After exposure to freeze-thaw cycles, scanning electron microscopy(SEM) and nuclear magnetic resonance(NMR) were used to test the four mixtures. The microstructure is qualitatively analyzed from the 2D SEM image and t...After exposure to freeze-thaw cycles, scanning electron microscopy(SEM) and nuclear magnetic resonance(NMR) were used to test the four mixtures. The microstructure is qualitatively analyzed from the 2D SEM image and the 3D pore distribution curve before and after freezing and thawing. The fractal dimension is utilized to characterize the two-dimensional topography image and the three-dimensional pore distribution, quantitatively. The results reveal that the surface porosity and volume porosity increase as the freeze-thaw action increases. Self-similarity characteristics exist in micro-damage inside the concrete. In the fractal dimension, it is possible to characterize pore evolution quantitatively. The fractal dimension correlates with pore damage evolution. The fractal dimension effectively quantitatively characterizes micro-damage features at various scales from the local to the global level.展开更多
The glacial history of Pico de Orizaba indicates that during the Last Glacial Maximum,its icecap covered up to~3000 m asl;due to the air temperature increasing,its main glacier has retreated to 5050 m asl.The retracti...The glacial history of Pico de Orizaba indicates that during the Last Glacial Maximum,its icecap covered up to~3000 m asl;due to the air temperature increasing,its main glacier has retreated to 5050 m asl.The retraction of the glacier has left behind an intense climatic instability that causes a high frequency of freeze-thaw cycles of great intensity;the resulting geomorphological processes are represented by the fragmentation of the bedrock that occupies the upper parts of the mountain.There is a notable lack of studies regarding the fragmentation and erosion occurring in tropical high mountains,and the associated geomorphological risks;for this reason,as a first stage of future continuous research,this study analyzes the freezing and thawing cycles that occur above 4000 m asl,through continuous monitoring of surface ground temperature.The results allow us to identify and characterize four zones:glacial,paraglacial,periglacial and proglacial.It was found that the paraglacial zone presents an intense drop of temperature,of up to~9℃ in only sixty minutes.The rock fatigue and intense freeze-thaw cycles that occur in this area are responsible for the high rate of rock disintegration and represent the main factor of the constant slope dynamics that occur at the site.This activity decreases,both in frequency and intensity,according to the distance to the glacier,which is where the temperature presents a certain degree of stability,until reaching the proglacial zone,where cycles are almost non-existent,and therefore there is no gelifraction activity.The geomorphological processes have resulted in significant alterations to the mountain slopes,which can have severe consequences in terms of risk and water.展开更多
We experimentally and theoretically present a paradigm for the accurate bilayer design of gradient metasurfaces for wave beam manipulation,producing an extremely asymmetric splitting effect by simply tailoring the int...We experimentally and theoretically present a paradigm for the accurate bilayer design of gradient metasurfaces for wave beam manipulation,producing an extremely asymmetric splitting effect by simply tailoring the interlayer size.This concept arises from anomalous diffraction in phase gradient metasurfaces and the precise combination of the phase gradient in bilayer metasurfaces.Ensured by different diffraction routes in momentum space for incident beams from opposite directions,extremely asymmetric acoustic beam splitting can be generated in a robust way,as demonstrated in experiments through a designed bilayer system.Our work provides a novel approach and feasible platform for designing tunable devices to control wave propagation.展开更多
Conversion of solar energy into H2 by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of phot...Conversion of solar energy into H2 by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of photoanodes is crucial to guarantee the high efficiency and stability of PEC reactions,which fundamentally rely on rationally designed semiconductors(as the active materials)and substrates(as the current collectors).In this review work,we start with a brief introduction of the roles of substrates in the PEC process.Then,we provide a systematic overview of representative strategies for the controlled fabrication of photoanodes on rationally designed substrates,including conductive glass,metal,sapphire,silicon,silicon carbide,and flexible substrates.Finally,some prospects concerning the challenges and research directions in this area are proposed.展开更多
A Pickering emulsion based on sodium starch octenyl succinate(SSOS)was prepared and its effects on the physicochemical properties of hairtail myofibrillar protein gels(MPGs)subjected to multiple freeze-thaw(F-T)cycles...A Pickering emulsion based on sodium starch octenyl succinate(SSOS)was prepared and its effects on the physicochemical properties of hairtail myofibrillar protein gels(MPGs)subjected to multiple freeze-thaw(F-T)cycles were investigated.The whiteness,water-holding capacity,storage modulus(G')and texture properties of the MPGs were significantly improved by adding 1%-2%Pickering emulsion(P<0.05).Meanwhile,Raman spectral analysis demonstrated that Pickering emulsion promoted the transformation of secondary structure,enhanced hydrogen bonds and hydrophobic interactions,and promoted the transition of disulfide bond conformation from g-g-g to g-g-t and t-g-t.At an emulsion concentration of 2%,theα-helix content decreased by 10.37%,while theβ-sheet content increased by 7.94%,compared to the control.After F-T cycles,the structure of the MPGs was destroyed,with an increase in hardness and a decrease in whiteness and water-holding capacity,however,the quality degradation of MPGs was reduced with 1%-2%Pickering emulsion.These findings demonstrated that SSOS-Pickering emulsions,as potential fat substitutes,can enhance the gel properties and the F-T stability of MPGs.展开更多
The reuse of waste recycled concrete from harsh environments has become a research hotspot in the field of construction.This study investigated the repair effect of carbonation treatment on second-generation recycled ...The reuse of waste recycled concrete from harsh environments has become a research hotspot in the field of construction.This study investigated the repair effect of carbonation treatment on second-generation recycled fine aggregate(SRFA)obtained from recycled fine aggregate concrete(RFAC)subjected to freeze-thaw(FT)cycles.Before and after carbonation,the properties of SRFA were evaluated.Carbonated second-generation recycled fine aggregate(CSRFA)at five substitution rates(0%,25%,50%,75%,100%)to replace SRFA was used to prepare carbonated second-generation recycled fine aggregate concrete(CSRFAC).The water absorption,porosity and mechanical properties of CSRFAC were tested,and its frost-resisting durability was evaluated.The results showed after carbonation treatment,the physical properties of SRFA was improved and met the requirements of II aggregate.The micro-hardness of the interfacial transition zone and attached mortar in CSRFA was 50.5%and 31.2%higher than that in SRFA,respectively.With the increase of CSRFA replacement rate,the water absorption and porosity of CSRFAC gradually decreased,and the mechanical properties and frost resistance of CSRFAC were gradually improved.Carbonation treatment effectively repairs the damage of SRFA caused by FT cycles and improves its application potential.展开更多
Moraines,characterized by the accumulation of rock and soil debris transported by glacial activity,present unique challenges for tunnel construction,particularly in portal sections,due to prevailing geographical and c...Moraines,characterized by the accumulation of rock and soil debris transported by glacial activity,present unique challenges for tunnel construction,particularly in portal sections,due to prevailing geographical and climatic conditions that facilitate freeze-thaw action.Despite these challenges,there is a dearth of studies investigating the influence of freeze-thaw action and water content on the mechanical properties of moraines,and no research on calculating surrounding rock pressure in moraine tunnels subjected to freeze-thaw conditions.In this study,direct shear tests under freeze-thaw cycles were conducted to examine the effects of freeze-thaw cycles and water content on the mechanical properties of frozen moraine.A comprehensive parameter K,integrating the number of freeze-thaws and water content,was introduced to model cohesion c.Drawing on Terzaghi Theory,we propose an improved algorithm for calculating surrounding rock pressure at the portal section of moraine tunnels.Using a tunnel as a case study,surrounding rock pressure was calculated under various conditions to validate the Improved Algorithm's efficacy.The results show that:(1)Strength loss exhibits a linear trend with the number of freeze-thaw cycles at water content levels of 4%and 8%,while at 12%water content,previous freeze-thaw cycles induce more significant damage to the soil.(2)Moraine saturation peaks between 8%and 12%water content.Following repeated freeze-thaw cycles,moraine shear strength initially increases before decreasing with varying water content.(3)The internal friction angle of moraine experiences slight reductions with prolonged freeze-thaw cycles,but both freeze-thaw cycles and water content significantly influence cohesion.(4)Vertical surrounding rock pressure increases after the initial freeze-thaw cycle,particularly with higher water content,although freeze-thaw cycles have minimal effect on it.(5)Freeze-thaw cycles lead to a substantial increase in lateral surrounding rock pressure,necessitating reinforced support structures at the arch wall,arch waist,and arch foot in engineering projects to mitigate freeze-thaw effects.This study provides a foundation for designing and selecting tunnel support structures in similar geological conditions.展开更多
Chloride (Cl−) ion erosion effects can seriously impact the safety and service life of marine liquefied natural gas(LNG) storage tanks and other polar offshore structures. This study investigates the impact of differe...Chloride (Cl−) ion erosion effects can seriously impact the safety and service life of marine liquefied natural gas(LNG) storage tanks and other polar offshore structures. This study investigates the impact of different low-temperaturecycles (20°C, –80°C, and −160°C) and concrete specimen crack widths (0, 0.3, and 0.6 mm) on the Cl−ion diffusion performance through rapid erosion tests conducted on pre-cracked concrete. The results show thatthe minimum temperature and crack width of freeze-thaw cycles enhance the erosive effect of chloride ions. TheCl− ion concentration and growth rate increased with the increasing crack width. Based on the experimental modeland in accordance with Fick’s second law of diffusion, the Cl− ion diffusion equation was modified by introducingcorrection factors in consideration of the freeze-thaw temperature, crack width, and their coupling effect.The experimental and fitting results obtained from this model can provide excellent reference for practical engineeringapplications.展开更多
Cobalt-based electrocatalysts take advantage of potentially harmonizable microstructure and flexible coupling effects compared to commercial noble metal-based catalytic materials.However,conventional water electrolysi...Cobalt-based electrocatalysts take advantage of potentially harmonizable microstructure and flexible coupling effects compared to commercial noble metal-based catalytic materials.However,conventional water electrolysis systems based on cobalt-based monofunctional hydrogen evolution reaction(HER)or oxygen evolution reaction(OER)catalysts have certain shortcomings in terms of resource utilization and universality.In contrast,cobalt-based bifunctional catalysts(CBCs)have attracted much attention in recent years for overall water splitting systems because of their practicality and reduced preparation cost of electrolyzer.This review aims to address the latest development in CBCs for total hydrolysis.The main modification strategies of CBCs are systematically classified in water electrolysis to provide an overview of how to regulate their morphology and electronic configuration.Then,the catalytic performance of CBCs in total-hydrolysis is summarized according to the types of cobalt-based phosphides,sulfides and oxides,and the mechanism of strengthened electrocatalytic ability is emphasized through combining experiments and theoretical calculations.Future efforts are finally suggested to focus on exploring the dynamic conversion of reaction intermediates and building near-industrial CBCs,designing advanced CBC materials through micro-modulation,and addressing commercial applications.展开更多
Arctic sea ice is broadly regarded as an indicator and amplifier of global climate change.The rapid changes in Arctic sea ice have been widely concerned.However,the spatiotemporal changes in the horizontal and vertica...Arctic sea ice is broadly regarded as an indicator and amplifier of global climate change.The rapid changes in Arctic sea ice have been widely concerned.However,the spatiotemporal changes in the horizontal and vertical dimensions of Arctic sea ice and its asymmetry during the melt and freeze seasons are rarely quantified simultaneously based on multiple sources of the same long time series.In this study,the spatiotemporal variation and freeze-thaw asymmetry of Arctic sea ice were investigated from both the horizontal and vertical dimensions during 1979–2020 based on remote sensing and assimilation data.The results indicated that Arctic sea ice was declining at a remarkably high rate of–5.4×10^(4) km^(2)/a in sea ice area(SIA)and–2.2 cm/a in sea ice thickness(SIT)during 1979 to 2020,and the reduction of SIA and SIT was the largest in summer and the smallest in winter.Spatially,compared with other sub-regions,SIA showed a sharper declining trend in the Barents Sea,Kara Sea,and East Siberian Sea,while SIT presented a larger downward trend in the northern Canadian Archipelago,northern Greenland,and the East Siberian Sea.Regarding to the seasonal trend of sea ice on sub-region scale,the reduction rate of SIA exhibited an apparent spatial heterogeneity among seasons,especially in summer and winter,i.e.,the sub-regions linked to the open ocean exhibited a higher decline rate in winter;however,the other sub-regions blocked by the coastlines presented a greater decline rate in summer.For SIT,the sub-regions such as the Beaufort Sea,East Siberian Sea,Chukchi Sea,Central Arctic,and Canadian Archipelago always showed a higher downward rate in all seasons.Furthermore,a striking freeze-thaw asymmetry of Arctic sea ice was also detected.Comparing sea ice changes in different dimensions,sea ice over most regions in the Arctic showed an early retreat and rapid advance in the horizontal dimension but late melting and gradual freezing in the vertical dimension.The amount of sea ice melting and freezing was disequilibrium in the Arctic during the considered period,and the rate of sea ice melting was 0.3×10^(4) km^(2)/a and 0.01 cm/a higher than that of freezing in the horizontal and vertical dimensions,respectively.Moreover,there were notable shifts in the melting and freezing of Arctic sea ice in 1997/2003 and 2000/2004,respectively,in the horizontal/vertical dimension.展开更多
Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy...Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.展开更多
Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have bee...Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.展开更多
Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formatio...Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formation of nickel single atoms(Ni-SAs) as exceptional bifunctional electrocatalyst toward UOR and hydrogen evolution reaction(HER) in urea-assisted water splitting.In UOR catalysis,Ni-SAs perform a superior catalytic performance than Ni-NP/NC and Pt/C ascribing to the formation of HOO-Ni-N_(4) structure evidenced by in-situ Raman spectroscopy,corresponding to a boosted mass activity by 175-fold at 1.4 V vs.RHE than Ni-NP/NC.Furthermore,Ni-SAs requires only 450 mV overpotential to obtain HER current density of 500 mA cm^(-2).136 mA cm^(-2) is achieved in urea-assisted water splitting at1.7 V for Ni-SAs,boosted by 5.7 times than Pt/C-IrO_(2) driven water splitting.展开更多
Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen e...Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.展开更多
Hematite(α-Fe_(2)O_(3)) based photoanodes have been extensively studied due to various intriguing features that make them viable candidates for a photoelectrochemical(PEC) water splitting photoanode.Herein,we propose...Hematite(α-Fe_(2)O_(3)) based photoanodes have been extensively studied due to various intriguing features that make them viable candidates for a photoelectrochemical(PEC) water splitting photoanode.Herein,we propose a Zr-doped Fe_(2)O_(3) photoanode decorated with facilely spin-coated Au nanoparticles(NPs) and microwave-assisted attached Si co-doping in conjunction with a SiO_(x) overlayer that displayed a remarkable photocurrent density of 2.01 mA/cm^(2) at 1.23 V vs.RHE.The kinetic dynamics at the photoelectrode/-electrolyte interface was examined by employing systematic electrochemical investigations.The Au NPs played a dual role in increasing PEC water splitting.First,the Schottky interface that was formed between Au NPs and Zr-Fe_(2)O_(3) lectrode ensured the prevention of electron flow from the photoanode to the metal,increasing the number of available charges as well as suppressing surface charge recombination.Second,Au extracted photoholes from the bulk of the Zr-Fe_(2)O_(3) and transported them to the outer SiO_(x) overlayer,while the SiO_(x) overlayer efficiently collected the photoholes and promoted the hole injection into the electrolyte.Further,Si co-doping enhanced bulk conductivity by reducing bulk charge transfer resistance and improving charge carrier density.This study outlines a technique to design a metallic charge transfer path with an overlayer for solar energy conversion.展开更多
Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high...Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high-performance electrocatalysts is crucial in making electrolyzed water technology commercially viable.Cobalt phosphide(Co-P)has emerged as a catalyst of high potential owing to its high catalytic activity and durability in water splitting.This paper systematically reviews the latest advances in the development of Co-P-based materials for use in water splitting.The essential effects of P in enhancing the catalytic performance of the hydrogen evolution reaction and oxygen evolution reaction are first outlined.Then,versatile synthesis techniques for Co-P electrocatalysts are summarized,followed by advanced strategies to enhance the electrocatalytic performance of Co-P materials,including heteroatom doping,composite construction,integration with well-conductive sub-strates,and structure control from the viewpoint of experiment.Along with these optimization strategies,the understanding of the inherent mechanism of enhanced catalytic performance is also discussed.Finally,some existing challenges in the development of highly active and stable Co-P-based materials are clarified,and pro-spective directions for prompting the wide commercialization of water electrolysis technology are proposed.展开更多
High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inhere...High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.展开更多
Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil fuels.Alkaline water electrolysis utilizing renewable energy sources has emerged as a means to...Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil fuels.Alkaline water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity hydrogen.Nevertheless,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment contamination.Therefore,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel foam.The synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline solution.Furthermore,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.展开更多
Hydrogen production from electrochemical water splitting is a promising strategy to generate green energy,which requires the development of efficient and stable electrocatalysts for the hydrogen evolution reaction and...Hydrogen production from electrochemical water splitting is a promising strategy to generate green energy,which requires the development of efficient and stable electrocatalysts for the hydrogen evolution reaction and the oxygen evolution reaction(HER and OER).Ionic liquids(ILs)or poly(ionic liquids)(PILs),containing heteroatoms,metal-based anions,and various structures,have been frequently involved as precursors to prepare electrocatalysts for water splitting.Moreover,ILs/PILs possess high conductivity,wide electrochemical windows,and high thermal and chemical stability,which can be directly applied in the electrocatalysis process with high durability.In this review,we focus on the studies of ILs/PILs-derived electrocatalysts for HER and OER,where ILs/PILs are applied as heteroatom dopants and metal precursors to prepare catalysts or are directly utilized as the electrocatalysts.Due to those attractive properties,IL/PIL-derived electrocatalysts exhibit excellent performance for electrochemical water splitting.All these accomplishments and developments are systematically summarized and thoughtfully discussed.Then,the overall perspectives for the current challenges and future developments of ILs/PILs-derived electrocatalysts are provided.展开更多
In order to understand the mechanical properties and the fracture surface roughness characteristics of thermally damaged granite under dynamic splitting,dynamic Brazilian splitting tests were conducted on granite samp...In order to understand the mechanical properties and the fracture surface roughness characteristics of thermally damaged granite under dynamic splitting,dynamic Brazilian splitting tests were conducted on granite samples after thermal treatment at 25,200,400,and 600℃.Results show that the dynamic peak splitting strength of thermally damaged granite samples increases with increasing strain rate,showing obvious strain‐rate sensitivity.With increasing temperature,thermally induced cracks in granite transform from intergranular cracks to intragranular cracks,and to a transgranular crack network.Thermally induced damages reduce the dynamic peak splitting strength and the maximum absorbed energy while increasing the peak radial strain.The fracture mode of the thermally damaged granite under dynamic loads is mode Ⅱ splitting failure.By using the axial roughness index Z2 a,the distribution ranges of the wedge‐shaped failure zones and the tensile failure zones in the fracture surfaces under dynamic Brazilian splitting can be effectively identified.The radial roughness index Z_(2)^(r)is sensitive to the strain rate and temperature.It shows a linear correlation with the peak splitting strength and the maximum absorbed energy and a linear negative correlation with the peak radial strain.Z_(2)^(r)can be used to quantitatively estimate the dynamic parameters based on the models proposed.展开更多
基金Funded by the Key Project of Science and Technology Research in Higher Educational Institutions of Inner Mongolia Autonomous Region (No.NJZZ22518)Inner Mongolia Natural Science Foundation Project (No.2022MS05043)Inner Mongolia Autonomous Region Water Conservancy Research Special Project(No.NSK2016-S11)。
文摘After exposure to freeze-thaw cycles, scanning electron microscopy(SEM) and nuclear magnetic resonance(NMR) were used to test the four mixtures. The microstructure is qualitatively analyzed from the 2D SEM image and the 3D pore distribution curve before and after freezing and thawing. The fractal dimension is utilized to characterize the two-dimensional topography image and the three-dimensional pore distribution, quantitatively. The results reveal that the surface porosity and volume porosity increase as the freeze-thaw action increases. Self-similarity characteristics exist in micro-damage inside the concrete. In the fractal dimension, it is possible to characterize pore evolution quantitatively. The fractal dimension correlates with pore damage evolution. The fractal dimension effectively quantitatively characterizes micro-damage features at various scales from the local to the global level.
基金support from the Programa de Apoyos para la Superación del Personal Académico (DGAPA)the support by the Alexander von Humboldt Foundationpart of the SIREI project num 531062023178 developed at CCT-UV
文摘The glacial history of Pico de Orizaba indicates that during the Last Glacial Maximum,its icecap covered up to~3000 m asl;due to the air temperature increasing,its main glacier has retreated to 5050 m asl.The retraction of the glacier has left behind an intense climatic instability that causes a high frequency of freeze-thaw cycles of great intensity;the resulting geomorphological processes are represented by the fragmentation of the bedrock that occupies the upper parts of the mountain.There is a notable lack of studies regarding the fragmentation and erosion occurring in tropical high mountains,and the associated geomorphological risks;for this reason,as a first stage of future continuous research,this study analyzes the freezing and thawing cycles that occur above 4000 m asl,through continuous monitoring of surface ground temperature.The results allow us to identify and characterize four zones:glacial,paraglacial,periglacial and proglacial.It was found that the paraglacial zone presents an intense drop of temperature,of up to~9℃ in only sixty minutes.The rock fatigue and intense freeze-thaw cycles that occur in this area are responsible for the high rate of rock disintegration and represent the main factor of the constant slope dynamics that occur at the site.This activity decreases,both in frequency and intensity,according to the distance to the glacier,which is where the temperature presents a certain degree of stability,until reaching the proglacial zone,where cycles are almost non-existent,and therefore there is no gelifraction activity.The geomorphological processes have resulted in significant alterations to the mountain slopes,which can have severe consequences in terms of risk and water.
文摘We experimentally and theoretically present a paradigm for the accurate bilayer design of gradient metasurfaces for wave beam manipulation,producing an extremely asymmetric splitting effect by simply tailoring the interlayer size.This concept arises from anomalous diffraction in phase gradient metasurfaces and the precise combination of the phase gradient in bilayer metasurfaces.Ensured by different diffraction routes in momentum space for incident beams from opposite directions,extremely asymmetric acoustic beam splitting can be generated in a robust way,as demonstrated in experiments through a designed bilayer system.Our work provides a novel approach and feasible platform for designing tunable devices to control wave propagation.
基金Natural Science Foundation of Zhejiang Province,Grant/Award Number:LY23E020002National Natural Science Foundation of China,Grant/Award Number:52272085 and 51972178+1 种基金Natural Science Foundation of Ningbo,Grant/Award Number:2021J145China Postdoctoral Science Foundation,Grant/Award Number:2020M681966。
文摘Conversion of solar energy into H2 by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of photoanodes is crucial to guarantee the high efficiency and stability of PEC reactions,which fundamentally rely on rationally designed semiconductors(as the active materials)and substrates(as the current collectors).In this review work,we start with a brief introduction of the roles of substrates in the PEC process.Then,we provide a systematic overview of representative strategies for the controlled fabrication of photoanodes on rationally designed substrates,including conductive glass,metal,sapphire,silicon,silicon carbide,and flexible substrates.Finally,some prospects concerning the challenges and research directions in this area are proposed.
基金supported by the National Natural Science Foundation of China(U20A2067,32272360)。
文摘A Pickering emulsion based on sodium starch octenyl succinate(SSOS)was prepared and its effects on the physicochemical properties of hairtail myofibrillar protein gels(MPGs)subjected to multiple freeze-thaw(F-T)cycles were investigated.The whiteness,water-holding capacity,storage modulus(G')and texture properties of the MPGs were significantly improved by adding 1%-2%Pickering emulsion(P<0.05).Meanwhile,Raman spectral analysis demonstrated that Pickering emulsion promoted the transformation of secondary structure,enhanced hydrogen bonds and hydrophobic interactions,and promoted the transition of disulfide bond conformation from g-g-g to g-g-t and t-g-t.At an emulsion concentration of 2%,theα-helix content decreased by 10.37%,while theβ-sheet content increased by 7.94%,compared to the control.After F-T cycles,the structure of the MPGs was destroyed,with an increase in hardness and a decrease in whiteness and water-holding capacity,however,the quality degradation of MPGs was reduced with 1%-2%Pickering emulsion.These findings demonstrated that SSOS-Pickering emulsions,as potential fat substitutes,can enhance the gel properties and the F-T stability of MPGs.
基金financially sponsored by Qing Lan Project in Jiangsu Province of China(2023)Scientific Research Project of Taizhou Polytechnic College(TZYKY-22-4).
文摘The reuse of waste recycled concrete from harsh environments has become a research hotspot in the field of construction.This study investigated the repair effect of carbonation treatment on second-generation recycled fine aggregate(SRFA)obtained from recycled fine aggregate concrete(RFAC)subjected to freeze-thaw(FT)cycles.Before and after carbonation,the properties of SRFA were evaluated.Carbonated second-generation recycled fine aggregate(CSRFA)at five substitution rates(0%,25%,50%,75%,100%)to replace SRFA was used to prepare carbonated second-generation recycled fine aggregate concrete(CSRFAC).The water absorption,porosity and mechanical properties of CSRFAC were tested,and its frost-resisting durability was evaluated.The results showed after carbonation treatment,the physical properties of SRFA was improved and met the requirements of II aggregate.The micro-hardness of the interfacial transition zone and attached mortar in CSRFA was 50.5%and 31.2%higher than that in SRFA,respectively.With the increase of CSRFA replacement rate,the water absorption and porosity of CSRFAC gradually decreased,and the mechanical properties and frost resistance of CSRFAC were gradually improved.Carbonation treatment effectively repairs the damage of SRFA caused by FT cycles and improves its application potential.
基金jointly supported by the National Natural Science Foundation of China(Grant Number 12262018)the Technology Funding Scheme of China Construction Second Engineering Bureau LTD(Grant Number 2020ZX150002)Special Funds for Guiding Local Scientific and Technological Development by The Central Government(Grant Number 22ZY1QA005)。
文摘Moraines,characterized by the accumulation of rock and soil debris transported by glacial activity,present unique challenges for tunnel construction,particularly in portal sections,due to prevailing geographical and climatic conditions that facilitate freeze-thaw action.Despite these challenges,there is a dearth of studies investigating the influence of freeze-thaw action and water content on the mechanical properties of moraines,and no research on calculating surrounding rock pressure in moraine tunnels subjected to freeze-thaw conditions.In this study,direct shear tests under freeze-thaw cycles were conducted to examine the effects of freeze-thaw cycles and water content on the mechanical properties of frozen moraine.A comprehensive parameter K,integrating the number of freeze-thaws and water content,was introduced to model cohesion c.Drawing on Terzaghi Theory,we propose an improved algorithm for calculating surrounding rock pressure at the portal section of moraine tunnels.Using a tunnel as a case study,surrounding rock pressure was calculated under various conditions to validate the Improved Algorithm's efficacy.The results show that:(1)Strength loss exhibits a linear trend with the number of freeze-thaw cycles at water content levels of 4%and 8%,while at 12%water content,previous freeze-thaw cycles induce more significant damage to the soil.(2)Moraine saturation peaks between 8%and 12%water content.Following repeated freeze-thaw cycles,moraine shear strength initially increases before decreasing with varying water content.(3)The internal friction angle of moraine experiences slight reductions with prolonged freeze-thaw cycles,but both freeze-thaw cycles and water content significantly influence cohesion.(4)Vertical surrounding rock pressure increases after the initial freeze-thaw cycle,particularly with higher water content,although freeze-thaw cycles have minimal effect on it.(5)Freeze-thaw cycles lead to a substantial increase in lateral surrounding rock pressure,necessitating reinforced support structures at the arch wall,arch waist,and arch foot in engineering projects to mitigate freeze-thaw effects.This study provides a foundation for designing and selecting tunnel support structures in similar geological conditions.
基金the Key Laboratory of Intelligent Health Perception and Lakes,Ministry of Education,Hubei University of Technology(No.2020EJB004)National Natural Science Foundation of China(No.51508171)Natural Science Foundation of Hubei Province(No.2020CFB860).
文摘Chloride (Cl−) ion erosion effects can seriously impact the safety and service life of marine liquefied natural gas(LNG) storage tanks and other polar offshore structures. This study investigates the impact of different low-temperaturecycles (20°C, –80°C, and −160°C) and concrete specimen crack widths (0, 0.3, and 0.6 mm) on the Cl−ion diffusion performance through rapid erosion tests conducted on pre-cracked concrete. The results show thatthe minimum temperature and crack width of freeze-thaw cycles enhance the erosive effect of chloride ions. TheCl− ion concentration and growth rate increased with the increasing crack width. Based on the experimental modeland in accordance with Fick’s second law of diffusion, the Cl− ion diffusion equation was modified by introducingcorrection factors in consideration of the freeze-thaw temperature, crack width, and their coupling effect.The experimental and fitting results obtained from this model can provide excellent reference for practical engineeringapplications.
基金financially supported by the National Natural Science Foundation of China(51572166,52102070)the Program for Professor of Special Appointment at Shanghai Institutions of Higher Learning(GZ2020012)+4 种基金the Key Research Project of Zhejiang Laboratory(2021PE0AC02)the China Postdoctoral Science Foundation(2021M702073)BAJC R&D Fund Projects(BA23011)Australian Research Council Future Fellowships(FT230100436)the Shanghai Technical Service Center for Advanced Ceramics Structure Design and Precision Manufacturing(20DZ2294000)。
文摘Cobalt-based electrocatalysts take advantage of potentially harmonizable microstructure and flexible coupling effects compared to commercial noble metal-based catalytic materials.However,conventional water electrolysis systems based on cobalt-based monofunctional hydrogen evolution reaction(HER)or oxygen evolution reaction(OER)catalysts have certain shortcomings in terms of resource utilization and universality.In contrast,cobalt-based bifunctional catalysts(CBCs)have attracted much attention in recent years for overall water splitting systems because of their practicality and reduced preparation cost of electrolyzer.This review aims to address the latest development in CBCs for total hydrolysis.The main modification strategies of CBCs are systematically classified in water electrolysis to provide an overview of how to regulate their morphology and electronic configuration.Then,the catalytic performance of CBCs in total-hydrolysis is summarized according to the types of cobalt-based phosphides,sulfides and oxides,and the mechanism of strengthened electrocatalytic ability is emphasized through combining experiments and theoretical calculations.Future efforts are finally suggested to focus on exploring the dynamic conversion of reaction intermediates and building near-industrial CBCs,designing advanced CBC materials through micro-modulation,and addressing commercial applications.
基金The Chinese Academy of Sciences(CAS)Key Deployment Project of Centre for Ocean Mega-Research of Science under contract No.COMS2020Q07the Open Fund Project of Key Laboratory of Marine Environmental Information Technology,Ministry of Natural Resourcesthe National Natural Science Foundation of China under contract No.41901133.
文摘Arctic sea ice is broadly regarded as an indicator and amplifier of global climate change.The rapid changes in Arctic sea ice have been widely concerned.However,the spatiotemporal changes in the horizontal and vertical dimensions of Arctic sea ice and its asymmetry during the melt and freeze seasons are rarely quantified simultaneously based on multiple sources of the same long time series.In this study,the spatiotemporal variation and freeze-thaw asymmetry of Arctic sea ice were investigated from both the horizontal and vertical dimensions during 1979–2020 based on remote sensing and assimilation data.The results indicated that Arctic sea ice was declining at a remarkably high rate of–5.4×10^(4) km^(2)/a in sea ice area(SIA)and–2.2 cm/a in sea ice thickness(SIT)during 1979 to 2020,and the reduction of SIA and SIT was the largest in summer and the smallest in winter.Spatially,compared with other sub-regions,SIA showed a sharper declining trend in the Barents Sea,Kara Sea,and East Siberian Sea,while SIT presented a larger downward trend in the northern Canadian Archipelago,northern Greenland,and the East Siberian Sea.Regarding to the seasonal trend of sea ice on sub-region scale,the reduction rate of SIA exhibited an apparent spatial heterogeneity among seasons,especially in summer and winter,i.e.,the sub-regions linked to the open ocean exhibited a higher decline rate in winter;however,the other sub-regions blocked by the coastlines presented a greater decline rate in summer.For SIT,the sub-regions such as the Beaufort Sea,East Siberian Sea,Chukchi Sea,Central Arctic,and Canadian Archipelago always showed a higher downward rate in all seasons.Furthermore,a striking freeze-thaw asymmetry of Arctic sea ice was also detected.Comparing sea ice changes in different dimensions,sea ice over most regions in the Arctic showed an early retreat and rapid advance in the horizontal dimension but late melting and gradual freezing in the vertical dimension.The amount of sea ice melting and freezing was disequilibrium in the Arctic during the considered period,and the rate of sea ice melting was 0.3×10^(4) km^(2)/a and 0.01 cm/a higher than that of freezing in the horizontal and vertical dimensions,respectively.Moreover,there were notable shifts in the melting and freezing of Arctic sea ice in 1997/2003 and 2000/2004,respectively,in the horizontal/vertical dimension.
基金supported by the National Natural Sci-ence Foundation of China(22272081),Jiangsu Provincial Specially Appointed Professors Foundation.
文摘Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.
文摘Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.
基金supported by the National Natural Science Foundation of China(No.22209126)。
文摘Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formation of nickel single atoms(Ni-SAs) as exceptional bifunctional electrocatalyst toward UOR and hydrogen evolution reaction(HER) in urea-assisted water splitting.In UOR catalysis,Ni-SAs perform a superior catalytic performance than Ni-NP/NC and Pt/C ascribing to the formation of HOO-Ni-N_(4) structure evidenced by in-situ Raman spectroscopy,corresponding to a boosted mass activity by 175-fold at 1.4 V vs.RHE than Ni-NP/NC.Furthermore,Ni-SAs requires only 450 mV overpotential to obtain HER current density of 500 mA cm^(-2).136 mA cm^(-2) is achieved in urea-assisted water splitting at1.7 V for Ni-SAs,boosted by 5.7 times than Pt/C-IrO_(2) driven water splitting.
基金supported by the Inner Mongolia R&D Program Plan(2021ZD0042,2021EEDSCXSFQZD006)the National Natural Science Foundation of China(21902123)the Natural Science Basic Research Program of Shaanxi(2023-JC-ZD-22)。
文摘Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2021R1A2C1095669,NRF-2021R1F1A1049366 and NRF2023R1A2C1003088)supported by the GRDC(Global Research Development Center)Cooperative Hub Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(RS-202300258911)。
文摘Hematite(α-Fe_(2)O_(3)) based photoanodes have been extensively studied due to various intriguing features that make them viable candidates for a photoelectrochemical(PEC) water splitting photoanode.Herein,we propose a Zr-doped Fe_(2)O_(3) photoanode decorated with facilely spin-coated Au nanoparticles(NPs) and microwave-assisted attached Si co-doping in conjunction with a SiO_(x) overlayer that displayed a remarkable photocurrent density of 2.01 mA/cm^(2) at 1.23 V vs.RHE.The kinetic dynamics at the photoelectrode/-electrolyte interface was examined by employing systematic electrochemical investigations.The Au NPs played a dual role in increasing PEC water splitting.First,the Schottky interface that was formed between Au NPs and Zr-Fe_(2)O_(3) lectrode ensured the prevention of electron flow from the photoanode to the metal,increasing the number of available charges as well as suppressing surface charge recombination.Second,Au extracted photoholes from the bulk of the Zr-Fe_(2)O_(3) and transported them to the outer SiO_(x) overlayer,while the SiO_(x) overlayer efficiently collected the photoholes and promoted the hole injection into the electrolyte.Further,Si co-doping enhanced bulk conductivity by reducing bulk charge transfer resistance and improving charge carrier density.This study outlines a technique to design a metallic charge transfer path with an overlayer for solar energy conversion.
基金the National Natural Science Foundation of China(21962008)Yunnan Province Excellent Youth Fund Project(202001AW070005)+1 种基金Candidate Talents Training Fund of Yunnan Province(2017PY269SQ,2018HB007)Yunnan Ten Thousand Talents Plan Young&Elite Talents Project(YNWR-QNBJ-2018-346).
文摘Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high-performance electrocatalysts is crucial in making electrolyzed water technology commercially viable.Cobalt phosphide(Co-P)has emerged as a catalyst of high potential owing to its high catalytic activity and durability in water splitting.This paper systematically reviews the latest advances in the development of Co-P-based materials for use in water splitting.The essential effects of P in enhancing the catalytic performance of the hydrogen evolution reaction and oxygen evolution reaction are first outlined.Then,versatile synthesis techniques for Co-P electrocatalysts are summarized,followed by advanced strategies to enhance the electrocatalytic performance of Co-P materials,including heteroatom doping,composite construction,integration with well-conductive sub-strates,and structure control from the viewpoint of experiment.Along with these optimization strategies,the understanding of the inherent mechanism of enhanced catalytic performance is also discussed.Finally,some existing challenges in the development of highly active and stable Co-P-based materials are clarified,and pro-spective directions for prompting the wide commercialization of water electrolysis technology are proposed.
基金support provided by the National Natural Science Foundation of China(Grant Nos.51972048,U23A20605)support provided by the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(Grant No.22567627H)the additional data in the revised manuscriptsupported by the National Key Research and Development Program of China(No.2022YFB3706300).
文摘High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.
基金financially supported by the National Natural Science Foundation of China(21975100).
文摘Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil fuels.Alkaline water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity hydrogen.Nevertheless,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment contamination.Therefore,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel foam.The synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline solution.Furthermore,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.
基金supported by the Natural Science Founda-tion of Chongqing(cstc2021jcyj-msxmX0420)Natural Science Foundation of Sichuan(2023NSFSC0088)。
文摘Hydrogen production from electrochemical water splitting is a promising strategy to generate green energy,which requires the development of efficient and stable electrocatalysts for the hydrogen evolution reaction and the oxygen evolution reaction(HER and OER).Ionic liquids(ILs)or poly(ionic liquids)(PILs),containing heteroatoms,metal-based anions,and various structures,have been frequently involved as precursors to prepare electrocatalysts for water splitting.Moreover,ILs/PILs possess high conductivity,wide electrochemical windows,and high thermal and chemical stability,which can be directly applied in the electrocatalysis process with high durability.In this review,we focus on the studies of ILs/PILs-derived electrocatalysts for HER and OER,where ILs/PILs are applied as heteroatom dopants and metal precursors to prepare catalysts or are directly utilized as the electrocatalysts.Due to those attractive properties,IL/PIL-derived electrocatalysts exhibit excellent performance for electrochemical water splitting.All these accomplishments and developments are systematically summarized and thoughtfully discussed.Then,the overall perspectives for the current challenges and future developments of ILs/PILs-derived electrocatalysts are provided.
基金supported by the National Natural Science Foundation of China(52174071,U1903216,52004052)the National Key R&D Program of China(2022YFC2903903).
文摘In order to understand the mechanical properties and the fracture surface roughness characteristics of thermally damaged granite under dynamic splitting,dynamic Brazilian splitting tests were conducted on granite samples after thermal treatment at 25,200,400,and 600℃.Results show that the dynamic peak splitting strength of thermally damaged granite samples increases with increasing strain rate,showing obvious strain‐rate sensitivity.With increasing temperature,thermally induced cracks in granite transform from intergranular cracks to intragranular cracks,and to a transgranular crack network.Thermally induced damages reduce the dynamic peak splitting strength and the maximum absorbed energy while increasing the peak radial strain.The fracture mode of the thermally damaged granite under dynamic loads is mode Ⅱ splitting failure.By using the axial roughness index Z2 a,the distribution ranges of the wedge‐shaped failure zones and the tensile failure zones in the fracture surfaces under dynamic Brazilian splitting can be effectively identified.The radial roughness index Z_(2)^(r)is sensitive to the strain rate and temperature.It shows a linear correlation with the peak splitting strength and the maximum absorbed energy and a linear negative correlation with the peak radial strain.Z_(2)^(r)can be used to quantitatively estimate the dynamic parameters based on the models proposed.