The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.A...The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.Accordingly,comprehensive kinetic study by employing thermalgravimetric analysis at various heating rates was presented in this paper.Two main weight loss regions were observed during heating.The initial region corresponded to the dehydration of crystal water,whereas the subsequent region with overlapping peaks involved complex decomposition reactions.The overlapping peaks were separated into two individual reaction peaks and the activation energy of each peak was calculated using isoconversional kinetics methods.The activation energy of peak 1 exhibited a continual increase as the reaction conversion progressed,while that of peak 2 steadily decreased.The optimal kinetic models,identified as belonging to the random nucleation and subsequent growth category,provided valuable insights into the mechanism of the decomposition reactions.Furthermore,the adjustment factor was introduced to reconstruct the kinetic mechanism models,and the reconstructed models described the kinetic mechanism model more accurately for the decomposition reactions.This study enhanced the understanding of the thermochemical behavior and kinetic parameters of the lepidolite sulfation product decomposition reactions,further providing theoretical basis for promoting the selective extraction of lithium.展开更多
The rapid expansion of lithium-ion batteries in electric vehicles and grid-scale energy storage intensify the demand for sustainable recycling strategies.Traditional metallurgical recycling methods face significant ch...The rapid expansion of lithium-ion batteries in electric vehicles and grid-scale energy storage intensify the demand for sustainable recycling strategies.Traditional metallurgical recycling methods face significant challenges,including high energy consumption,environmental pollution,and inefficient critical metals recovery.In contrast,advanced direct recycling can selectively extract valuable metals while preserving cathode structure,achieving over 99%lithium recovery from lithium iron phosphate.Moreover,by directly repairing defects and crystal structures of spent materials,their electrochemical performance can be effectively restored.Due to significantly reduced energy and reagent inputs,direct recycling cuts processing costs by over 20% and reduces waste emissions by at least 40% compared to conventional methods,making it a promising low-carbon alternative.This review systematically integrates the recent advances in direct recycling of spent batteries as well as the limitations and challenges of existing technologies,and proposes future research pathways to promote resource recycling and sustainable development.展开更多
Poly(ester amide)s(PEAs)represent promising biomaterials because of their well-balanced mechanical properties,biodegradability,and biocompatibility.However,practical applications of PEAs are still limited by challenge...Poly(ester amide)s(PEAs)represent promising biomaterials because of their well-balanced mechanical properties,biodegradability,and biocompatibility.However,practical applications of PEAs are still limited by challenges in functional versatility and environmental adaptability.Here,we present the first synthesis of periodic selenium-incorporated PEAs(Se-PEAs)via a rapid,catalyst-free selenol-yne click polymerization process.By harnessing the versatility of selenium,we achieved precise modulation of material properties.The resulting Se-PEAs demonstrated tunable mechanical behavior,spanning rigid plastics to elastomers,alongside exceptional thermal stability and high optical clarity.Programmable degradation profiles ensure long-term stability in physiological environments while facilitating rapid oxidative degradation at the end of the lifecycle.Surface selenoniumization further conferred robust antibacterial efficacy without compromising mechanical integrity.This multifunctionality positions Se-PEAs as transformative materials for biomedical implants,sustainable packaging,and high-refractiveindex optics.Our work advanced functional polymer design and underscored the potential of selenium chemistry in addressing global challenges in terms of plastic waste and ecological sustainability.展开更多
This review highlights the performance enhancement of polyvinyl alcohol(PVA)composites through the incorporation of nanofillers,focusing on mechanical,thermal,electrical and piezoelectric improvements.It examines bio-...This review highlights the performance enhancement of polyvinyl alcohol(PVA)composites through the incorporation of nanofillers,focusing on mechanical,thermal,electrical and piezoelectric improvements.It examines bio-based fillers such as nanocellulose cellulose nanofibrils(CNF)and cellulose nanocrystals(CNC),and carbon-based fillers like graphene nanoplatelets(GNP)and carbon nanotubes(CNT).CNF and CNC increase tensile strength by up to 40%and 17.9%,respectively,due to their ability to reinforce polymer networks.CNC also improves thermal stability,raising degradation temperatures to approximately 327℃through enhanced hydrogen bonding.Electrical and piezoelectric properties are significantly improved,with dielectric behaviour enhanced by up to 107%and open-circuit voltage reaching 25.6 V,suitable for energy harvesting.GNP and CNT contribute by forming conductive networks within the PVA matrix,enabling superior electrical conductivity and consistent piezoresistive responses under strain.These characteristics make such composites ideal for applications in flexible electronics,sensors,structural health monitoring and other advanced fields.This synthesis of experimental results and critical insights underscores the broad utility and future potential of nanofillerenhanced PVA composites across aerospace,automotive,healthcare,and defence sectors.展开更多
The rapid development of portable electronics,wearable technologies,and healthcare monitoring systems necessitates the innovation of flexible energy storage systems.Considering environmental pollution and the depletio...The rapid development of portable electronics,wearable technologies,and healthcare monitoring systems necessitates the innovation of flexible energy storage systems.Considering environmental pollution and the depletion of fossil resources,the utilization of renewable resources to engineer advanced flexible materials has become especially crucial.Cellulose,the most abundant natural polymer,has emerged as a promising precursor for advanced functional materials due to its unique structure and properties.Typically,the easy processability,tunable chemical structure,self-assembly behavior,mechanical strength,and reinforcing capability enable its utilization as binder,substrate,hybrid electrode,separator,and electrolyte reservoir for flexible energy storage devices.This review comprehensively summarizes the design,fabrication,and mechanical and electrochemical performances of cellulose-based materials.The structure and unique properties of cellulose are first briefly introduced.Then,the construction of cellulose-based materials in the forms of 1D fibers/filaments,2D films/membranes,3D hydrogels and aerogels is discussed,and the merits of cellulose in these materials are emphasized.After that,the various advanced applications in supercapacitors,lithium-ion batteries,lithium-sulfur batteries,sodium-ion batteries,metal-air batteries,and Zn-ion batteries are presented in detail.Finally,an outlook of the potential challenges and future perspectives in advanced cellulose-based materials for flexible energy storage systems is discussed.展开更多
Laser debonding technology has been widely used in advanced chip packaging,such as fan-out integration,2.5D/3D ICs,and MEMS devices.Typically,laser debonding of bonded pairs(R/R separation)is typically achieved by com...Laser debonding technology has been widely used in advanced chip packaging,such as fan-out integration,2.5D/3D ICs,and MEMS devices.Typically,laser debonding of bonded pairs(R/R separation)is typically achieved by completely removing the material from the ablation region within the release material layer at high energy densities.However,this R/R separation method often results in a significant amount of release material and carbonized debris remaining on the surface of the device wafer,severely reducing product yields and cleaning efficiency for ultra-thin device wafers.Here,we proposed an interfacial separation strategy based on laser-induced hot stamping effect and thermoelastic stress wave,which enables stress-free separation of wafer bonding pairs at the interface of the release layer and the adhesive layer(R/A separation).By comprehensively analyzing the micro-morphology and material composition of the release material,we elucidated the laser debonding behavior of bonded pairs under different separation modes.Additionally,we calculated the ablation threshold of the release material in the case of wafer bonding and established the processing window for different separation methods.This work offers a fresh perspective on the development and application of laser debonding technology.The proposed R/A interface separation method is versatile,controllable,and highly reliable,and does not leave release materials and carbonized debris on device wafers,demonstrating strong industrial adaptability,which greatly facilitates the application and development of advanced packaging for ultra-thin chips.展开更多
Type 2 diabetes markedly elevates fracture risk despite normal or high bone mineral density,a paradox reflecting qualitative skeletal deficits rather than loss of mass.Chronic hyperglycemia fosters the accumulation of...Type 2 diabetes markedly elevates fracture risk despite normal or high bone mineral density,a paradox reflecting qualitative skeletal deficits rather than loss of mass.Chronic hyperglycemia fosters the accumulation of advanced glycation end products in bone;their nonenzymatic crosslinks stiffen type I collagen,impair mineralization,and erode mechanical strength.By engaging the receptor for advanced glycation end products,these adducts activate nuclear factorκB and mitogen-activated protein kinase cascades,amplifying oxidative stress,inflammation,osteoblast dysfunction,and osteoclastogenesis.This review synthesizes epidemiological data from type 1 and type 2 diabetes,highlights the limits of densitybased skeletal assessment,and details the molecular pathology of the glycation-collagen axis.It also appraises antiglycation therapies,including formation inhibitors,crosslink breakers and receptor antagonists,with a particular focus on sodium-glucose cotransporter 2 inhibitors that couple glycemic control with modulation of the glycation pathway.By integrating recent basic and clinical advances,we propose a mechanistic framework for diabetic bone disease and outline strategies to mitigate glycationdriven skeletal fragility.展开更多
The rapid expansion of railways,especially High-Speed Railways(HSRs),has drawn considerable interest from both academic and industrial sectors.To meet the future vision of smart rail communications,the rail transport ...The rapid expansion of railways,especially High-Speed Railways(HSRs),has drawn considerable interest from both academic and industrial sectors.To meet the future vision of smart rail communications,the rail transport industry must innovate in key technologies to ensure high-quality transmissions for passengers and railway operations.These systems must function effectively under high mobility conditions while prioritizing safety,ecofriendliness,comfort,transparency,predictability,and reliability.On the other hand,the proposal of 6 G wireless technology introduces new possibilities for innovation in communication technologies,which may truly realize the current vision of HSR.Therefore,this article gives a review of the current advanced 6 G wireless communication technologies for HSR,including random access and switching,channel estimation and beamforming,integrated sensing and communication,and edge computing.The main application scenarios of these technologies are reviewed,as well as their current research status and challenges,followed by an outlook on future development directions.展开更多
Silicone rubber(SR)is a versatile material widely used across various advanced functional applications,such as soft actuators and robots,flexible electronics,and medical devices.However,most SR molding methods rely on...Silicone rubber(SR)is a versatile material widely used across various advanced functional applications,such as soft actuators and robots,flexible electronics,and medical devices.However,most SR molding methods rely on traditional thermal processing or direct ink writing three-dimensional(3D)printing.These methods are not conducive to manufacturing complex structures and present challenges such as time inefficiency,poor accuracy,and the necessity of multiple steps,significantly limiting SR applications.In this study,we developed an SR-based ink suitable for vat photopolymerization 3D printing using a multi-thiol monomer.This ink enables the one-step fabrication of complex architectures with high printing resolution at the micrometer scale,providing excellent mechanical strength and superior chemical stability.Specifically,the optimized 3D printing SR-20 exhibits a tensile stress of 1.96 MPa,an elongation at break of 487.9%,and an elastic modulus of 225.4 kPa.Additionally,the 3D-printed SR samples can withstand various solvents(acetone,toluene,and tetrahydrofuran)and endure temperatures ranging from-50℃ to 180℃,demonstrating superior stability.As a emonstration of the application,we successfully fabricated a series of SR-based soft pneumatic actuators and grippers in a single step with this technology,allowing for free assembly for the first time.This ultraviolet-curable SR,with high printing resolution and exceptional stability performance,has significant potential to enhance the capabilities of 3D printing for applications in soft actuators,robotics,flexible electronics,and medical devices.展开更多
Background:Immune checkpoint inhibitors(ICIs)are effective in a subset of patients with metastatic solid tumors.However,the patients who would benefit most from ICIs in biliary tract cancer(BTC)are still controversial...Background:Immune checkpoint inhibitors(ICIs)are effective in a subset of patients with metastatic solid tumors.However,the patients who would benefit most from ICIs in biliary tract cancer(BTC)are still controversial.Materials and methods:We molecularly characterized tissues and blood from 32 patients with metastatic BTC treated with the ICI pembrolizumab as second-line therapy.Results:All patients had microsatellite stable(MSS)type tumors.Three of the 32 patients achieved partial response(PR),with an objective response rate(ORR)of 9.4%(95%confidence interval[CI],2.0–25.2)and nine showed stable disease(SD),exhibiting a disease control rate(DCR)of 37.5%(95%CI,21.1–56.3).For the 31 patients who had access to PD-1 ligand 1(PD-L1)combined positive score(CPS)testing(cut-off value≥1%),the ORR was not different between those who had PD-L1-positive(PD-L1+;1/11,9.1%)and PDL1-(2/20,10.0%)tumors(p=1.000).The tumor mutational burden(TMB)of PD-L1+BTC was comparable to that of PD-L1-BTC(p=0.630).TMB and any exonic somatic mutations were also not predictive of pembrolizumab response.Molecular analysis of blood and tumor samples demonstrated a relatively high natural killer(NK)cell proportion in the peripheral blood before pembrolizumab treatment in patients who achieved tumor response.Moreover,the tumors of these patients presented high enrichment scores for NK cells,antitumor cytokines,and Th1 signatures,and a low enrichment score for cancer-associated fibroblasts.Conclusions:This study shows the molecular characteristics associated with the efficacy of pembrolizumab in BTC of the MSS type.展开更多
Employing two-dimensional(2D)synaptic devices to develop a brain-inspired neuromorphic computing system is a promising approach to overcoming the limitations of the von Neumann architecture.However,isotropic 2D materi...Employing two-dimensional(2D)synaptic devices to develop a brain-inspired neuromorphic computing system is a promising approach to overcoming the limitations of the von Neumann architecture.However,isotropic 2D materials are predominantly utilized to fabricate synaptic devices.Research on inherently anisotropic 2D materials in synaptic devices remains scarce.Here,we report an intrinsically anisotropic material,CrSBr,which exhibits optoelectronic properties with significant angular dependence,achieving a carrier mobility ratio as high as 7.83between the a-axis and b-axis.Based on this,we couple the in-plane anisotropy into the synaptic device and construct CrSBr/WSe_(2)multi-terminal device.This device can be regulated by the gate voltage and laser,exhibiting storage and synaptic behaviors dependent on the a and b axes.Furthermore,we apply the synaptic property to achieve image recognition.Due to the anisotropic response to identical external stimulus,the a-axis conductance trend transits from nonlinear to approximately linear within the multi-terminal conductance framework.This multi-terminal synapse model achieves a recognition rate of up to 91%on the Fashion-MNIST database,significantly outperforming single-terminal recognition performance.Our work introduces a novel approach to anisotropic artificial synapses for simulated image recognition and establishes a foundation for developing AI systems with enhanced recognition rates.展开更多
Si,as the most promising anode with high theoretical capacity for next-generation lithium-ion batteries(LIBs),is hampered in commercial application by its poor electrical conductivity and significant volume expansion....Si,as the most promising anode with high theoretical capacity for next-generation lithium-ion batteries(LIBs),is hampered in commercial application by its poor electrical conductivity and significant volume expansion.Herein,the core-shell Si@SiO_(x)/C@C-Ar(SSC-A)or Si@SiO_(x)/C@C-H_(2)/Ar(SSC-H)composites are purposefully designed by in situ introduction of inorganic SiO_(x)in pure Ar or H_(2)/Ar atmosphere to realize a Si-based anode for LIBs.By introducing different atmospheres,the valence states of SiO_(x)are regulated.The inorganic transition layer formed by the combination of SiO_(x)with higher average valence and asphalt-derived carbon demonstrates better performance in both stabilizing the core-shell structure and inhibiting the agglomeration of Si particles.Given these advantages,the SSC-A electrode exhibits excellent electrochemical performance(1163 mAh g^(-1)after 400 cycles at 1 A g^(-1)),and the commercial blended graphite-SSC-A electrode reaches a specific capacity of 442 mAh g^(-1)with 74.8%capacity retention under the same conditions.Even the SSC-A electrode without Super P maintains an ultrahigh discharge specific capacity of 803 mAh g^(-1)with 60.6%after cycling.Importantly,the full batteries based on SSC-A without Super P achieve a discharge specific capacity of 126 mAh g^(-1)with 28.2%capacity decay after 200 cycles,demonstrating the superior commercial application potential.展开更多
Fiber-shaped energy storage devices(FSESDs)with exceptional flexibility for wearable power sources should be applied with solid electrolytes over liquid electrolytes due to short circuits and leakage issue during defo...Fiber-shaped energy storage devices(FSESDs)with exceptional flexibility for wearable power sources should be applied with solid electrolytes over liquid electrolytes due to short circuits and leakage issue during deformation.Among the solid options,polymer electrolytes are particularly preferred due to their robustness and flexibility,although their low ionic conductivity remains a significant challenge.Here,we present a redox polymer electrolyte(HT_RPE)with 4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl(HT)as a multi-functional additive.HT acts as a plasticizer that transforms the glassy state into the rubbery state for improved chain mobility and provides distinctive ion conduction pathway by the self-exchange reaction between radical and oxidized species.These synergetic effects lead to high ionic conductivity(73.5 mS cm−1)based on a lower activation energy of 0.13 eV than other redox additives.Moreover,HT_RPE with a pseudocapacitive characteristic by HT enables an outstanding electrochemical performance of the symmetric FSESDs using carbon-based fiber electrodes(energy density of 25.4 W h kg^(−1) at a power density of 25,000 W kg^(−1))without typical active materials,along with excellent stability(capacitance retention of 91.2%after 8,000 bending cycles).This work highlights a versatile HT_RPE that utilizes the unique functionality of HT for both the high ionic conductivity and improved energy storage capability,providing a promising pathway for next-generation flexible energy storage devices.展开更多
A self-developed crack-free advanced superalloy ZGH451 fabricated by direct energy deposition(DED)was applied to investigate the microstructure evolution,stress rupture behavior,and deformation mech-anisms at moderate...A self-developed crack-free advanced superalloy ZGH451 fabricated by direct energy deposition(DED)was applied to investigate the microstructure evolution,stress rupture behavior,and deformation mech-anisms at moderate-high temperatures and high-low stress conditions.The high Ta/Al ratio induces large misfit lattice stress and low stacking fault energy of alloy,resulting in approximate cubicγ′phases in dendrites and the formation of initial dislocation tangles.After the stress rupture test at 760℃/780 MPa,high content cubicγ′phases,small size of voids as well as preserved dislocation tangles are observed,showing stable structures with high-stress rupture resistance.High content and suitable size of cubicγ′phases,initial dislocation tangles,and L-C locks hinder the dislocation motion,which decreases the minimum strain rate and prolongs life significantly,forming four stress rupture stages.Hence,the defor-mation mechanism is determined by dislocation piled-up onγ/γ′interface,formation of stacking faults inγ′phases,and dislocations shearingγ′phases.However,the microstructure exhibits uneven struc-tures composed of large sizes of raftedγ′phases and voids at 980℃/260 MPa.The rafted structure and high temperature provide continuous channels and enough energy for dislocation motion,resulting in the increase of minimum strain rate,decline of life,and typic three stress rupture stages,even though there are obstacles to dislocation movement caused by dislocation networks.The deformation mecha-nism transforms to form dislocation networks onγ/γ′interface and dislocations shearingγ′phases.Be-sides,the decomposition of carbides on GBs also depends on temperature,which decomposes into harm-ful chain-like M23 C6 carbides at moderate temperatures and reinforced granular-shaped M6 C carbides at high temperatures.The applied stress always decreases mechanical properties due to its degradation of microstructure induced by elongating the precipitates and defects.展开更多
Over the past several decades,the integration of IONs into EP emerged as an effective method for enhancing its mechanical properties.Nevertheless,challenges remain,especially with u-IONs,where the interfacial strength...Over the past several decades,the integration of IONs into EP emerged as an effective method for enhancing its mechanical properties.Nevertheless,challenges remain,especially with u-IONs,where the interfacial strength with EP is suboptimal,resulting in aggregation within the EP matrix and a subsequent deterioration in the mechanical performance of u-ION/EP nanocomposites.In this comprehensive review,we explored advanced chemical modification techniques tailored for IONs incorporated into EP,providing a detailed examination of the mechanical characteristics of surface cm-ION/EP nanocomposites.This review investigates various chemical modification methods and their distinct impacts on the mechanical attributes of the resulting EP nanocomposites.Special emphasis is given to addressing the persistent challenges of inadequate interfacial strength and aggregation.Furthermore,this article examines prospective surface modification approaches for inorganic oxide nanoparticles,offering a visionary outlook on methods to improve the mechanical performance of EP in future.展开更多
High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailo...High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailorable electronic structure,and entropy stabilization effect.The precise fabrication of HEMs with functional nanostructures provides a crucial avenue to optimize the adsorption strength and catalytic activity for electrocatalysis.This review comprehensively summarizes the development of HEMs,focusing on the principles and strategies of structural design,and the catalytic mechanism towards hydrogen evolution reaction,oxygen evolution reaction and oxygen reduction reaction for the development of high-performance electrocatalysts.The complexity inherent in the interactions between different elements,the changes in the d-band center and the Gibbs free energies during the catalytic progress,as well as the coordination environment of the active sites associated with the unique crystal structure to improve the catalytic performance are discussed.We also provide a perspective on the challenges and future development direction of HEMs in electrocatalysis.This review will contribute to the design and development of HEMs-based catalysts for the next generation of electrochemical applications.展开更多
The advancement of high-performance zinc-air battery systems necessitates the development of highly effective non-precious metal-based bifunctional electrocatalysts capable of synergistically enhancing both oxygen red...The advancement of high-performance zinc-air battery systems necessitates the development of highly effective non-precious metal-based bifunctional electrocatalysts capable of synergistically enhancing both oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).To address the critical limitations of conventional non-precious catalysts in balancing multiple active sites and structural stability,we introduce an innovative in situ synthesis approach for constructing Fe_(2)P/FeNi bimetallic heterogeneous nanoparticles encapsulated within nitrogen-phosphorus dual-doped carbon matrices featuring interconnected leaf-like nanostructures(Fe_(2)P/FeNi@NPC).This architecturally optimized configuration not only mitigates transition metal degradation through protective carbon confinement but also facilitates rapid charge transfer kinetics and efficient mass diffusion pathways,substantially improving both catalytic efficiency and operational durability.Through comprehensive characterizations combining insitu monitoring and ex-situ analysis,the dynamic evolution of active sites during electrochemical operations is systematically tracked,and the genuine catalytic centers and spin state are identified.The optimized Fe_(2)P/FeNi@NPC composite exhibited remarkable electrochemical performance in alkaline media,achieving a superior ORR half-wave potential of 0.83 V and requiring only 1.62 V to achieve a current density of 10 mA cm^(-2)for OER.Notably,the assembled rechargeable zinc-air batteries(ZABs)exhibited a high specific capacity of 755.08 mAh g^(-1),a low charge-discharge voltage difference of 0.79 V,and exceptional cycling stability of over 1400 h.Furthermore,the flexible ZAB maintains excellent cycling performance even when subjected to various bending conditions.This work provides valuable insights into atomic-and electronic-scale dual-regulation strategy,offering a promising pathway to overcome current limitations in non-precious metal-based electrocatalysts for practical applications in metal-air battery systems.展开更多
Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggis...Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggish CO_(2)reduction reaction(CO_(2)RR)/CO_(2)evolution reaction(CO_(2)ER)kinetics remains a huge challenge.In this work,an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation,which significantly improves the electrocatalytic activity for both CO_(2)RR and CO_(2)ER.Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface,which leads to optimized binding affinity towards reactants and preferred Li_(2)CO_(3)decomposition behavior,enabling excellent catalytic activity during CO_(2)redox.Benefiting from the enhanced charge transfer ability,the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%.This work provides an attractive strategy to construct robust catalysts by interface engineering,which could inspire further design of superior bidirectional catalysts for Li-CO_(2)batteries.展开更多
Rechargeable magnesium batteries(RMBs)have garnered significant attention in energy storage applications due to their high capacity,low cost,and high safety.However,the strong polarization effect and slow kinetic de-i...Rechargeable magnesium batteries(RMBs)have garnered significant attention in energy storage applications due to their high capacity,low cost,and high safety.However,the strong polarization effect and slow kinetic de-intercalation of Mg^(2+)in the cathode limit their commercial application.This study presents a novel interface-coupled V_(2)CT_(x)@VS_(4)heterostructure through a one-step hydrothermal process.In this architecture,V_(2)CT_(x)and VS_(4)can mutually support their structural framework,which effectively prevents the structural collapse of V_(2)CT_(x)MXene and the aggregation of VS_(4).Crucially,interfacial coupling between V_(2)CT_(x)and VS_(4)induces strong V-S bonds,substantially enhancing structural stability.Benefiting from these advantages,the heterostructure exhibits high specific capacity(226 mAh g^(-1)at 100 mA g^(-1))and excellent long-cycle stability(89% capacity retention after 1000 cycles at 500 mA g^(-1)).Furthermore,the Mg^(2+)storage mechanism in the V_(2)CT_(x)@VS_(4)composite was elucidated through a series of ex-situ characterizations.This work provides a feasible strategy for designing V_(2)CT_(x)MXene-based cathodes with high capacity and extended cyclability for RMBs.展开更多
The evolution of energy storage technology has seen remarkable progress,with a shift from pure metals to sophisticated,tailor-made active materials.The synthesis of nanostructures with exceptional properties is crucia...The evolution of energy storage technology has seen remarkable progress,with a shift from pure metals to sophisticated,tailor-made active materials.The synthesis of nanostructures with exceptional properties is crucial in the advancement of electrode materials.In this regard,our study highlights the fabrication of a novel,oriented heterostructure comprised of Zn-Mn-Co-telluride grown on a pre-oxidized copper mesh using a hydrothermal method followed by a solvothermal process.This innovative approach leads to the formation of the Zn-Mn-Cotelluride@CuO@Cu heterostructure,which demonstrates the unique oriented morphology.It outperforms both Zn-Mn-Co-telluride@Cu and CuO@Cu by exhibiting lower electrical resistivity,increased redox activity,higher specific capacity,and improved ion diffusion characteristics.The conductivity enhancements of the heterostructure are corroborated by density functional theory(DFT)calculations.When utilized in a hybrid supercapacitor(HSC)alongside activated carbon(AC)electrodes,the Zn-Mn-Co-telluride@CuO@Cu heterostructurebased HSC achieves an energy density of 75.7 Wh kg^(-1).Such findings underscore the potential of these novel electrode materials to significantly impact the design of next-generation supercapacitor devices.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52034002 and U2202254)the Fundamental Research Funds for the Central Universities,China(No.FRF-TT-19-001)。
文摘The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.Accordingly,comprehensive kinetic study by employing thermalgravimetric analysis at various heating rates was presented in this paper.Two main weight loss regions were observed during heating.The initial region corresponded to the dehydration of crystal water,whereas the subsequent region with overlapping peaks involved complex decomposition reactions.The overlapping peaks were separated into two individual reaction peaks and the activation energy of each peak was calculated using isoconversional kinetics methods.The activation energy of peak 1 exhibited a continual increase as the reaction conversion progressed,while that of peak 2 steadily decreased.The optimal kinetic models,identified as belonging to the random nucleation and subsequent growth category,provided valuable insights into the mechanism of the decomposition reactions.Furthermore,the adjustment factor was introduced to reconstruct the kinetic mechanism models,and the reconstructed models described the kinetic mechanism model more accurately for the decomposition reactions.This study enhanced the understanding of the thermochemical behavior and kinetic parameters of the lepidolite sulfation product decomposition reactions,further providing theoretical basis for promoting the selective extraction of lithium.
基金supported by the National Science Fund for Distinguished Young Scholars(52425706)。
文摘The rapid expansion of lithium-ion batteries in electric vehicles and grid-scale energy storage intensify the demand for sustainable recycling strategies.Traditional metallurgical recycling methods face significant challenges,including high energy consumption,environmental pollution,and inefficient critical metals recovery.In contrast,advanced direct recycling can selectively extract valuable metals while preserving cathode structure,achieving over 99%lithium recovery from lithium iron phosphate.Moreover,by directly repairing defects and crystal structures of spent materials,their electrochemical performance can be effectively restored.Due to significantly reduced energy and reagent inputs,direct recycling cuts processing costs by over 20% and reduces waste emissions by at least 40% compared to conventional methods,making it a promising low-carbon alternative.This review systematically integrates the recent advances in direct recycling of spent batteries as well as the limitations and challenges of existing technologies,and proposes future research pathways to promote resource recycling and sustainable development.
基金supported by the National Natural Science Foundation of China(21971177)the Natural Science Foundation of the Jiangsu Higher Education Institution of China(22KJA150004)+3 种基金the Suzhou Science and Technology Bureau(SZM2021008)the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutionsthe Jiangsu Key Laboratory of Advanced Functional Polymers Design and Application,Soochow University,Suzhou Medical and Industrial Cooperation Innovation Project(SZM2022011)the Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis and the Program of Innovative Research Team of Soochow University。
文摘Poly(ester amide)s(PEAs)represent promising biomaterials because of their well-balanced mechanical properties,biodegradability,and biocompatibility.However,practical applications of PEAs are still limited by challenges in functional versatility and environmental adaptability.Here,we present the first synthesis of periodic selenium-incorporated PEAs(Se-PEAs)via a rapid,catalyst-free selenol-yne click polymerization process.By harnessing the versatility of selenium,we achieved precise modulation of material properties.The resulting Se-PEAs demonstrated tunable mechanical behavior,spanning rigid plastics to elastomers,alongside exceptional thermal stability and high optical clarity.Programmable degradation profiles ensure long-term stability in physiological environments while facilitating rapid oxidative degradation at the end of the lifecycle.Surface selenoniumization further conferred robust antibacterial efficacy without compromising mechanical integrity.This multifunctionality positions Se-PEAs as transformative materials for biomedical implants,sustainable packaging,and high-refractiveindex optics.Our work advanced functional polymer design and underscored the potential of selenium chemistry in addressing global challenges in terms of plastic waste and ecological sustainability.
基金Ministry of Higher Education Malaysia(MoHE)and Universiti Putra Malaysia under the Fundamental Research Grant Scheme(FRGS)(Grant Nos.FRGS/1/2023/TK09/UPM/01/3 and 5540599。
文摘This review highlights the performance enhancement of polyvinyl alcohol(PVA)composites through the incorporation of nanofillers,focusing on mechanical,thermal,electrical and piezoelectric improvements.It examines bio-based fillers such as nanocellulose cellulose nanofibrils(CNF)and cellulose nanocrystals(CNC),and carbon-based fillers like graphene nanoplatelets(GNP)and carbon nanotubes(CNT).CNF and CNC increase tensile strength by up to 40%and 17.9%,respectively,due to their ability to reinforce polymer networks.CNC also improves thermal stability,raising degradation temperatures to approximately 327℃through enhanced hydrogen bonding.Electrical and piezoelectric properties are significantly improved,with dielectric behaviour enhanced by up to 107%and open-circuit voltage reaching 25.6 V,suitable for energy harvesting.GNP and CNT contribute by forming conductive networks within the PVA matrix,enabling superior electrical conductivity and consistent piezoresistive responses under strain.These characteristics make such composites ideal for applications in flexible electronics,sensors,structural health monitoring and other advanced fields.This synthesis of experimental results and critical insights underscores the broad utility and future potential of nanofillerenhanced PVA composites across aerospace,automotive,healthcare,and defence sectors.
基金supported by National Natural Science Foundation of China(Grant Nos.32201499,32222057,and 22478142)Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2023A1515012519,2023A0505050114,and 2024B1515040004)+1 种基金National Key Research and Development Project(Grant No 2023YFE0109600)State Key Laboratory of Advanced Papermaking and Paper-based Materials(2024C02).
文摘The rapid development of portable electronics,wearable technologies,and healthcare monitoring systems necessitates the innovation of flexible energy storage systems.Considering environmental pollution and the depletion of fossil resources,the utilization of renewable resources to engineer advanced flexible materials has become especially crucial.Cellulose,the most abundant natural polymer,has emerged as a promising precursor for advanced functional materials due to its unique structure and properties.Typically,the easy processability,tunable chemical structure,self-assembly behavior,mechanical strength,and reinforcing capability enable its utilization as binder,substrate,hybrid electrode,separator,and electrolyte reservoir for flexible energy storage devices.This review comprehensively summarizes the design,fabrication,and mechanical and electrochemical performances of cellulose-based materials.The structure and unique properties of cellulose are first briefly introduced.Then,the construction of cellulose-based materials in the forms of 1D fibers/filaments,2D films/membranes,3D hydrogels and aerogels is discussed,and the merits of cellulose in these materials are emphasized.After that,the various advanced applications in supercapacitors,lithium-ion batteries,lithium-sulfur batteries,sodium-ion batteries,metal-air batteries,and Zn-ion batteries are presented in detail.Finally,an outlook of the potential challenges and future perspectives in advanced cellulose-based materials for flexible energy storage systems is discussed.
基金the National Natural Science Foundation of China(62174170)the Natural Science Foundation of Guangdong Province(2024A1515010123)+4 种基金the Shenzhen Science and Technology Program(20220807020526001)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0670000)the Shenzhen Science and Technology Program(KJZD20230923114708018,KJZD20230923114710022)the Talent Support Project of Guangdong(2021TX06C101)the Shenzhen Basic Research(JCYJ20210324115406019).
文摘Laser debonding technology has been widely used in advanced chip packaging,such as fan-out integration,2.5D/3D ICs,and MEMS devices.Typically,laser debonding of bonded pairs(R/R separation)is typically achieved by completely removing the material from the ablation region within the release material layer at high energy densities.However,this R/R separation method often results in a significant amount of release material and carbonized debris remaining on the surface of the device wafer,severely reducing product yields and cleaning efficiency for ultra-thin device wafers.Here,we proposed an interfacial separation strategy based on laser-induced hot stamping effect and thermoelastic stress wave,which enables stress-free separation of wafer bonding pairs at the interface of the release layer and the adhesive layer(R/A separation).By comprehensively analyzing the micro-morphology and material composition of the release material,we elucidated the laser debonding behavior of bonded pairs under different separation modes.Additionally,we calculated the ablation threshold of the release material in the case of wafer bonding and established the processing window for different separation methods.This work offers a fresh perspective on the development and application of laser debonding technology.The proposed R/A interface separation method is versatile,controllable,and highly reliable,and does not leave release materials and carbonized debris on device wafers,demonstrating strong industrial adaptability,which greatly facilitates the application and development of advanced packaging for ultra-thin chips.
基金Supported by Clinical Medical Research Fund of the Zhejiang Medical Association,No.2025ZYC-Z32Henan Provincial Key Research and Development Program,No.231111311000+1 种基金Henan Provincial Science and Technology Research Project,No.232102310411Clinical Medical Research Fund of the Zhejiang Medical Association,2024ZYC-Z30.
文摘Type 2 diabetes markedly elevates fracture risk despite normal or high bone mineral density,a paradox reflecting qualitative skeletal deficits rather than loss of mass.Chronic hyperglycemia fosters the accumulation of advanced glycation end products in bone;their nonenzymatic crosslinks stiffen type I collagen,impair mineralization,and erode mechanical strength.By engaging the receptor for advanced glycation end products,these adducts activate nuclear factorκB and mitogen-activated protein kinase cascades,amplifying oxidative stress,inflammation,osteoblast dysfunction,and osteoclastogenesis.This review synthesizes epidemiological data from type 1 and type 2 diabetes,highlights the limits of densitybased skeletal assessment,and details the molecular pathology of the glycation-collagen axis.It also appraises antiglycation therapies,including formation inhibitors,crosslink breakers and receptor antagonists,with a particular focus on sodium-glucose cotransporter 2 inhibitors that couple glycemic control with modulation of the glycation pathway.By integrating recent basic and clinical advances,we propose a mechanistic framework for diabetic bone disease and outline strategies to mitigate glycationdriven skeletal fragility.
基金National Natural Science Foundation of China(U2468201,62122012,62221001).
文摘The rapid expansion of railways,especially High-Speed Railways(HSRs),has drawn considerable interest from both academic and industrial sectors.To meet the future vision of smart rail communications,the rail transport industry must innovate in key technologies to ensure high-quality transmissions for passengers and railway operations.These systems must function effectively under high mobility conditions while prioritizing safety,ecofriendliness,comfort,transparency,predictability,and reliability.On the other hand,the proposal of 6 G wireless technology introduces new possibilities for innovation in communication technologies,which may truly realize the current vision of HSR.Therefore,this article gives a review of the current advanced 6 G wireless communication technologies for HSR,including random access and switching,channel estimation and beamforming,integrated sensing and communication,and edge computing.The main application scenarios of these technologies are reviewed,as well as their current research status and challenges,followed by an outlook on future development directions.
基金supported by the Strategic Priority Program of the Chinese Academy of Sciences(XDB0470303)the National Key R&D Program of China(2022YFB4600102and 2023YFE0209900)+4 种基金the National Natural Science Foundation of China(52175201 and 51935012)the science and technology projects of Gansu province(22JR5RA093,24JRRA044,24YFFA014 and 24ZDGA014)the Innovation and Entrepreneurship Team Project of YEDA(2021TD007)the special supporting project for provincial leading talents of Yantaithe Taishan Scholars Program。
文摘Silicone rubber(SR)is a versatile material widely used across various advanced functional applications,such as soft actuators and robots,flexible electronics,and medical devices.However,most SR molding methods rely on traditional thermal processing or direct ink writing three-dimensional(3D)printing.These methods are not conducive to manufacturing complex structures and present challenges such as time inefficiency,poor accuracy,and the necessity of multiple steps,significantly limiting SR applications.In this study,we developed an SR-based ink suitable for vat photopolymerization 3D printing using a multi-thiol monomer.This ink enables the one-step fabrication of complex architectures with high printing resolution at the micrometer scale,providing excellent mechanical strength and superior chemical stability.Specifically,the optimized 3D printing SR-20 exhibits a tensile stress of 1.96 MPa,an elongation at break of 487.9%,and an elastic modulus of 225.4 kPa.Additionally,the 3D-printed SR samples can withstand various solvents(acetone,toluene,and tetrahydrofuran)and endure temperatures ranging from-50℃ to 180℃,demonstrating superior stability.As a emonstration of the application,we successfully fabricated a series of SR-based soft pneumatic actuators and grippers in a single step with this technology,allowing for free assembly for the first time.This ultraviolet-curable SR,with high printing resolution and exceptional stability performance,has significant potential to enhance the capabilities of 3D printing for applications in soft actuators,robotics,flexible electronics,and medical devices.
基金supported by the MISP program at Merck Sharp&Dohme Corp.,USAa grant of the Korea Health Technology R&D Project through the Korea Health Industry Development Institute(KHIDI)funded by the Ministry of Health&Welfare,Republic of Korea(Grant Number:HR20C0025).
文摘Background:Immune checkpoint inhibitors(ICIs)are effective in a subset of patients with metastatic solid tumors.However,the patients who would benefit most from ICIs in biliary tract cancer(BTC)are still controversial.Materials and methods:We molecularly characterized tissues and blood from 32 patients with metastatic BTC treated with the ICI pembrolizumab as second-line therapy.Results:All patients had microsatellite stable(MSS)type tumors.Three of the 32 patients achieved partial response(PR),with an objective response rate(ORR)of 9.4%(95%confidence interval[CI],2.0–25.2)and nine showed stable disease(SD),exhibiting a disease control rate(DCR)of 37.5%(95%CI,21.1–56.3).For the 31 patients who had access to PD-1 ligand 1(PD-L1)combined positive score(CPS)testing(cut-off value≥1%),the ORR was not different between those who had PD-L1-positive(PD-L1+;1/11,9.1%)and PDL1-(2/20,10.0%)tumors(p=1.000).The tumor mutational burden(TMB)of PD-L1+BTC was comparable to that of PD-L1-BTC(p=0.630).TMB and any exonic somatic mutations were also not predictive of pembrolizumab response.Molecular analysis of blood and tumor samples demonstrated a relatively high natural killer(NK)cell proportion in the peripheral blood before pembrolizumab treatment in patients who achieved tumor response.Moreover,the tumors of these patients presented high enrichment scores for NK cells,antitumor cytokines,and Th1 signatures,and a low enrichment score for cancer-associated fibroblasts.Conclusions:This study shows the molecular characteristics associated with the efficacy of pembrolizumab in BTC of the MSS type.
基金supported by the National Key R&D Program of China(No.2022YFA1203901)the National Natural Science Foundation of China(Nos.52450014,62174013,and 92265111)+1 种基金the National Science Foundation for Distinguished Young Scholars(No.JQ23007)the Beijing Natural Science Foundation(Nos.JQ23007 and L233003)
文摘Employing two-dimensional(2D)synaptic devices to develop a brain-inspired neuromorphic computing system is a promising approach to overcoming the limitations of the von Neumann architecture.However,isotropic 2D materials are predominantly utilized to fabricate synaptic devices.Research on inherently anisotropic 2D materials in synaptic devices remains scarce.Here,we report an intrinsically anisotropic material,CrSBr,which exhibits optoelectronic properties with significant angular dependence,achieving a carrier mobility ratio as high as 7.83between the a-axis and b-axis.Based on this,we couple the in-plane anisotropy into the synaptic device and construct CrSBr/WSe_(2)multi-terminal device.This device can be regulated by the gate voltage and laser,exhibiting storage and synaptic behaviors dependent on the a and b axes.Furthermore,we apply the synaptic property to achieve image recognition.Due to the anisotropic response to identical external stimulus,the a-axis conductance trend transits from nonlinear to approximately linear within the multi-terminal conductance framework.This multi-terminal synapse model achieves a recognition rate of up to 91%on the Fashion-MNIST database,significantly outperforming single-terminal recognition performance.Our work introduces a novel approach to anisotropic artificial synapses for simulated image recognition and establishes a foundation for developing AI systems with enhanced recognition rates.
基金financially supported by the National Natural Science Foundation of China(Nos.U22A20145,52072151,52171211,and 52271218)Jinan Independent Innovative Team(No.2020GXRC015)+3 种基金the Major Program of Shandong Province Natural Science Foundation(No.ZR2023ZD43)Natural Science Foumdation of Jiangsu Province(No.BK20241973)High-level Training Talents of'333'Project in Jiangsu Provincethe Science and Technology Program of University of Jinan(No.XKY2119)
文摘Si,as the most promising anode with high theoretical capacity for next-generation lithium-ion batteries(LIBs),is hampered in commercial application by its poor electrical conductivity and significant volume expansion.Herein,the core-shell Si@SiO_(x)/C@C-Ar(SSC-A)or Si@SiO_(x)/C@C-H_(2)/Ar(SSC-H)composites are purposefully designed by in situ introduction of inorganic SiO_(x)in pure Ar or H_(2)/Ar atmosphere to realize a Si-based anode for LIBs.By introducing different atmospheres,the valence states of SiO_(x)are regulated.The inorganic transition layer formed by the combination of SiO_(x)with higher average valence and asphalt-derived carbon demonstrates better performance in both stabilizing the core-shell structure and inhibiting the agglomeration of Si particles.Given these advantages,the SSC-A electrode exhibits excellent electrochemical performance(1163 mAh g^(-1)after 400 cycles at 1 A g^(-1)),and the commercial blended graphite-SSC-A electrode reaches a specific capacity of 442 mAh g^(-1)with 74.8%capacity retention under the same conditions.Even the SSC-A electrode without Super P maintains an ultrahigh discharge specific capacity of 803 mAh g^(-1)with 60.6%after cycling.Importantly,the full batteries based on SSC-A without Super P achieve a discharge specific capacity of 126 mAh g^(-1)with 28.2%capacity decay after 200 cycles,demonstrating the superior commercial application potential.
基金supported by Korea Institute of Science and Technology(KIST)Institutional Program and Open Research Program(ORP)This work was also supported by grant from the National Research Foundation(NRF)of Korea government(RS-2024-00433159 and RS-2023-00208313)from ITECH R&D program of MOTIE/KEIT(RS-2023-00257573).
文摘Fiber-shaped energy storage devices(FSESDs)with exceptional flexibility for wearable power sources should be applied with solid electrolytes over liquid electrolytes due to short circuits and leakage issue during deformation.Among the solid options,polymer electrolytes are particularly preferred due to their robustness and flexibility,although their low ionic conductivity remains a significant challenge.Here,we present a redox polymer electrolyte(HT_RPE)with 4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl(HT)as a multi-functional additive.HT acts as a plasticizer that transforms the glassy state into the rubbery state for improved chain mobility and provides distinctive ion conduction pathway by the self-exchange reaction between radical and oxidized species.These synergetic effects lead to high ionic conductivity(73.5 mS cm−1)based on a lower activation energy of 0.13 eV than other redox additives.Moreover,HT_RPE with a pseudocapacitive characteristic by HT enables an outstanding electrochemical performance of the symmetric FSESDs using carbon-based fiber electrodes(energy density of 25.4 W h kg^(−1) at a power density of 25,000 W kg^(−1))without typical active materials,along with excellent stability(capacitance retention of 91.2%after 8,000 bending cycles).This work highlights a versatile HT_RPE that utilizes the unique functionality of HT for both the high ionic conductivity and improved energy storage capability,providing a promising pathway for next-generation flexible energy storage devices.
基金financially supported by the Technology Area Fund of the Basic Strengthening Program(No.2021-JCJQ-JJ-0092)the Science Center for Gas Turbine Project(Project No.P2022-C-Ⅳ-002-001)+2 种基金the Defense Industrial Technology Development Program(No.JCKY2020130C024)the National Key R&D Program of China(Grant No.2021YFB3702503)the National Science and Tech-nology Major Project(No.Y2019-VII-0011-0151).
文摘A self-developed crack-free advanced superalloy ZGH451 fabricated by direct energy deposition(DED)was applied to investigate the microstructure evolution,stress rupture behavior,and deformation mech-anisms at moderate-high temperatures and high-low stress conditions.The high Ta/Al ratio induces large misfit lattice stress and low stacking fault energy of alloy,resulting in approximate cubicγ′phases in dendrites and the formation of initial dislocation tangles.After the stress rupture test at 760℃/780 MPa,high content cubicγ′phases,small size of voids as well as preserved dislocation tangles are observed,showing stable structures with high-stress rupture resistance.High content and suitable size of cubicγ′phases,initial dislocation tangles,and L-C locks hinder the dislocation motion,which decreases the minimum strain rate and prolongs life significantly,forming four stress rupture stages.Hence,the defor-mation mechanism is determined by dislocation piled-up onγ/γ′interface,formation of stacking faults inγ′phases,and dislocations shearingγ′phases.However,the microstructure exhibits uneven struc-tures composed of large sizes of raftedγ′phases and voids at 980℃/260 MPa.The rafted structure and high temperature provide continuous channels and enough energy for dislocation motion,resulting in the increase of minimum strain rate,decline of life,and typic three stress rupture stages,even though there are obstacles to dislocation movement caused by dislocation networks.The deformation mecha-nism transforms to form dislocation networks onγ/γ′interface and dislocations shearingγ′phases.Be-sides,the decomposition of carbides on GBs also depends on temperature,which decomposes into harm-ful chain-like M23 C6 carbides at moderate temperatures and reinforced granular-shaped M6 C carbides at high temperatures.The applied stress always decreases mechanical properties due to its degradation of microstructure induced by elongating the precipitates and defects.
基金supported by the National Key Research and Development of China(No.2018YFA0702804).
文摘Over the past several decades,the integration of IONs into EP emerged as an effective method for enhancing its mechanical properties.Nevertheless,challenges remain,especially with u-IONs,where the interfacial strength with EP is suboptimal,resulting in aggregation within the EP matrix and a subsequent deterioration in the mechanical performance of u-ION/EP nanocomposites.In this comprehensive review,we explored advanced chemical modification techniques tailored for IONs incorporated into EP,providing a detailed examination of the mechanical characteristics of surface cm-ION/EP nanocomposites.This review investigates various chemical modification methods and their distinct impacts on the mechanical attributes of the resulting EP nanocomposites.Special emphasis is given to addressing the persistent challenges of inadequate interfacial strength and aggregation.Furthermore,this article examines prospective surface modification approaches for inorganic oxide nanoparticles,offering a visionary outlook on methods to improve the mechanical performance of EP in future.
基金supported by the Guangdong Basic and Applied Basic Research Fund Project(2022A1515140061,No.11000-2344014)Startup Foundation for Postdoctor by Dongguan University of Technology(No.11000-221110149)the High-level Talents Program(contract number 2023JC10L014)of the Department of Science and Technology of Guangdong Province。
文摘High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailorable electronic structure,and entropy stabilization effect.The precise fabrication of HEMs with functional nanostructures provides a crucial avenue to optimize the adsorption strength and catalytic activity for electrocatalysis.This review comprehensively summarizes the development of HEMs,focusing on the principles and strategies of structural design,and the catalytic mechanism towards hydrogen evolution reaction,oxygen evolution reaction and oxygen reduction reaction for the development of high-performance electrocatalysts.The complexity inherent in the interactions between different elements,the changes in the d-band center and the Gibbs free energies during the catalytic progress,as well as the coordination environment of the active sites associated with the unique crystal structure to improve the catalytic performance are discussed.We also provide a perspective on the challenges and future development direction of HEMs in electrocatalysis.This review will contribute to the design and development of HEMs-based catalysts for the next generation of electrochemical applications.
基金supported by the National Natural Science Foundation of China(Nos.22008058,No 22279135)the Natural Science Foundation of Hubei Province(No.2023AFB1010)+1 种基金the Key Project of Scientific Plan of Education Department of Hubei Province(No.D20232501)the CAS Strategic Leading Science&Technology Program(B)(XDB1040203)。
文摘The advancement of high-performance zinc-air battery systems necessitates the development of highly effective non-precious metal-based bifunctional electrocatalysts capable of synergistically enhancing both oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).To address the critical limitations of conventional non-precious catalysts in balancing multiple active sites and structural stability,we introduce an innovative in situ synthesis approach for constructing Fe_(2)P/FeNi bimetallic heterogeneous nanoparticles encapsulated within nitrogen-phosphorus dual-doped carbon matrices featuring interconnected leaf-like nanostructures(Fe_(2)P/FeNi@NPC).This architecturally optimized configuration not only mitigates transition metal degradation through protective carbon confinement but also facilitates rapid charge transfer kinetics and efficient mass diffusion pathways,substantially improving both catalytic efficiency and operational durability.Through comprehensive characterizations combining insitu monitoring and ex-situ analysis,the dynamic evolution of active sites during electrochemical operations is systematically tracked,and the genuine catalytic centers and spin state are identified.The optimized Fe_(2)P/FeNi@NPC composite exhibited remarkable electrochemical performance in alkaline media,achieving a superior ORR half-wave potential of 0.83 V and requiring only 1.62 V to achieve a current density of 10 mA cm^(-2)for OER.Notably,the assembled rechargeable zinc-air batteries(ZABs)exhibited a high specific capacity of 755.08 mAh g^(-1),a low charge-discharge voltage difference of 0.79 V,and exceptional cycling stability of over 1400 h.Furthermore,the flexible ZAB maintains excellent cycling performance even when subjected to various bending conditions.This work provides valuable insights into atomic-and electronic-scale dual-regulation strategy,offering a promising pathway to overcome current limitations in non-precious metal-based electrocatalysts for practical applications in metal-air battery systems.
基金supported by the National Key Research and Development Program of China(2019YFA0705700)Guangdong Innovative and Entrepreneurial Research Team Program(2021ZT09L197)+2 种基金Shenzhen Science and Technology Program(KQTD20210811090112002)Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School,National Natural Science Foundation of China(No.52373233)the SIAT International Joint Lab Project(No.E3G113).
文摘Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggish CO_(2)reduction reaction(CO_(2)RR)/CO_(2)evolution reaction(CO_(2)ER)kinetics remains a huge challenge.In this work,an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation,which significantly improves the electrocatalytic activity for both CO_(2)RR and CO_(2)ER.Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface,which leads to optimized binding affinity towards reactants and preferred Li_(2)CO_(3)decomposition behavior,enabling excellent catalytic activity during CO_(2)redox.Benefiting from the enhanced charge transfer ability,the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%.This work provides an attractive strategy to construct robust catalysts by interface engineering,which could inspire further design of superior bidirectional catalysts for Li-CO_(2)batteries.
基金Financial support from the National Natural Science Foundation of China(52302317)is gratefully acknowledged。
文摘Rechargeable magnesium batteries(RMBs)have garnered significant attention in energy storage applications due to their high capacity,low cost,and high safety.However,the strong polarization effect and slow kinetic de-intercalation of Mg^(2+)in the cathode limit their commercial application.This study presents a novel interface-coupled V_(2)CT_(x)@VS_(4)heterostructure through a one-step hydrothermal process.In this architecture,V_(2)CT_(x)and VS_(4)can mutually support their structural framework,which effectively prevents the structural collapse of V_(2)CT_(x)MXene and the aggregation of VS_(4).Crucially,interfacial coupling between V_(2)CT_(x)and VS_(4)induces strong V-S bonds,substantially enhancing structural stability.Benefiting from these advantages,the heterostructure exhibits high specific capacity(226 mAh g^(-1)at 100 mA g^(-1))and excellent long-cycle stability(89% capacity retention after 1000 cycles at 500 mA g^(-1)).Furthermore,the Mg^(2+)storage mechanism in the V_(2)CT_(x)@VS_(4)composite was elucidated through a series of ex-situ characterizations.This work provides a feasible strategy for designing V_(2)CT_(x)MXene-based cathodes with high capacity and extended cyclability for RMBs.
基金supported by the Hong Kong Research Grants Council(No.CityU 11201522).
文摘The evolution of energy storage technology has seen remarkable progress,with a shift from pure metals to sophisticated,tailor-made active materials.The synthesis of nanostructures with exceptional properties is crucial in the advancement of electrode materials.In this regard,our study highlights the fabrication of a novel,oriented heterostructure comprised of Zn-Mn-Co-telluride grown on a pre-oxidized copper mesh using a hydrothermal method followed by a solvothermal process.This innovative approach leads to the formation of the Zn-Mn-Cotelluride@CuO@Cu heterostructure,which demonstrates the unique oriented morphology.It outperforms both Zn-Mn-Co-telluride@Cu and CuO@Cu by exhibiting lower electrical resistivity,increased redox activity,higher specific capacity,and improved ion diffusion characteristics.The conductivity enhancements of the heterostructure are corroborated by density functional theory(DFT)calculations.When utilized in a hybrid supercapacitor(HSC)alongside activated carbon(AC)electrodes,the Zn-Mn-Co-telluride@CuO@Cu heterostructurebased HSC achieves an energy density of 75.7 Wh kg^(-1).Such findings underscore the potential of these novel electrode materials to significantly impact the design of next-generation supercapacitor devices.
