Advanced 3D ordered electrodes for PEMFC applications: From structural features and fabrication methods to the controllable design of catalyst layers

The catalyst layers(CLs) electrode is the key component of the membrane electrode assembly(MEA) in proton exchange membrane fuel cells(PEMFCs). Conventional electrodes for PEMFCs are composed of carbon-supported, ionomer, and Pt nanoparticles, all immersed together and sprayed with a micron-level thickness of CLs. They have a performance trade-off where increasing the Pt loading leads to higher performance of abundant triple-phase boundary areas but increases the electrode cost. Major challenges must be overcome before realizing its wide commercialization. Literature research revealed that it is impossible to achieve performance and durability targets with only high-performance catalysts, so the controllable design of CLs architecture in MEAs for PEMFCs must now be the top priority to meet industry goals. From this perspective, a 3D ordered electrode circumvents this issue with a support-free architecture and ultrathin thickness while reducing noble metal Pt loadings. Herein, we discuss the motivation in-depth and summarize the necessary CLs structural features for designing ultralow Pt loading electrodes. Critical issues that remain in progress for 3D ordered CLs must be studied and characterized. Furthermore, approaches for 3D ordered CLs architecture electrode development, involving material design, structure optimization, preparation technology, and characterization techniques, are summarized and are expected to be next-generation CLs for PEMFCs. Finally, the review concludes with perspectives on possible research directions of CL architecture to address the significant challenges in the future.

Electrode-compatible fluorine-free multifunctional additive regulating solid electrolyte interphase and solvation structure for high-performance lithium-ion batteries

The rapid development and widespread application of lithium-ion batteries(LIBs) have increased demand for high-safety and high-performance LIBs. Accordingly, various additives have been used in commercial liquid electrolytes to severally adjust the solvation structure of lithium ions, control the components of solid electrolyte interphase, or reduce flammability. While it is highly desirable to develop low-cost multifunctional electrolyte additives integrally that address both safety and performance on LIBs, significant challenges remain. Herein, a novel phosphorus-containing organic small molecule, bis(2-methoxyethyl) methylphosphonate(BMOP), was rationally designed to serve as a fluorine-free and multifunctional additive in commercial electrolytes. This novel electrolyte additive is low-toxicity,high-efficiency, low-cost, and electrode-compatible, which shows the significant improvement to both electrochemical performance and fire safety for LIBs through regulating the electrolyte solvation structure, constructing the stable electrode-electrolyte interphase, and suppressing the electrolyte combustion. This work provides a new avenue for developing safer and high-performance LIBs.

Smart epidermal electrophysiological electrodes:Materials,structures,and algorithms

Epidermal electrophysiological monitoring has garnered significant attention for its potential in medical diagnosis and healthcare,particularly in continuous signal recording.However,simultaneously satisfying skin compliance,mechanical properties,environmental adaptation,and biocompatibility to avoid signal attenuation and motion artifacts is challenging,and accurate physiological feature extraction necessitates effective signal-processing algorithms.This review presents the latest advancements in smart electrodes for epidermal electrophysiological monitoring,focusing on materials,structures,and algorithms.First,smart materials incorporating self-adhesion,self-healing,and self-sensing functions offer promising solutions for long-term monitoring.Second,smart meso-structures,together with micro/nanostructures endowed the electrodes with self-adaption and multifunctionality.Third,intelligent algorithms give smart electrodes a“soul,”facilitating faster and more-accurate identification of required information via automatic processing of collected electrical signals.Finally,the existing challenges and future opportunities for developing smart electrodes are discussed.Recognized as a crucial direction for next-generation epidermal electrodes,intelligence holds the potential for extensive,effective,and transformative applications in the future.

Structures and electrochemical hydrogen storage performance of Si added A_2B_7-type alloy electrodes

In order to ameliorate the electrochemical hydrogen storage performance of La-Mg-Ni system A2B7-type electrode alloys, a small amount of Si was added. The La0.8Mg0.2Ni3.3Co0.2Six （x=0-0.2） electrode alloys were prepared by casting and annealing. The effects of adding Si on the structure and electrochemical hydrogen storage characteristics of the alloys were investigated systematically. The results indicate that the as-cast and annealed alloys hold multiple structures, involving two major phases of （La, Mg）2Ni7 with a Ce2Ni7-type hexagonal structure and LaNi5 with a CaCu5-type hexagonal structure as well as one residual phase LaNi3. The addition of Si results in a decrease in （La, Mg）2Ni7 phase and an increase in LaNi5 phase without changing the phase structure of the alloys. What is more, it brings on an obvious effect on electrochemical hydrogen storage characteristics of the alloys. The discharge capacities of the as-cast and annealed alloys decline with the increase of Si content, but their cycle stabilities clearly grow under the same condition. Furthermore, the measurements of the high rate discharge ability, the limiting current density, hydrogen diffusion coefficient as well as electrochemical impedance spectra all indicate that the electrochemical kinetic properties of the electrode alloys first increase and then decrease with the rising of Si content.

Flexible,high-density,laminated ECoG electrode array for high spatiotemporal resolution foci diagnostic localization of refractory epilepsy

High spatiotemporal resolution brain electrical signals are critical for basic neuroscience research and high-precision focus diagnostic localization,as the spatial scale of some pathologic signals is at the submillimeter or micrometer level.This entails connecting hundreds or thousands of electrode wires on a limited surface.This study reported a class of flexible,ultrathin,highdensity electrocorticogram(ECoG)electrode arrays.The challenge of a large number of wiring arrangements was overcome by a laminated structure design and processing technology improvement.The flexible,ultrathin,high-density ECoG electrode array was conformably attached to the cortex for reliable,high spatial resolution electrophysiologic recordings.The minimum spacing between electrodes was 15μm,comparable to the diameter of a single neuron.Eight hundred electrodes were prepared with an electrode density of 4444 mm^(-2).In focal epilepsy surgery,the flexible,high-density,laminated ECoG electrode array with 36 electrodes was applied to collect epileptic spike waves inrabbits,improving the positioning accuracy of epilepsy lesions from the centimeter to the submillimeter level.The flexible,high-density,laminated ECoG electrode array has potential clinical applications in intractable epilepsy and other neurologic diseases requiring high-precision electroencephalogram acquisition.

Micro-nano structural electrode architecture for high power energy storage

The necessity and superiorities of micro-nano structural electrodes toward high power:Electrochemical energy storage(EES)technologies have achieved great success in portable electronics and electric vehicles owing to their environmental friendliness and cost effectiveness.With the promotional concepts such as the Internet of Things and ultra-high efficiency self-powered systems in recent years,there are substantial demand for superior EES systems,including but not limited to high-performance,miniaturization and multifunction[1−4].In a particular EES cell,active materials are carried by electrodes as the basic building blocks of energy storage or release.Material innovation(includes composition,structure,size and morphology)has revealed remarkable energy density,power density and lifespan for associated devices in the lab setting of low mass loading slurry-coating electrodes[5].

A micromechanical model for efective conductivity in granular electrode structures

Optimization of composition and microstructure is important to enhance performance of solid oxide fuel cells （SOFC） and lithium-ion batteries （LIB）. For this, the porous electrode structures of both SOFC and LIB are modeled as a binary mixture of electronic and ionic conducting particles to estimate effective transport properties. Particle packings of 10000 spherical, binary sized and randomly positioned particles are created numerically and densified considering the different manufacturing processes in SOFC and LIB： the sintering of SOFC electrodes is approximated geometrically, whereas the calendering process and volume change due to intercalation in LIB are modeled physically by a discrete el- ement approach. A combination of a tracking algorithm and a resistor network approach is developed to predict the con- nectivity and effective conductivity for the various densified structures. For SOFC, a systematic study of the influence of morphology on connectivity and conductivity is performed on a large number of assemblies with different compositions and particle size ratios between 1 and 10. In comparison to percolation theory, an enlarged percolation area is found, es- pecially for large size ratios. It is shown that in contrast to former studies the percolation threshold correlates to varying coordination numbers. The effective conductivity shows not only an increase with volume fraction as expected but also with size ratio. For LIB, a general increase of conductivity during the intercalation process was observed in correlation with increasing contact forces. The positive influence of cal- endering on the percolation threshold and the effective conductivity of carbon black is shown. The anisotropy caused by the calendering process does not influence the carbon black phase.

Preparation optimization of multilayer-structured SnO_2–Sb–Ce/Ti electrode for efficient electrocatalytic oxidation of tetracycline in water

In this study, electrodeposition and thermal decomposition were alternatively used for the fabrication of a series of novel multilayer-structured SnO_2–Sb–Ce/Ti(SSCT) electrodes, and their physiochemical and electrochemical properties were investigated for electrochemical oxidation of tetracycline(TC) in aqueous medium.Experimentally, after the SnO_2–Sb–Ce(SSC) composite was electrodeposited for 120 s on the titanium substrate in aqueous solution, the outer thermal coatings composed of SSC were synthesized by a hydrothermal method.Both influences of electrodeposition time(T_(ed)) and thermal decomposition time(Ttd) were investigated to obtain the optimum preparation. It was found that when increasing T_(ed)to a certain extent a longer lifetime of electrode can be achieved, which was attributed to a more solid interlayer structure. A notable SSCTT_(ed),Ttdelectrode,i.e., SSCT3,10, which was prepared through three times of 120 s' electrodeposition(T_(ed)= 3) and ten times of thermal decomposition(Ttd= 10) obtained the highest oxygen evolution potential 3.141 V vs. SCE. In this selected electrode, when 10 mg·L^(-1) initial TC concentration was added to this wastewater, the highest color removal efficiency and mineralization rate of TC were 72.4% and 41.6%, respectively, with an applied electricity density of 20 m A·cm^(-2) and treatment time of 1 h. These results presented here demonstrate that the combined application of electrodeposition and thermal decomposition is effective in realization of enhanced electrocatalytic oxidation activity.

Structure and electrochemical hydrogen storage characteristics of La_(0.8-x)Pr_xMg_(0.2)Ni_(3.15)Co_(0.2)Al_(0.1)Si_(0.05) (x=0-0.4) electrode alloys

For the purpose of improving the electrochemical cycle stability of the La-Mg-Ni based A2BT-type electrode alloys, both reducing Mg content and substituting La with Pr were adopted. The Lao.8-xPrxMg0.2Ni3.15Co0.2A10.1Si0.05 （x=0, 0.1, 0.2, 0.3, 0.4） electrode alloys were fabricated by casting and annealing. The investigation on the structures and electrochemical performances of the alloys was performed. The obtained results reveal that the as-cast and annealed alloys comprise two major phases, （La, Mg）2Ni7 phase with the hexagonal Ce2NiT-type structure and LaNi5 phase with the hexagonal CaCus-type structure, as well as a little residual LaNi3 phase. It is also found that the addition of Pr element observably affects the electrochemical hydrogen storage characteristics of the alloys, just as the discharge capacity and high rate discharge ability （HRD） first rise then fall with the growing of Pr content, and among all the alloys, the as-cast and annealed （x=0.3） alloys generate the largest discharge capacities of 360.8 and 386.5 mA.h/g, respectively. Additionally, the electrochemical cycle stability of all the alloys markedly grows with the increase of Pr content. The capacity retaining rate （S100） at the 100th charging and discharging cycle is enhanced from 64.98% to 77.55% for the as-cast alloy, and from 76.60% to 95.72% for the as-annealed alloy by rising Pr content from 0 to 0.4. Furthermore, the substitution of Pr for La results in first increase and then decrease in the hydrogen diffusion coefficient （D）, the limiting current density （IL） as well as the electrochemical impedance.

Efficient direction-independent fog harvesting using a corona discharge device with a multi-electrode structure

Efflcient collection of water from fog can effectively alleviate the problem of water shortages in foggy but water-scarce areas,such as deserts,islands and so on.Unlike inefflcient fog meshes,corona discharge can charge water droplets and further enhance the water-collecting effect.This study proposes a novel multi-electrode collecting structure that can achieve efflcient and direction-independent water collection from fog.The multi-electrode structure consists of three parts:a charging electrode,an intercepting electrode and a ground electrode.Four types of watercollecting structures are compared experimentally,and the collection rates from a traditional fog mesh,a wire-mesh electrode with fog coming from a high-voltage electrode,a wire-mesh electrode with fog coming from a ground electrode and a multi-electrode structure are 2–3 g h^(-1),100–120 g h^(-1),60–80 g h^(-1)and 200–220 g h^(-1),respectively.The collection rate of the multielectrode structure is 100–150 times that of a traditional fog mesh and 2–4 times that of a wiremesh electrode.These results demonstrate the superiority of the multi-electrode structure in fog collection.In addition,the motion equation of charged droplets in an electric fleld is also derived,and the optimization strategy of electrode spacing is also discussed.This structure can be applied not only to fog collection,but also to air puriflcation,factory waste gas treatment and other flelds.

Hierarchical platinum–iridium neural electrodes structured by femtosecond laser for superwicking interface and superior charge storage capacity

The interfacial performance of implanted neural electrodes is crucial for stimulation safety and the recording quality of neuronal activity.This paper proposes a novel surface architecture and optimization strategy for the platinum–iridium(Pt–Ir)electrode to optimize electrochemical performance and wettability.A series of surface micro/nano structures were fabricated on Pt–Ir electrodes with different combinations of four adjustable laser-processing parameters.Subsequently,the electrodes were characterized by scanning electron microscopy,energy-dispersive X-ray spectroscopy,cyclic voltammetry,electrochemical impedance spectroscopy,and wetting behavior.The results show that electrode performance strongly depends on the surface morphology.Increasing scanning overlap along with moderate pulse energy and the right number of pulses leads to enriched surface micro/nano structures and improved electrode performance.It raises the maximum charge storage capacity to 128.2 mC/cm^(2) and the interface capacitance of electrodes to 3.0×10^(4)μF/cm^(2) for the geometric area,compared with 4.6 mC/cm^(2) and 443.1μF/cm2,respectively,for the smooth Pt–Ir electrode.The corresponding optimal results for the optically measured area are 111.8 mC/cm^(2) and 2.6×10^(4)μF/cm^(2),which indicate the contribution of fner structures to the ablation profle.The hierarchical structures formed by the femtosecond laser dramatically enhanced the wettability of the electrode interface,giving it superwicking properties.A wicking speed of approximately 80 mm/s was reached.Our optimization strategy,leading to superior performance of the superwicking Pt–Ir interface,is promising for use in new neural electrodes.

Effects of rapid quenching on structure and electrochemical characteristics of La_(0.5)Ce_(0.2)Mg_(0.3)Co_(0.4)Ni_(2.6-x)Mn_x(x=0-0.4) electrode alloys

The La-Mg-Ni system PuNi3-type La0.5Ce0.2Mg0.3Co0.4Ni2.6-xMnx(x=0,0.1,0.2,0.3,0.4) hydrogen storage alloys were prepared by casting and rapid quenching. The effects of the rapid quenching on the structure and electrochemical characteristics of the alloys were studied. The results obtained by XRD,SEM and TEM indicate that the as-cast and quenched alloys mainly consist of two major phases,(La,Mg)Ni3 and LaNi5,as well as a residual phase LaNi. The rapid quenching does not exert an obvious influence on the phase composition of the alloys,but it leads to an increase of the LaNi5 phase and a decrease of the(La,Mg)Ni3 phase. The as-quenched alloys have a nano-crystalline structure,and the grain sizes of the alloys are in the range of 20-30 nm. The results by the electrochemical measurements indicate that both the discharge capacity and the high rate discharge(HRD) ability of the alloy first increase and then decrease with the variety of quenching rate and obtain the maximum values at the special quenching rate which is changeable with the variety of Mn content. The rapid quenching significantly improves the cycle stabilities of the alloys,but it slightly impairs the activation capabilities of the alloys.

Efficient Terahertz Photoconductive Emitters with Improved Electrode Structures

We present the design, fabrication, and characterization of two new types of terahertz photoconductive emitters. One has an asymmetric four-contact electrode structure and the other has an arc-shaped electrode structure, which are all modified from a traditional strip line antenna. Numerical simulations and real experiments confirm the good performance of the proposed antennas. An amplitude increase of about 40% is experimentally observed for the terahertz signals generated from the new structures. The special electrode structure and its induced local bias field enhancement are responsible for this radiation efficiency improvement. Our work demonstrates the feasibility of developing highly efficient terahertz photoconductive emitters by optimizing the electrode structure.

A Self-Aligned Process to Fabricate a Metal Electrode-Quantum Dot/Nanowire-Metal Electrode Structure with 100% Yield

Using lateral phase change random access memory(PCRAM)for demonstration,we report a self-aligned process to fabricate a metal electrode-quantum dot(QD)/nanowire(NW)-metal electrode structure.Due to the good confinement and coupling between the Ge_(2)Sb_(2)Te_(5)(GST)QD and the tungsten electrodes,the device shows a threshold current and voltage as small as 2.50μA and 1.08 V,respectively.Our process is highlighted with good controllability and repeatability with 100%yield,making it a promising fabrication process for nanoelectronics.

Surface structure and catalytic activity of electrodeposited Ni-Fe-Co-Mo alloy electrode by partially leaching Mo and Fe

Ni-Fe-Mo-Co alloy electrode was prepared in a citrate solution by electrodeposition, and then Mo and Fe were partially leached out from the electrode in 30% KOH solution. The unique surface micromorphology of a hive-like structure was obtained with an average pore size of about 50 nm. The electrode has a very large real surface area and a stable structure. The effects of sodium molybdate concentration on the composition, surface morphology, and structure of electrodes were analyzed by EDS, SEM and XRD. The polarization curves of the different electrodes show that the catalytic activity of electrodes is strongly correlated with the mole fraction of alloy elements (Ni, Fe, Mo, Co), and the addition of cobalt element to Ni-Fe-Mo alloy improves the catalytic activity. The Ni35.63Fe24.67Mo23.52Co16.18 electrode has the best activity for hydrogen evolution reaction(HER), with an over-potential of 66.2 mV, in 30% KOH at 80 ℃ and 200 mA/cm2. The alloy maintains its good catalytic activity for HER during continuous or intermittent electrolysis. Its electrochemical activity and catalytic stability are much higher than the other iron-group with Mo alloy electrodes.

A STUDY OF STRUCTURE TRANSITION OF CHLORIDE LAYER ADSORBED ON Ag(100) ELECTRODES

The behavior of chloride adsorbed on Ag(100) electrode has been studied using chronoamperometric technique, and the structural transition of chloride layer has been confirmed.

EFFECT OF STRUCTURE OF FUNCTIONAL POLYMER ACTIVE MATERIALS ON PROPERTIES OF GADOLINIUM ION SELECTIVE ELECTRODE

In this paper,the functional polymeric active materials were prepared by the grafting copolymerization and their structure and properties were studied.The results show that the structure and properties of these ac- tive materials have the relative large effects on the properties of gadolinium ion selective electrodes.

Triboelectric nanogenerator based on electrodeposited Ag octahedral nano-assemblies

The tremendous potential of triboelectric generators-TENGs for converting mechanical energy into electrical energy places them as one of the most promising energy harvesting technologies. In this work, the fabrication of enhanced performance TENGs using Ag octahedron nano-assemblies on ITO as electrodes significantly increases the electric charge collection of the induced tribocharges. Thereby, nanostructured electrical contacts coated with Ag macroscale nano-assemblies with octahedral features were obtained by the electrodeposition technique on flexible PET/ITO substrates. Consequently, the nanostructured triboelectric generator-TENG exhibited 65 times more maximum output power, and almost 10 times more open circuit output voltage than that of a TENG with non-nanostructured contacts passing from μW to m W capabilities, which was attributed to the increment of intrinsic interface states due to a higher effective contact area in the former. Likewise, output performances of TENGs also displayed an asymptotic behavior on the output voltage as the operating frequency of the mechanical oscillations increased, which is attributed to a decrement in the internal impedance of the device with frequency. Furthermore, it is shown that the resulting electrical output power can successfully drive low power consumption electronic devices. On that account, the present research establishes a promising platform which contributes in an original way to the development of the TENGs technology.

Compared discharge characteristics and film modifications of atmospheric pressure plasma jets with two different electrode geometries

Atmospheric pressure plasma jet shows great potential for polymer film processing. The electrode geometry is the key factor to determine discharge characteristics and film modification of jets. In this paper, we compared the discharge characteristics and the film modifications of atmospheric pressure plasma jets with needle-ring electrode(NRE) and doublering electrode(DRE). The results show that jet with NRE has stronger electric field intensity and higher discharge power,making it present more reactive oxygen particles and higher electron temperature, but its discharge stability is insufficient.In contrast, the jet with DRE has uniform electric field distribution of lower field intensity, which allows it to maintain stable discharge over a wide range of applied voltages. Besides, the modification results show that the treatment efficiency of PET film by NRE is higher than that by DRE. These results provide a suitable atmospheric pressure plasma jets device selection scheme for polymer film processing process.

Micro/nano-wrinkled elastomeric electrodes enabling high energy storage performance and various form factors

Stretchable elastomer-based electrodes are considered promising energy storage electrodes for next-generation wearable/flexible electronics requiring various shape designs.However,these elastomeric electrodes suffer from the limited electrical conductivity of current collectors,low charge storage capacities,poor interfacial interactions between elastomers and conductive/active materials,and lack of shape controllability.In this study,we report hierarchically micro/nano-wrinkle-structured elastomeric electrodes with notably high energy storage performance and good mechanical/electrochemical stabilities,simultaneously allowing various form factors.For this study,a swelling/deswelling-involved metal nanoparticle(NP)assembly is first performed on thiol-functionalized polydimethylsiloxane(PDMS)elastomers,generating a micro-wrinkled structure and a conductive seed layer for subsequent electrodeposition.After the assembly of metal NPs,the conformal electrodeposition of Ni and NiCo layered double hydroxides layers with a homogeneous nanostructure on the micro-wrinkled PDMS induces the formation of a micro/nano-wrinkled surface morphology with a large active surface area and high electrical conductivity.Based on this unique approach,the formed elastomeric electrodes show higher areal capacity and superior rate capability than conventional elastomeric electrodes while maintaining their electrical/electrochemical properties under external mechanical deformation.This notable mechanical/electrochemical performance can be further enhanced by using spiral-structured PDMS(stretchability of~500%)and porous-structured PDMS(areal capacity of~280μAh cm^(-2)).