Aerogels are ultra-lightweight,porous materials defined by a complex network of interconnected pores and nanostructures,which effectively suppress heat transfer,making them exceptional for thermal insulation.Furthermo...Aerogels are ultra-lightweight,porous materials defined by a complex network of interconnected pores and nanostructures,which effectively suppress heat transfer,making them exceptional for thermal insulation.Furthermore,their porous architecture can trap and scatter light via multiple internal reflections,extending the optical path within the material.When combined with suitable light-absorbing materials,this feature significantly enhances light absorption(darkness).To validate this concept,mesoporous silica aerogel particles were incorporated into a resorcinol-formaldehyde(RF)sol,and the silica-to-RF ratio was optimized to achieve uniform carbon compound coatings on the silica pore walls.Notably,increasing silica loading raised the sol viscosity,enabling formulations ideal for direct ink writing processes with excellent shape fidelity for super-black topographical designs.The printed silica-RF green bodies exhibited remarkable mechanical strength and ultra-low thermal conductivity(15.8 m W m^(-1) K^(-1))prior to pyrolysis.Following pyrolysis,the composites maintained structural integrity and printed microcellular geometries while achieving super-black coloration(abs.99.56%in the 280-2500 nm range)and high photothermal conversion efficiency(94.2%).Additionally,these silica-carbon aerogel microcellulars demonstrated stable electrical conductivity and low electrochemical impedance.The synergistic combination of 3D printability and super-black photothermal features makes these composites highly versatile for multifunctional applications,including on-demand thermal management,and efficient solar-driven water production.展开更多
The all-vanadium redox flow battery(VRFB)plays an important role in the energy transition toward renewable technologies by providing grid-scale energy storage.Their deployment,however,is limited by the lack of membran...The all-vanadium redox flow battery(VRFB)plays an important role in the energy transition toward renewable technologies by providing grid-scale energy storage.Their deployment,however,is limited by the lack of membranes that provide both a high energy efficiency and capacity retention.Typically,the improvement of the battery’s energy efficiency comes at the cost of its capacity retention.Herein,novel N-alkylated and N-benzylated meta-polybenzimidazole(m-PBI)membranes are used to understand the molecular requirements of the polymer electrolyte in a vanadium redox flow battery,providing an important toolbox for future research toward next-generation membrane materials in energy storage devices.The addition of an ethyl side chain to the m-PBI backbone increases its affinity toward the acidic electrolyte,thereby increasing its ionic conductivity and the corresponding energy efficiency of the VRFB cell from 70%to 78%at a current density of 200 mA cm^(-2).In addition,cells equipped with ethylated m-PBI showed better capacity retention than their pristine counterpart,respectively 91%versus 87%,over 200 cycles at 200 mA cm^(-2).The outstanding VRFB cycling performance,together with the low-cost and fluorine-free chemistry of the N-alkylated m-PBI polymer,makes this material a promising membrane to be used in next-generation VRFB systems.展开更多
Tin perovskites are emerging as promising alternatives to their lead-based counterparts for high-performance and flexible perovskite solar cells.However,their rapid crystallization often leads to inadequate film quali...Tin perovskites are emerging as promising alternatives to their lead-based counterparts for high-performance and flexible perovskite solar cells.However,their rapid crystallization often leads to inadequate film quality and poor device performance.In this study,the role of GeI_(2) as an additive is investigated for controlling the nucleation and crystallization processes of formamidinium tin triiodide(FASnI3).The findings reveal the preferential formation of a Ge-rich layer at the bottom of the perovskite film upon the introduction of GeI_(2).It is proposed that the initial formation of the Ge complex acts as a crystallization regulator,promoting oriented growth of subsequent FASnI3 crystals and enhancing overall crystallinity.Through the incorporation of an optimal amount of GeI_(2),flexible Sn perovskite solar cells with an efficiency of 10.8%were achieved.Furthermore,it was observed that the GeI_(2) additive ensures a remarkable shelf-life for the devices,with the rigid cells retaining 91%of their initial performance after more than 13800 h of storage in an N_(2) gas environment.This study elucidates the mechanistic role of GeI_(2) in regulating the nucleation and crystallization process of tin perovskites,providing valuable insights into the significance of additive engineering for the development of high-performance flexible tin perovskite solar cells.展开更多
Acidic environments enhance CO_(2) utilization during CO_(2) electrolysis via a buffering effect that converts carbonates formed at the electrode surface back into CO_(2).Nevertheless,further investigation into acidic...Acidic environments enhance CO_(2) utilization during CO_(2) electrolysis via a buffering effect that converts carbonates formed at the electrode surface back into CO_(2).Nevertheless,further investigation into acidic CO_(2) electrolysis is required to improve its selectivity towards certain CO_(2) reduction reaction(CO_(2)RR)products,such as multicarbon(C2+)species,while enhancing its overall stability.In this study,liquid product recirculation in the catholyte and local OH−accumulation were identified as primary factors contributing to the degradation of gas diffusion electrodes mounted in closed‐loop catholyte configurations.We demonstrate that a single‐pass catholyte configuration prevents liquid product recirculation and maintains a continuous flow of acidic‐pH catholyte throughout the reaction while using the same volume as a closed‐loop setup.This approach improves electrode durability and maintains a Faradaic efficiency of 67%for multicarbon products over 4 h of CO_(2) electrolysis at−600 mA cm^(-2).展开更多
The present work reports on microscopic analyses of recombination at grain boundaries(GBs)in polycrystalline Li-doped(Ag,Cu)_(2)ZnSn(S,Se)_(4)(LiACZTSSe)and Cu_(2)ZnSnS_(4)(CZTS)absorber layers in high-efficiency sola...The present work reports on microscopic analyses of recombination at grain boundaries(GBs)in polycrystalline Li-doped(Ag,Cu)_(2)ZnSn(S,Se)_(4)(LiACZTSSe)and Cu_(2)ZnSnS_(4)(CZTS)absorber layers in high-efficiency solar cells(conversion efficiencies of 14.4%and 10.8%).Recombination velocities sG B were determined at a large number of GBs by evaluating profiles extracted from cathodoluminescence intensity distributions across GBs in these polycrystalline layers.In both Li-ACZTSSe and CZTS absorber layers,the sG B values exhibited wide ranges over several orders of magnitude with a median values of 680 and 1100 cm s^(-1)for the Li-ACZTSSe and CZTS absorbers.展开更多
A novel approach for fabricating multi-principal element alloys with adjustable phase configurations and mechanical properties was developed using laser-aided additive manufacturing(LAAM),combining FCC-structured(face...A novel approach for fabricating multi-principal element alloys with adjustable phase configurations and mechanical properties was developed using laser-aided additive manufacturing(LAAM),combining FCC-structured(face-centered cubic)CoCrNi and BCC-structured(body-centered cubic)CoCrNiAl0.6TiFe feedstocks.During fabrication,CoCrNi powders and CoCrNiAl0.6TiFe powders were simultaneously fed into the melt pool at individually adjustable rates,allowing for controlled phase transitions.The resulting phase evolution demonstrated a gradual transition from a single FCC structure CoCrNi(A10.6TiFe)x(x=0,0.1,0.2,0.3)to a dual FCCB2 structure CoCrNi(Al0.6TiFe)x(x=0.4,0.5)as the proportion of BCC-structured powders increased.The B2 phase,enriched in Ti and Al due to their larger atomic radii and negative segregation enthalpy,precipitated around the FCC matrix,with volume fractions of 0.5%and 5.7%for CoCrNi(A10.6TiFe)0.4 and CoCrNi(A10.6TiFe)0.5,respectively.This phase transition resulted in significant mechanical enhancements.Yield and ultimate tensile strengths increased from 486.0 and 781.2 MPa(CoCrNi)to 887.2 and 1165.2 MPa(CoCrNi(A10.6TiFe)0.5).Dislocation-mediated hardening prevailed in single-phase FCC alloys,exhibiting a characteristic dislocation density of 2.5×10^(15)m^(-2)for CoCrNi(A10.6TiFe)0.3 alloy.Once the B2 phase precipitated,precipitation strengthening became dominant,as observed in transmission electron microscopy(TEM),where dislocations accumulated around B2 precipitates.This study presents an innovative alloy fabrication strategy that enables precise tuning of FCC-BCC dualphase structures,facilitating the direct fabrication of components with spatially customized properties.These findings provide valuable insights for developing multiprincipal element alloys with heterogeneous microstructures for advanced engineering applications.展开更多
Two-dimensional(2D) transition metal carbides, carbonitrides and nitrides, known as MXenes, are emerging quickly at the frontiers of 2D materials world. Their exotic properties such as the highest electrical conductiv...Two-dimensional(2D) transition metal carbides, carbonitrides and nitrides, known as MXenes, are emerging quickly at the frontiers of 2D materials world. Their exotic properties such as the highest electrical conductivity among all solution-processed 2 D materials, the best electromagnetic interference shielding performance outperforming that of copper or aluminum at a nanoscale thickness, as well as the highest volumetric capacitance for pseudocapacitors, have been attracting extensive fundamental research and applications. Their unique surface chemistries, that is, hydrophilic groups terminated on the surface of MXenes after etching and delamination, enable plenty of opportunities for assembling into MXene building blocks. Particularly, assembling at liquid–liquid, liquid–solid, liquid–air, and solid–solid interfaces allows the efficient fabrication of various structures, including MXene surfactants, MXene heterostructures, MXene transparent films. Interfacial assembly of MXenes is of significance in unveiling more versatilities of MXenes as well as impacts on novel MXene-based architectures, based on which enhanced performance of devices is achieved. As such, this review focuses on the interfacial assembly of MXenes, explaining mechanisms behind various assembling and providing classical examples for corresponding interfacial assembling techniques. Applications of these as-assembled architectures are also discussed in brief. We believe this review may shed light on the interfacial chemistry of MXenes, thus guiding more efficient fabrication of MXene-based functional films/coatings/electrodes/devices.展开更多
Lightweight,ultra-flexible,and robust crosslinked transition metal carbide(Ti3C2 MXene)coated polyimide(PI)(C-MXene@PI)porous composites are manufactured via a scalable dip-coating followed by chemical crosslinking ap...Lightweight,ultra-flexible,and robust crosslinked transition metal carbide(Ti3C2 MXene)coated polyimide(PI)(C-MXene@PI)porous composites are manufactured via a scalable dip-coating followed by chemical crosslinking approach.In addition to the hydrophobicity,anti-oxidation and extreme-temperature stability,efficient utilization of the intrinsic conductivity of MXene,the interfacial polarization between MXene and PI,and the micrometer-sized pores of the composite foams are achieved.Consequently,the composites show a satisfactory X-band electromagnetic interference(EMI)shielding effectiveness of 22.5 to 62.5 dB at a density of 28.7 to 48.7 mg cm−3,leading to an excellent surface-specific SE of 21,317 dB cm^(2)g^(−1).Moreover,the composite foams exhibit excellent electrothermal performance as flexible heaters in terms of a prominent,rapid reproducible,and stable electrothermal effect at low voltages and superior heat performance and more uniform heat distribution compared with the commercial heaters composed of alloy plates.Furthermore,the composite foams are well attached on a human body to check their electromechanical sensing performance,demonstrating the sensitive and reliable detection of human motions as wearable sensors.The excellent EMI shielding performance and multifunctionalities,along with the facile and easy-to-scalable manufacturing techniques,imply promising perspectives of the porous C-MXene@PI composites in next-generation flexible electronics,aerospace,and smart devices.展开更多
Stability of borohydrides is determined by the localization of the negative charge on the boron atom.Ionic liquids(ILs) allow to modify the stability of the borohydrides and promote new dehydrogenation pathways with a...Stability of borohydrides is determined by the localization of the negative charge on the boron atom.Ionic liquids(ILs) allow to modify the stability of the borohydrides and promote new dehydrogenation pathways with a lower activation energy. The combination of borohydride and IL is very easy to realize and no expensive rare earth metals are required. The composite of the ILs with complex hydrides decreases the enthalpy and activation energy for the hydrogen desorption. The Coulomb interaction between borohydride and IL leads to a destabilization of the materials with a significantly lower enthalpy for hydrogen desorption. Here, we report a simple ion exchange reaction using various ILs, such as vinylbenzyltrimethylammonium chloride([VBTMA][Cl]), 1-butyl-3-methylimidazolium chloride([bmim][Cl]), and 1-ethyl-1-methylpyrrolidinium bromide([EMPY][Br]) with NaBH4 to decrease the hydrogen desorption temperature. Dehydrogenation of 1-butyl-3-methylimidazolium borohydride([bmim][BH4]) starts below 100℃. The quantity of desorbed hydrogen ranges between 2.4 wt% and 2.9 wt%, which is close to the theoretical content of hydrogen. The improvement in dehydrogenation is due to the strong amine cation that destabilizes borohydride by charge transfer.展开更多
AIM: To investigate collagen patches seeded with mesenchymal stem cells(MSCs) and/or tenocytes(TCs) with regards to their suitability for anterior cruciate ligament(ACL) repair. METHODS: Dynamic intraligamentary stabi...AIM: To investigate collagen patches seeded with mesenchymal stem cells(MSCs) and/or tenocytes(TCs) with regards to their suitability for anterior cruciate ligament(ACL) repair. METHODS: Dynamic intraligamentary stabilization utilizes a dynamic screw system to keep ACL remnants in place and promote biological healing, supplemented by collagen patches. How these scaffolds interact with cells and what type of benefit they provide has not yet been investigated in detail. Primary ACL-derived TCs and human bone marrow derived MSCs were seeded onto two different types of 3D collagen scaffolds, Chondro-Gide?(CG) and Novocart?(NC). Cells were seeded onto the scaffolds and cultured for 7 d either as a pure populations or as "premix" containing a 1:1 ratio of TCs to MSCs. Additionally, as controls, cells were seeded in monolayers and in co-cultures on both sides of porous high-density membrane inserts(0.4 μm). We analyzed the patches by real time polymerase chain reaction, glycosaminoglycan(GAG), DNA and hydroxyproline(HYP) content. To determine cell spreading and adherence in the scaffolds microscopic imaging techniques, i.e., confocal laser scanning microscopy(c LSM) and scanning electron microscopy(SEM), were applied.RESULTS: CLSM and SEM imaging analysis confirmed cell adherence onto scaffolds. The metabolic cell activity revealed that patches promote adherence and proliferation of cells. The most dramatic increase in absolute metabolic cell activity was measured for CG samples seeded with tenocytes or a 1:1 cell premix. Analysis of DNA content and c LSM imaging also indicated MSCs were not proliferating as nicely as tenocytes on CG. The HYP to GAG ratio significantly changed for the premix group, resulting from a slightly lower GAG content, demonstrating that the cells are modifying the underlying matrix. Real-time quantitativepolymerase chain reaction data indicated that MSCs showed a trend of differentiation towards a more tenogenic-like phenotype after 7 d.CONCLUSION: CG and NC are both cyto-compatible with primary MSCs and TCs; TCs seemed to perform better on these collagen patches than MSCs.展开更多
A new self-repairing membrane for inflatable light weight structures such as rubber boats or Tensairity constructions is presented. Inspired by rapid self-sealing processes in plants, a thin soft cellular polyurethane...A new self-repairing membrane for inflatable light weight structures such as rubber boats or Tensairity constructions is presented. Inspired by rapid self-sealing processes in plants, a thin soft cellular polyurethane foam coating is applied on the inside of a fabric substrate, which closes the fissure if the membrane is punctured with a spike. Experimental tests are carried out with a purpose built setup by measuring the air mass flow through a leak in a damaged membrane sample. It is shown that the weight per unit area of the self-repairing foam as well as the curing of the two component PU-foam under an overpressure influence the repair efficiency. Curing the foam under overpressure affects the relative density as well as the microstructure of the foam coatings. Maximal median repair efficiencies of 0.999 have been obtained with 0.16 g.cm 2 foam cured at 1 bar overpressure. These results suggest that the bio-inspired technique has the potential to extend the functional integrity of injured inflatable structures dramatically.展开更多
Functionally graded（FG） carbon nanotubes（CNT） and nano-silicon carbide（nSiC） reinforced aluminium（Al）matrix composites have been successfully fabricated using high-energy ball milling followed by solid-state s...Functionally graded（FG） carbon nanotubes（CNT） and nano-silicon carbide（nSiC） reinforced aluminium（Al）matrix composites have been successfully fabricated using high-energy ball milling followed by solid-state spark plasma sintering processes.The CNTs were well-dispersed in the Al particles using the nSiC as a solid mixing agent.Two different types of multi-walled CNTs were used to add different amounts of CNTs in the same volume.The ball milled Al—CNT—nSiC and Al—CNT powder mixtures were fully densified and demonstrated good adhesion with no serious microcracks and pores within an FG multilayer composite.Each layer contained different amounts of the CNTs,and the nSiC additions showed different microstructures and hardness.It is possible to control the characteristics of the FG multilayer composite through the efficient design of an Al—CNT—nSiC gradient layer.This concept offers a feasible approach for fabricating the dualnanoparticulate-reinforced Al matrix nanocomposites and can be applied to other scenarios such as polymer and ceramic systems.展开更多
The significant positive green environment influence of magnesium alloy usage in transport could be compromised by catastrophic fast fracture caused by stress corrosion cracking(SCC). Transgranular stress corrosion cr...The significant positive green environment influence of magnesium alloy usage in transport could be compromised by catastrophic fast fracture caused by stress corrosion cracking(SCC). Transgranular stress corrosion cracking(TGSCC) of AZ91 was evaluated using the linearly increasing stress test(LIST) and the constant extension rate test(CERT). The TGSCC threshold stress was 55-75 MPa in distilled water and in 5 g/L NaCl. The TGSCC velocity was 7×10-10-5×10-9 m/s. A delayed hydride-cracking(DHC) model for TGSCC was implemented using a finite element script in MATLAB and the model predictions were compared with experiment. A key outcome is that,during steady state TGSCC propagation,a high dynamic hydrogen concentration is expected to build up behind the crack tip. A number of recommendations are given for preventing SCC of Mg alloys in service. One of the most important recommendations might be that the total stress in service(i.e. the stress from the service loading + the fabrication stress + the residual stress) should be below a threshold level,which,in the absence of other data,could be(conservatively) estimated to be about 50% of the tensile yield strength.展开更多
In this work, the morphology, phase composition, and corrosion properties of microarc oxidized (MAO) gas tungsten arc (GTA) weldments of AZ31 alloy were investigated. Autogenous gas tungsten arc welds were made as ful...In this work, the morphology, phase composition, and corrosion properties of microarc oxidized (MAO) gas tungsten arc (GTA) weldments of AZ31 alloy were investigated. Autogenous gas tungsten arc welds were made as full penetration bead-on-plate welding under the alternating-current mode. A uniform oxide layer was developed on the surface of the specimens with MAO treatment in silicate-based alkaline electrolytes for different oxidation times. The corrosion behavior of the samples was evaluated by potentiodynamic polarization and electrochemical impedance spectroscopy. The oxide film improved the corrosion resistance substantially compared to the uncoated specimens. The sample coated for 10 min exhibited better corrosion properties. The corrosion resistance of the coatings was concluded to strongly depend on the morphology, whereas the phase composition and thickness were concluded to only slightly affect the corrosion resistance.展开更多
Ammonia is the most basic raw material in industrial and agricultural production.The current industrial production of ammonia relies on the Haber-Bosch process with high energy consumption.To overcome this shortcoming...Ammonia is the most basic raw material in industrial and agricultural production.The current industrial production of ammonia relies on the Haber-Bosch process with high energy consumption.To overcome this shortcoming,the development of electrocatalytic ammonia synthesis under moderate conditions is considered as a potential alternative technology.The two-dimensional(2D)MXenes family has been proved promising as electrocatalysts,but from the currently available literature,it is hard to find a systematic review on MXenes-catalyzed ammonia synthesis.So in the present review,we summarize the key perspectives on that topic in recent years as well as outline,from a prospective view,strategies of catalyst design.We analyze in detail the methods for preparing high performance MXenes-based catalysts and the corresponding underlying mechanisms,and also discuss the criteria and potential challenges,expecting to provide inspiration for the development of efficient MXenes-based route to electrochemical ammonia fixation.展开更多
基金financially supported by the Swiss National Science Foundation(grant number IZLRZ2_164058)the China Scholarship Council Ph.D.student exchange programthe Priority Academic Program Development of Jiangsu Higher Education Institution(PAPD)。
文摘Aerogels are ultra-lightweight,porous materials defined by a complex network of interconnected pores and nanostructures,which effectively suppress heat transfer,making them exceptional for thermal insulation.Furthermore,their porous architecture can trap and scatter light via multiple internal reflections,extending the optical path within the material.When combined with suitable light-absorbing materials,this feature significantly enhances light absorption(darkness).To validate this concept,mesoporous silica aerogel particles were incorporated into a resorcinol-formaldehyde(RF)sol,and the silica-to-RF ratio was optimized to achieve uniform carbon compound coatings on the silica pore walls.Notably,increasing silica loading raised the sol viscosity,enabling formulations ideal for direct ink writing processes with excellent shape fidelity for super-black topographical designs.The printed silica-RF green bodies exhibited remarkable mechanical strength and ultra-low thermal conductivity(15.8 m W m^(-1) K^(-1))prior to pyrolysis.Following pyrolysis,the composites maintained structural integrity and printed microcellular geometries while achieving super-black coloration(abs.99.56%in the 280-2500 nm range)and high photothermal conversion efficiency(94.2%).Additionally,these silica-carbon aerogel microcellulars demonstrated stable electrical conductivity and low electrochemical impedance.The synergistic combination of 3D printability and super-black photothermal features makes these composites highly versatile for multifunctional applications,including on-demand thermal management,and efficient solar-driven water production.
基金supported by the Swiss National Science Foundation(grant number 188631).
文摘The all-vanadium redox flow battery(VRFB)plays an important role in the energy transition toward renewable technologies by providing grid-scale energy storage.Their deployment,however,is limited by the lack of membranes that provide both a high energy efficiency and capacity retention.Typically,the improvement of the battery’s energy efficiency comes at the cost of its capacity retention.Herein,novel N-alkylated and N-benzylated meta-polybenzimidazole(m-PBI)membranes are used to understand the molecular requirements of the polymer electrolyte in a vanadium redox flow battery,providing an important toolbox for future research toward next-generation membrane materials in energy storage devices.The addition of an ethyl side chain to the m-PBI backbone increases its affinity toward the acidic electrolyte,thereby increasing its ionic conductivity and the corresponding energy efficiency of the VRFB cell from 70%to 78%at a current density of 200 mA cm^(-2).In addition,cells equipped with ethylated m-PBI showed better capacity retention than their pristine counterpart,respectively 91%versus 87%,over 200 cycles at 200 mA cm^(-2).The outstanding VRFB cycling performance,together with the low-cost and fluorine-free chemistry of the N-alkylated m-PBI polymer,makes this material a promising membrane to be used in next-generation VRFB systems.
基金funding from the European Union’s Horizon Europe research and innovation program under grant agreement no.101075605(SuPer-Tandem)financially supported by Swiss National Science Foundation(grant no.200021_213073)+3 种基金Swiss Federal Office of Energy(SFOE,grant no.SI/502549-01)partially financially supported by the National Natural Science Foundation of China(nos.62104163 and 62174112)the Natural Science Foundation of Sichuan Province(no.2022NSFSC1183)the China Scholarship Council(CSC)funding from the Ministry of Education of P.R.China.
文摘Tin perovskites are emerging as promising alternatives to their lead-based counterparts for high-performance and flexible perovskite solar cells.However,their rapid crystallization often leads to inadequate film quality and poor device performance.In this study,the role of GeI_(2) as an additive is investigated for controlling the nucleation and crystallization processes of formamidinium tin triiodide(FASnI3).The findings reveal the preferential formation of a Ge-rich layer at the bottom of the perovskite film upon the introduction of GeI_(2).It is proposed that the initial formation of the Ge complex acts as a crystallization regulator,promoting oriented growth of subsequent FASnI3 crystals and enhancing overall crystallinity.Through the incorporation of an optimal amount of GeI_(2),flexible Sn perovskite solar cells with an efficiency of 10.8%were achieved.Furthermore,it was observed that the GeI_(2) additive ensures a remarkable shelf-life for the devices,with the rigid cells retaining 91%of their initial performance after more than 13800 h of storage in an N_(2) gas environment.This study elucidates the mechanistic role of GeI_(2) in regulating the nucleation and crystallization process of tin perovskites,providing valuable insights into the significance of additive engineering for the development of high-performance flexible tin perovskite solar cells.
基金supported by the EPFL,EMPA and the National Research Foundation of Singapore(Urban Solutions and Sustainability,Industry Alignment Fund[Pre‐Positioning]Programme)(A‐0004543‐00‐00)。
文摘Acidic environments enhance CO_(2) utilization during CO_(2) electrolysis via a buffering effect that converts carbonates formed at the electrode surface back into CO_(2).Nevertheless,further investigation into acidic CO_(2) electrolysis is required to improve its selectivity towards certain CO_(2) reduction reaction(CO_(2)RR)products,such as multicarbon(C2+)species,while enhancing its overall stability.In this study,liquid product recirculation in the catholyte and local OH−accumulation were identified as primary factors contributing to the degradation of gas diffusion electrodes mounted in closed‐loop catholyte configurations.We demonstrate that a single‐pass catholyte configuration prevents liquid product recirculation and maintains a continuous flow of acidic‐pH catholyte throughout the reaction while using the same volume as a closed‐loop setup.This approach improves electrode durability and maintains a Faradaic efficiency of 67%for multicarbon products over 4 h of CO_(2) electrolysis at−600 mA cm^(-2).
基金support by the German-Israeli Helmholtz International Research School HI-SCORE(HIRS-0008)by the project“EFFCISⅡ”funded by the Federal Ministry for Economic Affairs and Climate Action(BMWK)under contract numbers 03EE1059B+9 种基金the Australian Renewable Energy Agency(ARENA)as part of ARENA’s Transformative Research Accelerating Commercialization(TRAC)Programthe Australian Research Council(ARC)Discovery Project(DP230102463)Linkage Project(LP200301593)Baosteel-Australia Joint Research and Development Center(BA19010)support from the Australian Center of Advanced Photovoltaics(ACAP)as a recipient of the ACAP Fel owship(RG172864-B)financial support of the Australian Research Council(ARC)Future Fel owship(FT190100756)funding from the European Union’s H2020 ERC-Consolidator program under grant agreement number no.866018(SENSATE)by the Science and Innovation Ministry of Spain projects number PID2023-148976OB-C41(CURIO-CITY)and PCI2023-145971-2(ACT-FAST,CET-Partnership 2023 program)the European Union’s Horizon research and innovation program under the Marie Skøodowska-Curie grant agreement no.10115148(LEK-PV)part of Maria de Maeztu Units of Excel ence Program CEX2023-001300-M/funded by MICIU/AEI/10.13039/501100011033
文摘The present work reports on microscopic analyses of recombination at grain boundaries(GBs)in polycrystalline Li-doped(Ag,Cu)_(2)ZnSn(S,Se)_(4)(LiACZTSSe)and Cu_(2)ZnSnS_(4)(CZTS)absorber layers in high-efficiency solar cells(conversion efficiencies of 14.4%and 10.8%).Recombination velocities sG B were determined at a large number of GBs by evaluating profiles extracted from cathodoluminescence intensity distributions across GBs in these polycrystalline layers.In both Li-ACZTSSe and CZTS absorber layers,the sG B values exhibited wide ranges over several orders of magnitude with a median values of 680 and 1100 cm s^(-1)for the Li-ACZTSSe and CZTS absorbers.
基金financially supported by the following sources:Guangdong Basic and Applied Basic Research Foundation(No.2023B1515120045)Yangjiang City Key Industry Talent Revitalization Plan Project for Alloy Materials and Hardware Scissors(No.RCZX202302)+7 种基金GDAS'Project of Science and Technology Development(Nos.2022GDASZH-2022010108,2022GD ASZH-2022010107 and 2024GD ASZH-2024010102)GDAS'Young Talent Project(No.2024GDASQNRC-0314)Guangzhou Basic and Applied Basic Research Foundation(No.2023A04J1628)the National Key R&D Program of China(No.2022YFB4600700)National Natural Science Foundation of China(No.52371110)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011510)Shenzhen Science and Technology Program(Nos.JCYJ20220530115011026 and JCYJ20230807093410021)Shanxi Province Key R&D Project(No.202302050201011)
文摘A novel approach for fabricating multi-principal element alloys with adjustable phase configurations and mechanical properties was developed using laser-aided additive manufacturing(LAAM),combining FCC-structured(face-centered cubic)CoCrNi and BCC-structured(body-centered cubic)CoCrNiAl0.6TiFe feedstocks.During fabrication,CoCrNi powders and CoCrNiAl0.6TiFe powders were simultaneously fed into the melt pool at individually adjustable rates,allowing for controlled phase transitions.The resulting phase evolution demonstrated a gradual transition from a single FCC structure CoCrNi(A10.6TiFe)x(x=0,0.1,0.2,0.3)to a dual FCCB2 structure CoCrNi(Al0.6TiFe)x(x=0.4,0.5)as the proportion of BCC-structured powders increased.The B2 phase,enriched in Ti and Al due to their larger atomic radii and negative segregation enthalpy,precipitated around the FCC matrix,with volume fractions of 0.5%and 5.7%for CoCrNi(A10.6TiFe)0.4 and CoCrNi(A10.6TiFe)0.5,respectively.This phase transition resulted in significant mechanical enhancements.Yield and ultimate tensile strengths increased from 486.0 and 781.2 MPa(CoCrNi)to 887.2 and 1165.2 MPa(CoCrNi(A10.6TiFe)0.5).Dislocation-mediated hardening prevailed in single-phase FCC alloys,exhibiting a characteristic dislocation density of 2.5×10^(15)m^(-2)for CoCrNi(A10.6TiFe)0.3 alloy.Once the B2 phase precipitated,precipitation strengthening became dominant,as observed in transmission electron microscopy(TEM),where dislocations accumulated around B2 precipitates.This study presents an innovative alloy fabrication strategy that enables precise tuning of FCC-BCC dualphase structures,facilitating the direct fabrication of components with spatially customized properties.These findings provide valuable insights for developing multiprincipal element alloys with heterogeneous microstructures for advanced engineering applications.
文摘Two-dimensional(2D) transition metal carbides, carbonitrides and nitrides, known as MXenes, are emerging quickly at the frontiers of 2D materials world. Their exotic properties such as the highest electrical conductivity among all solution-processed 2 D materials, the best electromagnetic interference shielding performance outperforming that of copper or aluminum at a nanoscale thickness, as well as the highest volumetric capacitance for pseudocapacitors, have been attracting extensive fundamental research and applications. Their unique surface chemistries, that is, hydrophilic groups terminated on the surface of MXenes after etching and delamination, enable plenty of opportunities for assembling into MXene building blocks. Particularly, assembling at liquid–liquid, liquid–solid, liquid–air, and solid–solid interfaces allows the efficient fabrication of various structures, including MXene surfactants, MXene heterostructures, MXene transparent films. Interfacial assembly of MXenes is of significance in unveiling more versatilities of MXenes as well as impacts on novel MXene-based architectures, based on which enhanced performance of devices is achieved. As such, this review focuses on the interfacial assembly of MXenes, explaining mechanisms behind various assembling and providing classical examples for corresponding interfacial assembling techniques. Applications of these as-assembled architectures are also discussed in brief. We believe this review may shed light on the interfacial chemistry of MXenes, thus guiding more efficient fabrication of MXene-based functional films/coatings/electrodes/devices.
基金support of the Qilu Young Scholar Program of Shandong University(No.31370082163127)the authors acknowledge funding from the support from the Chinese Scholarship Council(to NW,project#201709370040).
文摘Lightweight,ultra-flexible,and robust crosslinked transition metal carbide(Ti3C2 MXene)coated polyimide(PI)(C-MXene@PI)porous composites are manufactured via a scalable dip-coating followed by chemical crosslinking approach.In addition to the hydrophobicity,anti-oxidation and extreme-temperature stability,efficient utilization of the intrinsic conductivity of MXene,the interfacial polarization between MXene and PI,and the micrometer-sized pores of the composite foams are achieved.Consequently,the composites show a satisfactory X-band electromagnetic interference(EMI)shielding effectiveness of 22.5 to 62.5 dB at a density of 28.7 to 48.7 mg cm−3,leading to an excellent surface-specific SE of 21,317 dB cm^(2)g^(−1).Moreover,the composite foams exhibit excellent electrothermal performance as flexible heaters in terms of a prominent,rapid reproducible,and stable electrothermal effect at low voltages and superior heat performance and more uniform heat distribution compared with the commercial heaters composed of alloy plates.Furthermore,the composite foams are well attached on a human body to check their electromechanical sensing performance,demonstrating the sensitive and reliable detection of human motions as wearable sensors.The excellent EMI shielding performance and multifunctionalities,along with the facile and easy-to-scalable manufacturing techniques,imply promising perspectives of the porous C-MXene@PI composites in next-generation flexible electronics,aerospace,and smart devices.
基金part of the activities of SCCER HeE, which is financially supported by Innosuisse – Swiss Innovation Agency
文摘Stability of borohydrides is determined by the localization of the negative charge on the boron atom.Ionic liquids(ILs) allow to modify the stability of the borohydrides and promote new dehydrogenation pathways with a lower activation energy. The combination of borohydride and IL is very easy to realize and no expensive rare earth metals are required. The composite of the ILs with complex hydrides decreases the enthalpy and activation energy for the hydrogen desorption. The Coulomb interaction between borohydride and IL leads to a destabilization of the materials with a significantly lower enthalpy for hydrogen desorption. Here, we report a simple ion exchange reaction using various ILs, such as vinylbenzyltrimethylammonium chloride([VBTMA][Cl]), 1-butyl-3-methylimidazolium chloride([bmim][Cl]), and 1-ethyl-1-methylpyrrolidinium bromide([EMPY][Br]) with NaBH4 to decrease the hydrogen desorption temperature. Dehydrogenation of 1-butyl-3-methylimidazolium borohydride([bmim][BH4]) starts below 100℃. The quantity of desorbed hydrogen ranges between 2.4 wt% and 2.9 wt%, which is close to the theoretical content of hydrogen. The improvement in dehydrogenation is due to the strong amine cation that destabilizes borohydride by charge transfer.
基金Supported by A grant of the Swiss Orthopaedics Society(SGOT)to Ahmad SS,No.S99083814080618560
文摘AIM: To investigate collagen patches seeded with mesenchymal stem cells(MSCs) and/or tenocytes(TCs) with regards to their suitability for anterior cruciate ligament(ACL) repair. METHODS: Dynamic intraligamentary stabilization utilizes a dynamic screw system to keep ACL remnants in place and promote biological healing, supplemented by collagen patches. How these scaffolds interact with cells and what type of benefit they provide has not yet been investigated in detail. Primary ACL-derived TCs and human bone marrow derived MSCs were seeded onto two different types of 3D collagen scaffolds, Chondro-Gide?(CG) and Novocart?(NC). Cells were seeded onto the scaffolds and cultured for 7 d either as a pure populations or as "premix" containing a 1:1 ratio of TCs to MSCs. Additionally, as controls, cells were seeded in monolayers and in co-cultures on both sides of porous high-density membrane inserts(0.4 μm). We analyzed the patches by real time polymerase chain reaction, glycosaminoglycan(GAG), DNA and hydroxyproline(HYP) content. To determine cell spreading and adherence in the scaffolds microscopic imaging techniques, i.e., confocal laser scanning microscopy(c LSM) and scanning electron microscopy(SEM), were applied.RESULTS: CLSM and SEM imaging analysis confirmed cell adherence onto scaffolds. The metabolic cell activity revealed that patches promote adherence and proliferation of cells. The most dramatic increase in absolute metabolic cell activity was measured for CG samples seeded with tenocytes or a 1:1 cell premix. Analysis of DNA content and c LSM imaging also indicated MSCs were not proliferating as nicely as tenocytes on CG. The HYP to GAG ratio significantly changed for the premix group, resulting from a slightly lower GAG content, demonstrating that the cells are modifying the underlying matrix. Real-time quantitativepolymerase chain reaction data indicated that MSCs showed a trend of differentiation towards a more tenogenic-like phenotype after 7 d.CONCLUSION: CG and NC are both cyto-compatible with primary MSCs and TCs; TCs seemed to perform better on these collagen patches than MSCs.
文摘A new self-repairing membrane for inflatable light weight structures such as rubber boats or Tensairity constructions is presented. Inspired by rapid self-sealing processes in plants, a thin soft cellular polyurethane foam coating is applied on the inside of a fabric substrate, which closes the fissure if the membrane is punctured with a spike. Experimental tests are carried out with a purpose built setup by measuring the air mass flow through a leak in a damaged membrane sample. It is shown that the weight per unit area of the self-repairing foam as well as the curing of the two component PU-foam under an overpressure influence the repair efficiency. Curing the foam under overpressure affects the relative density as well as the microstructure of the foam coatings. Maximal median repair efficiencies of 0.999 have been obtained with 0.16 g.cm 2 foam cured at 1 bar overpressure. These results suggest that the bio-inspired technique has the potential to extend the functional integrity of injured inflatable structures dramatically.
文摘Functionally graded（FG） carbon nanotubes（CNT） and nano-silicon carbide（nSiC） reinforced aluminium（Al）matrix composites have been successfully fabricated using high-energy ball milling followed by solid-state spark plasma sintering processes.The CNTs were well-dispersed in the Al particles using the nSiC as a solid mixing agent.Two different types of multi-walled CNTs were used to add different amounts of CNTs in the same volume.The ball milled Al—CNT—nSiC and Al—CNT powder mixtures were fully densified and demonstrated good adhesion with no serious microcracks and pores within an FG multilayer composite.Each layer contained different amounts of the CNTs,and the nSiC additions showed different microstructures and hardness.It is possible to control the characteristics of the FG multilayer composite through the efficient design of an Al—CNT—nSiC gradient layer.This concept offers a feasible approach for fabricating the dualnanoparticulate-reinforced Al matrix nanocomposites and can be applied to other scenarios such as polymer and ceramic systems.
文摘The significant positive green environment influence of magnesium alloy usage in transport could be compromised by catastrophic fast fracture caused by stress corrosion cracking(SCC). Transgranular stress corrosion cracking(TGSCC) of AZ91 was evaluated using the linearly increasing stress test(LIST) and the constant extension rate test(CERT). The TGSCC threshold stress was 55-75 MPa in distilled water and in 5 g/L NaCl. The TGSCC velocity was 7×10-10-5×10-9 m/s. A delayed hydride-cracking(DHC) model for TGSCC was implemented using a finite element script in MATLAB and the model predictions were compared with experiment. A key outcome is that,during steady state TGSCC propagation,a high dynamic hydrogen concentration is expected to build up behind the crack tip. A number of recommendations are given for preventing SCC of Mg alloys in service. One of the most important recommendations might be that the total stress in service(i.e. the stress from the service loading + the fabrication stress + the residual stress) should be below a threshold level,which,in the absence of other data,could be(conservatively) estimated to be about 50% of the tensile yield strength.
基金the Department of Metallurgical and Materials Engineering,National Institute of Technology,Tiruchirapalli for providing the funds and facilities to conduct this research work
文摘In this work, the morphology, phase composition, and corrosion properties of microarc oxidized (MAO) gas tungsten arc (GTA) weldments of AZ31 alloy were investigated. Autogenous gas tungsten arc welds were made as full penetration bead-on-plate welding under the alternating-current mode. A uniform oxide layer was developed on the surface of the specimens with MAO treatment in silicate-based alkaline electrolytes for different oxidation times. The corrosion behavior of the samples was evaluated by potentiodynamic polarization and electrochemical impedance spectroscopy. The oxide film improved the corrosion resistance substantially compared to the uncoated specimens. The sample coated for 10 min exhibited better corrosion properties. The corrosion resistance of the coatings was concluded to strongly depend on the morphology, whereas the phase composition and thickness were concluded to only slightly affect the corrosion resistance.
基金supports from ETH board,Empa internal research call 2019(IRC-2019-CupSupercap)and 2020(IRC-2020-NitfixMX)supports from Xi'an Jiaotong University,and China Scholarship Council(202106280247).
文摘Ammonia is the most basic raw material in industrial and agricultural production.The current industrial production of ammonia relies on the Haber-Bosch process with high energy consumption.To overcome this shortcoming,the development of electrocatalytic ammonia synthesis under moderate conditions is considered as a potential alternative technology.The two-dimensional(2D)MXenes family has been proved promising as electrocatalysts,but from the currently available literature,it is hard to find a systematic review on MXenes-catalyzed ammonia synthesis.So in the present review,we summarize the key perspectives on that topic in recent years as well as outline,from a prospective view,strategies of catalyst design.We analyze in detail the methods for preparing high performance MXenes-based catalysts and the corresponding underlying mechanisms,and also discuss the criteria and potential challenges,expecting to provide inspiration for the development of efficient MXenes-based route to electrochemical ammonia fixation.
