Hydrogen peroxide(H_(2)O_(2)),an environmentally friendly chemical with high value,is extensively used in industrial production and daily life.However,the traditional anthraquinone method for H_(2)O_(2) production is ...Hydrogen peroxide(H_(2)O_(2)),an environmentally friendly chemical with high value,is extensively used in industrial production and daily life.However,the traditional anthraquinone method for H_(2)O_(2) production is associated with a highly energy-consuming and heavily polluting process.Solor-driven photocatalytic evolution of H_(2)O_(2) is a promising,eco-friendly,and energy-efficient strategy that holds great potential to substitute the traditional approach.Here,a ternary photocatalyst,NiS/CdS/Halloysite nanotubes(NiS/CdS/HNTs)is designed and prepared with an earth-abundant clay mineral HNTs as the support and NiS as a co-catalyst.The pivotal roles of HNTs and NiS in the photocatalytic process are elucidated by experiments and theoretical calculations.HNTs serve as the carrier,which allows CdS to be uniformly dispersed onto its surface as small particles,increasing effective contact with H_(2)O and O_(2) for H_(2)O_(2) formation.Simultaneously,it resulted in the formation of a Schottky junction between NiS and CdS,which not only favors photogenerated charges separating efficiently but also provides a unidirectional path to transfer electrons.Consequently,the optimized NiS/CdS/HNTs composite demonstrates an H_(2)O_(2) evolution rate of 380.5μmol·g^(-1)·h^(-1) without adding any sacrificial agent or extra O_(2),nearly 5.0 times that of pure CdS.This work suggests a feasible idea for designing and developing highly active and low-cost solar energy catalytic composite materials.展开更多
Ni−Co−C alloy coatings with exceptional properties were fabricated via electrodeposition using an ammonium oxalate−ammonium citrate system.The optimized coatings exhibited dense crystallization with a distinct granula...Ni−Co−C alloy coatings with exceptional properties were fabricated via electrodeposition using an ammonium oxalate−ammonium citrate system.The optimized coatings exhibited dense crystallization with a distinct granular surface,where large particles were covered with nanoscale clusters.Additionally,C atoms primarily existed within the coatings as a solid solution,maintaining the FCC structures.Compared to binary Ni−Co coatings,the Ni−Co−C alloy coatings exhibited significantly improved hardness,wear resistance,and adhesion strength,which could be attributed to the potential strengthening effect of the C atoms.Specifically,the introduction of C atoms optimized the local charge density and electron distribution in the alloy,transforming local weak ionic bonds into strong covalent interactions,thereby enhancing the bonding capability between the corresponding atoms in the NiCo bulk.展开更多
Owing to the complexity of droughts,detailed assessments of drought events have become a key issue in water resource management and planning.In this study,three-dimensional copula models at Standard Precipitation Evap...Owing to the complexity of droughts,detailed assessments of drought events have become a key issue in water resource management and planning.In this study,three-dimensional copula models at Standard Precipitation Evapotranspiration Index(SPEI)-1,SPEI-3,SPEI-6,and SPEI-12 were used to assess drought risks in the Haihe River Basin(HRB)of China from 1961–2020.Drought duration,severity,and peak,as indicated by SPEI,were extracted based on run theory and fitted with suitable marginal distributions.The difference between the joint return period(Tor)and the co-occurrence return period(Tand)could explain the intrinsic correlation between drought characteristics.The smaller the difference,the stronger the correlation.The results showed that droughts in the north-western region of the HRB were characterized by high peak,intense severity,and long duration.In contrast,the eastern region exhibited a higher frequency of drought occurrence.Furthermore,the decreasing trend in precipitation dominated droughts,and topography of the northwest region creates the features of low annual precipitation with more days of precipitation.The drought events in the HRB were influenced by the phase shift between El Niño and La Niña.There was a strong negative phase coupling between SPEI-12 and Niño3.4(R^(2)≥0.77).The transition from La Niña to El Niño was responsible for severe droughts in the HRB.The El Niño-Southern Oscillation could predict droughts with lag times of 0.15–4.35 mon in mountainous areas.展开更多
Marine heatwaves(MHWs)have become increasingly frequent and persistent in the context of global warming and the related underlying mechanisms are strongly region-dependent.We employed the NOAA(National Oceanic and Atm...Marine heatwaves(MHWs)have become increasingly frequent and persistent in the context of global warming and the related underlying mechanisms are strongly region-dependent.We employed the NOAA(National Oceanic and Atmospheric Administration)CRW(Coral Reef Watch)daily mean sea surface temperature dataset spanning from 1985 to 2022 to comprehensively analyze the fundamental attributes and evolving patterns of marine heatwaves in the offshore waters of China.Eight pronounced marine heatwaves from frequently affected sensitive regions were investigated to explore their formation mechanisms.The relationship between the occurrences of marine heatwave and large-scale climate mode in the region was explored.Results show that the western Pacific subtropical high plays an essential role in triggering marine heatwaves in Chinese offshore waters,with an anomalous downward shortwave radiation flux acting to warm the sea surface,which is remotely associated to the large-scale sea surface temperature state.Distinct mechanisms for the MHWs were identified in the northern and southern offshore waters of China.MHWs in high latitudes(such as the Bohai Sea and the Yellow Sea)mainly occur during the negative phase of the Pacific Decadal Oscillation(PDO),while those in low latitudes(such as the South China Sea)are more common in about 5-month lags behind the El Niño,for which we purposed a mechanism to describe the main differences in the formation of MHWs in China and discussed the related implications.展开更多
Flash drought is characterized by a period of rapid drought intensification with impacts on agriculture,water resources,ecosystems,and human environment.In the Qilian Mountains,northwestern China,flash droughts are be...Flash drought is characterized by a period of rapid drought intensification with impacts on agriculture,water resources,ecosystems,and human environment.In the Qilian Mountains,northwestern China,flash droughts are becoming more frequently due to the global climate warming.However,the spatiotemporal variations and their driving factors of flash droughts are not clear in this region.In this study,the European Centre for Medium-range Weather Forecasts(ECMWF)Reanalysis v5-Land(ERA5-Land)dataset was utilized to identify two types of flash drought events(heatwave-induced and water scarcity-induced flash drought events)that occurred in the growing season(April‒September)during 1981-2020 in this area.The results showed that the frequency of heatwave-induced flash droughts has decreased since 2010,while the frequency of water scarcity-induced flash droughts has declined markedly.Spatially,heatwave-induced flash droughts were predominantly concentrated in the western Qilian Mountains,whereas water scarcity-induced flash droughts were primarily concentrated in the central and eastern Qilian Mountains.A significantly increasing temporal trend in both types of flash droughts in the eastern Qilian Mountains was found.Meanwhile,there was a decreasing temporal trend of heatwave-induced flash droughts in the southwestern part of the region.Additionally,the influence of two major atmospheric modes,i.e.,the El Niño‒Southern Oscillation(ENSO)and North Atlantic Oscillation(NAO),on these two types of flash droughts was explored by the Superposed Epoch Analysis.The ENSO mainly influences flash droughts in the central and eastern parts of the Qilian Mountains by altering the strength of the East Asian monsoon,while the NAO mainly affects flash droughts in the entire parts of the Qilian Mountains by inducing anomalous westerlies activity.Our findings have important implications for predicting the evolution of flash drought events in the Qilian Mountains region under continued climate warming.展开更多
In 2023,the majority of the Earth witnessed its warmest boreal summer and autumn since 1850.Whether 2023 will indeed turn out to be the warmest year on record and what caused the astonishingly large margin of warming ...In 2023,the majority of the Earth witnessed its warmest boreal summer and autumn since 1850.Whether 2023 will indeed turn out to be the warmest year on record and what caused the astonishingly large margin of warming has become one of the hottest topics in the scientific community and is closely connected to the future development of human society.We analyzed the monthly varying global mean surface temperature(GMST)in 2023 and found that the globe,the land,and the oceans in 2023 all exhibit extraordinary warming,which is distinct from any previous year in recorded history.Based on the GMST statistical ensemble prediction model developed at the Institute of Atmospheric Physics,the GMST in 2023 is predicted to be 1.41℃±0.07℃,which will certainly surpass that in 2016 as the warmest year since 1850,and is approaching the 1.5℃ global warming threshold.Compared to 2022,the GMST in 2023 will increase by 0.24℃,with 88%of the increment contributed by the annual variability as mostly affected by El Niño.Moreover,the multidecadal variability related to the Atlantic Multidecadal Oscillation(AMO)in 2023 also provided an important warming background for sparking the GMST rise.As a result,the GMST in 2023 is projected to be 1.15℃±0.07℃,with only a 0.02℃ increment,if the effects of natural variability—including El Niño and the AMO—are eliminated and only the global warming trend is considered.展开更多
Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehic...Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible capacity.Herein,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic.Specifically,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff voltage.Furthermore,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal architecture.Whereas,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated polarization.Notably,Co-free NM can exhibit better safety performance than that of NCM cathode.These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.展开更多
MgH_(2),albeit with slow desorption kinetics,has been extensively studied as one of the most ideal solid hydrogen storage materials.Adding such catalyst as Ni can improve the desorption kinetics of MgH_(2),whereas the...MgH_(2),albeit with slow desorption kinetics,has been extensively studied as one of the most ideal solid hydrogen storage materials.Adding such catalyst as Ni can improve the desorption kinetics of MgH_(2),whereas the catalytic role has been attributed to different substances such as Ni,Mg_(2)Ni,Mg_(2)NiH0.3,and Mg_(2)NiH4.In the present study,Ni nanoparticles(Ni-NPs)supported on mesoporous carbon(Ni@C)have been synthesized to improve the hydrogen desorption kinetics of MgH_(2).The utilization of Ni@C largely decreases the dehydrogenation activation energy from 176.9 to 79.3 kJ mol^(−1) and the peak temperature of dehydrogenation from 375.5 to 235℃.The mechanism of Ni catalyst is well examined by advanced aberration-corrected environmental transmission electron microscopy and/or x-ray diffraction.During the first dehydrogenation,detailed microstructural studies reveal that the decomposition of MgH_(2)is initially triggered by the Ni-NPs,which is the rate-limiting step.Subsequently,the generated Mg reacts rapidly with Ni-NPs to form Mg_(2)Ni,which further promotes the dehydrogenation of residual MgH_(2).In the following dehydrogenation cycle,Mg_(2)NiH4 can rapidly decompose into Mg_(2)Ni,which continuously promotes the decomposition of MgH_(2).Our study not only elucidates the mechanism of Ni catalyst but also helps design and assemble catalysts with improved dehydriding kinetics of MgH_(2).展开更多
To explain the recent three-year La Niña event from 2020 to 2022,which has caused catastrophic weather events worldwide,Fasullo et al.(2023)demonstrated that the increase in biomass aerosol resulting from the 201...To explain the recent three-year La Niña event from 2020 to 2022,which has caused catastrophic weather events worldwide,Fasullo et al.(2023)demonstrated that the increase in biomass aerosol resulting from the 2019-20 Australian wildfire season could have triggered this multi-year La Niña.Here,we present compelling evidence from paleo-proxies,utilizing a substantial sample size of 26 volcanic eruptions in the Southern Hemisphere(SH),to support the hypothesis that ocean cooling in the SH can lead to a multi-year La Niña event.This research highlights the importance of focusing on the Southern Ocean,as current climate models struggle to accurately simulate the Pacific response driven by the Southern Ocean.展开更多
The aging embrittlement of 30Cr2Ni4MoV steel during service at high temperature has been attributed to the segregation of Si and Mn at grain boundary(GB).We report an alternative mechanism of aging embrittlement of 30...The aging embrittlement of 30Cr2Ni4MoV steel during service at high temperature has been attributed to the segregation of Si and Mn at grain boundary(GB).We report an alternative mechanism of aging embrittlement of 30Cr2Ni4MoV steel.Using atom probe tomography,it is found that the quenched and tempered(QT)30Cr2Ni4MoV steel has already contained obvious Si and Mn segregations at GB,which means that the Si and Mn segregations at GB are not sufficient to induce aging embrittlement.It is discovered for the first time in aged 30Cr2Ni4MoV there newly precipitate many G-phases along GB,and Si and Mn segregations at GB of QT30Cr2Ni4MoV steel are the main reason for the precipitation of G-phase.The hard and brittle G-phase helps to promote crack initiation during impact deformation.Subsequently,the cracks can rapidly propagate along GB due to the distribution of G-phase and the segregation of Si and Mn along the GB,which leads to intergranular cracking and low impact energy as for aged 30Cr2Ni4MoV steel.展开更多
NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the mic...NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the microstructures of the g-C3N4 photocatalysts.In this study,a facile and low-temperature（80 ℃） impregnation method was developed to prepare NiS2/g-C3N4 photocatalysts.First,the g-C3N4 powders were processed by the hydrothermal method in order to introduce oxygen-containing functional groups（such as-OH and-C0NH-） to the surface of g-C3N4.Then,the Ni^2＋ ions could be adsorbed near the g-C3N4 via strong electrostatic interaction between g-C3N4 and Ni^2＋ ions upon the addition of Ni（NO3）2 solution.Finally,NiS2 nanoparticles were formed on the surface of g-C3N4 upon the addition of TAA.It was found that the NiS2 nanoparticles were solidly and homogeneously grafted on the surface of g-C3N4,resulting in greatly improved photocatalytic H2production.When the amount of NiS2 was 3 wt%,the resultant NiS2/g-C3N4 photocatalyst showed the highest H2 evolution rate（116.343 μmol h^-1 g^-1）,which is significantly higher than that of the pure g-C3N4（3 μmol h^-1 g^-1）.Moreover,the results of a recycling test for the NiS2/g-C3N4（3 wt%）sample showed that this sample could maintain a stable and effective photocatalytic H2-evolution performance under visible-light irradiation.Based on the above results,a possible mechanism of the improved photocatalytic performance was proposed for the presented NiS2/g-C3N4 photocatalysts,in which the photogenerated electrons of g-C3N4 can be rapidly transferred to the NiS2 nanoparticles via the close and continuous contact between them;then,the photogenerated electrons rapidly react with H2O adsorbed on the surface of NiS2,which has a surficial metallic character and high catalytic activity,to produce H2.Considering the mild and facile synthesis method,the presented low-cost and highly efficient NiS2-modified g-C3N4 photocatalysts would have great potential for practical use in photocatalytic H2 production.展开更多
文摘Hydrogen peroxide(H_(2)O_(2)),an environmentally friendly chemical with high value,is extensively used in industrial production and daily life.However,the traditional anthraquinone method for H_(2)O_(2) production is associated with a highly energy-consuming and heavily polluting process.Solor-driven photocatalytic evolution of H_(2)O_(2) is a promising,eco-friendly,and energy-efficient strategy that holds great potential to substitute the traditional approach.Here,a ternary photocatalyst,NiS/CdS/Halloysite nanotubes(NiS/CdS/HNTs)is designed and prepared with an earth-abundant clay mineral HNTs as the support and NiS as a co-catalyst.The pivotal roles of HNTs and NiS in the photocatalytic process are elucidated by experiments and theoretical calculations.HNTs serve as the carrier,which allows CdS to be uniformly dispersed onto its surface as small particles,increasing effective contact with H_(2)O and O_(2) for H_(2)O_(2) formation.Simultaneously,it resulted in the formation of a Schottky junction between NiS and CdS,which not only favors photogenerated charges separating efficiently but also provides a unidirectional path to transfer electrons.Consequently,the optimized NiS/CdS/HNTs composite demonstrates an H_(2)O_(2) evolution rate of 380.5μmol·g^(-1)·h^(-1) without adding any sacrificial agent or extra O_(2),nearly 5.0 times that of pure CdS.This work suggests a feasible idea for designing and developing highly active and low-cost solar energy catalytic composite materials.
基金supported by the National Natural Science Foundation of China(Nos.52274320,52074053)。
文摘Ni−Co−C alloy coatings with exceptional properties were fabricated via electrodeposition using an ammonium oxalate−ammonium citrate system.The optimized coatings exhibited dense crystallization with a distinct granular surface,where large particles were covered with nanoscale clusters.Additionally,C atoms primarily existed within the coatings as a solid solution,maintaining the FCC structures.Compared to binary Ni−Co coatings,the Ni−Co−C alloy coatings exhibited significantly improved hardness,wear resistance,and adhesion strength,which could be attributed to the potential strengthening effect of the C atoms.Specifically,the introduction of C atoms optimized the local charge density and electron distribution in the alloy,transforming local weak ionic bonds into strong covalent interactions,thereby enhancing the bonding capability between the corresponding atoms in the NiCo bulk.
基金Under the auspices of the Shandong Provincial Natural Science Foundation(No.ZR2024ME171,ZR2024QD207)the National Natural Science Foundation of China(No.41471160,42377077)。
文摘Owing to the complexity of droughts,detailed assessments of drought events have become a key issue in water resource management and planning.In this study,three-dimensional copula models at Standard Precipitation Evapotranspiration Index(SPEI)-1,SPEI-3,SPEI-6,and SPEI-12 were used to assess drought risks in the Haihe River Basin(HRB)of China from 1961–2020.Drought duration,severity,and peak,as indicated by SPEI,were extracted based on run theory and fitted with suitable marginal distributions.The difference between the joint return period(Tor)and the co-occurrence return period(Tand)could explain the intrinsic correlation between drought characteristics.The smaller the difference,the stronger the correlation.The results showed that droughts in the north-western region of the HRB were characterized by high peak,intense severity,and long duration.In contrast,the eastern region exhibited a higher frequency of drought occurrence.Furthermore,the decreasing trend in precipitation dominated droughts,and topography of the northwest region creates the features of low annual precipitation with more days of precipitation.The drought events in the HRB were influenced by the phase shift between El Niño and La Niña.There was a strong negative phase coupling between SPEI-12 and Niño3.4(R^(2)≥0.77).The transition from La Niña to El Niño was responsible for severe droughts in the HRB.The El Niño-Southern Oscillation could predict droughts with lag times of 0.15–4.35 mon in mountainous areas.
基金Supported by the National Natural Science Foundation of China(No.41905089)the Laoshan Laboratory(No.LSKJ202202404)+1 种基金the Startup Foundation for Introducing Talent of NUIST,Jiangsu Innovation Research Group(No.JSSCTD202346)the Undergraduates Innovation and Entrepreneurship Training Program of Jiangsu Province(No.202310300087Y)。
文摘Marine heatwaves(MHWs)have become increasingly frequent and persistent in the context of global warming and the related underlying mechanisms are strongly region-dependent.We employed the NOAA(National Oceanic and Atmospheric Administration)CRW(Coral Reef Watch)daily mean sea surface temperature dataset spanning from 1985 to 2022 to comprehensively analyze the fundamental attributes and evolving patterns of marine heatwaves in the offshore waters of China.Eight pronounced marine heatwaves from frequently affected sensitive regions were investigated to explore their formation mechanisms.The relationship between the occurrences of marine heatwave and large-scale climate mode in the region was explored.Results show that the western Pacific subtropical high plays an essential role in triggering marine heatwaves in Chinese offshore waters,with an anomalous downward shortwave radiation flux acting to warm the sea surface,which is remotely associated to the large-scale sea surface temperature state.Distinct mechanisms for the MHWs were identified in the northern and southern offshore waters of China.MHWs in high latitudes(such as the Bohai Sea and the Yellow Sea)mainly occur during the negative phase of the Pacific Decadal Oscillation(PDO),while those in low latitudes(such as the South China Sea)are more common in about 5-month lags behind the El Niño,for which we purposed a mechanism to describe the main differences in the formation of MHWs in China and discussed the related implications.
基金supported by the National Natural Science Foundation of China(42477481,42477483)the Science and Technology Program in Gansu Province(23JRRA599)the Chinese Academy of Sciences(CAS)"Light of West China"Program.
文摘Flash drought is characterized by a period of rapid drought intensification with impacts on agriculture,water resources,ecosystems,and human environment.In the Qilian Mountains,northwestern China,flash droughts are becoming more frequently due to the global climate warming.However,the spatiotemporal variations and their driving factors of flash droughts are not clear in this region.In this study,the European Centre for Medium-range Weather Forecasts(ECMWF)Reanalysis v5-Land(ERA5-Land)dataset was utilized to identify two types of flash drought events(heatwave-induced and water scarcity-induced flash drought events)that occurred in the growing season(April‒September)during 1981-2020 in this area.The results showed that the frequency of heatwave-induced flash droughts has decreased since 2010,while the frequency of water scarcity-induced flash droughts has declined markedly.Spatially,heatwave-induced flash droughts were predominantly concentrated in the western Qilian Mountains,whereas water scarcity-induced flash droughts were primarily concentrated in the central and eastern Qilian Mountains.A significantly increasing temporal trend in both types of flash droughts in the eastern Qilian Mountains was found.Meanwhile,there was a decreasing temporal trend of heatwave-induced flash droughts in the southwestern part of the region.Additionally,the influence of two major atmospheric modes,i.e.,the El Niño‒Southern Oscillation(ENSO)and North Atlantic Oscillation(NAO),on these two types of flash droughts was explored by the Superposed Epoch Analysis.The ENSO mainly influences flash droughts in the central and eastern parts of the Qilian Mountains by altering the strength of the East Asian monsoon,while the NAO mainly affects flash droughts in the entire parts of the Qilian Mountains by inducing anomalous westerlies activity.Our findings have important implications for predicting the evolution of flash drought events in the Qilian Mountains region under continued climate warming.
基金supported by the Key Research Program of Frontier Sciences,Chinese Academy of Sciences(Grant No.ZDBS-LY-DQC010)the National Natural Science Foundation of China(Grant No.42175045).
文摘In 2023,the majority of the Earth witnessed its warmest boreal summer and autumn since 1850.Whether 2023 will indeed turn out to be the warmest year on record and what caused the astonishingly large margin of warming has become one of the hottest topics in the scientific community and is closely connected to the future development of human society.We analyzed the monthly varying global mean surface temperature(GMST)in 2023 and found that the globe,the land,and the oceans in 2023 all exhibit extraordinary warming,which is distinct from any previous year in recorded history.Based on the GMST statistical ensemble prediction model developed at the Institute of Atmospheric Physics,the GMST in 2023 is predicted to be 1.41℃±0.07℃,which will certainly surpass that in 2016 as the warmest year since 1850,and is approaching the 1.5℃ global warming threshold.Compared to 2022,the GMST in 2023 will increase by 0.24℃,with 88%of the increment contributed by the annual variability as mostly affected by El Niño.Moreover,the multidecadal variability related to the Atlantic Multidecadal Oscillation(AMO)in 2023 also provided an important warming background for sparking the GMST rise.As a result,the GMST in 2023 is projected to be 1.15℃±0.07℃,with only a 0.02℃ increment,if the effects of natural variability—including El Niño and the AMO—are eliminated and only the global warming trend is considered.
基金the National Natural Science Foundation of China(52070194,52073309,51902347,51908555)Natural Science Foundation of Hunan Province(2022JJ20069,2020JJ5741).
文摘Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible capacity.Herein,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic.Specifically,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff voltage.Furthermore,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal architecture.Whereas,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated polarization.Notably,Co-free NM can exhibit better safety performance than that of NCM cathode.These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.
基金supported by the National Natural Science Foundation of China(Nos.22279111,51971195,and 11935004)the Natural Science Foundation of Hebei Province(No.B2020203037)Subsidy for Hebei Key Laboratory of Applied Chemistry after Operation Performance(No.22567616H).
文摘MgH_(2),albeit with slow desorption kinetics,has been extensively studied as one of the most ideal solid hydrogen storage materials.Adding such catalyst as Ni can improve the desorption kinetics of MgH_(2),whereas the catalytic role has been attributed to different substances such as Ni,Mg_(2)Ni,Mg_(2)NiH0.3,and Mg_(2)NiH4.In the present study,Ni nanoparticles(Ni-NPs)supported on mesoporous carbon(Ni@C)have been synthesized to improve the hydrogen desorption kinetics of MgH_(2).The utilization of Ni@C largely decreases the dehydrogenation activation energy from 176.9 to 79.3 kJ mol^(−1) and the peak temperature of dehydrogenation from 375.5 to 235℃.The mechanism of Ni catalyst is well examined by advanced aberration-corrected environmental transmission electron microscopy and/or x-ray diffraction.During the first dehydrogenation,detailed microstructural studies reveal that the decomposition of MgH_(2)is initially triggered by the Ni-NPs,which is the rate-limiting step.Subsequently,the generated Mg reacts rapidly with Ni-NPs to form Mg_(2)Ni,which further promotes the dehydrogenation of residual MgH_(2).In the following dehydrogenation cycle,Mg_(2)NiH4 can rapidly decompose into Mg_(2)Ni,which continuously promotes the decomposition of MgH_(2).Our study not only elucidates the mechanism of Ni catalyst but also helps design and assemble catalysts with improved dehydriding kinetics of MgH_(2).
基金the National Key Research and Development Program of China(Grant No.2020YFA0608803)the National Natural Science Foundation of China(Grant Nos.41975107,41875092 and 42005020).
文摘To explain the recent three-year La Niña event from 2020 to 2022,which has caused catastrophic weather events worldwide,Fasullo et al.(2023)demonstrated that the increase in biomass aerosol resulting from the 2019-20 Australian wildfire season could have triggered this multi-year La Niña.Here,we present compelling evidence from paleo-proxies,utilizing a substantial sample size of 26 volcanic eruptions in the Southern Hemisphere(SH),to support the hypothesis that ocean cooling in the SH can lead to a multi-year La Niña event.This research highlights the importance of focusing on the Southern Ocean,as current climate models struggle to accurately simulate the Pacific response driven by the Southern Ocean.
基金supported by the Youth Innovation Promotion Association CAS(No.Y2021059)the LingChuang Research Project of China National Nuclear Corporation,the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA28040200)+1 种基金the Liaoning Unveiling and Commanding Program(2022JH1/10400017)the Innovation Foundation of Institute of Metal Research,CAS(No.2022-PY13).
文摘The aging embrittlement of 30Cr2Ni4MoV steel during service at high temperature has been attributed to the segregation of Si and Mn at grain boundary(GB).We report an alternative mechanism of aging embrittlement of 30Cr2Ni4MoV steel.Using atom probe tomography,it is found that the quenched and tempered(QT)30Cr2Ni4MoV steel has already contained obvious Si and Mn segregations at GB,which means that the Si and Mn segregations at GB are not sufficient to induce aging embrittlement.It is discovered for the first time in aged 30Cr2Ni4MoV there newly precipitate many G-phases along GB,and Si and Mn segregations at GB of QT30Cr2Ni4MoV steel are the main reason for the precipitation of G-phase.The hard and brittle G-phase helps to promote crack initiation during impact deformation.Subsequently,the cracks can rapidly propagate along GB due to the distribution of G-phase and the segregation of Si and Mn along the GB,which leads to intergranular cracking and low impact energy as for aged 30Cr2Ni4MoV steel.
基金supported by the National Natural Science Foundation of China (21277107, 21477094, 51672203, 51472192)the Program for New Century Excellent Talents in University (NCET-13-0944)the Fundamental Research Funds for the Central Universities (WUT 2015IB002)~~
文摘NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the microstructures of the g-C3N4 photocatalysts.In this study,a facile and low-temperature（80 ℃） impregnation method was developed to prepare NiS2/g-C3N4 photocatalysts.First,the g-C3N4 powders were processed by the hydrothermal method in order to introduce oxygen-containing functional groups（such as-OH and-C0NH-） to the surface of g-C3N4.Then,the Ni^2＋ ions could be adsorbed near the g-C3N4 via strong electrostatic interaction between g-C3N4 and Ni^2＋ ions upon the addition of Ni（NO3）2 solution.Finally,NiS2 nanoparticles were formed on the surface of g-C3N4 upon the addition of TAA.It was found that the NiS2 nanoparticles were solidly and homogeneously grafted on the surface of g-C3N4,resulting in greatly improved photocatalytic H2production.When the amount of NiS2 was 3 wt%,the resultant NiS2/g-C3N4 photocatalyst showed the highest H2 evolution rate（116.343 μmol h^-1 g^-1）,which is significantly higher than that of the pure g-C3N4（3 μmol h^-1 g^-1）.Moreover,the results of a recycling test for the NiS2/g-C3N4（3 wt%）sample showed that this sample could maintain a stable and effective photocatalytic H2-evolution performance under visible-light irradiation.Based on the above results,a possible mechanism of the improved photocatalytic performance was proposed for the presented NiS2/g-C3N4 photocatalysts,in which the photogenerated electrons of g-C3N4 can be rapidly transferred to the NiS2 nanoparticles via the close and continuous contact between them;then,the photogenerated electrons rapidly react with H2O adsorbed on the surface of NiS2,which has a surficial metallic character and high catalytic activity,to produce H2.Considering the mild and facile synthesis method,the presented low-cost and highly efficient NiS2-modified g-C3N4 photocatalysts would have great potential for practical use in photocatalytic H2 production.
