HBV)-carrier mice were generated and used to confirm changes in cholesterol metabolism and cell-surface lipid raft formation in dendritic cells(DCs)in the context of CHB.Additionally,HBV-carrier mice were immunized with a recombinant HBV vaccine(rHBVvac)combined with lipophilic statins and evaluated for vaccine efficacy against HBV.Serum samples were analyzed for HBsAg,anti-HBs,and alanine aminotransferase levels,and liver samples were evaluated for HBV DNA and RNA and HBcAg.CHB reduced free cholesterol levels and suppressed lipid raft formation on DCs in patients with CHB and HBV-carrier mice,whereas administration of lipophilic statins promoted free cholesterol accumulation and restored lipid rafts on DCs accompanied by an enhanced antigen-presentation ability in vitro and in vivo.Cholesterol accumulation on DCs improved the rHBVvac-mediated elimination of serum HBV DNA and intrahepatic HBV DNA,HBV RNA,and HBcAg and promoted the rHBVvac-mediated generation and polyfunctionality of HBV-specific CD11a^(hi) CD8α^(lo) cells,induction of the development of memory responses against HBV reinfection,and seroconversion from HBsAg to anti-HBs.The results demonstrated the important role of cholesterol levels in DC dysfunction during CHB,suggesting that strategies to increase cholesterol accumulation on DCs might enhance therapeutic vaccine efficacy against HBV and support development toward clinical CHB treatment.展开更多
Single-atom materials(SAMs)have become one of the most important power sources to push the field of energy conversion forward.Among the main types of energy,including thermal energy,electrical energy,solar energy,and ...Single-atom materials(SAMs)have become one of the most important power sources to push the field of energy conversion forward.Among the main types of energy,including thermal energy,electrical energy,solar energy,and biomass energy,SAMs have realized ultra-high efficiency and show an appealing future in practical application.More than high activity,the uniform active sites also provide a convincible model for chemists to design and comprehend the mechanism behind the phenomenon.Therefore,we presented an insightful review of the application of the single-atom material in the field of energy conversion.The challenges(e.g.,accurate synthesis and practical application)and future directions(e.g.,machine learning and efficient design)of the applications of SAMs in energy conversion are included,aiming to provide guidance for the research in the next step.展开更多
Deep learning models demonstrate impressive performance in rapidly predicting urban floods,but there are still limitations in enhancing physical connectivity and interpretability.This study proposed an innovative mode...Deep learning models demonstrate impressive performance in rapidly predicting urban floods,but there are still limitations in enhancing physical connectivity and interpretability.This study proposed an innovative modeling approach that integrates convolutional neural networks with weighted cellular automaton(CNN-WCA)to achieve the precise and rapid prediction of urban pluvial flooding processes and enhance the physical connectivity and reliability of modeling results.The study began by generating a rainfall-inundation dataset using WCA and LISFLOOD-FP,and the CNN-WCA model was trained using outputs from LISFLOOD-FP and WCA.Subsequently,the pre-trained model was applied to simulate the flood caused by the 20 July 2021 rainstorm in Zhengzhou City.The predicted inundation spatial distribution and depth by CNN-WCA closely aligned with those of LISFLOOD-FP,with the mean absolute error concentrated within 5 mm,and the prediction time of CNN-WCA was only 0.8%that of LISFLOOD-FP.The CNN-WCA model displays a strong capacity for accurately predicting changes in inundation depths within the study area and at susceptible points for urban flooding,with the Nash-Sutcliffe e fficiency values of most flood-prone points exceeding 0.97.Furthermore,the physical connectivity of the inundation distribution predicted by CNN-WCA is better than that of the distribution obtained with a CNN.The CNN-WCA model with additional physical constraints exhibits a reduction of around 34%in instances of physical discontinuity compared to CNN.Our results prove that the CNN model with multiple physical constraints has signifi cant potential to rapidly and accurately simulate urban flooding processes and improve the reliability of prediction.展开更多
基金the financial support from the National Natural Science Foundation of China(52203123 and 52473248)State Key Laboratory of Polymer Materials Engineering(sklpme2024-2-04)+1 种基金the Fundamental Research Funds for the Central Universitiessponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.
基金financial support from the National Natural Science Foundation of China(52203123)the Sichuan Science and Technology Program(2023NSFSC0991)+2 种基金the State Key Laboratory of Polymer Materials Engineering(sklpme 2023-1-05 and sklpme 2024-2-04)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.
基金National Natural Science Foundation of China (52203123)Sichuan Science and Technology Program (2023NSFSC0991)+2 种基金State Key Laboratory of Polymer Materials Engineering (sklpme-2023-1-05 and sklpme-2024-2-04)Fundamental Research Funds for the Central UniversitiesThis research was also partially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.
文摘With the rapid advancement of portable energy devices and sensor technologies,enhancing their catalytic performance,sensing capabilities,and application reliability has become a critical challenge in the fields of materials and energy science.Single-atom catalysts(SACs),owing to their high atomic utilization,outstanding catalytic activity,and precisely engineered structures enabled by density functional theory and enhanced by artificial intelligence,have shown tremendous potential in advancing portable energy and sensing technologies.While existing reviews predominantly focus on the application of SACs in individual portable devices,systematic discussions on their overall development prospects and challenges within portable energy and sensor fields remain scarce.Therefore,this review comprehensively explores the application potential and recent advancements of SACs in portable zinc-air batteries,proton exchange membrane fuel cells,and sensor technologies.The article highlights the influence of key factors such as material design,structural optimization,and packaging integration on device performance,while also addressing the primary bottlenecks and challenges encountered in current practical applications.Furthermore,it suggests possible future development directions,aiming to offer theoretical insights and engineering guidance for the large-scale deployment of SACs in wearable electronic devices,portable energy systems,and smart sensing technologies.
基金the National Key R&D Program of China(2018YFA0702003)the National Natural Science Foundation of China(21890383,21671117,21871159 and21901135)the Science and Technology Key Project of Guangdong Province of China(2020B010188002)。
文摘The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.
基金supported by the National Key Research and Development Programme (2021YFC2300603)the National Postdoctoral Programme for Innovative Talents (No.BX20190192)+1 种基金the China Postdoctoral Science Foundation (No.2020M672064)the National Science Foundation for Young Scientists of China (No.82001687).
文摘Chronic hepatitis B(CHB)infection remains a serious public health problem worldwide;however,the relationship between cholesterol levels and CHB remains unclear.We isolated peripheral blood mononuclear cells from healthy blood donors and CHB patients to analyze free cholesterol levels,lipid raft formation,and cholesterol metabolism-related pathways.Hepatitis B virus(HBV)-carrier mice were generated and used to confirm changes in cholesterol metabolism and cell-surface lipid raft formation in dendritic cells(DCs)in the context of CHB.Additionally,HBV-carrier mice were immunized with a recombinant HBV vaccine(rHBVvac)combined with lipophilic statins and evaluated for vaccine efficacy against HBV.Serum samples were analyzed for HBsAg,anti-HBs,and alanine aminotransferase levels,and liver samples were evaluated for HBV DNA and RNA and HBcAg.CHB reduced free cholesterol levels and suppressed lipid raft formation on DCs in patients with CHB and HBV-carrier mice,whereas administration of lipophilic statins promoted free cholesterol accumulation and restored lipid rafts on DCs accompanied by an enhanced antigen-presentation ability in vitro and in vivo.Cholesterol accumulation on DCs improved the rHBVvac-mediated elimination of serum HBV DNA and intrahepatic HBV DNA,HBV RNA,and HBcAg and promoted the rHBVvac-mediated generation and polyfunctionality of HBV-specific CD11a^(hi) CD8α^(lo) cells,induction of the development of memory responses against HBV reinfection,and seroconversion from HBsAg to anti-HBs.The results demonstrated the important role of cholesterol levels in DC dysfunction during CHB,suggesting that strategies to increase cholesterol accumulation on DCs might enhance therapeutic vaccine efficacy against HBV and support development toward clinical CHB treatment.
基金National Natural Science Foundation of China,Grant/Award Number:22325101。
文摘Single-atom materials(SAMs)have become one of the most important power sources to push the field of energy conversion forward.Among the main types of energy,including thermal energy,electrical energy,solar energy,and biomass energy,SAMs have realized ultra-high efficiency and show an appealing future in practical application.More than high activity,the uniform active sites also provide a convincible model for chemists to design and comprehend the mechanism behind the phenomenon.Therefore,we presented an insightful review of the application of the single-atom material in the field of energy conversion.The challenges(e.g.,accurate synthesis and practical application)and future directions(e.g.,machine learning and efficient design)of the applications of SAMs in energy conversion are included,aiming to provide guidance for the research in the next step.
基金supported by the General Program of National Natural Science Foundation of China(Grant No.42377467)。
文摘Deep learning models demonstrate impressive performance in rapidly predicting urban floods,but there are still limitations in enhancing physical connectivity and interpretability.This study proposed an innovative modeling approach that integrates convolutional neural networks with weighted cellular automaton(CNN-WCA)to achieve the precise and rapid prediction of urban pluvial flooding processes and enhance the physical connectivity and reliability of modeling results.The study began by generating a rainfall-inundation dataset using WCA and LISFLOOD-FP,and the CNN-WCA model was trained using outputs from LISFLOOD-FP and WCA.Subsequently,the pre-trained model was applied to simulate the flood caused by the 20 July 2021 rainstorm in Zhengzhou City.The predicted inundation spatial distribution and depth by CNN-WCA closely aligned with those of LISFLOOD-FP,with the mean absolute error concentrated within 5 mm,and the prediction time of CNN-WCA was only 0.8%that of LISFLOOD-FP.The CNN-WCA model displays a strong capacity for accurately predicting changes in inundation depths within the study area and at susceptible points for urban flooding,with the Nash-Sutcliffe e fficiency values of most flood-prone points exceeding 0.97.Furthermore,the physical connectivity of the inundation distribution predicted by CNN-WCA is better than that of the distribution obtained with a CNN.The CNN-WCA model with additional physical constraints exhibits a reduction of around 34%in instances of physical discontinuity compared to CNN.Our results prove that the CNN model with multiple physical constraints has signifi cant potential to rapidly and accurately simulate urban flooding processes and improve the reliability of prediction.
