ABSTRACT
Chromium-plated diamond/copper composite materials, with Cr layer thicknesses of 150 nm and 200 nm, were synthesized using a vacuum hot-press sintering process. Comparative analysis revealed that the thermal conductivity of the composite material with a Cr layer thickness of 150 nm increased by 266%, while that with a Cr layer thickness of 200 nm increased by 242%, relative to the diamond/copper composite materials without Cr plating. This indicates that the introduction of the Cr layer significantly enhanced the thermal conductivity of the composite material. The thermal properties of the composite material initially increased and subsequently decreased with rising sintering temperature. At a sintering temperature of 1050 °C and a diamond particle size of 210 µm, the thermal conductivity of the chromium-plated diamond/copper composite material reached a maximum value of 593.67 Wâm-1âK-1. This high thermal conductivity is attributed to the formation of chromium carbide at the interface. Additionally, the surface of the diamond particles in contact with the carbide layer exhibited a continuous serrated morphology due to the interface reaction. This "pinning effect" at the interface strengthened the bonding between the diamond particles and the copper matrix, thereby enhancing the overall thermal conductivity of the composite material.
ABSTRACT
Soft magnetic spinel ferrites are indispensable parts in devices such as transformers and inductors. Mechanical surface processing is a necessary step to realize certain shapes and surface roughness in producing the ferrite but also has a negative effect on the magnetic properties of the ferrite. In the past few years, a new surface layer was always believed to form during the mechanical surface processing, but the change of atomic structure on the surface and its effect on the magnetic structure remain unclear. Herein, an interface structure consisting of a rock-salt sublayer, distorted NiFe2O4 sublayer, and pristine NiFe2O4 was found to form on mechanically polished single-crystal NiFe2O4 ferrite. Such an interface structure is produced by phase transformation and lattice distortion induced by the mechanical processing. The magnetic domain observation and electrical property measurement also indicate that the magnetic and electrical anisotropy are both enhanced by the interface structure. This work provides deep insight into the surface structure evolution of spinel ferrite by mechanical processing.
ABSTRACT
Microsphere-based embolic agents have gained prominence in transarterial embolization (TAE) treatment, a critical minimally invasive therapy widely applied for a variety of diseases such as hypervascular tumors and acute bleeding. However, the development of microspheres with long-term, real-time, and repeated X-ray imaging as well as ultrasound imaging remains challenging. In this study, emulsion-based dual-modal imaging microbeads with a unique internal multi-interface structure is developed for TAE treatment. The embolic microbeads are fabricated from a solidified oil-in-water (O/W) emulsion composed of crosslinked CaAlg-based aqueous matrix and dispersed radiopaque iodinated oil (IO) droplets through a droplet-based microfluidic fabrication method. The CaAlg-IO microbeads exhibit superior X-ray imaging visibility due to the incorporation of exceptionally high iodine level up to 221 mgI mL-1, excellent ultrasound imaging capability attributed to the multi-interface structure of the O/W emulsion, great microcatheter deliverability thanks to their appropriate biomechanical properties and optimal microbead density, and extended drug release behavior owing to the biodegradation nature of the embolics. Such an embolic agent presents a promising emulsion-based platform to utilize multi-phased structures for improving endovascular embolization performance and assessment capabilities.
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For N-type tunnel-oxide-passivated-contact silicon solar cells, optimal Ag/Al-Si contact interface is crucial to improve the efficiency. However, the specific roles of Ag and Al at the interface have not been clearly elucidated. Hence, this work delves into the sintering process of Ag/Al paste and examines the impact of the Ag/Al-Si interface structure on contact quality. By incorporating TeO2 into PbO-based Ag/Al paste, the Ag/Al-Si interface structure can be modulated. It can be found that TeO2 accelerates the sintering of Ag powder and increases Ag colloids within glass layer, while it simultaneously impedes the diffusion of molten Al. It leads to a reduced Al content near the Ag/Al-Si interface and a shorter diffusion distance of Al into Si. Notably, it can be demonstrated that the diffusion of Al in Si layer is more effective to reduce the contact resistance than the precipitation of Ag colloids. Therefore, the PbO-based Ag/Al paste, which favors Al diffusion, leads to solar cells with lower contact resistance and series resistance, higher fill factor, and superior photoelectric conversion efficiency. In brief, this work is significant for optimizing metallization of silicon solar cells and other semiconductor devices.
ABSTRACT
A challenge facing the chlor-alkali process is the lack of electrocatalyst with high activity and selectivity for the efficient industrial production of chlorine. Herein the authors report a new electrocatalyst that can generate multi-interface structure by in situ growth of graphdiyne on the surface of cobalt oxides (GDY/Co3O4), which shows great potential in highly selective and efficient chlorine production. This result is due to the strong electron transfer and high density charge transport between GDY and Co3O4 and the interconversion of the mixed valence states of the Co atoms itself. These intrinsic characteristics efficiently enhance the conductivity of the catalyst, facilitate the reaction kinetics, and improve the overall catalytic selectivity and activity. Besides, the protective effect of the formed GDY layer is remarkable endowing the catalyst with excellent stability. The catalyst can selectively produce chlorine in low-concentration of NaCl aqueous solution at room temperature and pressure with the highest Faraday efficiency of 80.67% and an active chlorine yield rate of 184.40 mg h-1 cm-2, as well as superior long-term stability.
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The main strengthening mechanism for Inconel 718 (IN718), a Ni-based superalloy, is precipitation hardening by γ' and γⳠparticles. It is thus essential, for good alloy performance, that precipitates with the desired chemical composition have adequate size and dispersion. The distribution of the γ' and γⳠphases and their chemical composition were investigated in the nickel-based Inconel 718 superalloy by taking advantage of the new capabilities of scanning transmission electron microscopy and energy-dispersive X-ray spectrometry using a windowless multiple detector, a high-brightness Schottky electron gun, and a spherical aberration corrector in the illumination probe optics. A small routine was developed to deconvolute the respective compositions of γ' and γⳠnanoprecipitates embedded in the γ matrix. Keeping the electron probe current low enough-a few hundred pA-prevented excessive irradiation damage during the acquisition of element maps and brought their spatial resolution down to the atomic column level to track their element compositions. The present results agree with and complement atomic probe tomography observations and Thermo-Calc predictions from the literature. The presence of an Al enrichment at the γ'/γⳠinterface-which may control the γⳠphase coarsening-is observed in the last row of Al-Nb-Ti columns along this interface. In addition, a few columns with similar composition changes are found randomly distributed in the γ' phase.
ABSTRACT
Recently, the TiAlSiN/TiAlN coatings with excellent mechanical and thermal properties have great potential for protective applications that face deteriorated service environments. Here, we systematically investigate the interface structure, mechanical properties, and thermal stability of TiAlSiN/TiAlN multilayers with varied Al and Si contents of TiAlSiN sublayer. Both Ti0.53Al0.38Si0.09N/Ti0.52Al0.48N (ML_1) and Ti0.48Al0.38Si0.14N/Ti0.52Al0.48N (ML_2) exhibit the face-centered cubic structure through epitaxial growth, whereas the Ti0.43Al0.48Si0.09N/Ti0.52Al0.48N (ML_3) shows a mixed cubic/wurtzite (c/w) structure. This mechanism is explored by first-principles calculations that the increased content of Al and Si within the TiAlSiN sublayer is detrimental to the formation of a coherent interface. Meanwhile, the change of interfacial structure leads to a variation in hardness from â¼35.6 GPa of ML_1 to â¼35.4 GPa of ML_2 and then to â¼30.9 GPa of ML_3. In addition, ML_1 presents a delayed thermal decomposition by â¼100 °C, compared to those of ML_2 and ML_3 multilayers.
ABSTRACT
Polyethylene film mulching is a key technology for soil water retention in dryland agriculture, but the aging of the films can generate a large number of microplastics with different shapes. There exists a widespread misunderstanding that the concentrations of microplastics might be the determinant affecting the diversity and assembly of soil bacterial communities, rather than their shapes. Here, we examined the variations of soil bacteria community composition and functioning under two-year field incubation by four shapes (ball, fiber, fragment and powder) of microplastics along the concentration gradients (0.01%, 0.1% and 1%). Data showed that specific surface area of microplastics was significantly positively correlated with the variations of bacterial community abundance and diversity (r=0.505, p<0.05). The fragment- and fiber-shape microplastics displayed more pronounced interfacial continuity with soil particles and induced greater soil bacterial α-diversity, relative to the powder- and ball-shape ones. Strikingly, microplastic concentrations were not significantly correlated with bacterial community indices (r=0.079, p>0.05). Based on the variations of the ßNTI, bacterial community assembly actually followed both stochastic and deterministic processes, and microplastic shapes significantly modified soil biogeochemical cycle and ecological functions. Therefore, the shapes of microplastics, rather than the concentration, significantly affected soil bacterial community assembly, in association with microplastic-soil-water interfaces.
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The harm of electromagnetic waves on human daily life has gradually received attention, and electromagnetic waves absorption materials have been used to address this issue. MXene, as a new type of 2D material, is a very promising electromagnetic wave absorption material. In this study, NiS nanoparticles were grown on the surface of S terminated Ti3C2Tx, and -S group acted as sulfur sources to construct Ti-S-Ni covalent interface directly in NiS/Ti3C2Tx composites. To further regulate the interface structure and electromagnetic properties, -P and -NH2 groups were also introduced onto the surface of MXene to achieve the N, P co-doping NiS/Ti3C2Tx composites with covalent interface. By investigating the electromagnetic wave absorption performance of the composites, it was found that N and P doping could effectively enhance the electron transfer rate at the interface and optimize the conduction loss, resulting in a significant improvement in performance. The minimum reflection loss was -50.6 dB at a frequency of 15.6 GHz, and the matching thickness was only 1.14 mm with an effective absorption bandwidth of 3.6 GHz. These results provide an important references and guidance for further research and development of high-performance electromagnetic wave absorption materials.
ABSTRACT
Electric-driven freshwater/seawater splitting is an attractive and sustainable route to realize the generation of H2 and O2. Molybdenum-based oxides exhibit poor activity toward freshwater/seawater electrolysis. Herein, we adjusted the electronic structure of MoO2 by constructing N-doped carbon sheets supported P-Fe3O4-MoO2 nanosheets (P-Fe3O4-MoO2/NC). P-Fe3O4-MoO2/N-doped carbon sheets were precisely prepared by pyrolysis of Schiff base Fe complex and MoO3 nanosheets through phosphorization. Benefiting from the unique structures of the samples, it required 119/145 mV to drive freshwater/seawater reduction reaction at 10 mA/cm2. P-Fe3O4-MoO2/NC catalysts exhibited superior freshwater/seawater oxidation reactivity with 180/189 mV at 10 mA/cm2 compared with commercial RuO2. The low cell voltages for P-Fe3O4-MoO2/NC were 1.47 and 1.59 V towards freshwater and seawater electrolysis, respectively. Our work might shed light on the structural modulation of Mo-based oxides for enhancing freshwater and seawater electrolysis activity.
ABSTRACT
During a practical battery manufacture process, the LiCoO2 (LCO) electrodes are usually rolled with high pressure to achieve better performance, including reducing electrode polarization, increasing compact density, enhancing mechanical toughness, etc. In this work, a high-voltage LCO (HV-LCO) is achieved via modulating a commercialized LCO with an Al/F enriched and spinel reinforced surface structure. We reveal that the rolling can more or less introduce risk of grain-boundary-cracking (GBC) inside the HV-LCO and accelerate the capacity decay when cycled at 3-4.6 V vs Li/Li+. In particular, the concept of interface structure is proposed to explain the reason for the deteriorated cycle stability. As the GBC is generated, the interface structure of HV-LCO alters from a surface spinel phase to a hybrid of surface spinel plus boundary layer phases, leading to the exposure of some the nonprotective layer phase against the electrolyte. This alternation causes serious bulk structure damage upon cycles, including expanding GBC among the primary crystals, forming intragranular cracks and inactive spinel phases inside the bulk regions, etc., eventually leading to the deteriorated cycle stability. Above all, we realize that it is far from enough to achieve a eligible high-voltage LCO via only applying surface modification. This work provides a new insight for developing more advanced LCO cathodes.
ABSTRACT
Sluggish storage kinetics and insufficient performance are the major challenges that restrict the transition metal dichalcogenides (TMDs) applied for zinc ion storage, especially at the extreme temperature conditions. Herein, a multiscale interface structure-integrated modulation concept was presented, to unlock the omnidirectional storage kinetics-enhanced porous VSe2-x â n H2 O host. Theory research indicated that the co-modulation of H2 O intercalation and selenium vacancy enables enhancing the interfacial zinc ion capture ability and decreasing the zinc ion diffusion barrier. Moreover, an interfacial adsorption-intercalation pseudocapacitive storage mechanism was uncovered. Such cathode displayed remarkable storage performance at the wide temperature range (-40-60 °C) in aqueous and solid electrolytes. In particular, it can retain a high specific capacity of 173â mAh g-1 after 5000â cycles at 10â A g-1 , as well as a high energy density of 290â Wh kg-1 and a power density of 15.8â kW kg-1 at room temperature. Unexpectedly, a remarkably energy density of 465â Wh kg-1 and power density of 21.26â kW kg-1 at 60 °C also can be achieved, as well as 258â Wh kg-1 and 10.8â kW kg-1 at -20 °C. This work realizes a conceptual breakthrough for extending the interfacial storage limit of layered TMDs to construct all-climate high-performance Zn-ion batteries.
ABSTRACT
Next-generation materials for fast ion conduction have the potential to revolutionize battery technology. Metal-organic frameworks (MOFs) are promising candidates for achieving this goal. Given their structural diversity, the design of efficient MOF-based conductors can be accelerated by a detailed understanding and accurate prediction of ion conductivity. However, the polycrystalline nature of solid-state materials requires consideration of grain boundary effects, which is complicated by challenges in characterizing grain boundary structures and simulating ensemble transport processes. To address this, we have developed an approach for modeling ion transport at grain boundaries and predicting their contribution to conductivity. Mg2+ conduction in the Mg-MOF-74 thin film was studied as a representative system. Using computational techniques and guided by experiments, we investigated the structural details of MOF grain boundary interfaces to determine accessible Mg2+ transport pathways. Computed transport kinetics were input into a simplified MOF nanocrystal model, which combines ion transport in the bulk structure and at grain boundaries. The model predicts Mg2+ conductivity in the MOF-74 film within chemical accuracy (<1 kcal/mol activation energy difference), validating our approach. Physically, Mg2+ conduction in MOF-74 is inhibited by strong Mg2+ binding at grain boundaries, such that only a small fraction of grain boundary alignments allow for fast Mg2+ transport. This results in a 2-3 order-of-magnitude reduction in conductivity, illustrating the critical impact of the grain boundary contribution. Overall, our work provides a computation-aided platform for molecular-level understanding of grain boundary effects and quantitative prediction of ion conductivity. Combined with experimental measurements, it can serve as a synergistic tool for characterizing the grain boundary composition of MOF-based conductors.
ABSTRACT
Flexible supercapacitors have attracted more and more attention because of their promising applications in wearable electronics, however, it is still important to harmonize their mechanical and electrochemical properties for practical applications. In the present work, a seamless transition between polyaniline (PANI) electrode and NH4VO3_FeSO4 dual redox-mediated gel polymer electrolyte (GPE) is presented through in situ formation of gradient interface structure. Multiple physical interactions make the GPE excellent mechanical and self-healing properties. Meanwhile, double role functions of Fe2+ ions greatly relieve the traditional contradiction between mechanical and electrochemical properties of GPE. Moreover, benefiting from the structure and reversible redox reactions of VO3- and Fe2+, the integrated supercapacitor delivers an exceptional specific capacitance of 441.8 mF/cm2, a high energy density of 63.1 µWh/cm2, remarkable cyclic stability. Simultaneously, the gradient structure from PANI electrode to GPE greatly improves the electrode/electrolyte interface compatibility and ion transport, which endows the supercapacitor with stable electrochemical performance. Furthermore, the supercapacitor well-maintains the specific capacitance even at -20 °C with over 89.19 % retention after 6 cutting/healing cycles. The gradient interface structure design will promote the development of high-performance supercapacitor.
ABSTRACT
Diamond/copper composites with high thermal conductivity and a variable thermal expansion coefficient are promising materials for thermal management applications. However, achieving the desired thermal conductivity of the composite material is difficult due to detachment or weak bonding between diamond and Cu. The interfacial properties of diamond/Cu composites can be improved using metal matrix alloying methods. In this study, we investigate the effects of alloying elements (B, Cr, Hf, Mo, Nb, Si, Ti, V, Zr) on the interfacial properties of diamond/Cu using first-principles calculations. Results showed that all alloying components could increase the interfacial bonding of diamond/Cu. Analysis of the electronic structure revealed that increased interfacial bonding strength after doping was the result of the stronger bonding of the alloying element atoms to the C atoms. The C atoms in the first layer of diamond at the interface formed wave peaks near the Fermi energy level after doping with B or Si atoms, facilitating electron-phonon interaction at the interface. The phonon properties of B4C and SiC were similar to those of diamond, which facilitated phonon-phonon coupling. B and Si were shown to be better alloying elements when interfacial bond strength and heat transfer were considered.
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It is widely recognized that designing a special micro/nanostructure of microwave absorption materials for enhancing interface polarization benefits dielectric loss capability. In this work, a facile charge-driven self-assembly strategy is reported to prepare wrinkled reduced graphene oxide wrapped polymer-derived carbon (CS@rGO) microspheres. Noticeably, the unique three-dimensional (3D) multi-interface structure imparts CS@rGO microspheres with promoted microwave absorption capability. Adjusting the charge-driven self-assembly cycle times, the dielectric properties and impedance matching characteristics of the CS@rGO microspheres can be optimized. The minimum reflection loss (RLmin) of the sample can reach up to -55.24 dB at 13.75 GHz and the effective absorption bandwidth (RL ≤ -10 dB) is 4.30 GHz (11.55-15.85 GHz) at only a thickness of 1.85 mm. This research provides a pathway to explore the high-performance microwave absorber through the construction of the unique 3D multi-interface structure.
Subject(s)
Carbon , Microwaves , Microspheres , PolymersABSTRACT
Electrocatalytic upgrading of biomass-derived platform molecules has emerged as a sustainable and environmentally benign route to produce high-value chemicals. The main challenge lies in developing efficient catalysts for the selective activation of designated chemical bonds in the presence of various reducible groups. This work demonstrated a high-efficiency electrochemical conversion of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF), an important industrial synthetic reagent. A highly porous Cu-based catalyst was developed that achieved nearly 100% BHMF selectivity and long-term stability. Through comprehensive operando and ex-situ structural characterizations, an electrochemically generated catalyst with abundant Cu/Cu2O interfaces was identified as a catalytically active phase for HMF conversion. Deuterated BHMF, with the potential to produce deuterated drugs, was also synthesized using D2O as the deuterium source. Density functional theory calculations show that the Cu/Cu2O interface structure exhibits relatively low energy barriers for the hydrogenation of HMF to BHMF. This work provides insights into the origin of electrocatalytic hydrogenation activity and highlights the promising potential of the electrocatalytic synthesis of high-value chemicals.
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Insufficient catalyst utilization, limited mass transport, and high ohmic resistance of the conventional membrane electrode assembly (MEA) lead to significant performance losses of proton exchange membrane water electrolysis (PEMWE). Herein we propose a novel ordered MEA based on anode with a 3D membrane/catalytic layer (CL) interface and gradient tapered arrays by the nanoimprinting method, confirmed by energy dispersive spectroscopy. Benefiting from the maximized triple-phase interface, rapid mass transport, and gradient CL by overall design, such an ordered structure with Ir loading of 0.2 mg cm-2 not only greatly increases the electrochemical active area by 4.2 times but also decreases the overpotentials of both mass transport and ohmic polarization by 13.9% and 8.7%, respectively, compared with conventional MEA with an Ir loading of 2 mg cm-2, thus ensuring a superior performance (1.801 V at 2 A cm-2) and good stability. This work provides a new strategy of designing MEA for high-performance PEMWE.
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Organic-inorganic hybrid perovskite solar cells (PeSCs) attract much attention in the field of solar cells due to their excellent photovoltaic performance. Many efforts have been devoted to improving their power conversion efficiency (PCE). However, few works focus on simultaneously improving their electrical and optical property. Herein, a simple strategy is proposed to improve the PCE from 19.8% of a reference device to 22.9%, by utilizing cesium carbonate (Cs2CO3) to modify indium tin oxide (ITO) substrate. The insertion of a Cs2CO3-modification layer between ITO substrate and SnO2 electron transport layer simultaneously offers two benefits: improving the electron extraction capability and adjusting the light field distribution in the device. The optical optimization effect of Cs2CO3 revealed in this work has not been reported before. This work provides a new and simple strategy to obtain high performance PeSCs by improving the electrical and optical properties of the devices at the same time.
ABSTRACT
The detailed investigation of food-grade emulsions, which possess considerable structural and functional advantages, remains ongoing to enhance our understanding of these dispersion systems and to expand their application scope. This work reviews the applications of food-grade emulsions on the dispersed phase, interface structure, and macroscopic scales; further, it discusses the corresponding factors of influence, the selection and design of food dispersion systems, and the expansion of their application scope. Specifically, applications on the dispersed-phase scale mainly include delivery by soft matter carriers and auxiliary extraction/separation, while applications on the scale of the interface structure involve biphasic systems for enzymatic catalysis and systems that can influence substance digestion/absorption, washing, and disinfection. Future research on these scales should therefore focus on surface-active substances, real interface structure compositions, and the design of interface layers with antioxidant properties. By contrast, applications on the macroscopic scale mainly include the design of soft materials for structured food, in addition to various material applications and other emerging uses. In this case, future research should focus on the interactions between emulsion systems and food ingredients, the effects of food process engineering, safety, nutrition, and metabolism. Considering the ongoing research in this field, we believe that this review will be useful for researchers aiming to explore the applications of food-grade emulsions.