Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent year...Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.展开更多
Thermo-poro-mechanical responses along sliding zone/surface have been extensively studied.However,it has not been recognized that the potential contribution of other crucial engineering geological interfaces beyond th...Thermo-poro-mechanical responses along sliding zone/surface have been extensively studied.However,it has not been recognized that the potential contribution of other crucial engineering geological interfaces beyond the slip surface to progressive failure.Here,we aim to investigate the subsurface multiphysics of reservoir landslides under two extreme hydrologic conditions(i.e.wet and dry),particularly within sliding masses.Based on ultra-weak fiber Bragg grating(UWFBG)technology,we employ specialpurpose fiber optic sensing cables that can be implanted into boreholes as“nerves of the Earth”to collect data on soil temperature,water content,pore water pressure,and strain.The Xinpu landslide in the middle reach of the Three Gorges Reservoir Area in China was selected as a case study to establish a paradigm for in situ thermo-hydro-poro-mechanical monitoring.These UWFBG-based sensing cables were vertically buried in a 31 m-deep borehole at the foot of the landslide,with a resolution of 1 m except for the pressure sensor.We reported field measurements covering the period 2021 and 2022 and produced the spatiotemporal profiles throughout the borehole.Results show that wet years are more likely to motivate landslide motions than dry years.The annual thermally active layer of the landslide has a critical depth of roughly 9 m and might move downward in warmer years.The dynamic groundwater table is located at depths of 9e15 m,where the peaked strain undergoes a periodical response of leap and withdrawal to annual hydrometeorological cycles.These interface behaviors may support the interpretation of the contribution of reservoir regulation to slope stability,allowing us to correlate them to local damage events and potential global destabilization.This paper also offers a natural framework for interpreting thermo-hydro-poro-mechanical signatures from creeping reservoir bank slopes,which may form the basis for a landslide monitoring and early warning system.展开更多
The Jiangchuan Biota from the Jiucheng Member(Mb.)of the Dengying Formation(Fm.),discovered in Jiangchuan,eastern Yunnan,China,is marked by copious macrofossils at the apex of the Ediacaran strata.This fauna features ...The Jiangchuan Biota from the Jiucheng Member(Mb.)of the Dengying Formation(Fm.),discovered in Jiangchuan,eastern Yunnan,China,is marked by copious macrofossils at the apex of the Ediacaran strata.This fauna features benthic algae with varied holdfasts and other fossils of indeterminate taxonomic affinity and is compositionally unique compared to the Shibantan and Gaojiashan biotas of the Dengying Fm.and the Miaohe and Wenghui biotas of the Doushantuo Fm.,elsewhere in China.One novel benthic saccular macroalgal fossil,named here Houjiashania yuxiensis gen.and sp.nov.,from the Jiangchuan Biota is based on fossils that are sausage-shaped,elongate,tubular,ranging from 0.3 to 4 cm in length,and up to 0.8 cm in diameter.One terminus is blunt and rounded to an obtuse angle,the other is bent with a spread-out surface resembling a holdfast,suggesting a three-dimensional thallus.Thin,stipe-shaped outgrowths,likely vestiges of sessile saccular life forms,are prevalent in macroalgal fossils of analogous size and shape,as well as present brown algae Scytosiphonaceae,such as Colpomenia and Dactylosiphon.The new findings augment the diversity of benthic algae,such as those known from the Early Neoproterozoic Longfengshan Biota in North China.The benthic algal macrofossils in the Jiucheng Mb.add to knowledge of Late Ediacaran metaphyte diversification and offer more clues about the evolutionary positioning of primitive macroalgae.The co-occurrence of numerous planktonic and benthic multicellular algae and planktonic microbes might have facilitated ecologically the more extensive later Cambrian explosion evidenced by the Chengjiang Biota in Yunnan.展开更多
Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites...Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.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
Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performan...Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.展开更多
The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide incl...The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
Durable and efficient bi-functional catalyst,that is capable of both oxygen evolution reaction and hydrogen evolution reaction under acidic condition,are highly desired for the commercialization of proton exchange mem...Durable and efficient bi-functional catalyst,that is capable of both oxygen evolution reaction and hydrogen evolution reaction under acidic condition,are highly desired for the commercialization of proton exchange membrane water electrolysis.Herein,we report a robust L-Ru/HfO_(2)heterostructure constructed via confining crystalline Ru nanodomains by HfO_(2)matrix.When assembled with a proton exchange membrane,the bi-functional L-Ru/HfO_(2)catalyst-based electrolyzer presents a voltage of 1.57 and 1.67 V to reach 100 and 300 mA cm^(-2)current density,prevailing most of previously reported Ru-based materials as well as commercial Pt/C||RuO_(2)electrolyzer.It is revealed that the synergistic effect of HfO_(2)modification and small crystalline domain formation significantly alleviates the over-oxidation of Ru.More importantly,this synergistic effect facilitates a dual-site oxide path during the oxygen evolution procedure via optimization of the binding configurations of oxygenated adsorbates.As a result,the Ru active sites maintain the metallic state along with reduced energy barrier for the rate-determining step(^(*)O→^(*)OOH).Both of water adsorption and dissociation(Volmer step)are strengthened,while a moderate hydrogen binding is achieved to accelerate the hydrogen desorption procedure(Tafel step).Consequently,the activity and stability of acidic overall water splitting are simultaneously enhanced.展开更多
To investigate the mechanism of rockburst prevention by spraying water onto the surrounding rocks,15 experiments are performed considering different water absorption levels on a single face.High-speed photography and ...To investigate the mechanism of rockburst prevention by spraying water onto the surrounding rocks,15 experiments are performed considering different water absorption levels on a single face.High-speed photography and acoustic emission(AE)system are used to monitor the rockburst process.The effect of water on sandstone rockburst and the prevention mechanism of water on sandstone rockburst are analyzed from the perspective of energy and failure mode.The results show that the higher the ab-sorption degree,the lower the intensity of the rockburst after absorbing water on single side of sand-stone.This is reflected in the fact that with the increase in the water absorption level,the ejection velocity of rockburst fragments is smaller,the depth of the rockburst pit is shallower,and the AE energy is smaller.Under the water absorption level of 100%,the magnitude of rockburst intensity changes from medium to slight.The prevention mechanism of water on sandstone rockburst is that water reduces the capacity of sandstone to store strain energy and accelerates the expansion of shear cracks,which is not conducive to the occurrence of plate cracking before rockburst,and destroys the conditions for rockburst incubation.展开更多
The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional ...The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.展开更多
Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to wat...Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.展开更多
Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research ob...Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.展开更多
Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electr...Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.展开更多
Forty-five years after the Apollo and Luna missions, China’s Chang’e-5 (CE-5) mission collected ∼1.73 kg of new lunar materials from one ofthe youngest basalt units on the Moon. The CE-5 lunar samples provide oppor...Forty-five years after the Apollo and Luna missions, China’s Chang’e-5 (CE-5) mission collected ∼1.73 kg of new lunar materials from one ofthe youngest basalt units on the Moon. The CE-5 lunar samples provide opportunities to address some key scientific questions related to theMoon, including the discovery of high-pressure silica polymorphs (seifertite and stishovite) and a new lunar mineral, changesite-(Y). Seifertitewas found to be coexist with stishovite in a silica fragment from CE-5 lunar regolith. This is the first confirmed seifertite in returned lunarsamples. Seifertite has two space group symmetries (Pnc2 and Pbcn) and formed from an α-cristobalite-like phase during “cold” compressionduring a shock event. The aftershock heating process changes some seifertite to stishovite. Thus, this silica fragment records different stagesof an impact process, and the peak shock pressure is estimated to be ∼11 to 40 GPa, which is much lower than the pressure condition forcoexistence of seifertite and stishovite on the phase diagram. Changesite-(Y), with ideal formula (Ca_(8)Y)◻Fe^(2+)(PO_(4))_(7) (where ◻ denotes avacancy) is the first new lunar mineral to be discovered in CE-5 regolith samples. This newly identified phosphate mineral is in the form ofcolumnar crystals and was found in CE-5 basalt fragments. It contains high concentrations of Y and rare earth elements (REE), reaching upto ∼14 wt. % (Y,REE)2O3. The occurrence of changesite-(Y) marks the late-stage fractional crystallization processes of CE-5 basalts combinedwith silicate liquid immiscibility. These new findings demonstrate the significance of studies on high-pressure minerals in lunar materials andthe special nature of lunar magmatic evolution.展开更多
As an important factor that directly affects agricultural production, the social economy, and policy implementation,observed changes in dry/wet conditions have become a matter of widespread concern. However, previous ...As an important factor that directly affects agricultural production, the social economy, and policy implementation,observed changes in dry/wet conditions have become a matter of widespread concern. However, previous research has mainly focused on the long-term linear changes of dry/wet conditions, while the detection and evolution of the non-linear trends related to dry/wet changes have received less attention. The non-linear trends of the annual aridity index, obtained by the Ensemble Empirical Mode Decomposition(EEMD) method, reveal that changes in dry/wet conditions in China are asymmetric and can be characterized by contrasting features in both time and space in China. Spatially, most areas in western China have experienced transitions from drying to wetting, while opposite changes have occurred in most areas of eastern China. Temporally, the transitions occurred earlier in western China compared to eastern China. Research into the asymmetric spatial characteristics of dry/wet conditions compensates for the inadequacies of previous studies, which focused solely on temporal evolution;at the same time, it remedies the inadequacies of traditional research on linear trends over centennial timescales. Analyzing the non-linear trend also provides for a more comprehensive understanding of the drying/wetting changes in China.展开更多
We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resol...We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resolution transmission electron microscopy(HRTEM),and electron backscatter diffraction(EBSD).The findings reveal that annealing processing has a significant impact on diminishing residual stresses.As the annealing temperature rose from 950 to 1150℃,the majority of the residual stresses were relieved from 60.1 MPa down to 10.9 MPa.Moreover,the stress relaxation mechanism transitioned from being mainly controlled by dislocation slip to a combination of dislocation slip and grain boundary migration.Meanwhile,the annealing treatment promotes the decomposition of the Laves,accompanied by the precipitation ofμ-(Mo_(6)Co_(7))starting at 950℃ and reaching a maximum value at 1050℃.The tensile strength and plasticity of the annealing alloy at 1150℃ reached the maximum(1394 MPa,56.1%)which was 131%,200%fold than those of the as-cast alloy(1060 MPa,26.6%),but the oxidation process in the alloy was accelerated at 1150℃.The enhancement in durability and flexibility is primarily due to the dissolution of the brittle phase,along with the shape and dispersal of theγ′phase.展开更多
The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct ...The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.展开更多
High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion te...High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.展开更多
The development of effective antifreeze peptides to control ice growth has attracted a significant amount of attention yet still remains a great challenge.Here,we propose a novel design method based on in-depth invest...The development of effective antifreeze peptides to control ice growth has attracted a significant amount of attention yet still remains a great challenge.Here,we propose a novel design method based on in-depth investigation of repetitive motifs in various ice-binding proteins(IBPs)with evolution analysis.In this way,several peptides with notable antifreeze activity were developed.In particular,a designed antifreeze peptide named AVD exhibits ideal ice recrystallization inhibition(IRI),solubility,and biocompatibility,making it suitable for use as a cryoprotective agent(CPA).A mutation analysis and molecular dynamics(MD)simulations indicated that the Thr6 and Asn8 residues of the AVD peptide are fundamental to its ice-binding capacity,while the Ser18 residue can synergistically enhance their interaction with ice,revealing the antifreeze mechanism of AVD.Furthermore,to evaluate the cryoprotection potential of AVD,the peptide was successfully employed for the cryopreservation of various cells,which demonstrated significant post-freezing cell recovery.This work opens up a new avenue for designing antifreeze materials and provides peptide-based functional modules for synthetic biology.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51902101 and 21875203)the Natural Science Foundation of Hunan Province(Nos.2021JJ40044 and 2023JJ50287)Natural Science Foundation of Jiangsu Province(No.BK20201381).
文摘Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.
基金We acknowledge the funding support from the National Science Fund for Distinguished Young Scholars of National Natural Science Foundation of China(Grant No.42225702)the National Natural Science Foundation of China(Grant No.42077235).
文摘Thermo-poro-mechanical responses along sliding zone/surface have been extensively studied.However,it has not been recognized that the potential contribution of other crucial engineering geological interfaces beyond the slip surface to progressive failure.Here,we aim to investigate the subsurface multiphysics of reservoir landslides under two extreme hydrologic conditions(i.e.wet and dry),particularly within sliding masses.Based on ultra-weak fiber Bragg grating(UWFBG)technology,we employ specialpurpose fiber optic sensing cables that can be implanted into boreholes as“nerves of the Earth”to collect data on soil temperature,water content,pore water pressure,and strain.The Xinpu landslide in the middle reach of the Three Gorges Reservoir Area in China was selected as a case study to establish a paradigm for in situ thermo-hydro-poro-mechanical monitoring.These UWFBG-based sensing cables were vertically buried in a 31 m-deep borehole at the foot of the landslide,with a resolution of 1 m except for the pressure sensor.We reported field measurements covering the period 2021 and 2022 and produced the spatiotemporal profiles throughout the borehole.Results show that wet years are more likely to motivate landslide motions than dry years.The annual thermally active layer of the landslide has a critical depth of roughly 9 m and might move downward in warmer years.The dynamic groundwater table is located at depths of 9e15 m,where the peaked strain undergoes a periodical response of leap and withdrawal to annual hydrometeorological cycles.These interface behaviors may support the interpretation of the contribution of reservoir regulation to slope stability,allowing us to correlate them to local damage events and potential global destabilization.This paper also offers a natural framework for interpreting thermo-hydro-poro-mechanical signatures from creeping reservoir bank slopes,which may form the basis for a landslide monitoring and early warning system.
基金supported by the National Natural Science Foundation of China(Grant Nos.42172035,42062005 and 41572024)the China Geological Survey(Grant No.DD20221648)+1 种基金Yunnan Province Science and Technology Department(Grant No.202305AD160031,202401AT070012)the project entitled 1:50000 Regional Geological Survey of Dazhuang,Fabiao,Ditu,and Dianzhong Sheets in Yunnan Province(Grant No.D202207).
文摘The Jiangchuan Biota from the Jiucheng Member(Mb.)of the Dengying Formation(Fm.),discovered in Jiangchuan,eastern Yunnan,China,is marked by copious macrofossils at the apex of the Ediacaran strata.This fauna features benthic algae with varied holdfasts and other fossils of indeterminate taxonomic affinity and is compositionally unique compared to the Shibantan and Gaojiashan biotas of the Dengying Fm.and the Miaohe and Wenghui biotas of the Doushantuo Fm.,elsewhere in China.One novel benthic saccular macroalgal fossil,named here Houjiashania yuxiensis gen.and sp.nov.,from the Jiangchuan Biota is based on fossils that are sausage-shaped,elongate,tubular,ranging from 0.3 to 4 cm in length,and up to 0.8 cm in diameter.One terminus is blunt and rounded to an obtuse angle,the other is bent with a spread-out surface resembling a holdfast,suggesting a three-dimensional thallus.Thin,stipe-shaped outgrowths,likely vestiges of sessile saccular life forms,are prevalent in macroalgal fossils of analogous size and shape,as well as present brown algae Scytosiphonaceae,such as Colpomenia and Dactylosiphon.The new findings augment the diversity of benthic algae,such as those known from the Early Neoproterozoic Longfengshan Biota in North China.The benthic algal macrofossils in the Jiucheng Mb.add to knowledge of Late Ediacaran metaphyte diversification and offer more clues about the evolutionary positioning of primitive macroalgae.The co-occurrence of numerous planktonic and benthic multicellular algae and planktonic microbes might have facilitated ecologically the more extensive later Cambrian explosion evidenced by the Chengjiang Biota in Yunnan.
基金the financial support from the Natural Science Foundation of China(Grant No.52172106)Anhui Provincial Natural Science Foundation(Grant Nos.2108085QB60 and 2108085QB61)China Postdoctoral Science Foundation(Grant Nos.2020M682057 and 2023T160651).
文摘Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.
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funded by the National Natural Science Foundation of China (NSFC) (Nos. 22221001, 22201115, 21931001, and 21922105)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX–04)+3 种基金the 111 Project (B20027)by the Fundamental Research Funds for the Central Universities (lzujbky-2023-eyt03)support Natural Science Foundation of Gansu Providence (22JR5RA540)Gansu Province Youth Science and Technology Talent Promotion Project (GXH202220530-02)。
文摘Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.
基金Agency for Science,Technology and Research(A*STAR),under the RIE2020 Advanced Manufacturing and Engineering(AME)Programmatic Grant(Grant no.A18B1b0061)。
文摘The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金supported by the National Natural Science Foundation of China(Grant No.22279162,22261142664)Natural Science Fund for Colleges and Universities in Anhui Province(2022AH030057)CAS Project for Young Scientists in Basic Research(No.YSBR-094).
文摘Durable and efficient bi-functional catalyst,that is capable of both oxygen evolution reaction and hydrogen evolution reaction under acidic condition,are highly desired for the commercialization of proton exchange membrane water electrolysis.Herein,we report a robust L-Ru/HfO_(2)heterostructure constructed via confining crystalline Ru nanodomains by HfO_(2)matrix.When assembled with a proton exchange membrane,the bi-functional L-Ru/HfO_(2)catalyst-based electrolyzer presents a voltage of 1.57 and 1.67 V to reach 100 and 300 mA cm^(-2)current density,prevailing most of previously reported Ru-based materials as well as commercial Pt/C||RuO_(2)electrolyzer.It is revealed that the synergistic effect of HfO_(2)modification and small crystalline domain formation significantly alleviates the over-oxidation of Ru.More importantly,this synergistic effect facilitates a dual-site oxide path during the oxygen evolution procedure via optimization of the binding configurations of oxygenated adsorbates.As a result,the Ru active sites maintain the metallic state along with reduced energy barrier for the rate-determining step(^(*)O→^(*)OOH).Both of water adsorption and dissociation(Volmer step)are strengthened,while a moderate hydrogen binding is achieved to accelerate the hydrogen desorption procedure(Tafel step).Consequently,the activity and stability of acidic overall water splitting are simultaneously enhanced.
基金The financial support from the National Natural Science Foun-dation of China(Grant Nos.52074299 and 41941018)the Fundamental Research Funds for the Central Universities of China(Grant No.2023JCCXSB02)are gratefully acknowledged.
文摘To investigate the mechanism of rockburst prevention by spraying water onto the surrounding rocks,15 experiments are performed considering different water absorption levels on a single face.High-speed photography and acoustic emission(AE)system are used to monitor the rockburst process.The effect of water on sandstone rockburst and the prevention mechanism of water on sandstone rockburst are analyzed from the perspective of energy and failure mode.The results show that the higher the ab-sorption degree,the lower the intensity of the rockburst after absorbing water on single side of sand-stone.This is reflected in the fact that with the increase in the water absorption level,the ejection velocity of rockburst fragments is smaller,the depth of the rockburst pit is shallower,and the AE energy is smaller.Under the water absorption level of 100%,the magnitude of rockburst intensity changes from medium to slight.The prevention mechanism of water on sandstone rockburst is that water reduces the capacity of sandstone to store strain energy and accelerates the expansion of shear cracks,which is not conducive to the occurrence of plate cracking before rockburst,and destroys the conditions for rockburst incubation.
基金financial support from the National Natural Science Foundation of China (52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing (STRZ202203)the financial support provided by the China Scholarship Council (CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship,Australia。
文摘The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.
基金supported by the Australian Research Council (DE220100521 and DP200101217)supported by Fellow research grant of National University of Mongolia (No.P2021-4197)+2 种基金the support of Griffith University internal grantssupport from King Abdullah University of Science and Technology (KAUST)through the Ibn Rushd Postdoctoral Fellowship Awardsupport from the US Office of Naval Research (ONR),Office of Naval Research Global (ONRG)under the grant N62909-23-1-2035。
文摘Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.
基金Under the auspices of National Natural Science Foundation of China(No.42171230)。
文摘Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Excellent Scholars and Innovation Team of Guangxi Universities,the Innovation Project of Guangxi Graduate Education(YCBZ2022038)the High-performance Computing Platform of Guangxi University.
文摘Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.
基金supported by the B-Type Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB 41000000)the National Natural Science Foundation of China(Grant Nos.41773052,41973058,and 42003054)+2 种基金the Key Research Program of the Chinese Academy of Sciences(Grant No.ZDBS-SSWJSC007-10)the Pre-Research Project on Civil Aerospace Technologies funded by the CNSA(Grant No.D020201)the China Postdoctoral Science Foundation(Grant No.2020M680155).
文摘Forty-five years after the Apollo and Luna missions, China’s Chang’e-5 (CE-5) mission collected ∼1.73 kg of new lunar materials from one ofthe youngest basalt units on the Moon. The CE-5 lunar samples provide opportunities to address some key scientific questions related to theMoon, including the discovery of high-pressure silica polymorphs (seifertite and stishovite) and a new lunar mineral, changesite-(Y). Seifertitewas found to be coexist with stishovite in a silica fragment from CE-5 lunar regolith. This is the first confirmed seifertite in returned lunarsamples. Seifertite has two space group symmetries (Pnc2 and Pbcn) and formed from an α-cristobalite-like phase during “cold” compressionduring a shock event. The aftershock heating process changes some seifertite to stishovite. Thus, this silica fragment records different stagesof an impact process, and the peak shock pressure is estimated to be ∼11 to 40 GPa, which is much lower than the pressure condition forcoexistence of seifertite and stishovite on the phase diagram. Changesite-(Y), with ideal formula (Ca_(8)Y)◻Fe^(2+)(PO_(4))_(7) (where ◻ denotes avacancy) is the first new lunar mineral to be discovered in CE-5 regolith samples. This newly identified phosphate mineral is in the form ofcolumnar crystals and was found in CE-5 basalt fragments. It contains high concentrations of Y and rare earth elements (REE), reaching upto ∼14 wt. % (Y,REE)2O3. The occurrence of changesite-(Y) marks the late-stage fractional crystallization processes of CE-5 basalts combinedwith silicate liquid immiscibility. These new findings demonstrate the significance of studies on high-pressure minerals in lunar materials andthe special nature of lunar magmatic evolution.
基金supported by the National key research and development program (2019YFA0607104)National Natural Science Foundation of China (Grant Nos. 41991231, 42275034, 41975076, 42075029, 42075017, and 42075018)the Gansu Provincial Science and Technology Project (22JR5RA405)。
文摘As an important factor that directly affects agricultural production, the social economy, and policy implementation,observed changes in dry/wet conditions have become a matter of widespread concern. However, previous research has mainly focused on the long-term linear changes of dry/wet conditions, while the detection and evolution of the non-linear trends related to dry/wet changes have received less attention. The non-linear trends of the annual aridity index, obtained by the Ensemble Empirical Mode Decomposition(EEMD) method, reveal that changes in dry/wet conditions in China are asymmetric and can be characterized by contrasting features in both time and space in China. Spatially, most areas in western China have experienced transitions from drying to wetting, while opposite changes have occurred in most areas of eastern China. Temporally, the transitions occurred earlier in western China compared to eastern China. Research into the asymmetric spatial characteristics of dry/wet conditions compensates for the inadequacies of previous studies, which focused solely on temporal evolution;at the same time, it remedies the inadequacies of traditional research on linear trends over centennial timescales. Analyzing the non-linear trend also provides for a more comprehensive understanding of the drying/wetting changes in China.
基金This work was financially supported by the National Science and Technology Major Project of China(No.J2019-VI-0006-0120)the National Key R&D Program of China(No.2021YFB3700402)the National Natural Science Foundation of China(Nos.52074092 and 52274330).
文摘We discussed the decrease in residual stress,precipitation evolution,and mechanical properties of GH4151 alloy in different annealing temperatures,which were studied by the scanning electron microscope(SEM),high-resolution transmission electron microscopy(HRTEM),and electron backscatter diffraction(EBSD).The findings reveal that annealing processing has a significant impact on diminishing residual stresses.As the annealing temperature rose from 950 to 1150℃,the majority of the residual stresses were relieved from 60.1 MPa down to 10.9 MPa.Moreover,the stress relaxation mechanism transitioned from being mainly controlled by dislocation slip to a combination of dislocation slip and grain boundary migration.Meanwhile,the annealing treatment promotes the decomposition of the Laves,accompanied by the precipitation ofμ-(Mo_(6)Co_(7))starting at 950℃ and reaching a maximum value at 1050℃.The tensile strength and plasticity of the annealing alloy at 1150℃ reached the maximum(1394 MPa,56.1%)which was 131%,200%fold than those of the as-cast alloy(1060 MPa,26.6%),but the oxidation process in the alloy was accelerated at 1150℃.The enhancement in durability and flexibility is primarily due to the dissolution of the brittle phase,along with the shape and dispersal of theγ′phase.
基金supported by the Taishan Scholar Program of Shandong Province,China (tsqn202211162)the National Natural Science Foundation of China (22102079)the Natural Science Foundation of Shandong Province of China (ZR2021YQ10,ZR2022QB163)。
文摘The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.
基金the staff at Beamline (BL08U1-A and BL11B)of the Shanghai Synchrotron Radiation Facility (SSRF)the support from the National Key Research&Development Program of China (2022YFB3803700)+2 种基金the National Natural Science Foundation of China (52171186)the support through the Overseas Outstanding Youth Fund and Shanghai Pujiang Talent Project (21PJ1408500)the financial support from the Center of Hydrogen Science,Shanghai Jiao Tong University。
文摘High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.
基金supported by the National Key Research and Development Program of China (2021YFC2100800)the National Natural Science Foundation of China (22078238,21961132005,and 21908160)+1 种基金the Open Funding Project of the National Key Laboratory of Biochemical Engineeringthe Program of Introducing Talents of Discipline to Universities (BP0618007)。
文摘The development of effective antifreeze peptides to control ice growth has attracted a significant amount of attention yet still remains a great challenge.Here,we propose a novel design method based on in-depth investigation of repetitive motifs in various ice-binding proteins(IBPs)with evolution analysis.In this way,several peptides with notable antifreeze activity were developed.In particular,a designed antifreeze peptide named AVD exhibits ideal ice recrystallization inhibition(IRI),solubility,and biocompatibility,making it suitable for use as a cryoprotective agent(CPA).A mutation analysis and molecular dynamics(MD)simulations indicated that the Thr6 and Asn8 residues of the AVD peptide are fundamental to its ice-binding capacity,while the Ser18 residue can synergistically enhance their interaction with ice,revealing the antifreeze mechanism of AVD.Furthermore,to evaluate the cryoprotection potential of AVD,the peptide was successfully employed for the cryopreservation of various cells,which demonstrated significant post-freezing cell recovery.This work opens up a new avenue for designing antifreeze materials and provides peptide-based functional modules for synthetic biology.