This work investigated the microstructure,magnetic properties,and crystallization kinetics of the as-spun and annealed alloy ribbons of(Fe_(40-x)Co_xNi_(40)Si_(6.33)B_(12.66)Cu_1)_(0.97)Nb_(0.03),where x=0,6,7,8,9,pre...This work investigated the microstructure,magnetic properties,and crystallization kinetics of the as-spun and annealed alloy ribbons of(Fe_(40-x)Co_xNi_(40)Si_(6.33)B_(12.66)Cu_1)_(0.97)Nb_(0.03),where x=0,6,7,8,9,prepared using the meltspinning method.The results show that adding a moderate amount of Co can improve the glass forming ability(GFA),the first peak crystallization temperature,and thermal stability of the as-spun alloy ribbons.With x=7,the two-stage crystallization temperature interval△Tx=90 exhibits optimal thermal stability,and the alloy annealed at 673 K for 10 minutes shows the favorable combined magnetic properties,with H_(c)=0.12 A/m,M_(s)=88.7 A·m^(2)/kg,andμ_(e)=13800.The magnetic domain results show that annealing removes numerous pinning points in the magnetic domains of the alloy ribbons,making the domain walls smoother and effectively reducing the pinning effect.展开更多
Solid-state electrolyte Li_(10)GeP_(2)S_(12)(LGPS)has a high lithium ion conductivity of 12 mS cm^(-1)at room temperature,but its inferior chemical stability against lithium metal anode impedes its practical applicati...Solid-state electrolyte Li_(10)GeP_(2)S_(12)(LGPS)has a high lithium ion conductivity of 12 mS cm^(-1)at room temperature,but its inferior chemical stability against lithium metal anode impedes its practical application.Among all solutions,Ge atom substitution of the solid-state electrolyte LGPS stands out as the most promising solution to this interface problem.A systematic screening framework for Ge atom substitution including ionic conductivity,thermodynamic stability,electronic and mechanical properties is utilized to solve it.For fast screening,an enhanced model Dop Net FC using chemical formulas for the dataset is adopted to predict ionic conductivity.Finally,Li_(10)SrP_(2)S_(12)(LSrPS)is screened out,which has high lithium ion conductivity(12.58 mS cm^(-1)).In addition,an enhanced migration of lithium ion across the LSr PS/Li interface is found.Meanwhile,compared to the LGPS/Li interface,LSrPS/Li interface exhibits a larger Schottky barrier(0.134 eV),smaller electron transfer region(3.103?),and enhanced ability to block additional electrons,all of which contribute to the stabilized interface.The applied theoretical atom substitution screening framework with the aid of machine learning can be extended to rapid determination of modified specific material schemes.展开更多
In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterpart...In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterparts.The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications.In this context,the atomic substitution method has emerged as a favorable approach.It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting materials.In this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC materials.The effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are discussed.The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these advancements.Finally,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.展开更多
Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under pressure.This raises the question of whether the superconducting transition temperature T_(c) could be furt...Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under pressure.This raises the question of whether the superconducting transition temperature T_(c) could be further enhanced under suitable conditions.One possible route for achieving higher T_(c) is element substitution.Similar SC could appear in the Fmmm phase of rare-earth(RE)R_(3)Ni_(2)O_(7)(RNO,R=RE element)material series under suitable pressure.The electronic properties in the RNO materials are dominated by the Ni 3d orbitals in the bilayer NiO_(2) plane.In the strong coupling limit,the SC could be fully characterized by a bilayer single 3d_(x^(2)−y^(2))-orbital t–J‖–J⊥ model.With RE element substitution from La to other RE element,the lattice constant of the Fmmm RNO material decreases,and the resultant electronic hopping integral increases,leading to stronger superexchanges between the 3d_(x^(2)−y^(2)) orbitals.Based on the slave-boson mean-field theory,we explore the pairing nature and the evolution of T_(c) in RNO materials under pressure.Consequently,it is found that the element substitution does not alter the pairing nature,i.e.,the inter-layer s-wave pairing is always favored in the superconducting RNO under pressure.However,the T_(c) increases from La to Sm,and a nearly doubled T_(c) could be realized in SmNO under pressure.This work provides evidence for possible higher T_(c) R_(3)Ni_(2)O_(7) materials,which may be realized in further experiments.展开更多
Ion substitution has significantly improved the performance of ferrite magnets,and cobalt remains a key area of research.Studies on the mechanism of Co^(2+)in strontium ferrite,especially SrFe_(2n-x)Co_(x)O_(19-d)(n=6...Ion substitution has significantly improved the performance of ferrite magnets,and cobalt remains a key area of research.Studies on the mechanism of Co^(2+)in strontium ferrite,especially SrFe_(2n-x)Co_(x)O_(19-d)(n=6.1-5.4;x=0.05-0.20)synthesized using the ceramic method,showed that Co^(2+)preferentially enters the lattice as the Fe/Sr ratio decreases.This results in a decrease in the lattice constants a and c due to oxygen vacancies and iron ion deficiency.The impact of Co substitution on morphology is minor compared to the effect of the Fe/Sr ratio.As the Fe/Sr ratio decreases and the Co content increases,the saturation magnetization decreases.The magnetic anisotropy field exhibits a nonlinear change,generally increasing with higher Fe/Sr ratios and Co content.These changes in the performance of permanent magnets are attributed to the absence of Fe^(3+)ions at the 12k+2a and 2b sites and the substitution of Co^(2+)at the 2b site.This suggests that by adjusting the Fe/Sr ratio and appropriate Co substitution,the magnetic anisotropy field of M-type strontium ferrite can be effectively optimized.展开更多
Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behav...Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.展开更多
In this study,the impacts of egg consumption on mice model of metabolic syndrome(Met S)were comparatively investigated.Mice were divided into five groups(n=8):normal diet group(ND),high-fat diet group(HFD),HFD with wh...In this study,the impacts of egg consumption on mice model of metabolic syndrome(Met S)were comparatively investigated.Mice were divided into five groups(n=8):normal diet group(ND),high-fat diet group(HFD),HFD with whole egg group(WE),HFD with free-yolk egg substitute group(YFES),and HFD with lovastatin group(Lov).Main biochemical indexes and a non-targeted lipidomic analysis were employed to insight the lipid profile changes in serum.It was revealed that WE could significantly improve serum biochemical indexes by reducing body weight,low-density lipoprotein cholesterol(LDL-C)and total cholesterol(TC),while increasing high-density lipoprotein cholesterol.YFES exhibited remarkably better performance in increasing phosphatidylglycerol and phosphatidic acids,while decreasing phosphatidylinositol than WE.A total of 50 differential lipids biomarkers tightly related to glycerophospholipids metabolism were screened out.Carnitine C18:2 and C12:1,SM(d18:0/12:0),and SM(d18:1/14:1)were significantly upregulated in YFES compared to WE.YFES reduced expression of SREBP-1c and Cpt1a,while did not affect the expression of PPAR-α.Sphingomyelin biomarkers were positively related to the TC(|r|>0.6),while PPAR-αwas negatively correlated with triglyceride and LDL-C levels.To sum up,YFES attenuated HFD-induced Met S by improving the serum phospholipids,which account for its modulation of glycerophospholipid metabolism.展开更多
The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide(SiO)anodes.For the classic polyacrylic acid(PAA)binder,the self-association of-COOH g...The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide(SiO)anodes.For the classic polyacrylic acid(PAA)binder,the self-association of-COOH groups in PAA leads to the formation of intramolecular and intermolecular hydrogen bonds,greatly weakening the bonding force of the binder to SiO surface.However,strengthening the binder-material interaction from the perspective of binder molecular regulation poses a significant challenge.Herein,a modified PAA-Li_(x)(0.25≤x≤1)binder with prominent mechanical properties and adhesion strength is specifically synthesized for SiO anodes by quantitatively substituting the carboxylic hydrogen with lithium.The appropriate lithium substitution(x=0.25)not only effectively increases the number of hydrogen bonds between the PAA binder and SiO surface owing to charge repulsion effect between ions,but also guarantees moderate entanglement between PAA-Li_x molecular chains through the ion-dipole interaction.As such,the PAA-Li_(0.25)/SiO electrode exhibits exceptional mechanical properties and the lowest volume change,as well as the optimum cycling(1237.3 mA h g^(-1)after 100cycles at 0.1 C)and rate performance(1000.6 mA h g^(-1)at 1 C),significantly outperforming the electrode using pristine PAA binder.This work paves the way for quantitative regulation of binders at the molecular level.展开更多
It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced ...It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.展开更多
[目的]研究石灰性土壤上磷肥减施结合硫铵替代尿素措施的效果,为夏玉米-冬小麦体系合理施用磷肥和维持作物高产提供依据。[方法]在陕西关中设置3年田间定位试验,实施夏玉米-冬小麦轮作模式,共含有对照(CK,不施磷肥)、常规施磷(CP,年施磷...[目的]研究石灰性土壤上磷肥减施结合硫铵替代尿素措施的效果,为夏玉米-冬小麦体系合理施用磷肥和维持作物高产提供依据。[方法]在陕西关中设置3年田间定位试验,实施夏玉米-冬小麦轮作模式,共含有对照(CK,不施磷肥)、常规施磷(CP,年施磷量180 kg P_(2)O_(5)/hm^(2),撒施)、减施磷肥(RP,年施磷量134 kg P_(2)O_(5)/hm^(2),条施)、减磷结合硫铵替代尿素(RPSA,施磷量与RP相同,条施)4个处理。作物收获期采集植物和土壤样品,测定玉米和小麦产量、磷肥效率、pH及土壤磷水平。小麦拔节期测定根系形态、菌根侵染率等指标。[结果]与CK相比,施磷处理(CP,RP和RPSA)的玉米和小麦籽粒产量均显著提高,增幅分别为17.3%~24.8%和5.1%~19.0%;土壤有效磷(Olsen-P)和微生物量磷(MBP)显著提高;除RP外,施磷处理的土壤pH均显著降低。施磷处理间,2018-2019年度RP较CP产量显著降低14.6%,磷回收率和偏生产力显著提高。RPSA较RP土壤pH显著降低,有效磷、微生物量磷含量和根系形态及菌根侵染率均显著提高。土壤pH与土壤磷水平、小麦根系形态指标和产量均呈显著负相关。RDA结果表明:土壤pH是影响小麦菌根侵染率、根系形态和产量的最重要环境因子。[结论]磷肥减施结合硫铵替代尿素调控措施可以降低石灰性土壤pH,提高土壤有效磷和微生物量磷含量,促进小麦根系生长并提高菌根侵染率,是石灰性[土娄]土夏玉米-冬小麦体系有效的磷肥减施增效措施。展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.52275567)the Key Research and Development Program of Shanxi Province,China(Grant No.202202050201020)+3 种基金the Doctoral Starting-up Foundation of Taiyuan University of Science and Technology(Grant No.20192016)the Research Project Supported by Shanxi Scholarship Council(Grant No.2017-085)the Graduate Education and Teaching Reform Project of Shanxi Province,China(Grant No.2023JG136)the Special Fund for Science and Technology Innovation Teams of Shanxi Province,China(Grant No.202304051001036)。
文摘This work investigated the microstructure,magnetic properties,and crystallization kinetics of the as-spun and annealed alloy ribbons of(Fe_(40-x)Co_xNi_(40)Si_(6.33)B_(12.66)Cu_1)_(0.97)Nb_(0.03),where x=0,6,7,8,9,prepared using the meltspinning method.The results show that adding a moderate amount of Co can improve the glass forming ability(GFA),the first peak crystallization temperature,and thermal stability of the as-spun alloy ribbons.With x=7,the two-stage crystallization temperature interval△Tx=90 exhibits optimal thermal stability,and the alloy annealed at 673 K for 10 minutes shows the favorable combined magnetic properties,with H_(c)=0.12 A/m,M_(s)=88.7 A·m^(2)/kg,andμ_(e)=13800.The magnetic domain results show that annealing removes numerous pinning points in the magnetic domains of the alloy ribbons,making the domain walls smoother and effectively reducing the pinning effect.
基金support from the National Natural Science Foundation of China (No.51806072)。
文摘Solid-state electrolyte Li_(10)GeP_(2)S_(12)(LGPS)has a high lithium ion conductivity of 12 mS cm^(-1)at room temperature,but its inferior chemical stability against lithium metal anode impedes its practical application.Among all solutions,Ge atom substitution of the solid-state electrolyte LGPS stands out as the most promising solution to this interface problem.A systematic screening framework for Ge atom substitution including ionic conductivity,thermodynamic stability,electronic and mechanical properties is utilized to solve it.For fast screening,an enhanced model Dop Net FC using chemical formulas for the dataset is adopted to predict ionic conductivity.Finally,Li_(10)SrP_(2)S_(12)(LSrPS)is screened out,which has high lithium ion conductivity(12.58 mS cm^(-1)).In addition,an enhanced migration of lithium ion across the LSr PS/Li interface is found.Meanwhile,compared to the LGPS/Li interface,LSrPS/Li interface exhibits a larger Schottky barrier(0.134 eV),smaller electron transfer region(3.103?),and enhanced ability to block additional electrons,all of which contribute to the stabilized interface.The applied theoretical atom substitution screening framework with the aid of machine learning can be extended to rapid determination of modified specific material schemes.
基金supported by the Teli Fellowship from Beijing Institute of Technology,the National Natural Science Foundation of China(Nos.52303366,22173109).
文摘In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterparts.The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications.In this context,the atomic substitution method has emerged as a favorable approach.It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting materials.In this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC materials.The effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are discussed.The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these advancements.Finally,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.
基金supported by the National Natural Science Foundation of China(Grant Nos.12234016,12174317,and 12074031)the New Cornerstone Science Foundation.
文摘Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under pressure.This raises the question of whether the superconducting transition temperature T_(c) could be further enhanced under suitable conditions.One possible route for achieving higher T_(c) is element substitution.Similar SC could appear in the Fmmm phase of rare-earth(RE)R_(3)Ni_(2)O_(7)(RNO,R=RE element)material series under suitable pressure.The electronic properties in the RNO materials are dominated by the Ni 3d orbitals in the bilayer NiO_(2) plane.In the strong coupling limit,the SC could be fully characterized by a bilayer single 3d_(x^(2)−y^(2))-orbital t–J‖–J⊥ model.With RE element substitution from La to other RE element,the lattice constant of the Fmmm RNO material decreases,and the resultant electronic hopping integral increases,leading to stronger superexchanges between the 3d_(x^(2)−y^(2)) orbitals.Based on the slave-boson mean-field theory,we explore the pairing nature and the evolution of T_(c) in RNO materials under pressure.Consequently,it is found that the element substitution does not alter the pairing nature,i.e.,the inter-layer s-wave pairing is always favored in the superconducting RNO under pressure.However,the T_(c) increases from La to Sm,and a nearly doubled T_(c) could be realized in SmNO under pressure.This work provides evidence for possible higher T_(c) R_(3)Ni_(2)O_(7) materials,which may be realized in further experiments.
基金support from the Research Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(Grant No.E355B001)Key Research Program of the Chinese Academy of Sciences(Grant No.ZDRW-CN-2021-3)Science Center of the National Natural Science Foundation of China(Grant No.52088101).
文摘Ion substitution has significantly improved the performance of ferrite magnets,and cobalt remains a key area of research.Studies on the mechanism of Co^(2+)in strontium ferrite,especially SrFe_(2n-x)Co_(x)O_(19-d)(n=6.1-5.4;x=0.05-0.20)synthesized using the ceramic method,showed that Co^(2+)preferentially enters the lattice as the Fe/Sr ratio decreases.This results in a decrease in the lattice constants a and c due to oxygen vacancies and iron ion deficiency.The impact of Co substitution on morphology is minor compared to the effect of the Fe/Sr ratio.As the Fe/Sr ratio decreases and the Co content increases,the saturation magnetization decreases.The magnetic anisotropy field exhibits a nonlinear change,generally increasing with higher Fe/Sr ratios and Co content.These changes in the performance of permanent magnets are attributed to the absence of Fe^(3+)ions at the 12k+2a and 2b sites and the substitution of Co^(2+)at the 2b site.This suggests that by adjusting the Fe/Sr ratio and appropriate Co substitution,the magnetic anisotropy field of M-type strontium ferrite can be effectively optimized.
基金This work was supported by National Key R&D Program of China(2021YFF1200200)Peiyang Talents Project of Tianjin University.
文摘Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.
基金supported by the Applied Basic Research of Shanxi Province(201901D211381)the Innovation-driven Development Capacity Enhancement Fund of Shanxi Province(SXYBKY2019041)+2 种基金National Key Research and Development Program(2021YFD1600604-03)Shanxi Scholarship Council of China(2021-068)Shanxi Agricultural University High-Level Talent Project(2021XG013)。
文摘In this study,the impacts of egg consumption on mice model of metabolic syndrome(Met S)were comparatively investigated.Mice were divided into five groups(n=8):normal diet group(ND),high-fat diet group(HFD),HFD with whole egg group(WE),HFD with free-yolk egg substitute group(YFES),and HFD with lovastatin group(Lov).Main biochemical indexes and a non-targeted lipidomic analysis were employed to insight the lipid profile changes in serum.It was revealed that WE could significantly improve serum biochemical indexes by reducing body weight,low-density lipoprotein cholesterol(LDL-C)and total cholesterol(TC),while increasing high-density lipoprotein cholesterol.YFES exhibited remarkably better performance in increasing phosphatidylglycerol and phosphatidic acids,while decreasing phosphatidylinositol than WE.A total of 50 differential lipids biomarkers tightly related to glycerophospholipids metabolism were screened out.Carnitine C18:2 and C12:1,SM(d18:0/12:0),and SM(d18:1/14:1)were significantly upregulated in YFES compared to WE.YFES reduced expression of SREBP-1c and Cpt1a,while did not affect the expression of PPAR-α.Sphingomyelin biomarkers were positively related to the TC(|r|>0.6),while PPAR-αwas negatively correlated with triglyceride and LDL-C levels.To sum up,YFES attenuated HFD-induced Met S by improving the serum phospholipids,which account for its modulation of glycerophospholipid metabolism.
基金supported by the National Natural Science Foundation of China (Grant Nos.92372101,52162036 and 21875155)the Fundamental Research Funds for the Central Universities (Grant Nos.20720220010)the National Key Research and Development Program of China (Grant Nos.2021YFA1201502)。
文摘The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide(SiO)anodes.For the classic polyacrylic acid(PAA)binder,the self-association of-COOH groups in PAA leads to the formation of intramolecular and intermolecular hydrogen bonds,greatly weakening the bonding force of the binder to SiO surface.However,strengthening the binder-material interaction from the perspective of binder molecular regulation poses a significant challenge.Herein,a modified PAA-Li_(x)(0.25≤x≤1)binder with prominent mechanical properties and adhesion strength is specifically synthesized for SiO anodes by quantitatively substituting the carboxylic hydrogen with lithium.The appropriate lithium substitution(x=0.25)not only effectively increases the number of hydrogen bonds between the PAA binder and SiO surface owing to charge repulsion effect between ions,but also guarantees moderate entanglement between PAA-Li_x molecular chains through the ion-dipole interaction.As such,the PAA-Li_(0.25)/SiO electrode exhibits exceptional mechanical properties and the lowest volume change,as well as the optimum cycling(1237.3 mA h g^(-1)after 100cycles at 0.1 C)and rate performance(1000.6 mA h g^(-1)at 1 C),significantly outperforming the electrode using pristine PAA binder.This work paves the way for quantitative regulation of binders at the molecular level.
基金the National Natural Science Foundation of China (22209091)the Natural Science Foundation of Shandong Province (ZR2020QB057)+1 种基金the Key Program of National Natural Science Foundation of China (22133006)the Yankuang Group 2019 Science and Technology Program (YKKJ2019AJ05JG-R60)。
文摘It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.
文摘[目的]研究石灰性土壤上磷肥减施结合硫铵替代尿素措施的效果,为夏玉米-冬小麦体系合理施用磷肥和维持作物高产提供依据。[方法]在陕西关中设置3年田间定位试验,实施夏玉米-冬小麦轮作模式,共含有对照(CK,不施磷肥)、常规施磷(CP,年施磷量180 kg P_(2)O_(5)/hm^(2),撒施)、减施磷肥(RP,年施磷量134 kg P_(2)O_(5)/hm^(2),条施)、减磷结合硫铵替代尿素(RPSA,施磷量与RP相同,条施)4个处理。作物收获期采集植物和土壤样品,测定玉米和小麦产量、磷肥效率、pH及土壤磷水平。小麦拔节期测定根系形态、菌根侵染率等指标。[结果]与CK相比,施磷处理(CP,RP和RPSA)的玉米和小麦籽粒产量均显著提高,增幅分别为17.3%~24.8%和5.1%~19.0%;土壤有效磷(Olsen-P)和微生物量磷(MBP)显著提高;除RP外,施磷处理的土壤pH均显著降低。施磷处理间,2018-2019年度RP较CP产量显著降低14.6%,磷回收率和偏生产力显著提高。RPSA较RP土壤pH显著降低,有效磷、微生物量磷含量和根系形态及菌根侵染率均显著提高。土壤pH与土壤磷水平、小麦根系形态指标和产量均呈显著负相关。RDA结果表明:土壤pH是影响小麦菌根侵染率、根系形态和产量的最重要环境因子。[结论]磷肥减施结合硫铵替代尿素调控措施可以降低石灰性土壤pH,提高土壤有效磷和微生物量磷含量,促进小麦根系生长并提高菌根侵染率,是石灰性[土娄]土夏玉米-冬小麦体系有效的磷肥减施增效措施。