Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition be...Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.展开更多
As crucial carriers of culture,ancient paintings embody profound historical narratives and aesthetic values.Yet,the lack of professional expertise often hinders non-experts from fully appreciating these works.This dis...As crucial carriers of culture,ancient paintings embody profound historical narratives and aesthetic values.Yet,the lack of professional expertise often hinders non-experts from fully appreciating these works.This disconnect leads to misinterpretation and creates a barrier that diminishes the value of aesthetic education.Digital design is currently revolutionizing public engagement with ancient painting,offering transformative pathways to enhance aesthetic appreciation(Chen et al.,2025a;Tang et al.,2024).展开更多
The development of adsorbent materials for effective capture of radioactive iodomethane(CH_(3)I) from the off-gas of used nuclear fuel reprocessing, remains a significant and challenging line of research because curre...The development of adsorbent materials for effective capture of radioactive iodomethane(CH_(3)I) from the off-gas of used nuclear fuel reprocessing, remains a significant and challenging line of research because currently state-of-art adsorbents still suffer from low binding affinity with CH_(3)I. Here, we proposed a brand-new adsorption topological structure by developing a 2D interdigitated layered framework, named SCU-20, featuring slide-like channel with multiple active sites for CH_(3)I capture. The responsive rotating-adaptive aperture of SCU-20 enables the optimal utilization of all active sites within the pore for highly selective recognition and capture of CH_(3)I. A record-breaking CH_(3)I uptake capacity of 1.84 g/g was achieved under static sorption conditions with saturated CH_(3)I vapor. Both experimental and theoretical findings demonstrated that the exceptional uptake of SCU-20 towards CH_(3)I can be attributed to the confined physical electrostatic adsorption of F sites, coupled with the chemical nitrogen methylation reaction with uncoordinated N atoms of pyrazine. Moreover, dynamic CH_(3)I uptake capacity potentially allows for the capture of CH_(3)I in simulated real-world off gas reprocessing conditions. This study highlights the potential of SCU-20 as a promising candidate for efficient capture of iodine species and contributes to the development of effective solutions for radioactive iodine remediation.展开更多
The flexibility of metal-organic frameworks(MOFs)featuring stimuli-responsive structural transitions is often governed not only by the chemical composition and topology but also by orthogonal factors such as particle ...The flexibility of metal-organic frameworks(MOFs)featuring stimuli-responsive structural transitions is often governed not only by the chemical composition and topology but also by orthogonal factors such as particle size,desolvation method,and history of the sample.A precise understanding of the mechanism behind such observations has been lacking up to now,and there are still substantial open questions concerning the impact of sample treatment history.The DUT-8(M)family([M_(2)(2,6-ndc)2(dabco)]n,2,6-ndc=2,6-naphthalene dicarboxylate,dabco=1,4-diazabicyclo-[2.2.2]-octane),encompasses isostructural compounds based on Ni,Zn,Co,and Cu in the cluster node and is representative of pillared layer MOFs,often showing flexible behavior.In this contribution,we discuss a possible explanation for the differences in flexibility observed in desolvated phases of DUT-8(Cu).Theoretical calculations and crystallographic data shed light on the preferred formation of interpenetrated confined closed pore phases in DUT-8(Cu)in contrast to DUT-8(Ni,Co,Zn)where the closed pore phases are formed.展开更多
Metal-organic frameworks(MOFs)materials exhibit inherent advantages in microwave absorption(MA)due to their unique compositional and structural characteristics.However,it remains a significant challenge to systematica...Metal-organic frameworks(MOFs)materials exhibit inherent advantages in microwave absorption(MA)due to their unique compositional and structural characteristics.However,it remains a significant challenge to systematically elucidate the coordinated effects of component modulation and morphology design on electromagnetic parameters during the complex modification process to enhance the MA performance of MOFs.In this study,the twodimensional(2D)Co-based MOFs material,layered zeolitic imidazolate framework(ZIF-L),was meticulously selected as a structure design template and combined with an efficient ion-exchange component modulation method,aiming to stimulate the potential advantages between the two in the synergistic modulation of electromagnetic parameters.Specifically,the ion-exchange method enhanced various polarization mechanisms,including interface,dipole,and defect-induced polarizations.Meanwhile,the 2D template facilitates the formation of a robust conductive network on the surface and ensures the high efficiency and uniformity of the ion-exchange process.Ultimately,the resulting material achieved an adequate absorption bandwidth(EAB)of 6.47 GHz at a thickness of 2 mm,a 78% improvement over the untreated sample(EAB=3.64 GHz).This research not only provides valuable theoretical insights into the application of 2D MOFs materials in MA but also offers innovative perspectives for the design and development of energy-saving and environmentally friendly microwave absorption materials(MAMs).展开更多
Metal-organic framework(MOF)nanoparticles are successfully confined in the hollow mesoporous carbon spheres(HMCSs)through space-confined synthesis methods.The prepared ZIF-67@HMCSs nanocomposites act as effective sacr...Metal-organic framework(MOF)nanoparticles are successfully confined in the hollow mesoporous carbon spheres(HMCSs)through space-confined synthesis methods.The prepared ZIF-67@HMCSs nanocomposites act as effective sacrificial templates,which can afford Co^(2+)sources.After a facile solvothermal reaction and sequential cation etching,yolk-shell-structured layered double hydroxide@HMCSs(LDH@HMCSs)have been synthesized.The LDH@HMCSs nanocomposite possesses a three-dimensional(3D)hollow nanocage superstructure that effectively blocks the self-stacking of LDH nanosheets and promotes ion transport.Compared to CoFe-LDH@HMCSs,and Co-LDH@HMCSs,CoNi-LDH@HMCSs exhibit superior electrochemical performance and desalination performance due to the remarkable synergistic effect between the CoNi-LDH nanosheets and mesoporous N-doped carbon shells.The resultant CoNi-LDH@HMCSs-0.4-based capacitive deionization(CDI)device exhibits excellent salt adsorption capacity(SAC,36.41 mg·g^(-1))and good cycle stability.This work will confirm the significance of constructing superstructure and open new avenues for the practical application of CDI technology in water treatment.展开更多
Sodium-ion batteries are promising for large-scale energy storage due to sodium's low cost and infinite abundance. The most popular cathodes for sodium-ion batteries, i.e., the layered sodium-containing oxides, us...Sodium-ion batteries are promising for large-scale energy storage due to sodium's low cost and infinite abundance. The most popular cathodes for sodium-ion batteries, i.e., the layered sodium-containing oxides, usually exhibit reversible host rearrangement between P-type and O-type stacking upon charge/discharge. Herein we demonstrate that such host rearrangement is unfavorable and can be suppressed by introducing transition-metal ions into sodium layers. The electrode with stabilized P3-type stacking delivers superior rate capability, high energy efficiency, and excellent cycling performance. Owing to the cation-mixing nature, it performs the lowest lattice strain among all reported cathodes for sodium-ion batteries. Our findings highlight the significance of a stable host for sodium-ion storage and moreover underline the fundamental distinction in material design strategy between lithium-and sodium-ion batteries.展开更多
基金supported by the National Natural Science Foundation of China (52302292, 52302058, 52302085)the China Postdoctoral Science Foundation (2021M702225)+1 种基金the Anhui Province University Natural Science Research Project (2023AH030093, 2023AH040301)the Startup Research Fund of Chaohu University (KYQD-2023005, KYQD-2023051)。
文摘Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.
文摘As crucial carriers of culture,ancient paintings embody profound historical narratives and aesthetic values.Yet,the lack of professional expertise often hinders non-experts from fully appreciating these works.This disconnect leads to misinterpretation and creates a barrier that diminishes the value of aesthetic education.Digital design is currently revolutionizing public engagement with ancient painting,offering transformative pathways to enhance aesthetic appreciation(Chen et al.,2025a;Tang et al.,2024).
基金supported by the Intergovernmental International Cooperation of the National Key R&D Program of China(2022YFE0105300)the National Natural Science Foundation of China(21790374, 22276130, 22176139, 21825601)the New Cornerstone Science Foundation through the XPLORER PRIZE。
文摘The development of adsorbent materials for effective capture of radioactive iodomethane(CH_(3)I) from the off-gas of used nuclear fuel reprocessing, remains a significant and challenging line of research because currently state-of-art adsorbents still suffer from low binding affinity with CH_(3)I. Here, we proposed a brand-new adsorption topological structure by developing a 2D interdigitated layered framework, named SCU-20, featuring slide-like channel with multiple active sites for CH_(3)I capture. The responsive rotating-adaptive aperture of SCU-20 enables the optimal utilization of all active sites within the pore for highly selective recognition and capture of CH_(3)I. A record-breaking CH_(3)I uptake capacity of 1.84 g/g was achieved under static sorption conditions with saturated CH_(3)I vapor. Both experimental and theoretical findings demonstrated that the exceptional uptake of SCU-20 towards CH_(3)I can be attributed to the confined physical electrostatic adsorption of F sites, coupled with the chemical nitrogen methylation reaction with uncoordinated N atoms of pyrazine. Moreover, dynamic CH_(3)I uptake capacity potentially allows for the capture of CH_(3)I in simulated real-world off gas reprocessing conditions. This study highlights the potential of SCU-20 as a promising candidate for efficient capture of iodine species and contributes to the development of effective solutions for radioactive iodine remediation.
基金made possible as a result of a generous grant from the German Research Foundation(grant no.279409724).
文摘The flexibility of metal-organic frameworks(MOFs)featuring stimuli-responsive structural transitions is often governed not only by the chemical composition and topology but also by orthogonal factors such as particle size,desolvation method,and history of the sample.A precise understanding of the mechanism behind such observations has been lacking up to now,and there are still substantial open questions concerning the impact of sample treatment history.The DUT-8(M)family([M_(2)(2,6-ndc)2(dabco)]n,2,6-ndc=2,6-naphthalene dicarboxylate,dabco=1,4-diazabicyclo-[2.2.2]-octane),encompasses isostructural compounds based on Ni,Zn,Co,and Cu in the cluster node and is representative of pillared layer MOFs,often showing flexible behavior.In this contribution,we discuss a possible explanation for the differences in flexibility observed in desolvated phases of DUT-8(Cu).Theoretical calculations and crystallographic data shed light on the preferred formation of interpenetrated confined closed pore phases in DUT-8(Cu)in contrast to DUT-8(Ni,Co,Zn)where the closed pore phases are formed.
基金supported by the National Natural Science Foundation of China(No.52172295)Young talent lift project(No.2021-JCJQQT-064)+1 种基金the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_0571)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_0371).
文摘Metal-organic frameworks(MOFs)materials exhibit inherent advantages in microwave absorption(MA)due to their unique compositional and structural characteristics.However,it remains a significant challenge to systematically elucidate the coordinated effects of component modulation and morphology design on electromagnetic parameters during the complex modification process to enhance the MA performance of MOFs.In this study,the twodimensional(2D)Co-based MOFs material,layered zeolitic imidazolate framework(ZIF-L),was meticulously selected as a structure design template and combined with an efficient ion-exchange component modulation method,aiming to stimulate the potential advantages between the two in the synergistic modulation of electromagnetic parameters.Specifically,the ion-exchange method enhanced various polarization mechanisms,including interface,dipole,and defect-induced polarizations.Meanwhile,the 2D template facilitates the formation of a robust conductive network on the surface and ensures the high efficiency and uniformity of the ion-exchange process.Ultimately,the resulting material achieved an adequate absorption bandwidth(EAB)of 6.47 GHz at a thickness of 2 mm,a 78% improvement over the untreated sample(EAB=3.64 GHz).This research not only provides valuable theoretical insights into the application of 2D MOFs materials in MA but also offers innovative perspectives for the design and development of energy-saving and environmentally friendly microwave absorption materials(MAMs).
基金supported by the National Natural Science Foundation of China(No.52371240).
文摘Metal-organic framework(MOF)nanoparticles are successfully confined in the hollow mesoporous carbon spheres(HMCSs)through space-confined synthesis methods.The prepared ZIF-67@HMCSs nanocomposites act as effective sacrificial templates,which can afford Co^(2+)sources.After a facile solvothermal reaction and sequential cation etching,yolk-shell-structured layered double hydroxide@HMCSs(LDH@HMCSs)have been synthesized.The LDH@HMCSs nanocomposite possesses a three-dimensional(3D)hollow nanocage superstructure that effectively blocks the self-stacking of LDH nanosheets and promotes ion transport.Compared to CoFe-LDH@HMCSs,and Co-LDH@HMCSs,CoNi-LDH@HMCSs exhibit superior electrochemical performance and desalination performance due to the remarkable synergistic effect between the CoNi-LDH nanosheets and mesoporous N-doped carbon shells.The resultant CoNi-LDH@HMCSs-0.4-based capacitive deionization(CDI)device exhibits excellent salt adsorption capacity(SAC,36.41 mg·g^(-1))and good cycle stability.This work will confirm the significance of constructing superstructure and open new avenues for the practical application of CDI technology in water treatment.
基金The financial support from the National Basic Research Program of China(2014CB932300)Natural Science Foundation of Jiangsu Province of China(BK20170630)+1 种基金NSF of China(21633003 and 51602144)sponsored by the JST-CREST ‘‘Phase Interface Science for Highly Efficient Energy Utilization",JST(Japan)
文摘Sodium-ion batteries are promising for large-scale energy storage due to sodium's low cost and infinite abundance. The most popular cathodes for sodium-ion batteries, i.e., the layered sodium-containing oxides, usually exhibit reversible host rearrangement between P-type and O-type stacking upon charge/discharge. Herein we demonstrate that such host rearrangement is unfavorable and can be suppressed by introducing transition-metal ions into sodium layers. The electrode with stabilized P3-type stacking delivers superior rate capability, high energy efficiency, and excellent cycling performance. Owing to the cation-mixing nature, it performs the lowest lattice strain among all reported cathodes for sodium-ion batteries. Our findings highlight the significance of a stable host for sodium-ion storage and moreover underline the fundamental distinction in material design strategy between lithium-and sodium-ion batteries.
