Multilayer Electrode Research Articles

Multilayer Electrode Strategy Shorten Thermal Charging Time and Boost Energy Output in Gelatin‐Based i‐TE Cells

AbstractGel‐based ionic thermoelectric (i‐TE) cells provide alternative thermal energy harvesting from the environment, showing obvious advantages in voltage matching for self‐powered Internet‐of‐Things (IoT) sensors. However, the gel‐based i‐TE cells always suffer a long thermal charging time and poor output power performance. Herein, a multilayer electrode engineering strategy is proposed from the device‐design level, aiming to decrease the ions' diffusion distance, increase the electrode surface area, and facilitate the ions' reaction and recovery process. The thermal charging time is shortened from 27 to 8 min as the electrode layers increase from 2 to 8. An ultrahigh instantaneous power density of 15.8 mW m−2 K−2 and 2 h output energy density (E2h) of 403 J m−2 are achieved in an 8‐layer electrode i‐TE cell. Finally, A flexible and wearable i‐TE device with 20 units is demonstrated to generate a remarkable voltage of 3.8 V and output power of 282 µW by harvesting the human body heat. This work provides a feasible and effective route to design the i‐TE device, hopefully promoting its practical power generation application.

Magnetic tunnel junction based on bilayer LaI2 as perfect spin filter device

The discovery of van der Waals intrinsic magnets has expanded the possibilities of realizing spintronics devices. We investigate the transmission, tunneling magnetoresistance ratio, and spin injection efficiency of bilayer LaI2 using a combination of first-principles calculations and the non-equilibrium Green’s function method. Multilayer graphene electrodes are employed to build a magnetic tunnel junction with bilayer LaI2 as ferromagnetic barrier. The magnetic tunnel junction turns out to be a perfect spin filter device with an outstanding tunneling magnetoresistance ratio of 653% under a bias of 0.1 V and a still excellent performance in a wide bias range. In combination with the obtained high spin injection efficiency this opens up great potential from the application point of view.

Microconfined Assembly of High-Resolution and Mechanically Robust EGaIn Liquid Metal Stretchable Electrodes for Wearable Electronic Systems.

Stretchable electrodes based on liquid metals (LM) are widely used in human-machine interfacing, wearable bioelectronics, and other emerging technologies. However, realizing the high-precision patterning and mechanical stability remains challenging due to the poor wettability of LM. Herein, a method is reported to fabricate LM-based multilayer solid-liquid electrodes (m-SLE) utilizing electrohydrodynamic (EHD) printed confinement template. In these electrodes, LM self-assembled onto these high-resolution templates, assisted by selective wetting on the electrodeposited Cu layer. This study shows that a m-SLE composed of PDMS/Ag/Cu/EGaIn exhibits line width of ≈20µm, stretchability of ≈100%, mechanical stability ≈10000 times (stretch/relaxation cycles), and recyclability. The multi-layer structure of m-SLE enables the adjustability of strain sensing, in which the strain-sensitive Ag part can be used for non-distributed detection in human health monitoring and the strain-insensitive EGaIn part can be used as interconnects. In addition, this study demonstrates that near field communication (NFC) devices and multilayer displays integrated by m-SLEs exhibit stable wireless signal transmission capability and stretchability, suggesting its applicability in creating highly-integrated, large-scale commercial, and recyclable wearable electronics.

Dispersion of thermoelastic guided waves in multi-layered porous media

The mechanical properties of the graphite electrode will dynamically change during the charge-discharge cycle, which will affect the propagation characteristics of guided waves in lithium-ion batteries. Meanwhile, lithium-ion batteries experience fluctuations in operating temperature during cycling, which will also influence the propagation of guided waves. This research aims to investigate the guided wave propagation problem of porous electrode material with electrolyte versus temperature. The problem is under the framework of Green-Naghdi theory and Biot theory, and a numerical approach is presented to solve the thermoelastic wave propagation characteristics in such a multi-layered porous electrode. A frequency domain simulation for a multi-layered porous anode will be established. The simulation results confirm the feasibility and accuracy of the proposed approach. The porosity of the anode material shows obvious dynamic variation during cycling, which illustrates a strong correlation with the elastic modulus of the solid skeleton. Then, the effects of porosity and temperature variations on the propagation characteristics of thermoelastic guided waves in multi-layered porous graphite electrodes will be analyzed in detail. The phase velocity of fundamental modes appears regularly shift in the low frequency range. This may provide theoretical support for the acoustic nondestructive characterization of the operating states of the lithium-ion batteries.

Surface Acoustic Wave Sensors for Wireless Temperature Measurements above 1200 Degree Celsius.

High-temperature wireless sensing is crucial for monitoring combustion chambers and turbine stators in aeroengines, where surface temperatures can reach up to 1200 °C. Surface Acoustic Wave (SAW) temperature sensors are an excellent choice for these measurements. However, at extreme temperatures, they face issues such as agglomeration and recrystallization of electrodes, leading to loss of conductivity and reduced quality factor, hindering effective wireless signal transmission. This study develops an LGS SAW sensor with a Pt-10%Rh/Zr/Pt-10%Rh/Zr/Pt-10%Rh/Zr multilayer composite electrode structure to address these challenges. We demonstrate that the sensor can achieve wireless temperature measurements from room temperature to 1200 °C with an accuracy of 1.59%. The composite electrodes excite a quasi-shear wave on the LGS substrate, maintaining a Q-factor of 3526 at room temperature, providing an initial assurance for the strength of the wireless interrogation echo signal. The sensor operates stably for 2.18 h at 1200 °C before adhesion loss between the composite electrode and the substrate causes a sudden increase in resonant frequency. This study highlights the durability of the proposed electrode materials and structure at extreme temperatures and suggests future research to improve adhesion and extend the sensor's lifespan, thereby enhancing the reliability and effectiveness of high-temperature wireless sensing in aerospace applications.

Resistive Switching in Silver Iodide with Multi-Layer Graphene Electrodes

Resistive Switching in Silver Iodide with Multi-Layer Graphene Electrodes

Effect of interlayer thickness on electrochemical properties and corrosion resistance of sputtered TiNxnm/Tixnm multilayer thin films

Three multilayers [TiNxnm/Tixnm/p-type Si (100)] (x = 2.5, 5, 10) were fabricated using a dc-magnetron sputtering to evaluate surface and interfacial effect on electrochemical properties for possible application in supercapacitor electrode materials. The (111) and (101) planes of TiN and Ti were observed at 36.50° and 40.19° respectively. TA, LA, and TO phonon modes were found at 254.12, 306.15, and 637.94 cm−1, respectively. The defect state distribution of Ti, N, and O was investigated from PL. XPS confirmed the Ti at. % of TiNxnm/Tixnm multilayers decreased from 43.07 to 12.04 and N at. % increased from 42.79 to 72.53 % as the x value decreased from 10 nm to 2.5 nm. The areal specific capacitance (Ca) and energy density (E) of the TiNxnm/Tixnm multilayer electrode increased with decreasing multilayer thickness. E varied from 0.27 to 1.37 mWhcm−2 and the power density (P) from 5.04 to 25.4 mWcm−2 for the multilayers. The diffusion coefficient (D) and total accumulated charge (Qin) decreased from 6.48 × 10−17 to 1.56 × 10−18 cm2/s and 1.82 to 1.64 C/cm2, respectively, for TiNxnm/Tixnm multilayers. The capacitive contribution was the highest in x = 10 (2.181 Av−1s). However, the diffusion-limited contribution was maximum in x = 5 (3.541 Av−1/2s1/2). The cyclic stability maintained at 85.4 % capacitive retention over 1000 cycles and the expansive potential window (up to 0.8 V in 1 M H2SO4) makes the multilayer thin films ideal for supercapacitor electrodes. Among all the samples, the TiN2.5nm/Ti2.5nm exhibited the highest Ca, E, and diffusion coefficient, originating from the smaller layer thickness, leading to more ohmic conductivity and facilitating the supercapacitive performance.

Qualitative and quantitative protease activity tests based on protein degradation in three-dimensional structures

The pattern of the activity of proteases is related to distinct physiological states of living organisms. Often activity changes of a certain protease can be assigned to a specific disease. Hence, they are useful biomarkers and a simple and fast determination method of their activity could be a valuable tool for the efficient monitoring of numerous diseases. Here, two different methods for the qualitative and quantitative determination of protease activity are demonstrated using the model system of proteinase K. The first test system is based on a protein-modified and colored 3D silica structure that changes color when exposed to the enzyme. This method has also been used for the detection of matrix metallo-protease 2 (MMP2) with gelatine as protease substrate on the plates. The second detection system uses the decrease in the voltammetric signal of a cytochrome c/DNA multilayer electrode after incubation with a protease to quantitatively determine its proteolytic activity. While activities down to 0.15 U/ml can be detected with the first method, the second one provides detection limits of about 0.03U/ml (for proteinase K.) The functionality of both systems can be demonstrated and ways for further enhancement of sensitivity have been elucidated.

E-peroxone with a novel GDE decorated with hydrophobic membrane for the degradation of pyridine: Stability, byproducts and toxicity

E-peroxone process is an emerging electrochemical oxidation process, based on ozone and the in-situ cathodic generation of H2O2, but the stability of cathode is one of the key restraining factors. In this study, we designed a multilayer gas diffusion electrode (GDE) decorated with a commercial hydrophobic membrane for the degradation of pyridine. It was found that a proper control of membrane pore sizes and hot-pressing temperature can significantly promote the GDE stability. Subsequently, key operational parameters of the constructed E-peroxone system were investigated, including the ozone concentration, current density, pH value, electrolyte type and initial concentration of pyridine. The degradation pathways were proposed according to six identified transformation products. The toxicity variation along the degradation progress was evaluated with microbial respiration tests and Toxicity Estimation Software Tool (T.E.S.T.) calculation and an efficient detoxification capacity of E-peroxone was observed. This research provides a theoretical basis and technical support for the development of highly efficient and stable E-peroxone system for the elimination of toxic organic contaminants.

3-Dimensional numerical study on carbon based electrodes for vanadium redox flow battery

Electrode materials are critical in determining the performance of Vanadium redox flow batteries (VRFB). This work aims at elucidating the difference between carbon-based electrodes for VRFB. The electrodes considered for the present study are Graphite felt, Carbon felt, Carbon paper, and Carbon cloth. To study the characteristic behavior of different electrode materials, a 3D unit cell numerical model was developed by coupling electrolyte flow and electrochemical reactions and mass transfer module apart from considering the electrode structural and material information such as porosity, permeability, thickness, conductivity, and specific area. The simulation results of this study suggest that the Graphite felt is the optimum choice as an electrode material for VRFB as it offers higher electrocatalytic activity, lower pressure drop, better performance, and lower cost. The study is also extended to a multilayer configuration of Carbon Paper and Carbon Cloth. The performance of multi-layered electrodes by stacking single sheets of Carbon Paper and Carbon Cloth electrodes are matched to meet the performance obtained with the Graphite felt electrode. It has been shown with the help of polarization curve and the pressure drop study that the performance of five layers of carbon cloth and nine layers of carbon paper match the performance of Graphite felt, approximately. The present study provides practical guidance for the design and optimization of VRFB electrodes.

Simultaneous analysis of chloramphenicol, amoxicillin, and enrofloxacin using electrochemical sensors with multilayer graphene electrodes fabricated by electrochemical methods in an organic solvent

In this study, three antibiotics, chloramphenicol (CAP), amoxicillin (AMX), and enrofloxacin (ENR), were simultaneously analysed for the first time using electrochemical sensors. The multilayer graphene electrode used in the sensor was directly and rapidly fabricated from graphite through a one-step chronoamperometry method. Scanning electron microscopy and cyclic voltammetry techniques revealed the multilayer-graphene nanostructure of the prepared electrode with a large electrochemically active surface area and good electrochemical activity. The electrode exhibited the best electrochemical oxidation signals corresponding to the three antibiotics when fabricated at a potential of 5 V for 20 s. Under optimised conditions, the sensor demonstrated excellent multi-analyte analysis capability, with clear separation and good linearity of the signals of the three antibiotics (R2>0.99) in relation to their concentrations. The sensor exhibited high accuracy and sensitivity with detection limits of 0.060, 0.381, and 0.109 μM for CAP, AMX, and ENR, respectively. The applicability of the sensor was demonstrated through acceptable recoveries of all three antibiotics when simultaneously analysed in a lake water sample.

ZnO/Ag/ZnO multilayers as an n-type transparent conducting electrode for transparent organic light-emitting diodes

Alternative transparent conducting electrodes (TCEs) have gained significant attention in recent decades in an effort to replace costly indium-tin oxide (ITO) in organic optoelectronic devices. For example, state-of-the-art top-emitting and transparent organic light-emitting diodes (OLEDs) in the display industry require a transparent or semitransparent cathode for electron injection. Current OLED display technology employs ultrathin metallic (typically Mg:Ag) layers as semitransparent cathodes. However, recent studies have shown that metal oxide/metal/metal oxide multilayers can perform better optically and offer improved stability compared to semitransparent metal cathodes. Deposition of these multilayers with minimal damage to the underlying organic emissive layer is imperative. Here, we investigate a ZnO/Ag/ZnO TCE multilayer TCE deposited under mild sputtering conditions that are safe for the emissive layer. We demonstrate ∼ 85 % transparent electrodes with a sheet resistance of 1.47 Ω/sq, which is more conductive than the industry standard, ITO. We also integrate the multilayer TCE as the cathode in a transparent OLED device built on ITO, demonstrating the compatibility of this TCE with the existing OLED technology.

The analytical model of time-harmonic electric field and impedance spectrum in the multilayered interdigital electrode structure

Accurately determining the time-harmonic electric field and impedance spectrum in the multilayered interdigital electrode (IDE) transducers with lossy dielectrics is essential for the design of the structure, the property estimation of the dielectric, and performance optimization. This paper presents an analytical model of the electric field and impedance within a multilayered interdigitated electrode (IDE) when subjected to alternating excitation through the method of separation of variables (MSV). The equivalent circuit of IDE is established, where the impedance is the parallel of capacitive coupling and resistive coupling between electrodes. The general solutions for the electric field and impedance involving arbitrary numbers and complex permittivities of the dielectric layers are analytically derived. However, due to the approximation of boundary conditions, these physical quantities cannot be accurately obtained by the conventional analytical method using conformal mapping technique (CMT) and partial capacitance technique (PCT). The proposed model exhibits proficiency in generating precise electric field images and impedance values that closely correspond with simulated data, even when accounting for the frequency-dependent characteristics of permittivity and conductivity in lossy dielectrics. Moreover, the approaches to improve the sensitivity of a traditional three-layered IDE-based sensor are demonstrated. For a three-layered IDE-based capacitive sensor, improving the sensitivity can be accomplished through the incorporation of a ground plane at the substrate's bottom and increasing the metallization rate. Conversely, it is recommended to reduce the metallization rate, increase substrate thickness, and remove the ground plane in order to enhance the sensitivity of the IDE-based impedance sensor. The experimental results demonstrate that the proposed model generates outstanding impedance spectra (involving capacitance spectra and resistance spectra) results for various metallization ratios and top layers. This exemplifies the model's potential for predicting, designing, and enhancing a complex multilayered IDE-based transducer to achieve precise and sensitive detection.

Tailored multi-layer graphene arrays for precision detection of neurotransmitter

The development of sensitive dopamine (DA) sensors has significantly contributed to our understanding of DA-related disorders and has enabled advancements in medical diagnostics and neuroscience research. Therefore, in the present work, a novel electrochemical sensing platform was developed using multi-layer graphene arrays (MGA) modified electrodes for the selective detection of DA. The preparation of high-quality MGA was achieved using the plasma-enhanced chemical vapor deposition (PCVD) method and was confirmed using various physiochemical techniques such as transmission electron microscopy and Raman spectroscopy. The modified electrode, made of MGA, was utilized for the electrochemical detection of DA using cyclic voltammetry and amperometry i-t methods. DA’s electrochemical oxidation response and sensitivity at the MGA electrode were ≈9 and 3 times higher than observed with unmodified and commercially available multi-layer graphene-modified electrodes. The MGA sensor exhibited excellent analytical parameters for DA detection, including a wide linear range of up to 172.1 μM and a low detection limit of 1.3 nM. The sensor also demonstrated remarkable sensitivity, storage stability, and selectivity for DA detection, making it highly suitable for accurately detecting DA in medical diagnostics and neuroscience research. Furthermore, the practical application of the MGA sensor for DA detection was demonstrated in various real samples.

Fabrication and characterization of a novel multilayer heterojunction Si3N4-PbO2 nanocomposite electrode and its application on electrocatalysis degradation of sulfathiazole

To lengthen the lifetime and extend the potential commercial applications of lead dioxide electrode, herein, a novel multilayer heterojunction Ti/ SnO2-Sb2O3/ graphene oxide/ carbon nanotube/ Si3N4-PbO2 electrode (Si3N4-PbO2 electrode) was fabricated by co-electrodeposition process that doping Si3N4 nanoparticles in eletroplating solution. Various spectroscopic and microscopic techniques, including scanning electron microscopy (SEM) equipped with energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), were employed to characterize the surface of the fabricated electrode. The EDS analysis confirmed the successful attachment of 5.49 %wt Si and 2.46 %wt N elements from Si3N4 nanoparticles onto the PbO2 surface, while the XRD results indicated a shift in the preferred orientation of PbO2 grains from β(110) to β(101). The water adsorption energy and ·OH desorption energy in the electrocatalysis process were determined to be 0.71 eV and 0.241 eV through theoretical calculating. Subsequently, the Si3N4-PbO2 electrode was employed as an anode for the electrocatalytic degradation of sulfathiazole-simulated wastewater and real sulfonamides wastewater. Under optimized conditions determined via response surface methodology (RSM), the COD degradation efficiency reached 69.37 % for sulfathiazole and 62.35 % for real sulfonamides wastewater. The final COD concentration of the real sulfonamides wastewater was reduced to 77.05 mg/L, under the national urban sewage discharge standard. Finally, the degradation mechanism and pathway of sulfathiazole has been arranged based on the electron spin resonance (ESR), cyclic voltammetry (CV), while the intermediates were detected by Gas Chromatography-Mass Spectrometer (GC-MS) and the reactive sites of sulfathiazole were predicted by using Fukui function.

All‐Printed Electrically Driven Lighting via Electrochemiluminescence

AbstractElectrochemiluminescence (ECL) has attracted significant attention as a promising light‐emitting technology owing to its simple configuration and solution processability. ECL has wide applications in biological and chemical sensors, lighting, and displays. ECL lighting devices are fabricated as sandwiched structures with a transparent electrode on top, which limits their widespread adoption. Intricate structures with high precision and customizable designs can be directly fabricated using 3D printing. However, 3D printing of ECL devices is challenging because of poor printability and structural integrity of ECL luminophore inks. Here, all‐printed electrically driven lighting is demonstrated using the direct ink writing method. The ECL reactive layer and electrodes are directly printed using a side‐by‐side electrode configuration. A 3D printable ECL ink is developed by incorporating silica nanoparticles as rheological modifiers to realize well‐defined patterns with high structural integrity. Graphene is introduced on Ag multilayer electrodes to embrace both the electrical conductivity and electrochemical stability for efficient ECL operation. This all‐printing approach allows the fabrication of ECL devices with complex designs, such as combs and spirals. Moreover, it facilitates seamless printing on various substrate materials, making this technology an asset in the fields of biology, chemistry, and electronics.

A new ER valve composed of multilayer mesh electrodes

In many cases, ER valves are required to be used at lower operating voltages. For example, to develop a two-dimensional Braille matrix display, it is necessary to lay out many ER valves and control each Braille dot independently. If the commonly used parallel plate electrodes are applied, a low voltage can only be used when the electrode gap is very small, which will make the ER valve flow resistance very large, thus making it difficult to achieve effective control. A new type of ER valve composed of multilayer mesh electrodes was designed, which are arranged vertically in the direction of ER fluid flow. The flow rate of the ER valve is determined by the opening ratio of the mesh electrodes. This type of mesh electrode results in a more complex electric field distribution, which has a different action pattern on ER fluid yield stress compared to parallel electrodes. The non-uniform electric field generated by mesh electrodes under different operating voltages was simulated using COMSOL software, and the pressure drops of ER valves with various sizes of mesh electrodes under different voltages were experimentally investigated. The results indicate that the longitudinal electric field component plays a dominant role, and the stress of the ER fluid exhibits a periodic and gradient distribution. This valve exhibits good ER performance when the applied voltage is much lower than that of parallel electrodes. At the same time, the flow rate of the ER valve can be increased by enlarging the opening ratio of the mesh electrodes. Even if the applied voltage is 180 V, the pressure drop of the ER valve is large enough and the operation stability is good. This new type of ER valve makes the device small in size, easy to control intelligently and low cost. Multilayer mesh electrodes also have universal application value in ER technology.

Three-dimensional multi-layer carbon tube electrodes for AC line-filtering capacitors

Three-dimensional multi-layer carbon tube electrodes for AC line-filtering capacitors

Advanced multilayer model electrode for binder distribution within composite electrodes of lithium batteries

The loading levels of composite electrodes are increasing continuously to satisfy the energy density requirements of lithium-ion batteries (LIBs) in electric vehicles (EVs). Furthermore, a faster coating and drying process in the mass-production line yields a nonuniform binder distribution. Thus, it is necessary to understand its distribution within the composite electrode and control it for a better and more reliable electrochemical performance. Therefore, we propose the utilization of an advanced multilayer electrode model consisting of several electrode layers with different binder contents. Using these controlled electrode models, the adhesive strength within each layer was examined using a surface and interfacial cutting analysis system (SAICAS). This was followed by a composition analysis using EDX on each surface. Subsequently, the electronic conductivities of the model electrodes were measured using an electrode resistance meter to determine the bulk and interfacial electrode resistances. Furthermore, the electrochemical properties of each model electrode were evaluated to correlate their relationships and design the optimum binder distribution. Thus, this multilayer model provides a highly effective platform for determining the optimum binder distribution in highly loaded composite electrodes for high-energy–density and long-lasting LIBs.

Physically and Chemically Stable Molybdenum-Based Composite Electrodes for p-i-n Perovskite Solar Cells.

Metal halide perovskite solar cells (PSCs) have garnered much attention in recent years. Despite the remarkable advancements in PSCs utilizing traditional metal electrodes, challenges such as stability concerns and elevated costs have necessitated the exploration of innovative electrode designs to facilitate industrial commercialization. Herein, a physically and chemically stable molybdenum (Mo) electrode is developed to fundamentally tackle the instability factors introduced by electrodes. The combined spatially resolved element analyses and theoretical study demonstrate the high diffusion barrier of Mo ions within the device. Structural and morphology characterization also reveals the negligible plastic deformation and halide-metal reaction during aging when Mo is in contact with perovskite (PVSK). The electrode/underlayer junction is further stabilized by a thin seed layer of titanium (Ti) to improve Mo film's uniformity and adhesion. Based on a corresponding p-i-n PSCs (ITO/PTAA/PVSK/C60/SnO2/ITO/Ti/Mo), the champion sample could deliver an efficiency of 22.25%, which is among the highest value for PSCs based on Mo electrodes. Meanwhile, the device shows negligible performance decay after 2000 h operation, and retains 91% of the initial value after 1300 h at 50-60 °C. In summary, the multilayer Mo electrode opens an effective avenue to all-round stable electrode design in high-performance PSCs.