The functional properties of glasses are governed by their formation history and the complex relaxation processes they undergo.However,under extreme conditions,glass behaviors are still elusive.In this study,we employ...The functional properties of glasses are governed by their formation history and the complex relaxation processes they undergo.However,under extreme conditions,glass behaviors are still elusive.In this study,we employ simulations with varied protocols to evaluate the effectiveness of different descriptors in predicting mechanical properties across both low-and high-pressure regimes.Our findings demonstrate that conventional structural and configurational descriptors fail to correlate with the mechanical response following pressure release,whereas the activation energy descriptor exhibits robust linearity with shear modulus after correcting for pressure effects.Notably,the soft mode parameter emerges as an ideal and computationally efficient alternative for capturing this mechanical behavior.These findings provide critical insights into the influence of pressure on glassy properties,integrating the distinct features of compressed glasses into a unified theoretical framework.展开更多
Rare earth metal elements include lanthanide elements as well as scandium and yttrium,totaling seventeen metal elements.Due to the wide application prospects of rare earth metal elements in various fields such as lumi...Rare earth metal elements include lanthanide elements as well as scandium and yttrium,totaling seventeen metal elements.Due to the wide application prospects of rare earth metal elements in various fields such as luminescent materials,magnetic materials,catalytic materials,electronic devices,they have an important strategic position.In the field of electrocatalysis,rare earth metal elements have great potential for development due to their unique 4f electron layer structure,spin orbit coupling,high reactivity,controllable coordination number,and rich optical properties.However,there is currently a lack of systematic reviews on the modification strategies of rare earth metal elements and the latest developments in electrocatalysis.Therefore,in order to stimulate the enthusiasm of researchers,this review focuses on the application progress of rare earth metal element modified metal oxides in multiple fields such as wastewater treatment,hydrogen peroxide synthesis,hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and machine learning assisted research.In depth analysis of its electrocatalytic mechanism in various application scenarios and key factors affecting electrocatalytic performance.This review is of great significance for further developing high-performance and multifunctional electrocatalysts,and is expected to provide strong support for the development of energy,environment,and chemical industries.展开更多
The construction of rare earth(RE)alloy catalysts offers a route to harness the unique electronic structure of RE.Within the alloy,RE can fine-tune the electronic configuration of the active element,such as rhodium(Rh...The construction of rare earth(RE)alloy catalysts offers a route to harness the unique electronic structure of RE.Within the alloy,RE can fine-tune the electronic configuration of the active element,such as rhodium(Rh),via the ligand effect,optimizing the electrochemical reaction pathway.However,the challenging negative reduction potential of RE has impeded the progress in developing RE alloys,particularly nanoalloy catalysts.In this study,Rh_(3)Sc/C and Rh_(3)Y/C nanoalloys were synthesized using a sodium vapor reduction strategy for application as hydrogen evolution reaction(HER)catalysts.Elec-trochemical tests reveal that Rh-RE alloy catalysts exhibit significantly improved electrocatalytic activity in 1 mol/L KOH.Notably,Rh_(3)Y/C demonstrates exceptional HER performance,achieving a low over-potential of only 31 mV at 10 mA/cm^(2),surpassing the 50 mV observed for Rh/C.Furthermore,the current density of Rh_(3)Y/C at an 80 mV overpotential is 3.9 times that of Rh/C.This study sheds light on the remarkable catalytic potential of Rh-RE alloys,paving the way for the future expansion of RE nanoalloy systems.展开更多
In recent years,the development of ultrafast transmission electron microscopy(UTEM)has created new opportunities for studying dynamic processes at the nanoscale with unprecedented temporal resolution.~([1–3])The sign...In recent years,the development of ultrafast transmission electron microscopy(UTEM)has created new opportunities for studying dynamic processes at the nanoscale with unprecedented temporal resolution.~([1–3])The significant advances in femtosecond and even attosecond temporal resolution are achieved through the integration of the pump-probe principle with transmission electron microscopy(TEM).展开更多
Metal-organic frameworks(MOFs)with new topologies and enhanced properties can be obtained by connecting metal-organic layers(MOLs)using multifunctional linkers.However,new topologies constructed by this method using l...Metal-organic frameworks(MOFs)with new topologies and enhanced properties can be obtained by connecting metal-organic layers(MOLs)using multifunctional linkers.However,new topologies constructed by this method using linear-shaped ligands have not yet been explored.Herein,we present the design of NUT-123 by incorporating a near-linear perylene diimide(PDI)derivate,PDI-CH_(3)-COOH,into the preselected zirconium-based MOLs.3D electron diffraction confirms the successful construction of a novel topology in NUT-123.Furthermore,the uniformly dispersed PDI groups within the structure confer enhance photocatalytic capability while effectively circumventing the self-aggregation of PDI-CH_(3)-COOH.NUT-123 exhibits enhanced efficiency and selectivity in sulfide oxidation and demonstrates excellent substrate compatibility,achieving 100%conversion of various organic sulfides.Mechanistic studies indicate that the formation of sulfoxides is facilitated by concurrent electron and energy transfer.This work fills the gap in constructing a new topology by connecting MOLs with linear-shaped linkers and provides a photocatalyst for selective sulfide oxidation.展开更多
We demonstrate a bipolar graphene/F_(16)CuPc synaptic transistor(GFST)with matched p-type and n-type bipolar properties,which emulates multiplexed neurotransmission of the release of two excitatory neurotransmitters i...We demonstrate a bipolar graphene/F_(16)CuPc synaptic transistor(GFST)with matched p-type and n-type bipolar properties,which emulates multiplexed neurotransmission of the release of two excitatory neurotransmitters in graphene and F_(16)CuPc channels,separately.This process facilitates fast-switching plasticity by altering charge carriers in the separated channels.The complementary neural network for image recognition of Fashion-MNIST dataset was constructed using the matched relative amplitude and plasticity properties of the GFST dominated by holes or electrons to improve the weight regulation and recognition accuracy,achieving a pattern recognition accuracy of 83.23%.These results provide new insights to the construction of future neuromorphic systems.展开更多
On approaching the glass transition,the structural relaxation of glass-forming liquids slows down drastically,along with a significant growth of dynamic heterogeneity.Recent studies have achieved substantial advanceme...On approaching the glass transition,the structural relaxation of glass-forming liquids slows down drastically,along with a significant growth of dynamic heterogeneity.Recent studies have achieved substantial advancements in elucidating the quantitative correlations between structural relaxation and dynamic heterogeneity.Here,we present the discovery of a novel dynamic crossover with possibly universal dynamic signatures by investigating the relationship between structural relaxation and dynamic heterogeneity.Specifically,the structural relaxation time at the dynamic crossoverτ_(c)is equal to the time scale for the maximum non-Gaussian parameter,which could serve as a quantitative characterization of dynamic heterogeneity.The degree of dynamic heterogeneity at the crossover is approximately equivalent across all investigated glass-forming liquids,leading to a scaling collapse between structural relaxation and dynamic heterogeneity.Moreover,the mean squared displacement at the structural relaxation time is nearly constant across different temperatures as long as the structural relaxation time does not exceedτ_(c).We further observe that the temperature at the dynamic crossover is lower than the onset temperature of slow dynamics.Our findings thus suggest the existence of a novel dynamic crossover with possibly universal dynamic signatures in glass-forming liquids,which merits in-depth investigations.展开更多
Developing efficient and durable alkaline hydrogen evolution reaction(HER)catalysts is crucial for realizing high-performance,practical anion exchange membrane water electrolyzer(AEMWE)operating at ampere-level curren...Developing efficient and durable alkaline hydrogen evolution reaction(HER)catalysts is crucial for realizing high-performance,practical anion exchange membrane water electrolyzer(AEMWE)operating at ampere-level current densities.Although atomically dispersed Platinum(Pt)catalysts offer significant potential for enhancing atom utilization,their HER performance and durability are limited by the inflexibility in valence electron transfer between Pt and the support.In this study,we utilize asymmetrically single-atom copper(Cu)with tunable valence states as a valence electron reservoir(VER)to dynamically regulate the Pt 5d valence states,achieving efficient alkaline HER.In situ synchrotron radiation and theoretical calculations demonstrate that the dynamic evolution of the Pt 5d valence electron configuration optimizes the adsorption strengths of reaction intermediates.Meanwhile,single-atom Cu accelerates the rate-limiting water dissociation,and Pt facilitates subsequent^(*)H coupling.The catalyst requires only 23.5 and 177.2 mV overpotentials to achieve current densities of 10 and 500 mA cm^(-2)in 1 M KOH.Notably,the PtCu/NC exhibits a~57%lower hydrogen evolution barrier than Pt/NC.Moreover,the PtCu/NC-based AEMWE operates for over 600 h at an industrially relevant current density of 500 mA cm^(-2).展开更多
Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properti...Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.展开更多
Hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen ...Hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen evolution reaction(HER)/hydrazine oxidation reaction(HzOR)kinetics,is the key step.Herein,we demonstrate the development of ultrathin P/Fe co-doped NiSe_(2) nanosheets supported on modified Ni foam(P/Fe-NiSe_(2)) synthesized through a facile electrodeposition process and subsequent heat treatment.Based on electrochemical measurements,characterizations,and density functional theory calculations,a favorable“2+2”reaction mechanism with a two-step HER process and a two-step HzOR step was fully proved and the specific effect of P doping on HzOR kinetics was investigated.P/Fe-NiSe_(2) thus yields an impressive electrocatalytic performance,delivering a high current density of 100 mA cm^(−2) with potentials of−168 and 200 mV for HER and HzOR,respectively.Additionally,P/Fe-NiSe_(2) can work efficiently for hydrazine-assisted water electrolysis and Zn-Hydrazine(Zn-Hz)battery,making it promising for practical application.展开更多
Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH_(3) through the Haber-Bosch technique,carried out under severe ...Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH_(3) through the Haber-Bosch technique,carried out under severe reaction conditions,leads to substantial energy consumption and environmental pollution.It is thus imperative for NH_(3) synthesis methods to be investigated under more favorable conditions.Synthesis of ammonia by electrocatalysis can effectively reduce the environmental damage and other urgent problems,which is a promising solution.Metal-nitrogen series batteries(M-N batteries),such as metal-nitrogen gas batteries,metal-nitrogen oxide batteries and metal-oxynitride batteries have been regarded recently as an exemplar of concurrent NH_(3) synthesis and energy production.Nonetheless,the large-scale application of these batteries is still limited by numerous challenges are currently existing in building high-efficiency M-N batteries,including poor Faradic efficiency and low NH_(3) yield.Therefore,a comprehensive overview of M-N batteries is offered,specifically focusing on advanced strategies for designing highly efficient cathode catalysts in anticipation of future developments.The metal anodes,cathodic electro-reduction reactions,and design principles are encompassed in the discussion,offering detailed insights to enhance understanding.Mechanisms,feasibility analyses,technoeconomic assessments,device combinations,and comparative evaluations are delved into in the review,contributing to a thorough comprehension of diverse systems and their application potential.Perspectives and opportunities for future research directions are also delineated.展开更多
Recognized as one of the important active species involved in varicus ractions,singlet oxygen(^(1)O_(2))shows potential applications in chemical.blological,and environmental related fields.However,the con-trolled capt...Recognized as one of the important active species involved in varicus ractions,singlet oxygen(^(1)O_(2))shows potential applications in chemical.blological,and environmental related fields.However,the con-trolled capture and release of^(1)O_(2)are still facing huge challenges due to its short lifetime and high re-activity.Herein,a framework-interpenetration tuning strategy was applied on a metal-organic framework(MOF)that aiming to improve the capture and release rate of O.The porosity of the MOF was remark-ably enhanced with the structural evolution from seven-fold(termed NKM-181)to six-fold interpene-tration(termed NKM-182),and the active anthracene sites became much mare accessible.Such drastic process can be achieved as simple as exchanging the primitive MOF in selected solvent and occurred surprisingly as single-crystal to single-crystal transformation.Also,additionally owing to the unblocked regular channels,NKM-182 shown significantly improved^(1)O_(2)trapping and releasing rates compared to strates an unprecedented regulation of^(1)O_(2)capture and release that of in NKM-181.This work demon process,along with achieving the highest^(1)O_(2)capture and release rate among reported porous materi-als.furthermore.the obtalned endoperoxides with^(1)O_(2)loaded(termed EPO-NKM-181 and EPO-NKM-182)can be used as a high efficiency smart material for anti-fake application.展开更多
Artificial synapses are essential building blocks for neuromorphic electronics.Here,solid polymer electrolyte-gated artificial synapses(EGASs)were fabricated using ITO fibers as channels,which possess an ultra-high se...Artificial synapses are essential building blocks for neuromorphic electronics.Here,solid polymer electrolyte-gated artificial synapses(EGASs)were fabricated using ITO fibers as channels,which possess an ultra-high sensitivity of 5 m V and a long-term memory time exceeding 3 min.Notably,digitally printed ITO-fiber arrays exhibit an ultra-high transmittance of approximately 99.67%.Biological synaptic plasticity,such as excitatory postsynaptic current,paired-pulse facilitation,spike frequency-dependent plasticity,and synaptic potentiation and depression,were successfully mimicked using the EGASs.Based on the synaptic properties of the EGASs,an artificial neural network was constructed to perform supervised learning using the Fashion-MNIST dataset,achieving high pattern recognition rate(82.39%)due to the linear and symmetric synaptic plasticity.This work provides insights into high-sensitivity artificial synapses for future neuromorphic computing.展开更多
A flexible organic artificial synapse(OAS)for tunable time-frequency signal processing was fabricated using a tri-blend film that had been fabricated using a one-step solution method.When combined with a chitosan film...A flexible organic artificial synapse(OAS)for tunable time-frequency signal processing was fabricated using a tri-blend film that had been fabricated using a one-step solution method.When combined with a chitosan film,this OAS can achieve an ultrashort-term retention time of only 49 ms for instant electricalcomputing applications;this is the shortest retention time yet achieved by a two-terminal artificial synapse.An array of these flexible OASs can withstand a high bending strain of 5%for 10^(4) cycles;this deformation endurance is a new record.The OAS was also sensitive to the number and frequency of electrical inputs;a tunable cut-off frequency enables dynamic filtering for use in image detail enhancement.This work provides a new resource for development of future neuromorphic computing devices。展开更多
The anomalous non-Hermitian dynamical phenomenon with the non-Hermitian skin effect(NHSE)attracts wide attention due to its novel physics and promising applications.Here,we propose a new type of non-unitary discrete-t...The anomalous non-Hermitian dynamical phenomenon with the non-Hermitian skin effect(NHSE)attracts wide attention due to its novel physics and promising applications.Here,we propose a new type of non-unitary discrete-time quantum walk system demonstrating the NHSE and anomalous non-Hermitian dynamical phenomena,including the dynamical chiral phenomenon,the funneling phenomenon on the domain wall,and the anomalous reflection on the phase impurity.Furthermore,we design the quantum circuit experiments of these quantum walk systems and numerically simulate them with quantum noises to verify the robustness of the non-Hermitian dynamical phenomenon on the noisy intermediate-scale quantum(NISQ)devices.Our work paves the way for implementing the non-Hermitian dynamical phenomenon on the quantum circuit.展开更多
Electrophilic aromatic substitution(EAS)is a vital chemical reaction in organic chemistry that involves replacing substituent on an aromatic ring by an electrophile.Despite its widespread industrial applications in th...Electrophilic aromatic substitution(EAS)is a vital chemical reaction in organic chemistry that involves replacing substituent on an aromatic ring by an electrophile.Despite its widespread industrial applications in the production of substituted aromatic compounds,the reaction typically requires harsh reaction conditions,such as high temperature and potent Lewis acid catalysts,to activate the electrophile due to the stability of the aromatic ring[1].Recently,a study published by Yaping Zang and colleagues in Nature Communications demonstrates the use of an electric field as a catalyst to regulate EAS reactivity,replacing conventional chemical reagents.The research team discovered that an electric field could activate an otherwise unreactive electrophile and break inert nonpolar C-C bonds under mild conditions.These unprecedented results showcase the potential for broadening the scope of EAS reactions via electric field catalysis.展开更多
To promote the development of global carbon neutrality,perovskite solar cells(PSCs)have become a research hotspot in related fields.How to obtain PSCs with expected performance and explore the potential factors affect...To promote the development of global carbon neutrality,perovskite solar cells(PSCs)have become a research hotspot in related fields.How to obtain PSCs with expected performance and explore the potential factors affecting device performance are the research priorities in related fields.Although some classical computational methods can facilitate material development,they typically require complex mathematical approximations and manual feature screening processes,which have certain subjectivity and one-sidedness,limiting the performance of the model.In order to alleviate the above challenges,this paper proposes a machine learning(ML)model based on neural networks.The model can assist both PSCs design and analysis of their potential mechanism,demonstrating enhanced and comprehensive auxiliary capabilities.To make the model have higher feasibility and fit the real experimental process more closely,this paper collects the corresponding real experimental data from numerous research papers to develop the model.Compared with other classical ML methods,the proposed model achieved better overall performance.Regarding analysis of underlying mechanism,the relevant laws explored by the model are consistent with the actual experiment results of existing articles.The model exhibits great potential to discover complex laws that are difficult for humans to discover directly.In addition,we also fabricated PSCs to verify the guidance ability of the model in this paper for real experiments.Eventually,the model achieved acceptable results.This work provides new insights into integrating ML methods and PSC design techniques,as well as bridging photovoltaic power generation technology and other fields.展开更多
Manipulating magnetic domain structure plays a key role in advanced spintronics devices.Theoretical rationale is that the labyrinthine domain structure,normally appearing in ferromagnetic thin films with strong magnet...Manipulating magnetic domain structure plays a key role in advanced spintronics devices.Theoretical rationale is that the labyrinthine domain structure,normally appearing in ferromagnetic thin films with strong magnetic anisotropy,shows a great potential to increase data storage density for designing magnetic nonvolatile memory and logic devices.However,an electrical control of labyrinthine domain structure remains elusive.Here,we demonstrate the gate-driven evolution of labyrinthine domain structures in an itinerant ferromagnet Cr_(7)Te_(8).By combining electric transport measurements and micromagnetic finite difference simulations,we find that the hysteresis loop of anomalous Hall effect in Cr_(7)Te_(8)samples shows distinct features corresponding to the generation of labyrinthine domain structures.The labyrinthine domain structures are found to be electrically tunable via Li-electrolyte gating,and such gate-driven evolution in Cr_(7)Te_(8)originates from the reduction of the magnetic anisotropic energy with gating,revealed by our micromagnetic simulations.Our results on the gate control of anomalous Hall effect in an itinerant magnetic material provide an opportunity to understand the formation and evolution of labyrinthine domain structures,paving a new route towards electric-field driven spintronics.展开更多
Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality...Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality,hidden contamination,and complex treatment requirements.Current research focuses on advanced treatment technologies,among which the advanced oxidation process(AOPs) of peroxomonosulfate(PMS) has great potential.Although there are many reviews of PMS-based AOP,most of them focus on surface water.This review aims to explore the activation reaction of PMS to groundwater by in-situ chemical oxidation(ISCO) technology,further study the reaction mechanism,compare the treatment effect of characteristic pollutants in the groundwater of the chemical industry park,propose new activation methods and catalyst selection,and provide guidance for future groundwater treatment research.展开更多
Developing NO_(2)−reduction reaction(NO_(2)−RR)and oxygen evolution reaction(OER)bifunctional electrocatalysts at large current densities is crucial for decreasing energy consumption of electrocatalytic NH3 production...Developing NO_(2)−reduction reaction(NO_(2)−RR)and oxygen evolution reaction(OER)bifunctional electrocatalysts at large current densities is crucial for decreasing energy consumption of electrocatalytic NH3 production and booming sustainable nitrogenbased economy.In addition to increasing active sites of catalysts,bubble adhesion deserves more attention during high-current electrolysis,which can deteriorate mass transfer and block active sites in gas-involving environments.Herein,super-hydrophilic/aerophobic cobalt-nickel-iron layered double hydroxide[Co(OH)_(2)/NiFe LDH]core-shell heterostructures were developed as efficient NO_(2)−RR and OER electrocatalysts to optimize surface tension due to self-pumping effect and modify active hydrogen adsorption behavior owing to moderate work function difference between Co(OH)_(2)and NiFe LDH.The fabricated Co(OH)_(2)/NiFe LDH exhibited excellent NO_(2)−RR activity(yield:50 mg h^(−1)cm^(−2);FE:91%at−500 mA cm^(−2))and impressive OER behavior(η1000:340 mV)accompanied by remarkable application potential for renewable energy-driven two-electrode system to produce NH3.This effort revealed important insights into the development of electrodes for reaching cost-effective electrocatalytic ammonia production at large current densities.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos.T2325004 and 52161160330)the National Natural Science Foundation of China (Grants No.12504233)+2 种基金Advanced MaterialsNational Science and Technology Major Project (Grant No.2024ZD0606900)the Talent Hub for “AI+New Materials” Basic Researchthe Key Research and Development Program of Ningbo (Grant No.2025Z088)。
文摘The functional properties of glasses are governed by their formation history and the complex relaxation processes they undergo.However,under extreme conditions,glass behaviors are still elusive.In this study,we employ simulations with varied protocols to evaluate the effectiveness of different descriptors in predicting mechanical properties across both low-and high-pressure regimes.Our findings demonstrate that conventional structural and configurational descriptors fail to correlate with the mechanical response following pressure release,whereas the activation energy descriptor exhibits robust linearity with shear modulus after correcting for pressure effects.Notably,the soft mode parameter emerges as an ideal and computationally efficient alternative for capturing this mechanical behavior.These findings provide critical insights into the influence of pressure on glassy properties,integrating the distinct features of compressed glasses into a unified theoretical framework.
基金supported by the National Key Research and Development Program of China(No.2023YFC3708005)The Fundamental Research Funds for the Central Universities,Nankai University(No.63241208)supported by the National Natural Science Foundation of China(Nos.21872102 and 22172080)。
文摘Rare earth metal elements include lanthanide elements as well as scandium and yttrium,totaling seventeen metal elements.Due to the wide application prospects of rare earth metal elements in various fields such as luminescent materials,magnetic materials,catalytic materials,electronic devices,they have an important strategic position.In the field of electrocatalysis,rare earth metal elements have great potential for development due to their unique 4f electron layer structure,spin orbit coupling,high reactivity,controllable coordination number,and rich optical properties.However,there is currently a lack of systematic reviews on the modification strategies of rare earth metal elements and the latest developments in electrocatalysis.Therefore,in order to stimulate the enthusiasm of researchers,this review focuses on the application progress of rare earth metal element modified metal oxides in multiple fields such as wastewater treatment,hydrogen peroxide synthesis,hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and machine learning assisted research.In depth analysis of its electrocatalytic mechanism in various application scenarios and key factors affecting electrocatalytic performance.This review is of great significance for further developing high-performance and multifunctional electrocatalysts,and is expected to provide strong support for the development of energy,environment,and chemical industries.
基金the National Natural Science Foundation of China(22371131)the 111 Project from China(B18030)+5 种基金the Beijing-Tianjin-Hebei Collaborative Innovation Project(19YFSLQY00030)the Outstanding Youth Project of Tianjin Natural Science Foundation(20JCJQJC00130)the Key Project of Tianjin Natural Science Foundation(20JCZDJC00650)the opening fund of Key Laboratory of Rare Earths,Chinese Academy of Sciencesthe Functional Research Funds for the Central Universities,Nankai University(63186005)Tianjin Key Lab for Rare Earth Materials and Applications(ZB19500202).
文摘The construction of rare earth(RE)alloy catalysts offers a route to harness the unique electronic structure of RE.Within the alloy,RE can fine-tune the electronic configuration of the active element,such as rhodium(Rh),via the ligand effect,optimizing the electrochemical reaction pathway.However,the challenging negative reduction potential of RE has impeded the progress in developing RE alloys,particularly nanoalloy catalysts.In this study,Rh_(3)Sc/C and Rh_(3)Y/C nanoalloys were synthesized using a sodium vapor reduction strategy for application as hydrogen evolution reaction(HER)catalysts.Elec-trochemical tests reveal that Rh-RE alloy catalysts exhibit significantly improved electrocatalytic activity in 1 mol/L KOH.Notably,Rh_(3)Y/C demonstrates exceptional HER performance,achieving a low over-potential of only 31 mV at 10 mA/cm^(2),surpassing the 50 mV observed for Rh/C.Furthermore,the current density of Rh_(3)Y/C at an 80 mV overpotential is 3.9 times that of Rh/C.This study sheds light on the remarkable catalytic potential of Rh-RE alloys,paving the way for the future expansion of RE nanoalloy systems.
文摘In recent years,the development of ultrafast transmission electron microscopy(UTEM)has created new opportunities for studying dynamic processes at the nanoscale with unprecedented temporal resolution.~([1–3])The significant advances in femtosecond and even attosecond temporal resolution are achieved through the integration of the pump-probe principle with transmission electron microscopy(TEM).
基金supported by the Natural Science Foundation of Jiangsu Province(BK20231270)the National Science Fund for Distinguished Young Scholars(22125804).
文摘Metal-organic frameworks(MOFs)with new topologies and enhanced properties can be obtained by connecting metal-organic layers(MOLs)using multifunctional linkers.However,new topologies constructed by this method using linear-shaped ligands have not yet been explored.Herein,we present the design of NUT-123 by incorporating a near-linear perylene diimide(PDI)derivate,PDI-CH_(3)-COOH,into the preselected zirconium-based MOLs.3D electron diffraction confirms the successful construction of a novel topology in NUT-123.Furthermore,the uniformly dispersed PDI groups within the structure confer enhance photocatalytic capability while effectively circumventing the self-aggregation of PDI-CH_(3)-COOH.NUT-123 exhibits enhanced efficiency and selectivity in sulfide oxidation and demonstrates excellent substrate compatibility,achieving 100%conversion of various organic sulfides.Mechanistic studies indicate that the formation of sulfoxides is facilitated by concurrent electron and energy transfer.This work fills the gap in constructing a new topology by connecting MOLs with linear-shaped linkers and provides a photocatalyst for selective sulfide oxidation.
基金supported by the Shenzhen Science and Technology Program(No.JCYJ20210324121002008)the National Science Fund for Distinguished Young Scholars of China(No.T2125005)+5 种基金the National Key R&D Program of China(Nos.2022YFE0198200,2022YFA1204500,and 2022YFA1204504)the Natural Science Foundation of Tianjin(Nos.22JCYBJC01290 and 23JCQNJC01440)the Key Project of Natural Science Foundation of Tianjin(No.22JCZDJC00120)the Fundamental Research Funds for the Central Universities,Nankai University(Nos.BEG124901 and BEG124401)the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515110319)the Key Science and Technology Program of Henan Province(No.242102210171).
文摘We demonstrate a bipolar graphene/F_(16)CuPc synaptic transistor(GFST)with matched p-type and n-type bipolar properties,which emulates multiplexed neurotransmission of the release of two excitatory neurotransmitters in graphene and F_(16)CuPc channels,separately.This process facilitates fast-switching plasticity by altering charge carriers in the separated channels.The complementary neural network for image recognition of Fashion-MNIST dataset was constructed using the matched relative amplitude and plasticity properties of the GFST dominated by holes or electrons to improve the weight regulation and recognition accuracy,achieving a pattern recognition accuracy of 83.23%.These results provide new insights to the construction of future neuromorphic systems.
基金support from the National Natural Science Foundation of China(Grant Nos.12374202 and 12004001)Anhui Projects(Grant Nos.2022AH020009,S020218016,and Z010118169),and Hefei City(Grant No.Z020132009)+3 种基金support from the National Natural Science Foundation of China(Grant Nos.T2325004 and 52161160330)Advanced Materials-National Science and Technology Major Project(Grant No.2024ZD0606900)the Talent Hub for“AI+New Materials”Basic ResearchHefei Advanced Computing Center,Beijing Super Cloud Computing Center,and the High-Performance Computing Platform of Anhui University for providing computing resources.
文摘On approaching the glass transition,the structural relaxation of glass-forming liquids slows down drastically,along with a significant growth of dynamic heterogeneity.Recent studies have achieved substantial advancements in elucidating the quantitative correlations between structural relaxation and dynamic heterogeneity.Here,we present the discovery of a novel dynamic crossover with possibly universal dynamic signatures by investigating the relationship between structural relaxation and dynamic heterogeneity.Specifically,the structural relaxation time at the dynamic crossoverτ_(c)is equal to the time scale for the maximum non-Gaussian parameter,which could serve as a quantitative characterization of dynamic heterogeneity.The degree of dynamic heterogeneity at the crossover is approximately equivalent across all investigated glass-forming liquids,leading to a scaling collapse between structural relaxation and dynamic heterogeneity.Moreover,the mean squared displacement at the structural relaxation time is nearly constant across different temperatures as long as the structural relaxation time does not exceedτ_(c).We further observe that the temperature at the dynamic crossover is lower than the onset temperature of slow dynamics.Our findings thus suggest the existence of a novel dynamic crossover with possibly universal dynamic signatures in glass-forming liquids,which merits in-depth investigations.
基金supported by the Ningbo Top-Talent Team Program,Program for the National Natural Science Foundation of China(22106166)the Yongjiang Innovative Individual Introduction of China,and the China Postdoctoral Science Foundation(2022M723253)。
文摘Developing efficient and durable alkaline hydrogen evolution reaction(HER)catalysts is crucial for realizing high-performance,practical anion exchange membrane water electrolyzer(AEMWE)operating at ampere-level current densities.Although atomically dispersed Platinum(Pt)catalysts offer significant potential for enhancing atom utilization,their HER performance and durability are limited by the inflexibility in valence electron transfer between Pt and the support.In this study,we utilize asymmetrically single-atom copper(Cu)with tunable valence states as a valence electron reservoir(VER)to dynamically regulate the Pt 5d valence states,achieving efficient alkaline HER.In situ synchrotron radiation and theoretical calculations demonstrate that the dynamic evolution of the Pt 5d valence electron configuration optimizes the adsorption strengths of reaction intermediates.Meanwhile,single-atom Cu accelerates the rate-limiting water dissociation,and Pt facilitates subsequent^(*)H coupling.The catalyst requires only 23.5 and 177.2 mV overpotentials to achieve current densities of 10 and 500 mA cm^(-2)in 1 M KOH.Notably,the PtCu/NC exhibits a~57%lower hydrogen evolution barrier than Pt/NC.Moreover,the PtCu/NC-based AEMWE operates for over 600 h at an industrially relevant current density of 500 mA cm^(-2).
基金supported by the National Natural Science Foundation of China(21875118,22111530112)the support from the Smart Sensing Interdisciplinary Science Center,Nankai University。
文摘Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.
基金supported by the National Natural Science Foundation of China(22179065,22111530112,21875118)the Tianjin Graduate Research and Innovation Project(2022BKY018)the Ph.D.Candidate Research Innovation Fund of NKU School of Materials Science and Engineering.
文摘Hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen evolution reaction(HER)/hydrazine oxidation reaction(HzOR)kinetics,is the key step.Herein,we demonstrate the development of ultrathin P/Fe co-doped NiSe_(2) nanosheets supported on modified Ni foam(P/Fe-NiSe_(2)) synthesized through a facile electrodeposition process and subsequent heat treatment.Based on electrochemical measurements,characterizations,and density functional theory calculations,a favorable“2+2”reaction mechanism with a two-step HER process and a two-step HzOR step was fully proved and the specific effect of P doping on HzOR kinetics was investigated.P/Fe-NiSe_(2) thus yields an impressive electrocatalytic performance,delivering a high current density of 100 mA cm^(−2) with potentials of−168 and 200 mV for HER and HzOR,respectively.Additionally,P/Fe-NiSe_(2) can work efficiently for hydrazine-assisted water electrolysis and Zn-Hydrazine(Zn-Hz)battery,making it promising for practical application.
基金National Natural Science Foundation of China (22179065)Tianjin Graduate Research and Innovation Project (2022BKY018)。
文摘Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH_(3) through the Haber-Bosch technique,carried out under severe reaction conditions,leads to substantial energy consumption and environmental pollution.It is thus imperative for NH_(3) synthesis methods to be investigated under more favorable conditions.Synthesis of ammonia by electrocatalysis can effectively reduce the environmental damage and other urgent problems,which is a promising solution.Metal-nitrogen series batteries(M-N batteries),such as metal-nitrogen gas batteries,metal-nitrogen oxide batteries and metal-oxynitride batteries have been regarded recently as an exemplar of concurrent NH_(3) synthesis and energy production.Nonetheless,the large-scale application of these batteries is still limited by numerous challenges are currently existing in building high-efficiency M-N batteries,including poor Faradic efficiency and low NH_(3) yield.Therefore,a comprehensive overview of M-N batteries is offered,specifically focusing on advanced strategies for designing highly efficient cathode catalysts in anticipation of future developments.The metal anodes,cathodic electro-reduction reactions,and design principles are encompassed in the discussion,offering detailed insights to enhance understanding.Mechanisms,feasibility analyses,technoeconomic assessments,device combinations,and comparative evaluations are delved into in the review,contributing to a thorough comprehension of diverse systems and their application potential.Perspectives and opportunities for future research directions are also delineated.
基金the financial support of the National Natural Science Foundation of China(Nos.22035003 and 22201137)Nature Science Fund of Tianjin,China(No.19JCZDJC37200)+1 种基金Fundamental Research Funds for the Central Universities(No.63223020)the Haihe Laboratory of Sustainable Chemical Transformations(No.YYJC202101).
文摘Recognized as one of the important active species involved in varicus ractions,singlet oxygen(^(1)O_(2))shows potential applications in chemical.blological,and environmental related fields.However,the con-trolled capture and release of^(1)O_(2)are still facing huge challenges due to its short lifetime and high re-activity.Herein,a framework-interpenetration tuning strategy was applied on a metal-organic framework(MOF)that aiming to improve the capture and release rate of O.The porosity of the MOF was remark-ably enhanced with the structural evolution from seven-fold(termed NKM-181)to six-fold interpene-tration(termed NKM-182),and the active anthracene sites became much mare accessible.Such drastic process can be achieved as simple as exchanging the primitive MOF in selected solvent and occurred surprisingly as single-crystal to single-crystal transformation.Also,additionally owing to the unblocked regular channels,NKM-182 shown significantly improved^(1)O_(2)trapping and releasing rates compared to strates an unprecedented regulation of^(1)O_(2)capture and release that of in NKM-181.This work demon process,along with achieving the highest^(1)O_(2)capture and release rate among reported porous materi-als.furthermore.the obtalned endoperoxides with^(1)O_(2)loaded(termed EPO-NKM-181 and EPO-NKM-182)can be used as a high efficiency smart material for anti-fake application.
基金supported by the National Science Fund for Distinguished Young Scholars of China(No.T2125005)the National Key R&D Program of China(Nos.2022YFE0198200,2022YFA1204500,2022YFA1204504)+3 种基金the Shenzhen Science and Technology Project(No.JCYJ20210324121002008)the Natural Science Foundation of Tianjin(Nos.22JCYBJC01290,23JCQNJC01440)the Key Project of Nature Science Foundation of Tianjin(No.22JCZDJC00120)the Fundamental Research Funds for the Central Universities,Nankai University(Nos.BEG124901,BEG124401)。
文摘Artificial synapses are essential building blocks for neuromorphic electronics.Here,solid polymer electrolyte-gated artificial synapses(EGASs)were fabricated using ITO fibers as channels,which possess an ultra-high sensitivity of 5 m V and a long-term memory time exceeding 3 min.Notably,digitally printed ITO-fiber arrays exhibit an ultra-high transmittance of approximately 99.67%.Biological synaptic plasticity,such as excitatory postsynaptic current,paired-pulse facilitation,spike frequency-dependent plasticity,and synaptic potentiation and depression,were successfully mimicked using the EGASs.Based on the synaptic properties of the EGASs,an artificial neural network was constructed to perform supervised learning using the Fashion-MNIST dataset,achieving high pattern recognition rate(82.39%)due to the linear and symmetric synaptic plasticity.This work provides insights into high-sensitivity artificial synapses for future neuromorphic computing.
基金supported by the National Key R&D Program of China(Nos.2022YFE0198200,2022YFA1200044)the National Science Fund for Distinguished Young Scholars of China(No.T2125005)+1 种基金the Tianjin Science Foundation for Distinguished Young Scholars(No.19JCJQJC61000)the Shenzhen Science and Technology Project(No.JCYj20210324121002008).
文摘A flexible organic artificial synapse(OAS)for tunable time-frequency signal processing was fabricated using a tri-blend film that had been fabricated using a one-step solution method.When combined with a chitosan film,this OAS can achieve an ultrashort-term retention time of only 49 ms for instant electricalcomputing applications;this is the shortest retention time yet achieved by a two-terminal artificial synapse.An array of these flexible OASs can withstand a high bending strain of 5%for 10^(4) cycles;this deformation endurance is a new record.The OAS was also sensitive to the number and frequency of electrical inputs;a tunable cut-off frequency enables dynamic filtering for use in image detail enhancement.This work provides a new resource for development of future neuromorphic computing devices。
基金Project supported by the National Key R&D Program of China (Grant No. 2022YFA1403901)the National Natural Science Foundation of China (Grant No. NSFC-11888101)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences (Grant No. XDB28000000)New Cornerstone Investigator Programsupported by the fellowship of China National Postdoctoral Program for Innovative Talents (Grant No. BX2021300)
文摘The anomalous non-Hermitian dynamical phenomenon with the non-Hermitian skin effect(NHSE)attracts wide attention due to its novel physics and promising applications.Here,we propose a new type of non-unitary discrete-time quantum walk system demonstrating the NHSE and anomalous non-Hermitian dynamical phenomena,including the dynamical chiral phenomenon,the funneling phenomenon on the domain wall,and the anomalous reflection on the phase impurity.Furthermore,we design the quantum circuit experiments of these quantum walk systems and numerically simulate them with quantum noises to verify the robustness of the non-Hermitian dynamical phenomenon on the noisy intermediate-scale quantum(NISQ)devices.Our work paves the way for implementing the non-Hermitian dynamical phenomenon on the quantum circuit.
文摘Electrophilic aromatic substitution(EAS)is a vital chemical reaction in organic chemistry that involves replacing substituent on an aromatic ring by an electrophile.Despite its widespread industrial applications in the production of substituted aromatic compounds,the reaction typically requires harsh reaction conditions,such as high temperature and potent Lewis acid catalysts,to activate the electrophile due to the stability of the aromatic ring[1].Recently,a study published by Yaping Zang and colleagues in Nature Communications demonstrates the use of an electric field as a catalyst to regulate EAS reactivity,replacing conventional chemical reagents.The research team discovered that an electric field could activate an otherwise unreactive electrophile and break inert nonpolar C-C bonds under mild conditions.These unprecedented results showcase the potential for broadening the scope of EAS reactions via electric field catalysis.
基金financially supported by the National Natural Science Foundation of China(NSFC)project(Authorization Number:61771261)。
文摘To promote the development of global carbon neutrality,perovskite solar cells(PSCs)have become a research hotspot in related fields.How to obtain PSCs with expected performance and explore the potential factors affecting device performance are the research priorities in related fields.Although some classical computational methods can facilitate material development,they typically require complex mathematical approximations and manual feature screening processes,which have certain subjectivity and one-sidedness,limiting the performance of the model.In order to alleviate the above challenges,this paper proposes a machine learning(ML)model based on neural networks.The model can assist both PSCs design and analysis of their potential mechanism,demonstrating enhanced and comprehensive auxiliary capabilities.To make the model have higher feasibility and fit the real experimental process more closely,this paper collects the corresponding real experimental data from numerous research papers to develop the model.Compared with other classical ML methods,the proposed model achieved better overall performance.Regarding analysis of underlying mechanism,the relevant laws explored by the model are consistent with the actual experiment results of existing articles.The model exhibits great potential to discover complex laws that are difficult for humans to discover directly.In addition,we also fabricated PSCs to verify the guidance ability of the model in this paper for real experiments.Eventually,the model achieved acceptable results.This work provides new insights into integrating ML methods and PSC design techniques,as well as bridging photovoltaic power generation technology and other fields.
基金supported by the National Natural Science Foundation of China(Grant Nos.92365203,52072168,51861145201,52302180,and 12204232)the National Key Research and Development Program of China(Grant No.2021YFA1202901)+1 种基金the Science and Technology Development Project of Henan Province(Grant No.242102230140)the China Postdoctoral Science Foundation(Grant No.2024M750775)。
文摘Manipulating magnetic domain structure plays a key role in advanced spintronics devices.Theoretical rationale is that the labyrinthine domain structure,normally appearing in ferromagnetic thin films with strong magnetic anisotropy,shows a great potential to increase data storage density for designing magnetic nonvolatile memory and logic devices.However,an electrical control of labyrinthine domain structure remains elusive.Here,we demonstrate the gate-driven evolution of labyrinthine domain structures in an itinerant ferromagnet Cr_(7)Te_(8).By combining electric transport measurements and micromagnetic finite difference simulations,we find that the hysteresis loop of anomalous Hall effect in Cr_(7)Te_(8)samples shows distinct features corresponding to the generation of labyrinthine domain structures.The labyrinthine domain structures are found to be electrically tunable via Li-electrolyte gating,and such gate-driven evolution in Cr_(7)Te_(8)originates from the reduction of the magnetic anisotropic energy with gating,revealed by our micromagnetic simulations.Our results on the gate control of anomalous Hall effect in an itinerant magnetic material provide an opportunity to understand the formation and evolution of labyrinthine domain structures,paving a new route towards electric-field driven spintronics.
基金supported by the National Key Research and Development Program of China (No.2023YFC3708005)the National Natural Science Foundation of China (Nos.21872102,22172080)the Fundamental Research Funds for the Central Universities (Nankai University,No.63241208)。
文摘Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality,hidden contamination,and complex treatment requirements.Current research focuses on advanced treatment technologies,among which the advanced oxidation process(AOPs) of peroxomonosulfate(PMS) has great potential.Although there are many reviews of PMS-based AOP,most of them focus on surface water.This review aims to explore the activation reaction of PMS to groundwater by in-situ chemical oxidation(ISCO) technology,further study the reaction mechanism,compare the treatment effect of characteristic pollutants in the groundwater of the chemical industry park,propose new activation methods and catalyst selection,and provide guidance for future groundwater treatment research.
基金supported by the National Natural Science Foundation of China(NSFCgrant no.22179065).
文摘Developing NO_(2)−reduction reaction(NO_(2)−RR)and oxygen evolution reaction(OER)bifunctional electrocatalysts at large current densities is crucial for decreasing energy consumption of electrocatalytic NH3 production and booming sustainable nitrogenbased economy.In addition to increasing active sites of catalysts,bubble adhesion deserves more attention during high-current electrolysis,which can deteriorate mass transfer and block active sites in gas-involving environments.Herein,super-hydrophilic/aerophobic cobalt-nickel-iron layered double hydroxide[Co(OH)_(2)/NiFe LDH]core-shell heterostructures were developed as efficient NO_(2)−RR and OER electrocatalysts to optimize surface tension due to self-pumping effect and modify active hydrogen adsorption behavior owing to moderate work function difference between Co(OH)_(2)and NiFe LDH.The fabricated Co(OH)_(2)/NiFe LDH exhibited excellent NO_(2)−RR activity(yield:50 mg h^(−1)cm^(−2);FE:91%at−500 mA cm^(−2))and impressive OER behavior(η1000:340 mV)accompanied by remarkable application potential for renewable energy-driven two-electrode system to produce NH3.This effort revealed important insights into the development of electrodes for reaching cost-effective electrocatalytic ammonia production at large current densities.
