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
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
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
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
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
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
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
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
Stimuli-responsive coordination polymers(CPs)are among one of the most prolific research areas in developing the next-generation functional materials.Their capability of being accurately excited by particular external...Stimuli-responsive coordination polymers(CPs)are among one of the most prolific research areas in developing the next-generation functional materials.Their capability of being accurately excited by particular external changes with pre-determined and observable/characterizable behaviors correspond,are the so called“stimuli”and“responsive”.Abundant types of CP compounds,especially metal-organic frameworks(MOFs),are of rocketing interest owing to their compositional diversity,structural tunability,and in essence their highly engineerable functionality.This present review is aimed to sketch several common types of stimulation and the corresponding responses for CPs,accompanied with the broad logic and mechanisms underneath.And further from the aspect of material revolution,some representative progresses together with the latest advances of CP-based materials in various fields are covered in attempt to display a broader picture towards the possible prospects of this topic.展开更多
The development of renewable woods for power generation can help improve the energy efficiency of buildings,and promote the concept design and implementation of“smart buildings”.Here,with specific chemical treatment...The development of renewable woods for power generation can help improve the energy efficiency of buildings,and promote the concept design and implementation of“smart buildings”.Here,with specific chemical treatment and hydrothermal synthesis,we demonstrated the practical value of natural wood for thermoelectric power generation in smart buildings.The prepared wood-based thermoelectric sponges show high Seebeck coefficients of 320.5 and 436.6μV/K in the vertical and parallel directions of the longitudinal channel of wood.After 500 cycles of the compressive strain at 20%,the corresponding Seebeck coefficients increase up to 413.4 and 502.1μV/K,respectively,which is attributed to the improved contact and connection between tellurium thermoelectric nanowires.The Seebeck coefficients are much larger than those of most reported inorganic thermoelectric materials.Meanwhile,the thermoelectric sponges maintain excellent thermoelectric and mechanical stability.We further modeled the application value of wood-based thermoelectric sponges in smart buildings for power generation.Relatively high thermoelectric electricity can be obtained,such as in Beijing with over 1.5 million kWh every year,demonstrating the great potential in thermal energy harvest and energy supply.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
Flexible epidermal sensors assume an indispensable role in the field of wearable electronics,enabling the imperceptible detection of biomechanical signals for personalized health care.As an integral part,solution-proc...Flexible epidermal sensors assume an indispensable role in the field of wearable electronics,enabling the imperceptible detection of biomechanical signals for personalized health care.As an integral part,solution-processed ultrathin nanocomposite conductors with high strain sensitivity offer cost-effectiveness and scalability for sensor manufacturing.Nevertheless,their controllable fabrication remains a challenge,and the presence of abundant polymers usually lead to high hysteresis and unsatisfactory sensitivity for low strain detection.Here,a robust,unform,and highly conductive silver nanofilm is prepared through Layer-by-Layer(LbL)assembly by combining positively charged polyurethane and uniformly sized silver nanoparticles(AgNPs)on desired substrates.Subsequent photonic sintering is used to fuse the AgNPs into a cohesive structure and mitigate uncontrollable heat-induced cracks in the Ag nanofilm owing to continuous thermal expansion from underlying elastomeric substrates.Consequently,the Ag nanofilms achieve a conductivity of 5.1×10^(4)S cm^(−1),and demonstrate substrate-dependent electromechanical properties.In particular,the LbL assembled Ag nanofilms on oxygen plasma-treated polydimethylsiloxane(PDMS)can serve as hypersensitive sensors with gauge factors of more than 3000 at strains of less than 5%,or they are stretchable with small resistance variations to more than 50%on(3-aminopropyl)triethoxysilane modified PDMS or other thermoplastic elastomers.Mechanisms on this substrate dependent electromechanical properties are investigated,and the ultrasensitive strain sensors on PDMS are demonstrated for the detection of sound frequencies,pulses,and small forces.展开更多
Comprehensive Summary Herein,the temperature-and pressure-stimulated responsive behavior as well as crystal-glass phase transition of a new zero-dimensional hybrid manganese bromide[4-MTPP]2[MnBr4][4-MTPP+=(4-methoxyb...Comprehensive Summary Herein,the temperature-and pressure-stimulated responsive behavior as well as crystal-glass phase transition of a new zero-dimensional hybrid manganese bromide[4-MTPP]2[MnBr4][4-MTPP+=(4-methoxybenzyl)tris(phenyl)phosphonium]were reported.Our experiment results demonstrate that[4-MTPP]2[MnBr4]shows typical green photoluminescence emission centered at 522.4 nm excited by UV light.展开更多
The generation and amplification of chirality in inorganic nanomaterials have garnered significant attention due to their promising applications in enantioselective catalysis,chiral sensing,and optoelectronics.Interfa...The generation and amplification of chirality in inorganic nanomaterials have garnered significant attention due to their promising applications in enantioselective catalysis,chiral sensing,and optoelectronics.Interface-driven self-assembly has emerged as a robust and versatile strategy to induce and enhance chirality in these systems,offering precise control over the spatial organization of nanoscale building blocks.This review presents a comprehensive overview of recent advancements in interface-driven selfassembly techniques,focusing on how these methods facilitate the generation and amplification of chiroptical properties in inorganic nanomaterials.We examine the strategies of interface-driven self-assembly through external torsion,aggregation amplification,and chiral molecule induction,highlighting key mechanisms that contribute to enhanced chiral responses.Self-assembly processes at liquid-liquid,gas-liquid,and liquid-solid interfaces are critically discussed,along with the influence of parameters,such as nanoparticle shape,surface ligand composition,and external stimuli on the formation of chiral nanostructures.Additionally,theoretical models describing the emergence of chirality are examined,providing insights into the role of interfacial molecular interactions in driving observed chiroptical effects.Finally,we review the applications of these chiral nanomaterials in spintronics,chiral photonics,and beyond,and propose future directions for advancing the design and development of novel chiral inorganic nanomaterials.This robust strategy holds great potential for facilitating breakthroughs in both the fundamental understanding and the practical implementation of chiral nanostructures.展开更多
The conventional design of metal-organic frameworks(MOFs)with room-temperature phosphorescence(RTP)mostly relies on using heavy metals,as the heavy atom effect can effectively increase the efficiency of intersystem cr...The conventional design of metal-organic frameworks(MOFs)with room-temperature phosphorescence(RTP)mostly relies on using heavy metals,as the heavy atom effect can effectively increase the efficiency of intersystem crossing(ISC)to get a better phosphorescence performance.For the first time,we reported the highly efficient RTP of a lithium-based MOF IMU-101 with a lifetime(τ)of 299 ms and a quantum yield(QY)of 4.91%.In addition,MOFs IMU-102 and IMU-103,with sodium and cesium as metal nodes,were successfully synthesized.The phosphorescence properties of this series of alkali metal MOFs were systematically studied and compared.The crystallography and computational calculation show that the mechanism for achieving RTP for this material lies in the ultrashort coordination bond of Li,which enables the reduction of non-radiative transitions.IMU-101,as a cheap and environmentally friendly room-temperature phosphorescent material,has been further developed into composite polymer inks and bulk materials.This makes them promising for applications in anti-counterfeiting and information encryption.展开更多
Metabolism,transpiration,and invasion of pathogens during the storage and transportation of fruits can lead to significant waste and even food safety issues.Therefore,real-time,rapid,and accurate non-destructive monit...Metabolism,transpiration,and invasion of pathogens during the storage and transportation of fruits can lead to significant waste and even food safety issues.Therefore,real-time,rapid,and accurate non-destructive monitoring of physiological information during the storage of fruits and vegetables to assess fruit freshness is crucial.Herein,we engineered a degradable and multifunctional humidity sensing film for monitoring fruit freshness.The film is fabricated through the co-assembly of bagasse cellulose nanocrystals(CNC),okra polysaccharides(OPs),silver nanowires(Ag NWs),and phytic acid(PA),utilizing dynamic hydrogen and phosphate bonds.This innovative design endows the CNC/OPs/PA/Ag NWs(COPA)composite film with outstanding mechanical properties,water resistance,low water vapor permeability,antibacterial,degradability,and moisture-sensing ability.Notably,the proposed COPA humidity sensor exhibits high linearity(R^(2)=0.994),ultralow hysteresis(1.24%),and 32 days of operational stability across a 35%–98%relative humidity(RH)range,enabling precise freshness monitoring during fruit storage.Significantly,the COPA film prolonged the shelf-life of packaged fruit when compared to conventional PE film packaging.This research establishes a foundational framework for next-generation smart sensors in food quality management and biomedical monitoring applications.展开更多
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.
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.
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 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 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.
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This work was supported by the National Key Research and Development Program of China(2022YFA1502901)the National Natural Science Foundation of China[22035003,22371137 and 22201137]+3 种基金the Nature Science Fund of Tianjin,China[19JCZDJC37200]the Fundamental Research Funds for the Central Universities[63233040]the Haihe Laboratory of Sustainable Chemical Transformations[YYJC202101]the Science Foundation of State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter[20230029].
文摘Stimuli-responsive coordination polymers(CPs)are among one of the most prolific research areas in developing the next-generation functional materials.Their capability of being accurately excited by particular external changes with pre-determined and observable/characterizable behaviors correspond,are the so called“stimuli”and“responsive”.Abundant types of CP compounds,especially metal-organic frameworks(MOFs),are of rocketing interest owing to their compositional diversity,structural tunability,and in essence their highly engineerable functionality.This present review is aimed to sketch several common types of stimulation and the corresponding responses for CPs,accompanied with the broad logic and mechanisms underneath.And further from the aspect of material revolution,some representative progresses together with the latest advances of CP-based materials in various fields are covered in attempt to display a broader picture towards the possible prospects of this topic.
基金the National Key R&D Program of China(No.2020YFA0711500)the National Natural Science Fund of China(Nos.51973095,52273248,and 52303238)the Key Project of Natural Science Foundation of Tianjin City(No.21JCZDJC00010).
文摘The development of renewable woods for power generation can help improve the energy efficiency of buildings,and promote the concept design and implementation of“smart buildings”.Here,with specific chemical treatment and hydrothermal synthesis,we demonstrated the practical value of natural wood for thermoelectric power generation in smart buildings.The prepared wood-based thermoelectric sponges show high Seebeck coefficients of 320.5 and 436.6μV/K in the vertical and parallel directions of the longitudinal channel of wood.After 500 cycles of the compressive strain at 20%,the corresponding Seebeck coefficients increase up to 413.4 and 502.1μV/K,respectively,which is attributed to the improved contact and connection between tellurium thermoelectric nanowires.The Seebeck coefficients are much larger than those of most reported inorganic thermoelectric materials.Meanwhile,the thermoelectric sponges maintain excellent thermoelectric and mechanical stability.We further modeled the application value of wood-based thermoelectric sponges in smart buildings for power generation.Relatively high thermoelectric electricity can be obtained,such as in Beijing with over 1.5 million kWh every year,demonstrating the great potential in thermal energy harvest and energy supply.
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.
基金supported by the National Natural Science Foundation of China(NSFC,52273076 and 12004195)111 Project(B18030),and Natural Science Foundation of Tianjin(23JCQNJC00350).
文摘Flexible epidermal sensors assume an indispensable role in the field of wearable electronics,enabling the imperceptible detection of biomechanical signals for personalized health care.As an integral part,solution-processed ultrathin nanocomposite conductors with high strain sensitivity offer cost-effectiveness and scalability for sensor manufacturing.Nevertheless,their controllable fabrication remains a challenge,and the presence of abundant polymers usually lead to high hysteresis and unsatisfactory sensitivity for low strain detection.Here,a robust,unform,and highly conductive silver nanofilm is prepared through Layer-by-Layer(LbL)assembly by combining positively charged polyurethane and uniformly sized silver nanoparticles(AgNPs)on desired substrates.Subsequent photonic sintering is used to fuse the AgNPs into a cohesive structure and mitigate uncontrollable heat-induced cracks in the Ag nanofilm owing to continuous thermal expansion from underlying elastomeric substrates.Consequently,the Ag nanofilms achieve a conductivity of 5.1×10^(4)S cm^(−1),and demonstrate substrate-dependent electromechanical properties.In particular,the LbL assembled Ag nanofilms on oxygen plasma-treated polydimethylsiloxane(PDMS)can serve as hypersensitive sensors with gauge factors of more than 3000 at strains of less than 5%,or they are stretchable with small resistance variations to more than 50%on(3-aminopropyl)triethoxysilane modified PDMS or other thermoplastic elastomers.Mechanisms on this substrate dependent electromechanical properties are investigated,and the ultrasensitive strain sensors on PDMS are demonstrated for the detection of sound frequencies,pulses,and small forces.
基金supported by the National Natural Science Foundation of China(No.22375105)Natural Science Foundation for Young Scientists of Shanxi Province(No.202203021222293)+1 种基金the Fundamental Research Program of Shanxi Province(No.20210302124307)the Jinzhong University"1331 project"Collaborative Innovation Center(No.jzxyxtcxzx202105).
文摘Comprehensive Summary Herein,the temperature-and pressure-stimulated responsive behavior as well as crystal-glass phase transition of a new zero-dimensional hybrid manganese bromide[4-MTPP]2[MnBr4][4-MTPP+=(4-methoxybenzyl)tris(phenyl)phosphonium]were reported.Our experiment results demonstrate that[4-MTPP]2[MnBr4]shows typical green photoluminescence emission centered at 522.4 nm excited by UV light.
基金supported by the National Natural Science Foundation of China(Nos.22293030,22293032,91859123,22474064,and 22204082)the National Key Research and Development Program of China(No.2019YFA0210100)+3 种基金the National Postdoctoral Program for Innovative Talents(No.BX20220156)the China Postdoctoral Science Foundation(No.2023M731789)the Frontiers Science Center for New Organic Matter,Nankai University(No.63181206)the Haihe Laboratory of Sustainable Chemical Transformations.
文摘The generation and amplification of chirality in inorganic nanomaterials have garnered significant attention due to their promising applications in enantioselective catalysis,chiral sensing,and optoelectronics.Interface-driven self-assembly has emerged as a robust and versatile strategy to induce and enhance chirality in these systems,offering precise control over the spatial organization of nanoscale building blocks.This review presents a comprehensive overview of recent advancements in interface-driven selfassembly techniques,focusing on how these methods facilitate the generation and amplification of chiroptical properties in inorganic nanomaterials.We examine the strategies of interface-driven self-assembly through external torsion,aggregation amplification,and chiral molecule induction,highlighting key mechanisms that contribute to enhanced chiral responses.Self-assembly processes at liquid-liquid,gas-liquid,and liquid-solid interfaces are critically discussed,along with the influence of parameters,such as nanoparticle shape,surface ligand composition,and external stimuli on the formation of chiral nanostructures.Additionally,theoretical models describing the emergence of chirality are examined,providing insights into the role of interfacial molecular interactions in driving observed chiroptical effects.Finally,we review the applications of these chiral nanomaterials in spintronics,chiral photonics,and beyond,and propose future directions for advancing the design and development of novel chiral inorganic nanomaterials.This robust strategy holds great potential for facilitating breakthroughs in both the fundamental understanding and the practical implementation of chiral nanostructures.
基金supported by the National Natural Science Foundation of China(22261037)the Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT22091)+6 种基金the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2021BS02002)the Young Science and Technology Talents Cultivation Project of Inner Mongolia University(21221505)the Central Guidance on Local Science and Technology Development Fund of Inner Mongolia Autonomous Region(2023ZY0016)the Start-up Funding provided by Inner Mongolia Universitythe financial support from the National Natural Science Foundation of China(22361031)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2022QN02015)the Research Program of Science and Technology at Universities of Inner Mongolia Autonomous Region(NJZY22334)。
文摘The conventional design of metal-organic frameworks(MOFs)with room-temperature phosphorescence(RTP)mostly relies on using heavy metals,as the heavy atom effect can effectively increase the efficiency of intersystem crossing(ISC)to get a better phosphorescence performance.For the first time,we reported the highly efficient RTP of a lithium-based MOF IMU-101 with a lifetime(τ)of 299 ms and a quantum yield(QY)of 4.91%.In addition,MOFs IMU-102 and IMU-103,with sodium and cesium as metal nodes,were successfully synthesized.The phosphorescence properties of this series of alkali metal MOFs were systematically studied and compared.The crystallography and computational calculation show that the mechanism for achieving RTP for this material lies in the ultrashort coordination bond of Li,which enables the reduction of non-radiative transitions.IMU-101,as a cheap and environmentally friendly room-temperature phosphorescent material,has been further developed into composite polymer inks and bulk materials.This makes them promising for applications in anti-counterfeiting and information encryption.
基金financial support provided by the National Natural Science Foundation of China(Nos.52363014 and 22405179)the Science and Technology Project of Guangxi(GK AB23026136)the Open Fund Funding of Key Laboratory of New Processing Technology for Nonferrous Metal&Materials,Ministry of Education/Guangxi Key Laboratory of Optical and Electronic Materials and Devics(22AA-7).
文摘Metabolism,transpiration,and invasion of pathogens during the storage and transportation of fruits can lead to significant waste and even food safety issues.Therefore,real-time,rapid,and accurate non-destructive monitoring of physiological information during the storage of fruits and vegetables to assess fruit freshness is crucial.Herein,we engineered a degradable and multifunctional humidity sensing film for monitoring fruit freshness.The film is fabricated through the co-assembly of bagasse cellulose nanocrystals(CNC),okra polysaccharides(OPs),silver nanowires(Ag NWs),and phytic acid(PA),utilizing dynamic hydrogen and phosphate bonds.This innovative design endows the CNC/OPs/PA/Ag NWs(COPA)composite film with outstanding mechanical properties,water resistance,low water vapor permeability,antibacterial,degradability,and moisture-sensing ability.Notably,the proposed COPA humidity sensor exhibits high linearity(R^(2)=0.994),ultralow hysteresis(1.24%),and 32 days of operational stability across a 35%–98%relative humidity(RH)range,enabling precise freshness monitoring during fruit storage.Significantly,the COPA film prolonged the shelf-life of packaged fruit when compared to conventional PE film packaging.This research establishes a foundational framework for next-generation smart sensors in food quality management and biomedical monitoring applications.
