In this paper,we introduce the notion of G_(C)-X-injective modules,where X denotes a class of left S-modules and C represents a faithfully semidualizing bimodule.Under the condition that X satisfies certain hypotheses...In this paper,we introduce the notion of G_(C)-X-injective modules,where X denotes a class of left S-modules and C represents a faithfully semidualizing bimodule.Under the condition that X satisfies certain hypotheses,some properties and some equivalent characterizations of G_(C)-X-injective modules are investigated,and we also show that the triple(■,cores■,■)is a weak co-AB-context.As an application,two complete cotorsion pairs and a new model structure in Mod S are given.展开更多
Single-atom catalysts for alkyne semi-hydrogenation have been extensively investigated due to their high metal utilization and improved olefin selectivity.However,their reactivity is hindered by the sluggish activatio...Single-atom catalysts for alkyne semi-hydrogenation have been extensively investigated due to their high metal utilization and improved olefin selectivity.However,their reactivity is hindered by the sluggish activation of reactants on isolated sites.Herein,a non-precise metal catalyst consisting of Ni-Cu hetero-diatomic pairs was prepared using a sequential deposition method.The diatomic sites catalyst exhibited an unprecedented activity among non-precious catalysts with over 98%conversion and 77 mol_(C2H2) mol_(metal)^(-1) h^(-1) at 180℃,whereas the single-atom catalysts of Cu/C and Ni/C were almost inert under the same conditions.Experimental and theoretical results revealed the crucial diatomic synergy between the Ni-Cu pairs,wherein acetylene was adsorbed on Ni sites and hydrogen was adsorbed on Cu sites,and the diatomic site enabled spontaneous desorption of ethylene.The superior activity of the diatomic catalyst was observed,resulting from the enhanced dominance of d-electrons of Ni near the Fermi level.The research demonstrates an approach to designing non-precise metal catalysts with extraordinary catalytic performance for alkyne hydrogenation.展开更多
To fully utilize the resources provided by optical fiber networks,a cross-band quantum light source generating photon pairs,where one photon in a pair is at C band and the other is at O band,is proposed in this work.T...To fully utilize the resources provided by optical fiber networks,a cross-band quantum light source generating photon pairs,where one photon in a pair is at C band and the other is at O band,is proposed in this work.This source is based on spontaneous four-wave mixing(SFWM)in a piece of shallow-ridge silicon waveguide.Theoretical analysis shows that the waveguide dispersion could be tailored by adjusting the ridge width,enabling broadband photon pair generation by SFWM across C band and O band.The spontaneous Raman scattering(SpRS)in silicon waveguides is also investigated experimentally.It shows that there are two regions in the spectrum of generated photons from SpRS,which could be used to achieve cross-band photon pair generation.A chip of shallow-ridge silicon waveguide samples with different ridge widths has been fabricated,through which cross-band photon pair generation is demonstrated experimentally.The experimental results show that the source can be achieved using dispersion-optimized shallow-ridge silicon waveguides.This cross-band quantum light source provides a way to develop new fiber-based quantum communication functions utilizing both C band and O band and extends applications of quantum networks.展开更多
This paper proposes an innovative form of group reduction or similarity transformation involving off-diagonal block matrices. The proposed method is applied to the Ablowitz-Kaup-Newell-Segur(AKNS) matrix spectral prob...This paper proposes an innovative form of group reduction or similarity transformation involving off-diagonal block matrices. The proposed method is applied to the Ablowitz-Kaup-Newell-Segur(AKNS) matrix spectral problem, leading to the generation of reduced matrix AKNS integrable hierarchies. As a result, a variety of reduced multiple-component integrable nonlinear Schr??dinger and modified Korteweg-de Vries models are derived from the analysis of the reduced AKNS matrix spectral problem.展开更多
This paper presents a geometric perspective that connects reciprocal transformations with multidimensional integrable deformations.By interpreting conservation laws as closed 1-forms,we formalize reciprocal transforma...This paper presents a geometric perspective that connects reciprocal transformations with multidimensional integrable deformations.By interpreting conservation laws as closed 1-forms,we formalize reciprocal transformations as induced local diffeomorphisms on the jet bundle.This allows us to characterize higher-dimensional deformations as systematic fiber bundle extensions,where fiber coordinates are generated by potential functions of the conservation laws.This perspective provides an interpretation for the covariant lifting of Lax pairs to higher dimensions and reveals that auto-Backlund transformations are composite diffeomorphisms.These results are applied to several classical integrable models.展开更多
The spin-sensitive nature of redox reactions in energy conversion systems,such as the oxygen evolution reaction(OER),has attracted increasing attention due to its potential for enhancing catalytic efficiency.Magnetic ...The spin-sensitive nature of redox reactions in energy conversion systems,such as the oxygen evolution reaction(OER),has attracted increasing attention due to its potential for enhancing catalytic efficiency.Magnetic fields(MFs)have been proposed to enhance OER performance by influencing the spin states of oxygen intermediates.However,prior study has predominantly focused on MF effects mediated by the intrinsic magnetic properties of electrocatalysts or magnetohydrodynamics.In this work,we report a universal enhancement in OER activity,achieving over 150% increase in current density under a200 mT MF across diamagnetic,paramagnetic and magnetic electrocatalysts in 1 M KOH.Through systematic investigation of MF orientation and strength,pH,applied potentials,and the use of benzoquinone radical scavenger,we demonstrate that MF-driven performance improvements arise from direct modulation of oxygen radical spin states.Specifically,MFs promote the formation of spin-triplet oxygen intermediates(↑O–O↑),a critical step for O–O bond formation,independent of the catalyst's intrinsic magnetism.However,the local magnetic environment near the catalyst surface,governed by its magnetic properties,indirectly influences radical spin dynamics by alternating the effective field experienced by intermediates.These findings redefine the role of spin manipulation in electrocatalysis,advancing understanding of MF-driven spin effects in redox reactions.展开更多
Switchable polymerization is emerging as a powerful tool to construct block copolymers directly from mixtures of monomers.However,current achievements typically iterate between two polymerization cycles to afford prod...Switchable polymerization is emerging as a powerful tool to construct block copolymers directly from mixtures of monomers.However,current achievements typically iterate between two polymerization cycles to afford products with fixed sequences and compositions.Herein,we report the triethylborane/1,8-diazabicyclo[5.4.0]undec-7-ene(Et_3B/DBU)pair-mediated four-component switchable polymerization of propylene oxide(PO),CO_(2),phthalic anhydride(PA),and racemic lactide(rac-LA),which enables the on-demand synthesis of four different block copolymers,i.e.,poly(propylene phthalate)-b-polylactide(PPE-b-PLA),PPE-b-PLA-b-poly(propylene carbonate)(PPC),PPE-b-PPC-b-PLA,and PPE-b-PPCb-poly(propylene oxide)(PPO),through rationally modulating the Lewis pair(LP)ratio.Core to this protocol is that increasing the loading of Et_(3)B accelerates the ring-opening of PO while impeding the reactivity of rac-LA,thus allowing for fine-tuning of the thermodynamic and kinetic of the switchable polymerization.Therefore,the four polymerization cycles involving PO/PA ring-opening copolymerization(ROCOP),PO/CO_(2) ROCOP,rac-LA ring-opening polymerization(ROP),and PO ROP can be connected and discriminated in precisely programmed manners.展开更多
In this study,electrochemical C-H carboxylation of benzylamines with CO_(2) was reported.This linear paired electrolysis system enables efficient and economical synthesis of value-added α-amino acids(α-AAs) under mi...In this study,electrochemical C-H carboxylation of benzylamines with CO_(2) was reported.This linear paired electrolysis system enables efficient and economical synthesis of value-added α-amino acids(α-AAs) under mild conditions.Various substituted benzylamines containing diverse functional groups and even highly reactive moieties,such as cyano,amide and alkene groups could be successfully transformed to the carboxylated products.Notably,this method proved to be applicable to the late-stage modification of biorelevant compounds,highlighting its potential for synthetic chemistry.Mechanistic studies such as radical trapping experiments,kinetic isotope effect(KIE) tests and cyclic voltammetry(CV) studies provided useful insight into this transformation.展开更多
Achieving non-centrosymmetric(NCS) configurations in ABX3-type hybrid halides remains a critical challenge for nonlinear optical(NLO) materials due to the conflicting requirements of high second-harmonic generation(SH...Achieving non-centrosymmetric(NCS) configurations in ABX3-type hybrid halides remains a critical challenge for nonlinear optical(NLO) materials due to the conflicting requirements of high second-harmonic generation(SHG) response,wide bandgap,and phase-matching capabilities.Herein,we propose a triplesite modulation strategy by synergistically tailoring the A-site cations(2-methylimidazole cation/1-ethyl-3-methylimidazole cation),B-site metals(Sn^(2+)/Pb^(2+)),and X-site halogens(Cl/Br),which effectively disrupts lattice symmetry and enables NCS crystallization.Our results demonstrate a strong SHG response,an expanded optical bandgap and increased birefringence.The optimized compound C_(6)H_(11)N_(2)PbCl_(3) exhibits a moderately strong SHG efficiency of 3.8 × KDP,a wide bandgap(3.87 eV),and enhanced birefringence(0.139@1064 nm),surpassing majority hybrid NLO materials.The innovative anionic framework introduced here broadens the scope of hybrid NLO crystals,facilitating the integration of various aromatic heterocyclic cations.This research provides a robust strategic framework for the development of advanced NLO materials.展开更多
Motivated by the recent experimental discovery of superconductivity in rhombohedral tetralayer graphene,we investigate the pairing mechanism arising from the density–density interactions within the random-phase appro...Motivated by the recent experimental discovery of superconductivity in rhombohedral tetralayer graphene,we investigate the pairing mechanism arising from the density–density interactions within the random-phase approximation.This approach successfully highlights the dominance of the chiral p-wave pairing between electrons with the same spin and valley index at low densities,while also predicting the superconducting range in agreement with experimental findings.Furthermore,we examine the characteristics of distinct superconducting regions:SC1 and SC2 exhibit chiral finite-momentum superconductivity with pronounced phase fluctuations,whereas SC4 displays zero-momentum spin-singlet superconductivity.展开更多
Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy ...Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.展开更多
erized by a periodic real-space modulation of the superconducting pairing order parameter,is a novel quantum phase observed in superconducting(SC)systems.It is believed to play a key role in understanding the pseudoga...erized by a periodic real-space modulation of the superconducting pairing order parameter,is a novel quantum phase observed in superconducting(SC)systems.It is believed to play a key role in understanding the pseudogap phase of superconductors and has recently been discovered in bulk cuprates,transition-metal dichalcogenide,and other unconventional superconductors.However,artificially engineered PDW in designable two-dimensional materials remain rare.In this paper,we report a strain-assisted strategy to realize cooper-pair density modulation in a van der Waals heterostructure:graphene on SC 2H-NbSe2.Superconductivity is induced in graphene via the proximity effect.Meanwhile,the graphene membrane spontaneously buckles into a periodic structure owing to strain,featuring a spatially modulated local density of states(LDOS).The interplay between the spatially modulated LDOS and the proximity-induced superconductivity results in an oscillatory pair density determined by the buckled geometry,constituting an artificial PDW.This approach enables the engineering of PDWs with periodicities of up to tens of nanometers and allows their realization in a variety of heterostructures with tailored designs.Our work provides new insights into the investigation of PDW physics using predesigned two-dimensional materials.展开更多
The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solv...The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solvent-resistant Nitrate-coordinated electrolyte.The practical Ah-level graphite LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) pouch cell with the newly developed electrolyte demonstrates a significant breakthrough in cycling stability,exhibiting negligible capacity fade after 250 cycles at-30℃ and 0.1 C.NO_(3)^(-),as the functional additive,compresses the electric field around Li^(+)through electrostatic interactions,mimicking the Debye-screening effect and inducing the coordinative exclusion of free ethyl acetate molecules at low temperatures.The transformation from contact ion pairs(CIPs)formed by Pto solventseparated ion pairs is significantly restrained,which mitigates the continuous reactions between the electrolyte and inevitable lithium deposition at low temperature.Additionally,this customized inert CIPs form a solid electrolyte interphase on graphite that exhibits remarkable ionic conductivity and rigidity,preventing excessive Li dendrite growth.This finding offers new insights into the relationship of microstructure-performance for low-temperature electrolytes,demonstrating that relying solely on inert CIPs can also inhibit the decomposition of the interfacial electrolyte,and inspires a unique design concept for high-performance,commercially viable LIBs that operate reliably in sub-zero environments.展开更多
Following over 20 years of research,a direct measurement of the QGP temperature has been achieved at Relativistic Heavy-Ion Collider(RHIC),free from the blue-shift effect and contamination from strong interactions.Thi...Following over 20 years of research,a direct measurement of the QGP temperature has been achieved at Relativistic Heavy-Ion Collider(RHIC),free from the blue-shift effect and contamination from strong interactions.This viewpoint discusses a recent measurement of the QGP temperature at different stages at the Solenoidal Tracker at RHIC(STAR),which used e^(+)e^(-)pairs as penetrating probes.展开更多
Single Pair Ethernet(以下简称SPE)凭借极其显著的布线简化优势,正迅速成为工业通信领域的重要技术。该项创新技术仅需使用一对导线即可同时完成数据信号与电力的双重传输,这一特性使其特别适用于空间要求极为紧凑的微型设备、安装空...Single Pair Ethernet(以下简称SPE)凭借极其显著的布线简化优势,正迅速成为工业通信领域的重要技术。该项创新技术仅需使用一对导线即可同时完成数据信号与电力的双重传输,这一特性使其特别适用于空间要求极为紧凑的微型设备、安装空间受到严格限制的工业环境以及对网络架构灵活性有着较高要求的各类解决方案。然而长期以来,市场上多种互不兼容的连接接口严重制约了SPE技术的全面市场推广与普及应用。展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR),powered by advanced technologies such as solid oxide electrolysis cells(SOEC),is a promising method to convert CO_(2) into valuable carbon-based products usi...Electrochemical carbon dioxide reduction reaction(CO_(2)RR),powered by advanced technologies such as solid oxide electrolysis cells(SOEC),is a promising method to convert CO_(2) into valuable carbon-based products using renewable electricity.The high chemical stability of CO_(2) requires catalysts to exhibit both high activity and stable electrocatalytic performance.However,catalysts that deliver high performance in CO_(2)RR are rare and still require further improvement.Here,we report a strategy that can efficiently enhance catalyst activity through Zn doping,which introduces active frustrated Lewis pairs(FLP)to improve the catalyst's ability to activate small molecules.A high current density of-1.85 A cm^(-2)at 800℃under a bias voltage of 1.5 V was achieved using the Sr_(2)Fe_(0.8)Zn_(0.2)MoO_(6-δ)(SFZn_(0.2)M)cathode with pure CO_(2) feeding gas,surpassing previously reported results for perovskite oxide cathodes.This SOEC device also demonstrates excellent stability,with negligible degradation over tests lasting up to 110 h.展开更多
In the area of secure Web information system, mutual authentication and key agreement are essential between Web clients and servers. An efficient certificateless authenticated key agreement protocol for Web client/ser...In the area of secure Web information system, mutual authentication and key agreement are essential between Web clients and servers. An efficient certificateless authenticated key agreement protocol for Web client/server setting is proposed, which uses pairings on certain elliptic curves. We show that the newly proposed key agreement protocol is practical and of great efficiency, meanwhile, it satisfies every desired security require ments for key agreement protocols.展开更多
Signcryption is a cryptographic primitive that performs signature and encryption simultaneously, at lower computational costs and communication overheads than the signature-then- encryption approach. In this paper, we...Signcryption is a cryptographic primitive that performs signature and encryption simultaneously, at lower computational costs and communication overheads than the signature-then- encryption approach. In this paper, we propose an efficient multi-recipient signcryption scheme based on the bilinear pairings, which broadcasts a message to multiple users in a secure and authenticated manner. We prove its semantic security and unforgeability under the Gap Diffie-Hellman problem assumption in the random oracle model. The proposed scheme is more efficient than re-signcrypting a message n times using a signcryption scheme in terms of computational costs and communication overheads.展开更多
We argue that traditional identity-based systems from pairings seem unsuitable for designing group signature schemes due to the problem of key escrow. In this paper we first propose new ID-based public key systems wit...We argue that traditional identity-based systems from pairings seem unsuitable for designing group signature schemes due to the problem of key escrow. In this paper we first propose new ID-based public key systems without trusted PKG (Private Key Generator) from bilinear pairings. In our new ID-based systems, if the dishonest PKG impersonates an honest user to communicate with others, the user can provide a proof of treachery of the PKG afterwards, which is similar to certificate-based systems. Therefore, our systems reach the Girault’s trusted level 3. We then propose a group signature scheme under the new ID-based systems, the security and performance of which rely on the new systems. The size of the group public key and the length of the signature are independent on the numbers of the group.展开更多
文摘In this paper,we introduce the notion of G_(C)-X-injective modules,where X denotes a class of left S-modules and C represents a faithfully semidualizing bimodule.Under the condition that X satisfies certain hypotheses,some properties and some equivalent characterizations of G_(C)-X-injective modules are investigated,and we also show that the triple(■,cores■,■)is a weak co-AB-context.As an application,two complete cotorsion pairs and a new model structure in Mod S are given.
基金supported by the National Key R&D Program of China(Grant No.2021YFA1501803)the National Natural Science Foundation of China(NSFC,Grant No.21978148&52206156)。
文摘Single-atom catalysts for alkyne semi-hydrogenation have been extensively investigated due to their high metal utilization and improved olefin selectivity.However,their reactivity is hindered by the sluggish activation of reactants on isolated sites.Herein,a non-precise metal catalyst consisting of Ni-Cu hetero-diatomic pairs was prepared using a sequential deposition method.The diatomic sites catalyst exhibited an unprecedented activity among non-precious catalysts with over 98%conversion and 77 mol_(C2H2) mol_(metal)^(-1) h^(-1) at 180℃,whereas the single-atom catalysts of Cu/C and Ni/C were almost inert under the same conditions.Experimental and theoretical results revealed the crucial diatomic synergy between the Ni-Cu pairs,wherein acetylene was adsorbed on Ni sites and hydrogen was adsorbed on Cu sites,and the diatomic site enabled spontaneous desorption of ethylene.The superior activity of the diatomic catalyst was observed,resulting from the enhanced dominance of d-electrons of Ni near the Fermi level.The research demonstrates an approach to designing non-precise metal catalysts with extraordinary catalytic performance for alkyne hydrogenation.
基金supported by the Quantum Science and Technology-National Science and Technology Major Project (Grant No.2024ZD0302502 for WZ)the National Natural Science Foundation of China(Grant No.92365210 for WZ)+1 种基金Tsinghua Initiative Scientific Research Program (for WZ)the project of Tsinghua University-Zhuhai Huafa Industrial Share Company Joint Institute for Architecture Optoelectronic Technologies (JIAOT,for YH)。
文摘To fully utilize the resources provided by optical fiber networks,a cross-band quantum light source generating photon pairs,where one photon in a pair is at C band and the other is at O band,is proposed in this work.This source is based on spontaneous four-wave mixing(SFWM)in a piece of shallow-ridge silicon waveguide.Theoretical analysis shows that the waveguide dispersion could be tailored by adjusting the ridge width,enabling broadband photon pair generation by SFWM across C band and O band.The spontaneous Raman scattering(SpRS)in silicon waveguides is also investigated experimentally.It shows that there are two regions in the spectrum of generated photons from SpRS,which could be used to achieve cross-band photon pair generation.A chip of shallow-ridge silicon waveguide samples with different ridge widths has been fabricated,through which cross-band photon pair generation is demonstrated experimentally.The experimental results show that the source can be achieved using dispersion-optimized shallow-ridge silicon waveguides.This cross-band quantum light source provides a way to develop new fiber-based quantum communication functions utilizing both C band and O band and extends applications of quantum networks.
基金supported in part by the Ministry of Science and Technology of China (G2021016032L and G2023016011L)the National Natural Science Foundation of China (12271488 and 11975145)。
文摘This paper proposes an innovative form of group reduction or similarity transformation involving off-diagonal block matrices. The proposed method is applied to the Ablowitz-Kaup-Newell-Segur(AKNS) matrix spectral problem, leading to the generation of reduced matrix AKNS integrable hierarchies. As a result, a variety of reduced multiple-component integrable nonlinear Schr??dinger and modified Korteweg-de Vries models are derived from the analysis of the reduced AKNS matrix spectral problem.
基金sponsored by the National Natural Science Foundation of China(Nos.12235007,11975131)。
文摘This paper presents a geometric perspective that connects reciprocal transformations with multidimensional integrable deformations.By interpreting conservation laws as closed 1-forms,we formalize reciprocal transformations as induced local diffeomorphisms on the jet bundle.This allows us to characterize higher-dimensional deformations as systematic fiber bundle extensions,where fiber coordinates are generated by potential functions of the conservation laws.This perspective provides an interpretation for the covariant lifting of Lax pairs to higher dimensions and reveals that auto-Backlund transformations are composite diffeomorphisms.These results are applied to several classical integrable models.
基金supported by the Singapore Ministry of Education through MOE Tier 2 grant(MOE-T2EP10223-0006)the Australia Research Council(DP190100150,DE250100232)+2 种基金Singapore-International Synchrotron Access Programme(SG-SAP)the funding support from the RIE 2025 Industry Alignment FundIndustry Collaboration Projects(IAF-ICP)(Award I2301E0023),administered by A*STARsupported by Nanofilm Technologies International Limited。
文摘The spin-sensitive nature of redox reactions in energy conversion systems,such as the oxygen evolution reaction(OER),has attracted increasing attention due to its potential for enhancing catalytic efficiency.Magnetic fields(MFs)have been proposed to enhance OER performance by influencing the spin states of oxygen intermediates.However,prior study has predominantly focused on MF effects mediated by the intrinsic magnetic properties of electrocatalysts or magnetohydrodynamics.In this work,we report a universal enhancement in OER activity,achieving over 150% increase in current density under a200 mT MF across diamagnetic,paramagnetic and magnetic electrocatalysts in 1 M KOH.Through systematic investigation of MF orientation and strength,pH,applied potentials,and the use of benzoquinone radical scavenger,we demonstrate that MF-driven performance improvements arise from direct modulation of oxygen radical spin states.Specifically,MFs promote the formation of spin-triplet oxygen intermediates(↑O–O↑),a critical step for O–O bond formation,independent of the catalyst's intrinsic magnetism.However,the local magnetic environment near the catalyst surface,governed by its magnetic properties,indirectly influences radical spin dynamics by alternating the effective field experienced by intermediates.These findings redefine the role of spin manipulation in electrocatalysis,advancing understanding of MF-driven spin effects in redox reactions.
基金financially supported by National Key R&D Program Young Scientists Project(No.2023YFC3903100)the National Natural Science Foundation of China(No.22322503)analytical and testing assistance from the Analysis and Testing Center of HUST。
文摘Switchable polymerization is emerging as a powerful tool to construct block copolymers directly from mixtures of monomers.However,current achievements typically iterate between two polymerization cycles to afford products with fixed sequences and compositions.Herein,we report the triethylborane/1,8-diazabicyclo[5.4.0]undec-7-ene(Et_3B/DBU)pair-mediated four-component switchable polymerization of propylene oxide(PO),CO_(2),phthalic anhydride(PA),and racemic lactide(rac-LA),which enables the on-demand synthesis of four different block copolymers,i.e.,poly(propylene phthalate)-b-polylactide(PPE-b-PLA),PPE-b-PLA-b-poly(propylene carbonate)(PPC),PPE-b-PPC-b-PLA,and PPE-b-PPCb-poly(propylene oxide)(PPO),through rationally modulating the Lewis pair(LP)ratio.Core to this protocol is that increasing the loading of Et_(3)B accelerates the ring-opening of PO while impeding the reactivity of rac-LA,thus allowing for fine-tuning of the thermodynamic and kinetic of the switchable polymerization.Therefore,the four polymerization cycles involving PO/PA ring-opening copolymerization(ROCOP),PO/CO_(2) ROCOP,rac-LA ring-opening polymerization(ROP),and PO ROP can be connected and discriminated in precisely programmed manners.
基金Financial support from National Key R&D Program of China (No.2023YFA1507203)National Natural Science Foundation of China (Nos.22371149 and 22188101)+3 种基金the Fundamental Research Funds for the Central Universities (No.63224098)Frontiers Science Center for New Organic Matter,Nankai University (No.63181206)Nankai University are gratefully acknowledgedthe Haihe Laboratory of Sustainable Chemical Transformations for financial support。
文摘In this study,electrochemical C-H carboxylation of benzylamines with CO_(2) was reported.This linear paired electrolysis system enables efficient and economical synthesis of value-added α-amino acids(α-AAs) under mild conditions.Various substituted benzylamines containing diverse functional groups and even highly reactive moieties,such as cyano,amide and alkene groups could be successfully transformed to the carboxylated products.Notably,this method proved to be applicable to the late-stage modification of biorelevant compounds,highlighting its potential for synthetic chemistry.Mechanistic studies such as radical trapping experiments,kinetic isotope effect(KIE) tests and cyclic voltammetry(CV) studies provided useful insight into this transformation.
基金supported by the National Natural Science Foundation of China (No.22275052)Department of Science and Technology of Hubei Province (Nos.2025AFA111 and 2024CSA076)。
文摘Achieving non-centrosymmetric(NCS) configurations in ABX3-type hybrid halides remains a critical challenge for nonlinear optical(NLO) materials due to the conflicting requirements of high second-harmonic generation(SHG) response,wide bandgap,and phase-matching capabilities.Herein,we propose a triplesite modulation strategy by synergistically tailoring the A-site cations(2-methylimidazole cation/1-ethyl-3-methylimidazole cation),B-site metals(Sn^(2+)/Pb^(2+)),and X-site halogens(Cl/Br),which effectively disrupts lattice symmetry and enables NCS crystallization.Our results demonstrate a strong SHG response,an expanded optical bandgap and increased birefringence.The optimized compound C_(6)H_(11)N_(2)PbCl_(3) exhibits a moderately strong SHG efficiency of 3.8 × KDP,a wide bandgap(3.87 eV),and enhanced birefringence(0.139@1064 nm),surpassing majority hybrid NLO materials.The innovative anionic framework introduced here broadens the scope of hybrid NLO crystals,facilitating the integration of various aromatic heterocyclic cations.This research provides a robust strategic framework for the development of advanced NLO materials.
基金supported by the National Natural Science Foundation of China (Grant Nos.12447125,12234016,and 12174317)the New Cornerstone Science Foundation。
文摘Motivated by the recent experimental discovery of superconductivity in rhombohedral tetralayer graphene,we investigate the pairing mechanism arising from the density–density interactions within the random-phase approximation.This approach successfully highlights the dominance of the chiral p-wave pairing between electrons with the same spin and valley index at low densities,while also predicting the superconducting range in agreement with experimental findings.Furthermore,we examine the characteristics of distinct superconducting regions:SC1 and SC2 exhibit chiral finite-momentum superconductivity with pronounced phase fluctuations,whereas SC4 displays zero-momentum spin-singlet superconductivity.
基金supported by the National Natural Science Foundation of China(Grant No.52573299)the Natural Science Foundation of Jiangxi province(No.20242BAB25223,20232BCJ23025,20232BCJ25040,20232BAB214024)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594).
文摘Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.
基金supported by the National Natural Science Foundation of China (Grant Nos.12474477,12550405,and 61888102)the Beijing Outstanding Young Scientist Program+4 种基金the National Key R&D Program of China (Grant No.2024YFA1207700)the Fundamental Research Funds for the Central Universitiesthe Scientific Research Innovation Capability Support Project for Young Faculty (Grant No.SRICSPYF- ZY2025071)the Robotic AI-Scientist Platform of the Chinese Academy of Sciencesfinancial support from the Flemish Research Foundation (Grant Nos.FWO/11E5821N and FWO/G0A5921N)。
文摘erized by a periodic real-space modulation of the superconducting pairing order parameter,is a novel quantum phase observed in superconducting(SC)systems.It is believed to play a key role in understanding the pseudogap phase of superconductors and has recently been discovered in bulk cuprates,transition-metal dichalcogenide,and other unconventional superconductors.However,artificially engineered PDW in designable two-dimensional materials remain rare.In this paper,we report a strain-assisted strategy to realize cooper-pair density modulation in a van der Waals heterostructure:graphene on SC 2H-NbSe2.Superconductivity is induced in graphene via the proximity effect.Meanwhile,the graphene membrane spontaneously buckles into a periodic structure owing to strain,featuring a spatially modulated local density of states(LDOS).The interplay between the spatially modulated LDOS and the proximity-induced superconductivity results in an oscillatory pair density determined by the buckled geometry,constituting an artificial PDW.This approach enables the engineering of PDWs with periodicities of up to tens of nanometers and allows their realization in a variety of heterostructures with tailored designs.Our work provides new insights into the investigation of PDW physics using predesigned two-dimensional materials.
基金support from the Heilongjiang Touyan Innovation Team Program(HITTY-20190033)National Natural Science Foundation of China(22278096)Innovation Special Project on Science and Technology for Carbon Peaking and Carbon Neutrality in Jiangsu Province(WSSJH20230015)。
文摘The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solvent-resistant Nitrate-coordinated electrolyte.The practical Ah-level graphite LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) pouch cell with the newly developed electrolyte demonstrates a significant breakthrough in cycling stability,exhibiting negligible capacity fade after 250 cycles at-30℃ and 0.1 C.NO_(3)^(-),as the functional additive,compresses the electric field around Li^(+)through electrostatic interactions,mimicking the Debye-screening effect and inducing the coordinative exclusion of free ethyl acetate molecules at low temperatures.The transformation from contact ion pairs(CIPs)formed by Pto solventseparated ion pairs is significantly restrained,which mitigates the continuous reactions between the electrolyte and inevitable lithium deposition at low temperature.Additionally,this customized inert CIPs form a solid electrolyte interphase on graphite that exhibits remarkable ionic conductivity and rigidity,preventing excessive Li dendrite growth.This finding offers new insights into the relationship of microstructure-performance for low-temperature electrolytes,demonstrating that relying solely on inert CIPs can also inhibit the decomposition of the interfacial electrolyte,and inspires a unique design concept for high-performance,commercially viable LIBs that operate reliably in sub-zero environments.
文摘Following over 20 years of research,a direct measurement of the QGP temperature has been achieved at Relativistic Heavy-Ion Collider(RHIC),free from the blue-shift effect and contamination from strong interactions.This viewpoint discusses a recent measurement of the QGP temperature at different stages at the Solenoidal Tracker at RHIC(STAR),which used e^(+)e^(-)pairs as penetrating probes.
基金support from the National Key Research and Development Program of China(2024YFB4106400)the National Natural Science Foundation of China(22269019,52472202)Hubei Province(2024BCB073,2024EHA045).
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR),powered by advanced technologies such as solid oxide electrolysis cells(SOEC),is a promising method to convert CO_(2) into valuable carbon-based products using renewable electricity.The high chemical stability of CO_(2) requires catalysts to exhibit both high activity and stable electrocatalytic performance.However,catalysts that deliver high performance in CO_(2)RR are rare and still require further improvement.Here,we report a strategy that can efficiently enhance catalyst activity through Zn doping,which introduces active frustrated Lewis pairs(FLP)to improve the catalyst's ability to activate small molecules.A high current density of-1.85 A cm^(-2)at 800℃under a bias voltage of 1.5 V was achieved using the Sr_(2)Fe_(0.8)Zn_(0.2)MoO_(6-δ)(SFZn_(0.2)M)cathode with pure CO_(2) feeding gas,surpassing previously reported results for perovskite oxide cathodes.This SOEC device also demonstrates excellent stability,with negligible degradation over tests lasting up to 110 h.
基金Supported bythe National Natural Science Foundationof China (60225007 ,60572155) the Science and Technology ResearchProject of Shanghai (04DZ07067)
文摘In the area of secure Web information system, mutual authentication and key agreement are essential between Web clients and servers. An efficient certificateless authenticated key agreement protocol for Web client/server setting is proposed, which uses pairings on certain elliptic curves. We show that the newly proposed key agreement protocol is practical and of great efficiency, meanwhile, it satisfies every desired security require ments for key agreement protocols.
基金Supported by the National Natural Science Foundation of China (60473029)
文摘Signcryption is a cryptographic primitive that performs signature and encryption simultaneously, at lower computational costs and communication overheads than the signature-then- encryption approach. In this paper, we propose an efficient multi-recipient signcryption scheme based on the bilinear pairings, which broadcasts a message to multiple users in a secure and authenticated manner. We prove its semantic security and unforgeability under the Gap Diffie-Hellman problem assumption in the random oracle model. The proposed scheme is more efficient than re-signcrypting a message n times using a signcryption scheme in terms of computational costs and communication overheads.
基金Supported by National Natural Science Foundation of China (No.60503006 and No.60403007) and Natural Science Foundation of Guangdong, China (No. 04205407).
文摘We argue that traditional identity-based systems from pairings seem unsuitable for designing group signature schemes due to the problem of key escrow. In this paper we first propose new ID-based public key systems without trusted PKG (Private Key Generator) from bilinear pairings. In our new ID-based systems, if the dishonest PKG impersonates an honest user to communicate with others, the user can provide a proof of treachery of the PKG afterwards, which is similar to certificate-based systems. Therefore, our systems reach the Girault’s trusted level 3. We then propose a group signature scheme under the new ID-based systems, the security and performance of which rely on the new systems. The size of the group public key and the length of the signature are independent on the numbers of the group.
