It is well accepted that a lithiophilic interface can effectively regulate Li deposition behaviors,but the influence of the lithiophilic interface is gradually diminished upon continuous Li deposition that completely ...It is well accepted that a lithiophilic interface can effectively regulate Li deposition behaviors,but the influence of the lithiophilic interface is gradually diminished upon continuous Li deposition that completely isolates Li from the lithiophilic metals.Herein,we perform in-depth studies on the creation of dynamic alloy interfaces upon Li deposition,arising from the exceptionally high diffusion coefficient of Hg in the amalgam solid solution.As a comparison,other metals such as Au,Ag,and Zn have typical diffusion coefficients of 10-20 orders of magnitude lower than that of Hg in the similar solid solution phases.This difference induces compact Li deposition pattern with an amalgam substrate even with a high areal capacity of 55 mAh cm^(-2).This finding provides new insight into the rational design of Li anode substrate for the stable cycling of Li metal batteries.展开更多
The triboelectric nanogenerator(TENG)can effectively collect energy based on contact electrification(CE)at diverse interfaces,including solid–solid,liquid–solid,liquid–liquid,gas–solid,and gas–liquid.This enables...The triboelectric nanogenerator(TENG)can effectively collect energy based on contact electrification(CE)at diverse interfaces,including solid–solid,liquid–solid,liquid–liquid,gas–solid,and gas–liquid.This enables energy harvesting from sources such as water,wind,and sound.In this review,we provide an overview of the coexistence of electron and ion transfer in the CE process.We elucidate the diverse dominant mechanisms observed at different interfaces and emphasize the interconnectedness and complementary nature of interface studies.The review also offers a comprehensive summary of the factors influencing charge transfer and the advancements in interfacial modification techniques.Additionally,we highlight the wide range of applications stemming from the distinctive characteristics of charge transfer at various interfaces.Finally,this review elucidates the future opportunities and challenges that interface CE may encounter.We anticipate that this review can offer valuable insights for future research on interface CE and facilitate the continued development and industrialization of TENG.展开更多
Flexible and wearable pressure sensors hold immense promise for health monitoring,covering disease detection and postoperative rehabilitation.Developing pressure sensors with high sensitivity,wide detection range,and ...Flexible and wearable pressure sensors hold immense promise for health monitoring,covering disease detection and postoperative rehabilitation.Developing pressure sensors with high sensitivity,wide detection range,and cost-effectiveness is paramount.By leveraging paper for its sustainability,biocompatibility,and inherent porous structure,herein,a solution-processed all-paper resistive pressure sensor is designed with outstanding performance.A ternary composite paste,comprising a compressible 3D carbon skeleton,conductive polymer poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate),and cohesive carbon nanotubes,is blade-coated on paper and naturally dried to form the porous composite electrode with hierachical micro-and nano-structured surface.Combined with screen-printed Cu electrodes in submillimeter finger widths on rough paper,this creates a multiscale hierarchical contact interface between electrodes,significantly enhancing sensitivity(1014 kPa-1)and expanding the detection range(up to 300 kPa)of as-resulted all-paper pressure sensor with low detection limit and power consumption.Its versatility ranges from subtle wrist pulses,robust finger taps,to large-area spatial force detection,highlighting its intricate submillimetermicrometer-nanometer hierarchical interface and nanometer porosity in the composite electrode.Ultimately,this all-paper resistive pressure sensor,with its superior sensing capabilities,large-scale fabrication potential,and cost-effectiveness,paves the way for next-generation wearable electronics,ushering in an era of advanced,sustainable technological solutions.展开更多
Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new mater...Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new materials in this respect.In van der Waals(vdW)layered materials,these building blocks are charge neutral and can be isolated from their bulk phase(top-down),but usually grow on substrate.In ionic layered materials,they are charged and usually cannot exist independently but can serve as motifs to construct new materials(bottom-up).In this paper,we introduce our recently constructed databases for 2D material-substrate interface(2DMSI),and 2D charged building blocks.For 2DMSI database,we systematically build a workflow to predict appropriate substrates and their geometries at substrates,and construct the 2DMSI database.For the 2D charged building block database,1208 entries from bulk material database are identified.Information of crystal structure,valence state,source,dimension and so on is provided for each entry with a json format.We also show its application in designing and searching for new functional layered materials.The 2DMSI database,building block database,and designed layered materials are available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00188.展开更多
The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide incl...The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.展开更多
Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT...Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT aerogel structure shows nano-pore size(30-40 nm),high specific surface area(559 m^(2)g^(−1)),high void fraction(91.7%)and enhanced mechanical property:(1)the nano-pore size is beneficial for efficiently blocking thermal conduction and thermal convection via Knudsen effect(beneficial for infrared(IR)stealth);(2)the heterogeneous interface was beneficial for IR reflection(beneficial for IR stealth)and MWCNT polarization loss(beneficial for electromagnetic wave(EMW)attenuation);(3)the high void fraction was beneficial for enhancing thermal insulation(beneficial for IR stealth)and EMW impedance match(beneficial for EMW attenuation).Guided by the above theoretical design strategy,PVTMS@MWCNT nano-aerogel shows superior EMW absorption property(cover all Ku-band)and thermal IR stealth property(ΔT reached 60.7℃).Followed by a facial combination of the above nano-aerogel with graphene film of high electrical conductivity,an extremely high electromagnetic interference shielding material(66.5 dB,2.06 mm thickness)with superior absorption performance of an average absorption-to-reflection(A/R)coefficient ratio of 25.4 and a low reflection bandwidth of 4.1 GHz(A/R ratio more than 10)was experimentally obtained in this work.展开更多
A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and developme...A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and development have recently been conducted to form a stable interface between the electrode and electrolyte.Therefore,it is essential to investigate emerging knowledge and contextualize it.The nanoengineering of the electrode-electrolyte interface has been actively researched at the electrode/electrolyte and interphase levels.This review presents and summarizes some recent advances aimed at nanoengineering approaches to build a more stable electrode-electrolyte interface and assess the impact of each approach adopted.Furthermore,future perspectives on the feasibility and practicality of each approach will also be reviewed in detail.Finally,this review aids in projecting a more sustainable research pathway for a nanoengineered interphase design between electrode and electrolyte,which is pivotal for high-performance,thermally stable Li-ion batteries.展开更多
Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electro...Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electrochemical performance is greatly limited.In this study,a nickel/manganese sulfide material(Ni_(0.96)S_(x)/MnS_(y)-NC)with adjustable sulfur vacancies and heterogeneous hollow spheres was prepared using a simple method.The introduction of a concentration-adjustable sulfur vacancy enables the generation of a heterogeneous interface between bimetallic sulfide and sulfur vacancies.This interface collectively creates an internal electric field,improving the mobility of electrons and ions,increasing the number of electrochemically active sites,and further optimizing the performance of Na~+storage.The direction of electron flow is confirmed by Density functional theory(DFT)calculations.The hollow nano-spherical material provides a buffer for expansion,facilitating rapid transfer kinetics.Our innovative discovery involves the interaction between the ether-based electrolyte and copper foil,leading to the formation of Cu_9S_5,which grafts the active material and copper current collector,reinforcing mechanical supporting.This results in a new heterostructure of Cu_9S_5 with Ni_(0.96)S_(x)/MnS_(y),contributing to the stabilization of structural integrity for long-cycle performance.Therefore,Ni_(0.96)S_(x)/MnS_(y)-NC exhibits excellent electrochemical properties following our modification route.Regarding stability performance,Ni0_(.96)S_(x)/MnS_(y)-NC demonstrates an average decay rate of 0.00944%after 10,000 cycles at an extremely high current density of 10000 mA g^(-1),A full cell with a high capacity of 304.2 mA h g^(-1)was also successfully assembled by using Na_(3)V_(2)(PO_(4))_(3)/C as the cathode.This study explores a novel strategy for interface/vacancy co-modification in the fabrication of high-performance sodium-ion batteries electrode.展开更多
A study of the interfacial behavior and internal thermal stress distribution in fiber-reinforced composites is essential to assess their performance and reliability.CNT/carbon fiber(CF)hybrid fibers were constructed u...A study of the interfacial behavior and internal thermal stress distribution in fiber-reinforced composites is essential to assess their performance and reliability.CNT/carbon fiber(CF)hybrid fibers were constructed using electrophoretic deposition.The interfacial properties of CF/epoxy and CNT/CF/epoxy composites were statistically investigated and compared using in-situ thermal Raman mapping by dispersing CNTs as a Raman sensing medium(CNT_(R))in a resin.The associated local thermal stress changes can be simulated by capturing the G'band position distribution of CNT_(R) in the epoxy at different temperatures.It was found that the G'band shifted to lower positions with increasing temperature,reaching a maximum difference of 2.43 cm^(−1) at 100℃.The interfacial bonding between CNT/CF and the matrix and the stress distribution and changes during heat treatment(20-100℃)were investig-ated in detail.This work is important for studying thermal stress in fiber-reinforced composites by in-situ thermal Raman mapping technology.展开更多
Brain-computer interface(BCI)technology is rapidly advancing in medical research and application.As an emerging biomedical engineering technology,it has garnered significant attention in the clinical research of brain...Brain-computer interface(BCI)technology is rapidly advancing in medical research and application.As an emerging biomedical engineering technology,it has garnered significant attention in the clinical research of brain disease diagnosis and treatment,neurological rehabilitation,and mental health.However,BCI also raises several challenges and ethical concerns in clinical research.In this article,the authors investigate and discuss three aspects of BCI in medicine and healthcare:the state of international ethical governance,multidimensional ethical challenges pertaining to BCI in clinical research,and suggestive concerns for ethical review.Despite the great potential of frontier BCI research and development in the field of medical care,the ethical challenges induced by itself and the complexities of clinical research and brain function have put forward new special fields for ethics in BCI.To ensure"responsible innovation"in BCI research in healthcare and medicine,the creation of an ethical global governance framework and system,along with special guidelines for cutting-edge BCI research in medicine,is suggested.展开更多
In this paper,a new finite element and finite difference(FE-FD)method has been developed for anisotropic parabolic interface problems with a known moving interface using Cartesian meshes.In the spatial discretization,...In this paper,a new finite element and finite difference(FE-FD)method has been developed for anisotropic parabolic interface problems with a known moving interface using Cartesian meshes.In the spatial discretization,the standard P,FE discretization is applied so that the part of the coefficient matrix is symmetric positive definite,while near the interface,the maximum principle preserving immersed interface discretization is applied.In the time discretization,a modified Crank-Nicolson discretization is employed so that the hybrid FE-FD is stable and second order accurate.Correction terms are needed when the interface crosses grid lines.The moving interface is represented by the zero level set of a Lipschitz continuous function.Numerical experiments presented in this paper confirm second orderconvergence.展开更多
Cold-junction compensation(CJC)and disconnection detection circuit design of various thermocouples(TC)and multi-channel TC interface circuits were designed.The CJC and disconnection detection circuit consists of a CJC...Cold-junction compensation(CJC)and disconnection detection circuit design of various thermocouples(TC)and multi-channel TC interface circuits were designed.The CJC and disconnection detection circuit consists of a CJC semiconductor device,an instrumentation amplifier(IA),two resistors,and a diode for disconnection detection.Based on the basic circuit,a multi-channel interface circuit was also implemented.The CJC was implemented using compensation semiconductor and IA,and disconnection detection was detected by using two resistors and a diode so that IA input voltage became-0.42 V.As a result of the experiment using R-type TC,the error of the designed circuit was reduced from 0.14 mV to 3μV after CJC in the temperature range of 0°C to 1400°C.In addition,it was confirmed that the output voltage of IA was saturated from 88 mV to-14.2 V when TC was disconnected from normal.The output voltage of the designed circuit was 0 V to 10 V in the temperature range of 0°C to 1400°C.The results of the 4-channel interface experiment using R-type TC were almost identical to the CJC and disconnection detection results for each channel.The implemented multi-channel interface has a feature that can be applied equally to E,J,K,T,R,and S-type TCs by changing the terminals of CJC semiconductor devices and adjusting the IA gain.展开更多
Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield ...Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield with a passable CO_(2) conversion and lack insight into its reaction mechanism for guiding the design of catalysts.In this work,Cu^(+)/CeZrO_(x) interfaces are engineered by employing a series of ceria-zirconia solid solution catalysts with various Ce/Zr ratios,forming a Cu^(+)-O_(v)-Ce^(3+)structure where Cu^(+)atoms are bonded to the oxygen vacancies(O_(v))of ceria.Compared to Cu/CeO_(2) and Cu/ZrO_(2),the optimized catalyst(i.e.,Cu_(0.3)Ce_(0.3)Zr_(0.7))exhibits a much higher mass-specific methanol formation rate(192g_(MeOH)/kg_(cat)/h)at 240℃and 3 MPa.Through a series of in-situ and ex-situ characterization,it is revealed that oxygen vacancies in solid solutions can effectively assist the activation of CO_(2) and tune the electronic state of copper to promote the formation of Cu^(+)/CeZrO_(x) interfaces,which stabilizes the key*CO intermediate,inhibits its desorption and facilitates its further hydrogenation to methanol via the reverse watergas-shift(RWGS)+CO-Hydro pathway.Therefore,the concentration of*CO or the apparent Cu^(+)/(Cu^(+)+Cu^(0))ratio could be employed as a quantitative descriptor of the methanol formation rate.This work is expected to give a deep insight into the mechanism of metal/support interfaces in CO_(2) hydrogenation to methanol,offering an effective strategy to develop new catalysts with high performance.展开更多
Designing cost-effective and high-efficiency electrocatalysts is critical to the water splitting performance during hydrogen generation.Herein,we have developed Fe_(2)P-Co_(2)P heterostructure nanowire arrays with exc...Designing cost-effective and high-efficiency electrocatalysts is critical to the water splitting performance during hydrogen generation.Herein,we have developed Fe_(2)P-Co_(2)P heterostructure nanowire arrays with excellent lattice torsions and grain boundaries for highly efficient water splitting.According to the microstructural investigations and theoretical calculations,the lattice torsion interface not only contributes to the exposure of more active sites but also effectively tunes the adsorption energy of hydrogen/oxygen intermediates via the accumulation of charge redistribution.As a result,the Fe_(2)P-Co_(2)P heterostructure nanowire array exhibits exceptional bifunctional catalytic activity with overpotentials of 65 and 198 mV at 10 mA cm^(-2) for hydrogen and oxygen evolution reactions,respectively.Moreover,the Fe_(2)P-Co_(2)P/NF-assembled electrolyzer can deliver 10 mA cm^(-2) at an ultralow voltage of1.51 V while resulting in a high solar-to-hydrogen conversion efficiency of 19.8%in the solar-driven water electrolysis cell.展开更多
Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectificatio...Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectification phenomenon in an asymmetric solid–liquid–solid sandwiched system with a nano-structured interface.By using the non-equilibrium molecular dynamics simulations,the thermal transport through the solid–liquid–solid system is examined,and the thermal rectification phenomenon can be observed.It is revealed that the thermal rectification effect can be attributed to the significant difference in the interfacial thermal resistance between Cassie and Wenzel states when reversing the temperature bias.In addition,effects of the liquid density,solid–liquid bonding strength and nanostructure size on the thermal rectification are examined.The findings may provide a new way for designs of certain thermal devices.展开更多
The User Interface Transition Diagram (UITD) is a formal modeling notation that simplifies the specification and design of user-system interactions. It is a valuable communication tool for technical and non-technical ...The User Interface Transition Diagram (UITD) is a formal modeling notation that simplifies the specification and design of user-system interactions. It is a valuable communication tool for technical and non-technical stakeholders during the requirements elicitation phase, as it provides a simple yet technically complete notation that is easy to understand. In this paper, we investigated the efficiency of creating UITDs using draw.io, a widely used diagramming software, compared to a dedicated UITD editor. We conducted a study to compare the time required to use each tool to complete the task of creating a medium size UITD, as well as the subjective ease of use and satisfaction of participants with the dedicated Editor. Our results show that the UITD editor is more efficient and preferred by participants, highlighting the importance of using specialized tools for creating formal models such as UITDs. The findings of this study have implications for software developers, designers, and other stakeholders involved in the specification and design of user-system interactions.展开更多
Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this ...Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.展开更多
The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high c...The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.展开更多
Oriented ligand immobilization is one of the most effective strategies used in the design and construction of a high-capacity protein A chromatography. In this work, cysteine was introduced as anchoring sites by subst...Oriented ligand immobilization is one of the most effective strategies used in the design and construction of a high-capacity protein A chromatography. In this work, cysteine was introduced as anchoring sites by substituting a specific residue on Helix Ⅰ, Ⅱ, and at C-terminus of antibody binding domain Z from protein A, respectively, to investigate structural evolution and binding behavior of protein A ligands at liquid-solid interfaces. Among the three affinity dextran-coated Fe_(3)O_(4) magnetic nanoparticles(Fe_(3)O_(4)@Dx MNPs), affinity MNPs with the immobilized ligand via N11C on Helix Ⅰ(Fe_(3)O_(4)@Dx-Z_(1) MNPs) had the highest helical content, and MNPs with the immobilized ligand via G29C on Helix Ⅱ(Fe_(3)O_(4)@Dx-Z_(2) MNPs) had the lowest helical content at the same pHs. It was attributed to less electrostatic attraction of ligand to negatively charged surface on Fe_(3)O_(4)@Dx-Z_(1) MNPs because of less positive charged residues on Helix Ⅰ(K6) than Helix Ⅱ(R27/K35). Among the three affinity MNPs, moreover, the highest affinity to immunoglobulin G(IgG) binding was observed on Fe_(3)O_(4)@Dx-Z_(1) MNPs in isothermal titration calorimetry measurement, further validating greater structural integrity of the ligand on Fe_(3)O_(4)@Dx-Z_(1) MNPs. Finally,the study of IgG binding on MNPs and 96-well plates showed that anchoring sites for ligand immobilization had distinct influences on IgG binding and IgG-mediated antigen binding. This work illustrated that anchoring sites of the ligands had a striking significance for the molecular structure of the ligand at liquid-solid interfaces and raised an important implication for the design and optimization of protein A chromatography and protein A-based immunoassay analysis.展开更多
The electronic structures and properties of electrocatalysts,which depend on the physicochemical structure and metallic element components,could significantly affect their electrocatalytic performance and their future...The electronic structures and properties of electrocatalysts,which depend on the physicochemical structure and metallic element components,could significantly affect their electrocatalytic performance and their future applications in Zn-air battery(ZAB)and overall water splitting(OWS).Here,by combining vacancies and heterogeneous interfacial engineering,three-dimensional(3D)core-shell NiCoP/NiO heterostructures with dominated oxygen vacancies have been controllably in-situ grown on carbon cloth for using as highly efficient electrocatalysts toward hydrogen and oxygen electrochemical reactions.Theoretical calculation and electrochemical results manifest that the hybridization of NiCoP core with NiO shell produces a strong synergistic electronic coupling effect.The oxygen vacancy can enable the emergence of new electronic states within the band gap,crossing the Fermi levels of the two spin components and optimizing the local electronic structure.Besides,the hierarchical core-shell NiCoP/NiO nanoarrays also endow the catalysts with multiple exposed active sites,faster mass transfer behavior,optimized electronic strutures and improved electrochemical performance during ZAB and OWS applications.展开更多
基金supported by the National Key Research and Development Program of China(2019YFA0205700)Scientific Research Projects of Colleges and Universities in Hebei Province(JZX2023004)+2 种基金Research Program of Local Science and Technology Development under the Guidance of Central(216Z4402G)support from Ministry of Science and Higher Education of Russian Federation(project FFSG-2022-0001(122111700046-3),"Laboratory of perspective electrode materials for chemical power sources")support from"Yuanguang"Scholar Program of Hebei University of Technology
文摘It is well accepted that a lithiophilic interface can effectively regulate Li deposition behaviors,but the influence of the lithiophilic interface is gradually diminished upon continuous Li deposition that completely isolates Li from the lithiophilic metals.Herein,we perform in-depth studies on the creation of dynamic alloy interfaces upon Li deposition,arising from the exceptionally high diffusion coefficient of Hg in the amalgam solid solution.As a comparison,other metals such as Au,Ag,and Zn have typical diffusion coefficients of 10-20 orders of magnitude lower than that of Hg in the similar solid solution phases.This difference induces compact Li deposition pattern with an amalgam substrate even with a high areal capacity of 55 mAh cm^(-2).This finding provides new insight into the rational design of Li anode substrate for the stable cycling of Li metal batteries.
基金the National Natural Science Foundation of China for Excellent Young Scholar(Grant No.52322313)National Key R&D Project from Minister of Science and Technology(2021YFA1201601)+6 种基金National Science Fund of China(62174014)Beijing Nova program(Z201100006820063)Youth Innovation Promotion Association CAS(2021165)Innovation Project of Ocean Science and Technology(22-3-3-hygg-18-hy)State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(KFZD202202)Fundamental Research Funds for the Central Universities(292022000337)Young Top-Notch Talents Program of Beijing Excellent Talents Funding(2017000021223ZK03).
文摘The triboelectric nanogenerator(TENG)can effectively collect energy based on contact electrification(CE)at diverse interfaces,including solid–solid,liquid–solid,liquid–liquid,gas–solid,and gas–liquid.This enables energy harvesting from sources such as water,wind,and sound.In this review,we provide an overview of the coexistence of electron and ion transfer in the CE process.We elucidate the diverse dominant mechanisms observed at different interfaces and emphasize the interconnectedness and complementary nature of interface studies.The review also offers a comprehensive summary of the factors influencing charge transfer and the advancements in interfacial modification techniques.Additionally,we highlight the wide range of applications stemming from the distinctive characteristics of charge transfer at various interfaces.Finally,this review elucidates the future opportunities and challenges that interface CE may encounter.We anticipate that this review can offer valuable insights for future research on interface CE and facilitate the continued development and industrialization of TENG.
基金support by the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai(AMGM2021A03)the"Special Lubrication and Sealing for Aerospace"Shaanxi Provincial Science and Technology Innovation Team(2024RS-CXTD-63)+1 种基金the Xianyang2023 Key Research and Development Plan(L2023-ZDYF-QYCX-009)the World First Class University and First Class Academic Discipline Construction Funding 2023(0604024GH0201332,0604024SH0201332).
文摘Flexible and wearable pressure sensors hold immense promise for health monitoring,covering disease detection and postoperative rehabilitation.Developing pressure sensors with high sensitivity,wide detection range,and cost-effectiveness is paramount.By leveraging paper for its sustainability,biocompatibility,and inherent porous structure,herein,a solution-processed all-paper resistive pressure sensor is designed with outstanding performance.A ternary composite paste,comprising a compressible 3D carbon skeleton,conductive polymer poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate),and cohesive carbon nanotubes,is blade-coated on paper and naturally dried to form the porous composite electrode with hierachical micro-and nano-structured surface.Combined with screen-printed Cu electrodes in submillimeter finger widths on rough paper,this creates a multiscale hierarchical contact interface between electrodes,significantly enhancing sensitivity(1014 kPa-1)and expanding the detection range(up to 300 kPa)of as-resulted all-paper pressure sensor with low detection limit and power consumption.Its versatility ranges from subtle wrist pulses,robust finger taps,to large-area spatial force detection,highlighting its intricate submillimetermicrometer-nanometer hierarchical interface and nanometer porosity in the composite electrode.Ultimately,this all-paper resistive pressure sensor,with its superior sensing capabilities,large-scale fabrication potential,and cost-effectiveness,paves the way for next-generation wearable electronics,ushering in an era of advanced,sustainable technological solutions.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61888102,52272172,and 52102193)the Major Program of the National Natural Science Foundation of China(Grant No.92163206)+2 种基金the National Key Research and Development Program of China(Grant Nos.2021YFA1201501 and 2022YFA1204100)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB30000000)the Fundamental Research Funds for the Central Universities.
文摘Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new materials in this respect.In van der Waals(vdW)layered materials,these building blocks are charge neutral and can be isolated from their bulk phase(top-down),but usually grow on substrate.In ionic layered materials,they are charged and usually cannot exist independently but can serve as motifs to construct new materials(bottom-up).In this paper,we introduce our recently constructed databases for 2D material-substrate interface(2DMSI),and 2D charged building blocks.For 2DMSI database,we systematically build a workflow to predict appropriate substrates and their geometries at substrates,and construct the 2DMSI database.For the 2D charged building block database,1208 entries from bulk material database are identified.Information of crystal structure,valence state,source,dimension and so on is provided for each entry with a json format.We also show its application in designing and searching for new functional layered materials.The 2DMSI database,building block database,and designed layered materials are available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00188.
基金Agency for Science,Technology and Research(A*STAR),under the RIE2020 Advanced Manufacturing and Engineering(AME)Programmatic Grant(Grant no.A18B1b0061)。
文摘The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.
基金the National Natural Science Foundation(No.52073187)NSAF Foundation(No.U2230202)for their financial support of this project+3 种基金National Natural Science Foundation(No.51721091)Programme of Introducing Talents of Discipline to Universities(No.B13040)State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-2-03)support of China Scholarship Council
文摘Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT aerogel structure shows nano-pore size(30-40 nm),high specific surface area(559 m^(2)g^(−1)),high void fraction(91.7%)and enhanced mechanical property:(1)the nano-pore size is beneficial for efficiently blocking thermal conduction and thermal convection via Knudsen effect(beneficial for infrared(IR)stealth);(2)the heterogeneous interface was beneficial for IR reflection(beneficial for IR stealth)and MWCNT polarization loss(beneficial for electromagnetic wave(EMW)attenuation);(3)the high void fraction was beneficial for enhancing thermal insulation(beneficial for IR stealth)and EMW impedance match(beneficial for EMW attenuation).Guided by the above theoretical design strategy,PVTMS@MWCNT nano-aerogel shows superior EMW absorption property(cover all Ku-band)and thermal IR stealth property(ΔT reached 60.7℃).Followed by a facial combination of the above nano-aerogel with graphene film of high electrical conductivity,an extremely high electromagnetic interference shielding material(66.5 dB,2.06 mm thickness)with superior absorption performance of an average absorption-to-reflection(A/R)coefficient ratio of 25.4 and a low reflection bandwidth of 4.1 GHz(A/R ratio more than 10)was experimentally obtained in this work.
基金supported by funding from Bavarian Center for Battery Technology(Baybatt,Hightech Agenda Bayern)and Bayerisch-Tschechische Hochschulagentur(BTHA)(BTHA-AP-202245,BTHA-AP-2023-5,and BTHA-AP-2023-12)supported by the University of Bayreuth-Deakin University Joint Ph.D.Program+1 种基金supported by the Regional Innovation Strategy(RIS)through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(MOE)(2021RIS-003)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS2023-00213749)
文摘A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and development have recently been conducted to form a stable interface between the electrode and electrolyte.Therefore,it is essential to investigate emerging knowledge and contextualize it.The nanoengineering of the electrode-electrolyte interface has been actively researched at the electrode/electrolyte and interphase levels.This review presents and summarizes some recent advances aimed at nanoengineering approaches to build a more stable electrode-electrolyte interface and assess the impact of each approach adopted.Furthermore,future perspectives on the feasibility and practicality of each approach will also be reviewed in detail.Finally,this review aids in projecting a more sustainable research pathway for a nanoengineered interphase design between electrode and electrolyte,which is pivotal for high-performance,thermally stable Li-ion batteries.
基金financially supported by the National Nature Science Foundation of Jiangsu Province(BK20221259)。
文摘Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electrochemical performance is greatly limited.In this study,a nickel/manganese sulfide material(Ni_(0.96)S_(x)/MnS_(y)-NC)with adjustable sulfur vacancies and heterogeneous hollow spheres was prepared using a simple method.The introduction of a concentration-adjustable sulfur vacancy enables the generation of a heterogeneous interface between bimetallic sulfide and sulfur vacancies.This interface collectively creates an internal electric field,improving the mobility of electrons and ions,increasing the number of electrochemically active sites,and further optimizing the performance of Na~+storage.The direction of electron flow is confirmed by Density functional theory(DFT)calculations.The hollow nano-spherical material provides a buffer for expansion,facilitating rapid transfer kinetics.Our innovative discovery involves the interaction between the ether-based electrolyte and copper foil,leading to the formation of Cu_9S_5,which grafts the active material and copper current collector,reinforcing mechanical supporting.This results in a new heterostructure of Cu_9S_5 with Ni_(0.96)S_(x)/MnS_(y),contributing to the stabilization of structural integrity for long-cycle performance.Therefore,Ni_(0.96)S_(x)/MnS_(y)-NC exhibits excellent electrochemical properties following our modification route.Regarding stability performance,Ni0_(.96)S_(x)/MnS_(y)-NC demonstrates an average decay rate of 0.00944%after 10,000 cycles at an extremely high current density of 10000 mA g^(-1),A full cell with a high capacity of 304.2 mA h g^(-1)was also successfully assembled by using Na_(3)V_(2)(PO_(4))_(3)/C as the cathode.This study explores a novel strategy for interface/vacancy co-modification in the fabrication of high-performance sodium-ion batteries electrode.
文摘A study of the interfacial behavior and internal thermal stress distribution in fiber-reinforced composites is essential to assess their performance and reliability.CNT/carbon fiber(CF)hybrid fibers were constructed using electrophoretic deposition.The interfacial properties of CF/epoxy and CNT/CF/epoxy composites were statistically investigated and compared using in-situ thermal Raman mapping by dispersing CNTs as a Raman sensing medium(CNT_(R))in a resin.The associated local thermal stress changes can be simulated by capturing the G'band position distribution of CNT_(R) in the epoxy at different temperatures.It was found that the G'band shifted to lower positions with increasing temperature,reaching a maximum difference of 2.43 cm^(−1) at 100℃.The interfacial bonding between CNT/CF and the matrix and the stress distribution and changes during heat treatment(20-100℃)were investig-ated in detail.This work is important for studying thermal stress in fiber-reinforced composites by in-situ thermal Raman mapping technology.
基金supported by the Ministry of Science and Tech-nology of the People's Republic of China(2021ZD0201900),Project 5(2021ZD0201905).
文摘Brain-computer interface(BCI)technology is rapidly advancing in medical research and application.As an emerging biomedical engineering technology,it has garnered significant attention in the clinical research of brain disease diagnosis and treatment,neurological rehabilitation,and mental health.However,BCI also raises several challenges and ethical concerns in clinical research.In this article,the authors investigate and discuss three aspects of BCI in medicine and healthcare:the state of international ethical governance,multidimensional ethical challenges pertaining to BCI in clinical research,and suggestive concerns for ethical review.Despite the great potential of frontier BCI research and development in the field of medical care,the ethical challenges induced by itself and the complexities of clinical research and brain function have put forward new special fields for ethics in BCI.To ensure"responsible innovation"in BCI research in healthcare and medicine,the creation of an ethical global governance framework and system,along with special guidelines for cutting-edge BCI research in medicine,is suggested.
基金partially supported by the National Natural Science Foundation of China(Grant No.12261070)the Ningxia Key Research and Development Project of China(Grant No.2022BSB03048)+2 种基金partially supported by the Simons(Grant No.633724)and by Fundacion Seneca grant 21760/IV/22partially supported by the Spanish national research project PID2019-108336GB-I00by Fundacion Séneca grant 21728/EE/22.Este trabajo es resultado de las estancias(21760/IV/22)y(21728/EE/22)financiadas por la Fundacion Séneca-Agencia de Ciencia y Tecnologia de la Region de Murcia con cargo al Programa Regional de Movilidad,Colaboracion Internacional e Intercambio de Conocimiento"Jimenez de la Espada".(Plan de Actuacion 2022).
文摘In this paper,a new finite element and finite difference(FE-FD)method has been developed for anisotropic parabolic interface problems with a known moving interface using Cartesian meshes.In the spatial discretization,the standard P,FE discretization is applied so that the part of the coefficient matrix is symmetric positive definite,while near the interface,the maximum principle preserving immersed interface discretization is applied.In the time discretization,a modified Crank-Nicolson discretization is employed so that the hybrid FE-FD is stable and second order accurate.Correction terms are needed when the interface crosses grid lines.The moving interface is represented by the zero level set of a Lipschitz continuous function.Numerical experiments presented in this paper confirm second orderconvergence.
文摘Cold-junction compensation(CJC)and disconnection detection circuit design of various thermocouples(TC)and multi-channel TC interface circuits were designed.The CJC and disconnection detection circuit consists of a CJC semiconductor device,an instrumentation amplifier(IA),two resistors,and a diode for disconnection detection.Based on the basic circuit,a multi-channel interface circuit was also implemented.The CJC was implemented using compensation semiconductor and IA,and disconnection detection was detected by using two resistors and a diode so that IA input voltage became-0.42 V.As a result of the experiment using R-type TC,the error of the designed circuit was reduced from 0.14 mV to 3μV after CJC in the temperature range of 0°C to 1400°C.In addition,it was confirmed that the output voltage of IA was saturated from 88 mV to-14.2 V when TC was disconnected from normal.The output voltage of the designed circuit was 0 V to 10 V in the temperature range of 0°C to 1400°C.The results of the 4-channel interface experiment using R-type TC were almost identical to the CJC and disconnection detection results for each channel.The implemented multi-channel interface has a feature that can be applied equally to E,J,K,T,R,and S-type TCs by changing the terminals of CJC semiconductor devices and adjusting the IA gain.
基金sponsored by the National Natural Science Foundation of China(21808120,21978148)。
文摘Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield with a passable CO_(2) conversion and lack insight into its reaction mechanism for guiding the design of catalysts.In this work,Cu^(+)/CeZrO_(x) interfaces are engineered by employing a series of ceria-zirconia solid solution catalysts with various Ce/Zr ratios,forming a Cu^(+)-O_(v)-Ce^(3+)structure where Cu^(+)atoms are bonded to the oxygen vacancies(O_(v))of ceria.Compared to Cu/CeO_(2) and Cu/ZrO_(2),the optimized catalyst(i.e.,Cu_(0.3)Ce_(0.3)Zr_(0.7))exhibits a much higher mass-specific methanol formation rate(192g_(MeOH)/kg_(cat)/h)at 240℃and 3 MPa.Through a series of in-situ and ex-situ characterization,it is revealed that oxygen vacancies in solid solutions can effectively assist the activation of CO_(2) and tune the electronic state of copper to promote the formation of Cu^(+)/CeZrO_(x) interfaces,which stabilizes the key*CO intermediate,inhibits its desorption and facilitates its further hydrogenation to methanol via the reverse watergas-shift(RWGS)+CO-Hydro pathway.Therefore,the concentration of*CO or the apparent Cu^(+)/(Cu^(+)+Cu^(0))ratio could be employed as a quantitative descriptor of the methanol formation rate.This work is expected to give a deep insight into the mechanism of metal/support interfaces in CO_(2) hydrogenation to methanol,offering an effective strategy to develop new catalysts with high performance.
基金financially supported by the National Natural Science Foundation of China(U2002213)the Creative Project of Engineering Research Center of Alternative Energy Materials&Devices,Ministry of Education,Sichuan University(AEMD202207)+7 种基金the Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials of Guangxi University(2022GXYSOF10)the Guangdong Colleges&Universities Characteristic Innovation Project(2021KTSCX263)the Guangdong Education&Scientific Research Project(2021GXJK535)the Guangzhou Panyu Polytechnic Science&Technology Project(2021KJ01)the East-Land Middle-aged and Young Backbone Teacher of Yunnan University(C176220200)the Yunnan Applied Basic Research Projects(202001BB050006,202001BB050007)the Double Tops Joint Fund of the Yunnan Science and Technology Bureau and Yunnan University(2019FY003025)the Double First Class University Plan(C176220100042)。
文摘Designing cost-effective and high-efficiency electrocatalysts is critical to the water splitting performance during hydrogen generation.Herein,we have developed Fe_(2)P-Co_(2)P heterostructure nanowire arrays with excellent lattice torsions and grain boundaries for highly efficient water splitting.According to the microstructural investigations and theoretical calculations,the lattice torsion interface not only contributes to the exposure of more active sites but also effectively tunes the adsorption energy of hydrogen/oxygen intermediates via the accumulation of charge redistribution.As a result,the Fe_(2)P-Co_(2)P heterostructure nanowire array exhibits exceptional bifunctional catalytic activity with overpotentials of 65 and 198 mV at 10 mA cm^(-2) for hydrogen and oxygen evolution reactions,respectively.Moreover,the Fe_(2)P-Co_(2)P/NF-assembled electrolyzer can deliver 10 mA cm^(-2) at an ultralow voltage of1.51 V while resulting in a high solar-to-hydrogen conversion efficiency of 19.8%in the solar-driven water electrolysis cell.
基金the National Natural Science Foundation of China(Grant No.51976002)the Beijing Nova Program of Science and Technology(Grant No.Z191100001119033)。
文摘Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectification phenomenon in an asymmetric solid–liquid–solid sandwiched system with a nano-structured interface.By using the non-equilibrium molecular dynamics simulations,the thermal transport through the solid–liquid–solid system is examined,and the thermal rectification phenomenon can be observed.It is revealed that the thermal rectification effect can be attributed to the significant difference in the interfacial thermal resistance between Cassie and Wenzel states when reversing the temperature bias.In addition,effects of the liquid density,solid–liquid bonding strength and nanostructure size on the thermal rectification are examined.The findings may provide a new way for designs of certain thermal devices.
文摘The User Interface Transition Diagram (UITD) is a formal modeling notation that simplifies the specification and design of user-system interactions. It is a valuable communication tool for technical and non-technical stakeholders during the requirements elicitation phase, as it provides a simple yet technically complete notation that is easy to understand. In this paper, we investigated the efficiency of creating UITDs using draw.io, a widely used diagramming software, compared to a dedicated UITD editor. We conducted a study to compare the time required to use each tool to complete the task of creating a medium size UITD, as well as the subjective ease of use and satisfaction of participants with the dedicated Editor. Our results show that the UITD editor is more efficient and preferred by participants, highlighting the importance of using specialized tools for creating formal models such as UITDs. The findings of this study have implications for software developers, designers, and other stakeholders involved in the specification and design of user-system interactions.
基金supported by the National Natural Science Foundation of China(grant nos.21975026 and 22005033)the National Postdoctoral Program of China(no.BX20180037)+1 种基金China Postdoctoral Science Foundation(no.2018M640077)the Beijing Institute of Technology Research Fund Program for Young Scholars(no.XSQD-202108005).
文摘Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.
基金supported by the National Natural Science Foundation of China (NSFC)(22075201)the National Key Research and Development Program of China (2022YFB4101800)。
文摘The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.
基金supported by the National Natural Science Foundation of China (Nos. 21878221 and 21476166)the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (No. 21621004)。
文摘Oriented ligand immobilization is one of the most effective strategies used in the design and construction of a high-capacity protein A chromatography. In this work, cysteine was introduced as anchoring sites by substituting a specific residue on Helix Ⅰ, Ⅱ, and at C-terminus of antibody binding domain Z from protein A, respectively, to investigate structural evolution and binding behavior of protein A ligands at liquid-solid interfaces. Among the three affinity dextran-coated Fe_(3)O_(4) magnetic nanoparticles(Fe_(3)O_(4)@Dx MNPs), affinity MNPs with the immobilized ligand via N11C on Helix Ⅰ(Fe_(3)O_(4)@Dx-Z_(1) MNPs) had the highest helical content, and MNPs with the immobilized ligand via G29C on Helix Ⅱ(Fe_(3)O_(4)@Dx-Z_(2) MNPs) had the lowest helical content at the same pHs. It was attributed to less electrostatic attraction of ligand to negatively charged surface on Fe_(3)O_(4)@Dx-Z_(1) MNPs because of less positive charged residues on Helix Ⅰ(K6) than Helix Ⅱ(R27/K35). Among the three affinity MNPs, moreover, the highest affinity to immunoglobulin G(IgG) binding was observed on Fe_(3)O_(4)@Dx-Z_(1) MNPs in isothermal titration calorimetry measurement, further validating greater structural integrity of the ligand on Fe_(3)O_(4)@Dx-Z_(1) MNPs. Finally,the study of IgG binding on MNPs and 96-well plates showed that anchoring sites for ligand immobilization had distinct influences on IgG binding and IgG-mediated antigen binding. This work illustrated that anchoring sites of the ligands had a striking significance for the molecular structure of the ligand at liquid-solid interfaces and raised an important implication for the design and optimization of protein A chromatography and protein A-based immunoassay analysis.
基金financially supported by the National Natural Science Foundation of China(No.22179014,21603019)program for the Hundred Talents Program of Chongqing University。
文摘The electronic structures and properties of electrocatalysts,which depend on the physicochemical structure and metallic element components,could significantly affect their electrocatalytic performance and their future applications in Zn-air battery(ZAB)and overall water splitting(OWS).Here,by combining vacancies and heterogeneous interfacial engineering,three-dimensional(3D)core-shell NiCoP/NiO heterostructures with dominated oxygen vacancies have been controllably in-situ grown on carbon cloth for using as highly efficient electrocatalysts toward hydrogen and oxygen electrochemical reactions.Theoretical calculation and electrochemical results manifest that the hybridization of NiCoP core with NiO shell produces a strong synergistic electronic coupling effect.The oxygen vacancy can enable the emergence of new electronic states within the band gap,crossing the Fermi levels of the two spin components and optimizing the local electronic structure.Besides,the hierarchical core-shell NiCoP/NiO nanoarrays also endow the catalysts with multiple exposed active sites,faster mass transfer behavior,optimized electronic strutures and improved electrochemical performance during ZAB and OWS applications.