Wearable electronics face a significant challenge related to the limited permeability of electronic materials/devices.This issue results in sweat accumulation across the interface of the device and skin following a sp...Wearable electronics face a significant challenge related to the limited permeability of electronic materials/devices.This issue results in sweat accumulation across the interface of the device and skin following a specific period of use[1−3].Not only does it bring about discomfort for users regarding thermos-physiology,but it also has a detrimental effect on interface adhesion and signal quality,thus hindering exact sig-nal monitoring during prolonged periods[4−6].展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use i...High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use in soft electronics.To resolve these issues,a method involving freeze–thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network(DN)ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol)(PMP DN ICH)system.The well-designed ICH exhibits outstanding ionic conductivity(63.89 mS cm^(-1) at 25℃),excellent temperature resistance(-60–80℃),prolonged stability(30 d at ambient temperature),high oxidation resist-ance,remarkable antibacterial activity,decent mechanical performance,and adhesion.Additionally,the ICH performs effectively in a flexible wireless strain sensor,thermal sensor,all-solid-state supercapacitor,and single-electrode triboelectric nanogenerator,thereby highlighting its viability in constructing soft electronic devices.The highly integrated gel structure endows these flexible electronic devices with stable,reliable signal output performance.In particular,the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm^(-2)(current density,1 mA cm^(-2))and excellent environmental adaptability.This study paves the way for the design and fabrication of high-performance mul-tifunctional/flexible ICHs for wearable sensing,energy-storage,and energy-harvesting applications.展开更多
The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct ...The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.展开更多
Electromagnetic interference shielding(EMI SE)modules are the core com-ponent of modern electronics.However,the tra-ditional metal-based SE modules always take up indispensable three-dimensional space inside electroni...Electromagnetic interference shielding(EMI SE)modules are the core com-ponent of modern electronics.However,the tra-ditional metal-based SE modules always take up indispensable three-dimensional space inside electronics,posing a major obstacle to the integra-tion of electronics.The innovation of integrating 3D-printed conformal shielding(c-SE)modules with packaging materials onto core electronics offers infinite possibilities to satisfy ideal SE func-tion without occupying additional space.Herein,the 3D printable carbon-based inks with various proportions of graphene and carbon nanotube nanoparticles are well-formulated by manipulating their rheological peculiarity.Accordingly,the free-constructed architectures with arbitrarily-customized structure and multifunctionality are created via 3D printing.In particular,the SE performance of 3D-printed frame is up to 61.4 dB,simultaneously accompanied with an ultralight architecture of 0.076 g cm^(-3) and a superhigh specific shielding of 802.4 dB cm3 g^(-1).Moreover,as a proof-of-concept,the 3D-printed c-SE module is in situ integrated into core electronics,successfully replacing the traditional metal-based module to afford multiple functions for electromagnetic compatibility and thermal dissipa-tion.Thus,this scientific innovation completely makes up the blank for assembling carbon-based c-SE modules and sheds a brilliant light on developing the next generation of high-performance shielding materials with arbitrarily-customized structure for integrated electronics.展开更多
PrBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(PrBSCF) has attracted much research interest as a potential triple ionic and electronic conductor(TIEC) electrode for protonic ceramic fuel cells(PCFCs). The chemical formula...PrBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(PrBSCF) has attracted much research interest as a potential triple ionic and electronic conductor(TIEC) electrode for protonic ceramic fuel cells(PCFCs). The chemical formula for Pr BSCF is AA'B_(2)O_(5+δ), with Pr(A-site) and Ba/Sr(A'-site) alternately stacked along the c-axis. Due to these structural features, the bulk oxygen ion diffusivity is significantly enhanced through the disorder-free channels in the PrO layer;thus, the A site cations(lanthanide ions) play a pivotal role in determining the overall electrochemical properties of layered perovskites. Consequently, previous research has predominantly focused on the electrical properties and oxygen bulk/surface kinetics of Ln cation effects,whereas the hydration properties for PCFC systems remain unidentified. Here, we thoroughly examined the proton uptake behavior and thermodynamic parameters for the hydration reaction to conclusively determine the changes in the electrochemical performances depending on LnBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(LnBSCF,Ln=Pr, Nd, and Gd) cathodes. At 500 ℃, the quantitative proton concentration of PrBSCF was 2.04 mol% and progressively decreased as the Ln cation size decreased. Similarly, the Gibbs free energy indicated that less energy was required for the formation of protonic defects in the order of Pr BSCF < Nd BSCF < Gd BSCF. To elucidate the close relationship between hydration properties and electrochemical performances in LnBSCF cathodes, PCFC single cell measurements and analysis of the distribution of relaxation time were further investigated.展开更多
Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composite...Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.展开更多
The sensory perception of food is a dynamic process,which is closely related to the release of flavor substances during oral processing.It’s not only affected by the food material,but also subjected to the individual...The sensory perception of food is a dynamic process,which is closely related to the release of flavor substances during oral processing.It’s not only affected by the food material,but also subjected to the individual oral environment.To explore the oral processing characteristics of soft-boiled chicken,the sensory properties,texture,particle size,viscosity,characteristic values of electronic nose and tongue of different chicken samples were investigated.The correlation analysis showed that the physical characteristics especially the cohesiveness,springiness,resilience of the sample determined oral processing behavior.The addition of chicken skin played a role in lubrication during oral processing.The particle size of the bolus was heightened at the early stage,and the fluidity was enhanced in the end,which reduced the chewing time to the swallowing point and raised the aromatic compounds signal of electronic nose.But the effect of chicken skin on chicken thigh with relatively high fat content,was opposite in electronic nose,which had a certain masking effect on the perception of umami and sweet taste.In conclusion,fat played a critical role in chicken oral processing and chicken thigh had obvious advantages in comprehensive evaluation of soft-boiled chicken,which was more popular among people.展开更多
This review summarizes recent progress in developing wireless,batteryless,fully implantable biomedical devices for real-time continuous physiological signal monitoring,focusing on advancing human health care.Design co...This review summarizes recent progress in developing wireless,batteryless,fully implantable biomedical devices for real-time continuous physiological signal monitoring,focusing on advancing human health care.Design considerations,such as biological constraints,energy sourcing,and wireless communication,are discussed in achieving the desired performance of the devices and enhanced interface with human tissues.In addition,we review the recent achievements in materials used for developing implantable systems,emphasizing their importance in achieving multi-functionalities,biocompatibility,and hemocompatibility.The wireless,batteryless devices offer minimally invasive device insertion to the body,enabling portable health monitoring and advanced disease diagnosis.Lastly,we summarize the most recent practical applications of advanced implantable devices for human health care,highlighting their potential for immediate commercialization and clinical uses.展开更多
Hydride ion(H-)conductors have drawn much attention due to their potential applications in hydrideion-based devices.Rare earth metal hydrides(REH_(x))have fast H-conduction which,unfortunately,is accompanied by detrim...Hydride ion(H-)conductors have drawn much attention due to their potential applications in hydrideion-based devices.Rare earth metal hydrides(REH_(x))have fast H-conduction which,unfortunately,is accompanied by detrimental electron conduction preventing their application as ion conductors.Here,REH_(x)(RE=Nd,Ce,and Pr)with varied grain sizes,rich grain boundaries,and defects have been prepared by ball milling and subsequent sintering.The electronic conductivity of the ball-milled REH_(x)samples can be reduced by 2-4 orders of magnitude compared with the non-ball-milled samples.The relationship of electron conduction and miscrostructures in REH_(x)is studied and discussed based on experimental data and previously-proposed classical and quantum theories.The H-conductivity of all REH_(x)is about 10^(-4)to 10^(-3)S cm^(-1)at room temperature,showing promise for the development of H-conductors and their applications in clean energy storage and conversion.展开更多
Bioelectronic interventions,specifically trigeminal nerve st imulat ion(TNS),have attracted considerable attention in conditions where cortical spreading depolarizations(CSDs)accompanied by compromised cerebral perfus...Bioelectronic interventions,specifically trigeminal nerve st imulat ion(TNS),have attracted considerable attention in conditions where cortical spreading depolarizations(CSDs)accompanied by compromised cerebral perfusion may exacerbate neurological damage.While pharmacological interventions have demonstrated initial potential in addressing CSDs,a standardized treatment approach has not yet been established.The objective of this perspective is to explore emerging bioelectronic methodologies for addressing CSDs,particularly emphasizing TNS,and to underscore TNS’s capacity to enhance neurovascular coupling and cerebral perfusion.展开更多
Recently,an extreme narrowband spectral response of only 8 nm in electronic-grade diamond-based photodetectors has been observed by Zheng Wei and his colleagues from Sun Yat-sen University for the first time.A charge ...Recently,an extreme narrowband spectral response of only 8 nm in electronic-grade diamond-based photodetectors has been observed by Zheng Wei and his colleagues from Sun Yat-sen University for the first time.A charge collection narrowing mechanism assisted by free exciton radiative recombination is proposed,which well reveals the characteristic spectral response of diamond.展开更多
Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7...Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7−δ)(SF)exhibits superior proton uptake and rapid ionic conduction,boosting activity.However,excessive proton uptake during RePCC operation degrades SF’s crystal structure,impacting durability.This study introduces a novel A/B-sites co-substitution strategy for modifying air electrodes,incorporating Sr-deficiency and Nb-substitution to create Sr_(2.8)Fe_(1.8)Nb_(0.2)O_(7−δ)(D-SFN).Nb stabilizes SF’s crystal,curbing excessive phase formation,and Sr-deficiency boosts oxygen vacancy concentration,optimizing oxygen transport.The D-SFN electrode demonstrates outstanding activity and durability,achieving a peak power density of 596 mW cm^(−2)in fuel cell mode and a current density of−1.19 A cm^(−2)in electrolysis mode at 1.3 V,650℃,with excellent cycling durability.This approach holds the potential for advancing robust and efficient air electrodes in RePCCs for renewable energy storage.展开更多
The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on...The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.展开更多
Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of hos...Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce6O6 or Zr6O6).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce6 clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99%and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pdδ+,which not only enhances the adsorption of H2 and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.展开更多
Cross-sections for electronic excitation and de-excitation among the ground state and lowest-lying seven electronic excited states of carbon monoxide(CO)by low-energy electron impact are computed using the R-matrix me...Cross-sections for electronic excitation and de-excitation among the ground state and lowest-lying seven electronic excited states of carbon monoxide(CO)by low-energy electron impact are computed using the R-matrix method.The excitation cross-sections from the ground state to the electronic states a^(3)Π,a'^(3)Σ^(+)+and A^(1)Πagree with previous experimental and theoretical results.In addition,the cross-sections for the I^(1)Σ^(+)-and D^(1)Δstates of CO,which will cascade to CO a'^(3)Σ^(+)+and A^(1)Πstates,are calculated.Furthermore,in contrast to the typical increase in electronic excitation cross-sections with collision energy,the de-excitation cross-sections show a negative trend with increasing energy.展开更多
In the information age,electronic documents(e-documents)have become a popular alternative to paper documents due to their lower costs,higher dissemination rates,and ease of knowledge sharing.However,digital copyright ...In the information age,electronic documents(e-documents)have become a popular alternative to paper documents due to their lower costs,higher dissemination rates,and ease of knowledge sharing.However,digital copyright infringements occur frequently due to the ease of copying,which not only infringes on the rights of creators but also weakens their creative enthusiasm.Therefore,it is crucial to establish an e-document sharing system that enforces copyright protection.However,the existing centralized system has outstanding vulnerabilities,and the plagiarism detection algorithm used cannot fully detect the context,semantics,style,and other factors of the text.Digital watermark technology is only used as a means of infringement tracing.This paper proposes a decentralized framework for e-document sharing based on decentralized autonomous organization(DAO)and non-fungible token(NFT)in blockchain.The use of blockchain as a distributed credit base resolves the vulnerabilities inherent in traditional centralized systems.The e-document evaluation and plagiarism detection mechanisms based on the DAO model effectively address challenges in comprehensive text information checks,thereby promoting the enhancement of e-document quality.The mechanism for protecting and circulating e-document copyrights using NFT technology ensures effective safeguarding of users’e-document copyrights and facilitates e-document sharing.Moreover,recognizing the security issues within the DAO governance mechanism,we introduce an innovative optimization solution.Through experimentation,we validate the enhanced security of the optimized governance mechanism,reducing manipulation risks by up to 51%.Additionally,by utilizing evolutionary game analysis to deduce the equilibrium strategies of the framework,we discovered that adjusting the reward and penalty parameters of the incentive mechanism motivates creators to generate superior quality and unique e-documents,while evaluators are more likely to engage in assessments.展开更多
Organic–inorganic lead halide perovskites(LHPs) have attracted great interest owing to their outstanding optoelectronic properties.Typically,the underlying electronic structure would determinate the physical properti...Organic–inorganic lead halide perovskites(LHPs) have attracted great interest owing to their outstanding optoelectronic properties.Typically,the underlying electronic structure would determinate the physical properties of materials.But as for now,limited studies have been done to reveal the underlying electronic structure of this material system,comparing to the huge amount of investigations on the material synthesis.The effective mass of the valance band is one of the most important physical parameters which plays a dominant role in charge transport and photovoltaic phenomena.In pristine CsPbBr_(3),the Fr?hlich polarons associated with the Pb–Br stretching modes are proposed to be responsible for the effective mass renormalization.In this regard,it would be very interesting to explore the electronic structure in doped LHPs.Here,we report high-resolution angle-resolved photoemission spectroscopy(ARPES) studies on both pristine and Cl-doped CsPbBr_(3).The experimental band dispersions are extracted from ARPES spectra along both ■ and ■ high symmetry directions.DFT calculations are performed and directly compared with the ARPES data.Our results have revealed the band structure of Cl-doped CsPbBr_(3) for the first time,which have also unveiled the effective mass renormalization in the Cl-doped CsPbBr_(3) compound.Doping dependent measurements indicate that the chlorine doping could moderately tune the renormalization strength.These results will help understand the physical properties of LHPs as a function of doping.展开更多
TiNi-based shape memory alloys have been extensively investigated due to their significant applications,but a comprehensive understanding of the evolution of electronic structure and electrical transport in a system w...TiNi-based shape memory alloys have been extensively investigated due to their significant applications,but a comprehensive understanding of the evolution of electronic structure and electrical transport in a system with martensitic transformations(MT) is still lacking.In this work,we focused on the electronic transport behavior of three phases in Ni_(50-x)Fe_xTi_(50)across the MT.A phase diagram of Ni_(50-x)Fe_xTi_(50) was established based on x-ray diffraction,calorimetric,magnetic,and electrical measurements.To reveal the driving force of MT,phonon softening was revealed using first-principles calculations.Notably,the transverse and longitudinal transport behavior changed significantly across the phase transition,which can be attributed to the reconstruction of electronic structures.This work promotes the understanding of phase transitions and demonstrates the sensitivity of electron transport to phase transition.展开更多
The first-principles calculations are performed to examine structural,mechanical,and electronic properties at large strain for a monolayer C_(4)N_(4),which has been predicted as an anchoring promising material to atte...The first-principles calculations are performed to examine structural,mechanical,and electronic properties at large strain for a monolayer C_(4)N_(4),which has been predicted as an anchoring promising material to attenuate shuttle effect in Li–S batteries stemming from its large absorption energy and low diffusion energy barrier.Our results show that the ideal strengths of C_(4)N_(4)under tension and pure shear deformation conditions reach 13.9 GPa and 12.5 GPa when the strains are 0.07 and 0.28,respectively.The folded five-membered rings and diverse bonding modes between carbon and nitrogen atoms enhance the ability to resist plastic deformation of C_(4)N_(4).The orderly bond-rearranging behaviors under the weak tensile loading path along the[100]direction cause the impressive semiconductor–metal transition and inverse semiconductor–metal transition.The present results enrich the knowledge of the structure and electronic properties of C_(4)N_(4)under deformations and shed light on exploring other two-dimensional materials under diverse loading conditions.展开更多
文摘Wearable electronics face a significant challenge related to the limited permeability of electronic materials/devices.This issue results in sweat accumulation across the interface of the device and skin following a specific period of use[1−3].Not only does it bring about discomfort for users regarding thermos-physiology,but it also has a detrimental effect on interface adhesion and signal quality,thus hindering exact sig-nal monitoring during prolonged periods[4−6].
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金the National Natural Science Foundation of China(11875138,52077095).
文摘High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use in soft electronics.To resolve these issues,a method involving freeze–thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network(DN)ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol)(PMP DN ICH)system.The well-designed ICH exhibits outstanding ionic conductivity(63.89 mS cm^(-1) at 25℃),excellent temperature resistance(-60–80℃),prolonged stability(30 d at ambient temperature),high oxidation resist-ance,remarkable antibacterial activity,decent mechanical performance,and adhesion.Additionally,the ICH performs effectively in a flexible wireless strain sensor,thermal sensor,all-solid-state supercapacitor,and single-electrode triboelectric nanogenerator,thereby highlighting its viability in constructing soft electronic devices.The highly integrated gel structure endows these flexible electronic devices with stable,reliable signal output performance.In particular,the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm^(-2)(current density,1 mA cm^(-2))and excellent environmental adaptability.This study paves the way for the design and fabrication of high-performance mul-tifunctional/flexible ICHs for wearable sensing,energy-storage,and energy-harvesting applications.
基金supported by the Taishan Scholar Program of Shandong Province,China (tsqn202211162)the National Natural Science Foundation of China (22102079)the Natural Science Foundation of Shandong Province of China (ZR2021YQ10,ZR2022QB163)。
文摘The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.
基金This work is financially supported by the National Natural Science Foundation of China(52303036)the Natural Science Foundation of Guangxi Province(2020GXNSFAA297028)+4 种基金the Guangxi Science and Technology Base and Talent Special Project(GUIKE AD23026179)the International Science&Technology Cooperation Project of Chengdu(2021-GH03-00009-HZ)the Program of Innovative Research Team for Young Scientists of Sichuan Province(22CXTD0019)the Natural Science Foundation of Sichuan Province(2023NSFSC0986)the Opening Project of State Key Laboratory of Polymer Materials Engineering(Sichuan University)(Sklpme2023-3-18).
文摘Electromagnetic interference shielding(EMI SE)modules are the core com-ponent of modern electronics.However,the tra-ditional metal-based SE modules always take up indispensable three-dimensional space inside electronics,posing a major obstacle to the integra-tion of electronics.The innovation of integrating 3D-printed conformal shielding(c-SE)modules with packaging materials onto core electronics offers infinite possibilities to satisfy ideal SE func-tion without occupying additional space.Herein,the 3D printable carbon-based inks with various proportions of graphene and carbon nanotube nanoparticles are well-formulated by manipulating their rheological peculiarity.Accordingly,the free-constructed architectures with arbitrarily-customized structure and multifunctionality are created via 3D printing.In particular,the SE performance of 3D-printed frame is up to 61.4 dB,simultaneously accompanied with an ultralight architecture of 0.076 g cm^(-3) and a superhigh specific shielding of 802.4 dB cm3 g^(-1).Moreover,as a proof-of-concept,the 3D-printed c-SE module is in situ integrated into core electronics,successfully replacing the traditional metal-based module to afford multiple functions for electromagnetic compatibility and thermal dissipa-tion.Thus,this scientific innovation completely makes up the blank for assembling carbon-based c-SE modules and sheds a brilliant light on developing the next generation of high-performance shielding materials with arbitrarily-customized structure for integrated electronics.
基金supported by the National Research Foundation (NRF) grant funded by the Korea government (NRF2022R1C1C1007619, NRF-2021M3H4A1A01002921, NRF2021M3I3A1084292)supported by the KIST Institutional Program (Project No. 2E32592-23-069)。
文摘PrBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(PrBSCF) has attracted much research interest as a potential triple ionic and electronic conductor(TIEC) electrode for protonic ceramic fuel cells(PCFCs). The chemical formula for Pr BSCF is AA'B_(2)O_(5+δ), with Pr(A-site) and Ba/Sr(A'-site) alternately stacked along the c-axis. Due to these structural features, the bulk oxygen ion diffusivity is significantly enhanced through the disorder-free channels in the PrO layer;thus, the A site cations(lanthanide ions) play a pivotal role in determining the overall electrochemical properties of layered perovskites. Consequently, previous research has predominantly focused on the electrical properties and oxygen bulk/surface kinetics of Ln cation effects,whereas the hydration properties for PCFC systems remain unidentified. Here, we thoroughly examined the proton uptake behavior and thermodynamic parameters for the hydration reaction to conclusively determine the changes in the electrochemical performances depending on LnBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(LnBSCF,Ln=Pr, Nd, and Gd) cathodes. At 500 ℃, the quantitative proton concentration of PrBSCF was 2.04 mol% and progressively decreased as the Ln cation size decreased. Similarly, the Gibbs free energy indicated that less energy was required for the formation of protonic defects in the order of Pr BSCF < Nd BSCF < Gd BSCF. To elucidate the close relationship between hydration properties and electrochemical performances in LnBSCF cathodes, PCFC single cell measurements and analysis of the distribution of relaxation time were further investigated.
基金We acknowledge the support from the National Key Research and Development Program of China(Grant No.2022YFA1405000)the Natural Science Foundation of Jiangsu Province,Major Project(Grant No.BK20212004)+1 种基金the National Natural Science Foundation of China(Grant No.62374083)the State Key Laboratory of Analytical Chemistry for Life Science(Grant No.5431ZZXM2205).
文摘Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.
基金supported by China Agriculture Research System of MOF and MARA(CARS-41)Wens Fifth Five R&D Major Project(WENS-2020-1-ZDZX-007)。
文摘The sensory perception of food is a dynamic process,which is closely related to the release of flavor substances during oral processing.It’s not only affected by the food material,but also subjected to the individual oral environment.To explore the oral processing characteristics of soft-boiled chicken,the sensory properties,texture,particle size,viscosity,characteristic values of electronic nose and tongue of different chicken samples were investigated.The correlation analysis showed that the physical characteristics especially the cohesiveness,springiness,resilience of the sample determined oral processing behavior.The addition of chicken skin played a role in lubrication during oral processing.The particle size of the bolus was heightened at the early stage,and the fluidity was enhanced in the end,which reduced the chewing time to the swallowing point and raised the aromatic compounds signal of electronic nose.But the effect of chicken skin on chicken thigh with relatively high fat content,was opposite in electronic nose,which had a certain masking effect on the perception of umami and sweet taste.In conclusion,fat played a critical role in chicken oral processing and chicken thigh had obvious advantages in comprehensive evaluation of soft-boiled chicken,which was more popular among people.
基金the NSF CCSS-2152638 and the IEN Center Grant from the Institute for Electronics and Nanotechnology at Georgia Tech.
文摘This review summarizes recent progress in developing wireless,batteryless,fully implantable biomedical devices for real-time continuous physiological signal monitoring,focusing on advancing human health care.Design considerations,such as biological constraints,energy sourcing,and wireless communication,are discussed in achieving the desired performance of the devices and enhanced interface with human tissues.In addition,we review the recent achievements in materials used for developing implantable systems,emphasizing their importance in achieving multi-functionalities,biocompatibility,and hemocompatibility.The wireless,batteryless devices offer minimally invasive device insertion to the body,enabling portable health monitoring and advanced disease diagnosis.Lastly,we summarize the most recent practical applications of advanced implantable devices for human health care,highlighting their potential for immediate commercialization and clinical uses.
基金supported by the National Key Research and Development Program of China(2021YFB4000602)the National Natural Science Foundation of China(21988101,22279130,21633011)+1 种基金the Dalian Science and Technology Innovation Fund(2023RJ016)the Liaoning Revitalization Talents Program(x LYC2002076)。
文摘Hydride ion(H-)conductors have drawn much attention due to their potential applications in hydrideion-based devices.Rare earth metal hydrides(REH_(x))have fast H-conduction which,unfortunately,is accompanied by detrimental electron conduction preventing their application as ion conductors.Here,REH_(x)(RE=Nd,Ce,and Pr)with varied grain sizes,rich grain boundaries,and defects have been prepared by ball milling and subsequent sintering.The electronic conductivity of the ball-milled REH_(x)samples can be reduced by 2-4 orders of magnitude compared with the non-ball-milled samples.The relationship of electron conduction and miscrostructures in REH_(x)is studied and discussed based on experimental data and previously-proposed classical and quantum theories.The H-conductivity of all REH_(x)is about 10^(-4)to 10^(-3)S cm^(-1)at room temperature,showing promise for the development of H-conductors and their applications in clean energy storage and conversion.
基金supported by National Institute of Neurological Disorders and Stroke of the National Institutes of Health under award number R21NS114763US Army Medical Research and Materiel Command (USAMRMC) under award#W81XWH-18-1-0773merit-based career enhancement award at the Feinstein Institutes for Medical Research (to CL)
文摘Bioelectronic interventions,specifically trigeminal nerve st imulat ion(TNS),have attracted considerable attention in conditions where cortical spreading depolarizations(CSDs)accompanied by compromised cerebral perfusion may exacerbate neurological damage.While pharmacological interventions have demonstrated initial potential in addressing CSDs,a standardized treatment approach has not yet been established.The objective of this perspective is to explore emerging bioelectronic methodologies for addressing CSDs,particularly emphasizing TNS,and to underscore TNS’s capacity to enhance neurovascular coupling and cerebral perfusion.
文摘Recently,an extreme narrowband spectral response of only 8 nm in electronic-grade diamond-based photodetectors has been observed by Zheng Wei and his colleagues from Sun Yat-sen University for the first time.A charge collection narrowing mechanism assisted by free exciton radiative recombination is proposed,which well reveals the characteristic spectral response of diamond.
基金supported by the Research Grants Council,University Grants Committee,Hong Kong SAR(Project Number:N_PolyU552/20)supported by the National Nature Science Foundation of China(22209138)Guangdong Basic and Applied Basic Research Foundation(2021A1515110464).
文摘Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7−δ)(SF)exhibits superior proton uptake and rapid ionic conduction,boosting activity.However,excessive proton uptake during RePCC operation degrades SF’s crystal structure,impacting durability.This study introduces a novel A/B-sites co-substitution strategy for modifying air electrodes,incorporating Sr-deficiency and Nb-substitution to create Sr_(2.8)Fe_(1.8)Nb_(0.2)O_(7−δ)(D-SFN).Nb stabilizes SF’s crystal,curbing excessive phase formation,and Sr-deficiency boosts oxygen vacancy concentration,optimizing oxygen transport.The D-SFN electrode demonstrates outstanding activity and durability,achieving a peak power density of 596 mW cm^(−2)in fuel cell mode and a current density of−1.19 A cm^(−2)in electrolysis mode at 1.3 V,650℃,with excellent cycling durability.This approach holds the potential for advancing robust and efficient air electrodes in RePCCs for renewable energy storage.
文摘The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.
文摘Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce6O6 or Zr6O6).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce6 clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99%and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pdδ+,which not only enhances the adsorption of H2 and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.
基金Project supported by the National Natural Science Foundation of China (Grant No.11974253)。
文摘Cross-sections for electronic excitation and de-excitation among the ground state and lowest-lying seven electronic excited states of carbon monoxide(CO)by low-energy electron impact are computed using the R-matrix method.The excitation cross-sections from the ground state to the electronic states a^(3)Π,a'^(3)Σ^(+)+and A^(1)Πagree with previous experimental and theoretical results.In addition,the cross-sections for the I^(1)Σ^(+)-and D^(1)Δstates of CO,which will cascade to CO a'^(3)Σ^(+)+and A^(1)Πstates,are calculated.Furthermore,in contrast to the typical increase in electronic excitation cross-sections with collision energy,the de-excitation cross-sections show a negative trend with increasing energy.
基金This work is supported by the National Key Research and Development Program(2022YFB2702300)National Natural Science Foundation of China(Grant No.62172115)+2 种基金Innovation Fund Program of the Engineering Research Center for Integration and Application of Digital Learning Technology of Ministry of Education under Grant Number No.1331005Guangdong Higher Education Innovation Group 2020KCXTD007Guangzhou Fundamental Research Plan of Municipal-School Jointly Funded Projects(No.202102010445).
文摘In the information age,electronic documents(e-documents)have become a popular alternative to paper documents due to their lower costs,higher dissemination rates,and ease of knowledge sharing.However,digital copyright infringements occur frequently due to the ease of copying,which not only infringes on the rights of creators but also weakens their creative enthusiasm.Therefore,it is crucial to establish an e-document sharing system that enforces copyright protection.However,the existing centralized system has outstanding vulnerabilities,and the plagiarism detection algorithm used cannot fully detect the context,semantics,style,and other factors of the text.Digital watermark technology is only used as a means of infringement tracing.This paper proposes a decentralized framework for e-document sharing based on decentralized autonomous organization(DAO)and non-fungible token(NFT)in blockchain.The use of blockchain as a distributed credit base resolves the vulnerabilities inherent in traditional centralized systems.The e-document evaluation and plagiarism detection mechanisms based on the DAO model effectively address challenges in comprehensive text information checks,thereby promoting the enhancement of e-document quality.The mechanism for protecting and circulating e-document copyrights using NFT technology ensures effective safeguarding of users’e-document copyrights and facilitates e-document sharing.Moreover,recognizing the security issues within the DAO governance mechanism,we introduce an innovative optimization solution.Through experimentation,we validate the enhanced security of the optimized governance mechanism,reducing manipulation risks by up to 51%.Additionally,by utilizing evolutionary game analysis to deduce the equilibrium strategies of the framework,we discovered that adjusting the reward and penalty parameters of the incentive mechanism motivates creators to generate superior quality and unique e-documents,while evaluators are more likely to engage in assessments.
基金Project supported by the International Partnership Program of the Chinese Academy of Sciences(Grant No.123GJHZ2022035MI)the Fundamental Research Funds for the Central Universities(Grant Nos.WK3510000015 and WK3510000012)。
文摘Organic–inorganic lead halide perovskites(LHPs) have attracted great interest owing to their outstanding optoelectronic properties.Typically,the underlying electronic structure would determinate the physical properties of materials.But as for now,limited studies have been done to reveal the underlying electronic structure of this material system,comparing to the huge amount of investigations on the material synthesis.The effective mass of the valance band is one of the most important physical parameters which plays a dominant role in charge transport and photovoltaic phenomena.In pristine CsPbBr_(3),the Fr?hlich polarons associated with the Pb–Br stretching modes are proposed to be responsible for the effective mass renormalization.In this regard,it would be very interesting to explore the electronic structure in doped LHPs.Here,we report high-resolution angle-resolved photoemission spectroscopy(ARPES) studies on both pristine and Cl-doped CsPbBr_(3).The experimental band dispersions are extracted from ARPES spectra along both ■ and ■ high symmetry directions.DFT calculations are performed and directly compared with the ARPES data.Our results have revealed the band structure of Cl-doped CsPbBr_(3) for the first time,which have also unveiled the effective mass renormalization in the Cl-doped CsPbBr_(3) compound.Doping dependent measurements indicate that the chlorine doping could moderately tune the renormalization strength.These results will help understand the physical properties of LHPs as a function of doping.
基金supported by the State Key Development Program for Basic Research of China(Grant Nos.2019YFA0704900 and 2022YFA1403800)the Fundamental Science Center of the National Natural Science Foundation of China(Grant No.52088101)+2 种基金the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(CAS)(Grant No.XDB33000000)the Synergetic Extreme Condition User Facility(SECUF)the Scientific Instrument Developing Project of CAS(Grant No.ZDKYYQ20210003)。
文摘TiNi-based shape memory alloys have been extensively investigated due to their significant applications,but a comprehensive understanding of the evolution of electronic structure and electrical transport in a system with martensitic transformations(MT) is still lacking.In this work,we focused on the electronic transport behavior of three phases in Ni_(50-x)Fe_xTi_(50)across the MT.A phase diagram of Ni_(50-x)Fe_xTi_(50) was established based on x-ray diffraction,calorimetric,magnetic,and electrical measurements.To reveal the driving force of MT,phonon softening was revealed using first-principles calculations.Notably,the transverse and longitudinal transport behavior changed significantly across the phase transition,which can be attributed to the reconstruction of electronic structures.This work promotes the understanding of phase transitions and demonstrates the sensitivity of electron transport to phase transition.
基金Project support by the National Natural Science Foundation of China(Grant Nos.11704044 and 12074140)。
文摘The first-principles calculations are performed to examine structural,mechanical,and electronic properties at large strain for a monolayer C_(4)N_(4),which has been predicted as an anchoring promising material to attenuate shuttle effect in Li–S batteries stemming from its large absorption energy and low diffusion energy barrier.Our results show that the ideal strengths of C_(4)N_(4)under tension and pure shear deformation conditions reach 13.9 GPa and 12.5 GPa when the strains are 0.07 and 0.28,respectively.The folded five-membered rings and diverse bonding modes between carbon and nitrogen atoms enhance the ability to resist plastic deformation of C_(4)N_(4).The orderly bond-rearranging behaviors under the weak tensile loading path along the[100]direction cause the impressive semiconductor–metal transition and inverse semiconductor–metal transition.The present results enrich the knowledge of the structure and electronic properties of C_(4)N_(4)under deformations and shed light on exploring other two-dimensional materials under diverse loading conditions.