Flexible capacitive pressure sensor based on interdigital electrodes with porous microneedle arrays for physiological signal monitoring

Flexible pressure sensors have many potential applications in the monitoring of physiological signals because of their good biocompatibil-ity and wearability.However,their relatively low sensitivity,linearity,and stability have hindered their large-scale commercial application.Herein,aflexible capacitive pressure sensor based on an interdigital electrode structure with two porous microneedle arrays(MNAs)is pro-posed.The porous substrate that constitutes the MNA is a mixed product of polydimethylsiloxane and NaHCO3.Due to its porous and interdigital structure,the maximum sensitivity(0.07 kPa-1)of a porous MNA-based pressure sensor was found to be seven times higher than that of an imporous MNA pressure sensor,and it was much greater than that of aflat pressure sensor without a porous MNA structure.Finite-element analysis showed that the interdigital MNA structure can greatly increase the strain and improve the sensitivity of the sen-sor.In addition,the porous MNA-based pressure sensor was found to have good stability over 1500 loading cycles as a result of its bilayer parylene-enhanced conductive electrode structure.Most importantly,it was found that the sensor could accurately monitor the motion of afinger,wrist joint,arm,face,abdomen,eye,and Adam’s apple.Furthermore,preliminary semantic recognition was achieved by monitoring the movement of the Adam’s apple.Finally,multiple pressure sensors were integrated into a 33 array to detect a spatial pressure distribu-×tion.Compared to the sensors reported in previous works,the interdigital electrode structure presented in this work improves sensitivity and stability by modifying the electrode layer rather than the dielectric layer.

Capacitive energy storage from single pore to porous electrode identified by frequency response analysis

Rate capability,peak power,and energy density are of vital importance for the capacitive energy storage(CES)of electrochemical energy devices.The frequency response analysis(FRA)is regarded as an efficient tool in studying the CES.In the present work,a bi-scale impedance transmission line model(TLM)is firstly developed for a single pore to a porous electrode.Not only the TLM of the single pore is reparameterized but also the particle packing compactness is defined in the bi-scale.Subsequently,the CES properties are identified by FRA,focused on rate capability vs.characteristic frequency,peak power vs.equivalent series resistance,and energy density vs.low frequency limiting capacitance for a single pore to a porous electrode.Based on these relationships,the CES properties are numerically simulated and theoretically predicted for a single pore to a porous electrode in terms of intra-particle pore length,intra-particle pore diameter,inter-particle pore diameter,electrolyte conductivity,interfacial capacitance&exponent factor,electrode thickness,electrode apparent surface area,and particle packing compactness.Finally,the experimental diagnosis of four supercapacitors(SCs)with different electrode thicknesses is conducted for validating the bi-scale TLM and gaining an insight into the CES properties for a porous electrode to a single pore.The calculating results suggest,to some extent,the inter-particle pore plays a more critical role than the intra-particle pore in the CES properties such as the rate capability and the peak power density for a single pore to a porous electrode.Hence,in order to design a better porous electrode,more attention should be given to the inter-particle pore.

Multiscale modeling of electrolytes in porous electrode:From equilibrium structure to non-equilibrium transport

Understanding the mechanisms and properties of various transport processes in the electrolyte,porous electrode,and at the interface between electrode and electrolyte plays a crucial role in guiding the improvement of electrolytes,materials and microstructures of electrode.Nanoscale equilibrium properties and nonequilibrium ion transport are substantially different to that in the bulk,which are difficult to observe from experiments directly.In this paper,we introduce equilibrium and no-equilibrium thermodynamics for electrolyte in porous electrodes or electrolyte-electrode interface.The equilibrium properties of electrical double layer(EDL)including the EDL structure and capacitance are discussed.In addition,classical non-equilibrium thermodynamic theory is introduced to help us understand the coupling effect of different transport processes.We also review the recent studies of nonequilibrium ion transport in porous electrode by molecular and continuum methods,among these methods,dynamic density functional theory(DDFT)shows tremendous potential as its high efficiency and high accuracy.Moreover,some opportunities for future development and application of the non-equilibrium thermodynamics in electrochemical system are prospected.

Functional porous carbon-based composite electrode materials for lithium secondary batteries

The synthetic routes of porous carbons and the applications of the functional porous carbon-based composite electrode materials for lithium secondary batteries are reviewed. The synthetic methods have made great breakthroughs to control the pore size and volume, wall thickness, surface area, and connectivity of porous carbons, which result in the development of functional porous carbon-based composite electrode materials. The effects of porous carbons on the electrochemical properties are further discussed. The porous carbons as ideal matrixes to incorporate active materials make a great improvement on the electrochemical properties because of high surface area and pore volume, excellent electronic conductivity, and strong adsorption capacity. Large numbers of the composite electrode materials have been used for the devices of electrochemical energy conversion and storage, such as lithium-ion batteries （LIBs）, Li-S batteries, and Li-O2 batteries. It is believed that functional porous carbon-based composite electrode materials will continuously contribute to the field of lithium secondary batteries.

Analytical modeling and simulation of porous electrodes: Li-ion distribution and diffusion-induced stress

A new model of porous electrodes based on the Gibbs free energy is developed, in which lithium-ion(Liion) diffusion, diffusion-induced stress(DIS), Butler–Volmer(BV) reaction kinetics, and size polydispersity of electrode particles are considered. The influence of BV reaction kinetics and concentration-dependent exchange current density(ECD) on concentration profile and DIS evolution are numerically investigated. BV reaction kinetics leads to a decrease in Li-ion concentration and DIS. In addition, concentrationdependent ECD results in a decrease in Li-ion concentration and an increase in DIS. Size polydispersity of electrode particles significantly affects the concentration profile and DIS.Optimal macroscopic state of charge(SOC) should consider the influence of the microscopic SOC values and mass fractions of differently sized particles.

Two-Phase Flow in Porous Electrodes of Proton Exchange Membrane Fuel Cell

Water management in porous electrodes bears significance due to its strong potential in determining the performance of proton exchange membrane fuel cell.In terms of porous electrodes,internal water distribution and removal process have extensively attracted attention in both experimental and numerical studies.However,the structural difference among the catalyst layer(CL),microporous layer(MPL),and gas diffusion layer(GDL)leads to significant challenges in studying the two-phase flow behavior.Given the different porosities and pore scales of the CL,MPL,and GDL,the model scales in simulating each component are inconsistent.This review emphasizes the numerical simulation related to porous electrodes in the water transport process and evaluates the effectiveness and weakness of the conventional methods used during the investigation.The limitations of existing models include the following:(i)The reconstruction of geometric models is difficult to achieve when using the real characteristics of the components;(ii)the computational domain size is limited due to massive computational loads in three-dimensional(3 D)simulations;(iii)numerical associations among 3 D models are lacking because of the separate studies for each component;(iv)the effects of vapor condensation and heat transfer on the two-phase flow are disregarded;(v)compressive deformation during assembly and vibration in road conditions should be considered in two-phase flow studies given the real operating conditions.Therefore,this review is aimed at critical research gaps which need further investigation.Insightful potential research directions are also suggested for future improvements.

Flexible heteroatom-doped porous carbon nanofiber cages for electrode scaffolds

Porous carbon nanofibers(PCNFs)with rich functionalities and high surface areas are important electrode scaffolds to load active materials,but increasing their pore volumes and strength simultaneously is a challenge.Here,we report a scalable method to fabricate B-F-N triply doped PCNF cages with high porosity of greater than 92.8%and small bending stiffness of 10 mN by electrospinning the mixed sol of poly(tetrafluoroethylene),poly(vinyl alcohol),boric acid,and carbon nanotubes(CNTs)followed by pyrolysis.The macromicro dual-phase separation creates well-controlled macropores(>60 nm)and meso-micropores with large pore volumes(0.55 cm3/g)on carbon nanofibers,while the interior CNTs can cushion the applied stress and render the PCNF films with superior flexibility.Fabricated symmetrical supercapacitors with the PCNF cages exhibit high gravimetric capacitance of 164 F/g at 20 mV/s and 92.5%capacity retention after 20000 cycles at 2 A/g.The reported approach allows the green synthesis of a new PCNF scaffold material with properties appealing for applications.

Preparation and Electrochemical Properties of Porous Platinum Electrode

Porous platinum electrodes were prepared by adding YSZ,as an active material,in platinum paste.Relationship between microstructure and electrochemical performance of O 2(g),Pt/YSZ electrode have been characterized by SEM and cyclic voltammetry.Results showed that the microstructure of platinum electrode is a significant impact on the cyclic voltammetry.With the increase of platinum electrode's porosity,the area of three-phase boundary of O 2(g) /Pt/YSZ was increased.The electrochemical reactivity was also enhanced.These were presented as the increase of current density and cathode voltage in cyclic voltammetry.

Newly Design Porous/Sponge Red Phosphorus@Graphene and Highly Conductive Ni2P Electrode for Asymmetric Solid State Supercapacitive Device With Excellent Performance

Supercapacitors have attracted much attention in the field of electrochemical energy storage.However,material preparation,stability,performance as well as power density limit their applications in many fields.Herein,a sponge-like red phosphorus@graphene(rP@rGO)negative electrode and a Ni2P positive electrode were prepared using a simple one-step method.Both electrodes showed excellent performances(294 F g^−1 and 1526.6 F g^−1 for rP@rGO and Ni2P,respectively),which seem to be the highest among all rP@rGO-and Ni2P-based electrodes reported so far.The asymmetric solid-state supercapacitor was assembled by sandwiching a gel electrolyte-soaked cellulose paper between rP@rGO and Ni2P as the negative and positive electrodes.Compared to other asymmetric devices,the device,which attained a high operating window of up to 1.6 V,showed high energy and power density values of 41.66 and 1200 W kg−1,respectively.It also has an excellent cyclic stability up to 88%after various consecutive charge/discharge tests.Additionally,the device could power commercial light emitting diodes and fans for 30 s.So,the ease of the synthesis method and excellent performance of the prepared electrode materials mat have significant potential for energy storage applications.

Self-templating synthesis of biomass-based porous carbon nanotubes for energy storage and catalytic degradation applications

Dwindling energy sources and a worsening environment are huge global problems,and biomass wastes are an under-exploited source of material for both energy and material generation.Herein,self-template decoction dregs of Ganoderma lucidum-derived porous carbon nanotubes(ST-DDLGCs)were synthesized via a facile and scalable strategy in response to these challenges.ST-DDLGCs exhibited a large surface area(1731.51 m^(2)g^(-1))and high pore volume(0.76 cm^(3)g^(-1)),due to the interlacing tubular structures of precursors and extra-hierarchical porous structures on tube walls.In the ST-DDLGC/PMS system,the degradation efficiency of capecitabine(CAP)reached~97.3%within 120 min.Moreover,ST-DDLGCs displayed high catalytic activity over a wide pH range of 3–9,and strong anti-interference to these typical and ubiquitous anions in wastewater and natural water bodies(i.e.,H_(2)PO_(4)^(-),NO_(3)^(-),Cl^(-) and HCO_(3)^(-)),in which a ^(1)O_(2)-dominated oxidation was identified and non-radical mechanisms were deduced.Additionally,ST-DDLGC-based coin-type symmetrical supercapacitors exhibited outstanding electrochemical performance,with specific capacitances of up to 328.1 F g^(-1)at 0.5 A g^(-1),and cycling stability of up to 98.6%after 10,000 cycles at a current density of 2 A g^(-1).The superior properties of ST-DDLGCs could be attributed to the unique porous tubular structure,which facilitated mass transfer and presented numerous active sites.The results highlight ST-DDLGCs as a potential candidate for constructing inexpensive and advanced environmentally functional materials and energy storage devices.

Study of the electrochemical properties of a transition metallic ions modified electrode in acidic VOSO_4 solution

Graphite material was used as the electrode for an all-vanadium redox flow battery, and the electrode was modified by transition metallic ions to enhance its electrochemical behavior. An porous graphite composite electrode has high specific surface area and high current density. The electrode modified by transition metallic ions has improved catalysis behavior that can catalyze the V（Ⅱ）-V（Ⅴ） redox reaction showed by cyclic voltammograms. This article studied the impedance of the modified electrode by electrochemical impedance spectroscopy （EIS）, and approved that the electrode modified by Co^2＋ and Mn^2＋ has a lower charge transfer resistance than the non-modified electrode. The effect of average particle size distribution is at lower frequencies that the slope of Warburg impedance is reduced by large particle size distribution. The voltage efficiency of the Co^2＋ modified electrode test cell is 81.5%, which is higher than that of the non-modified electrode.

Optimization of LiMn_2O_4 electrode properties in a gradient-and surrogate-based framework

In this study, the effects of discharge rate and LiMn2O4 cathode properties （thickness, porosity, particle size, and solid-state diffusivity and conductivity） on the gravimetric energy and power density of a lithium-ion battery cell are analyzed simultaneously using a cell-level model. Surrogate-based analysis tools are applied to simulation data to construct educed-order models, which are in turn used to perform global sensitivity analysis to compare the relative importance of cathode properties. Based on these results, the cell is then optimized for several distinct physical scenarios using gradient-based methods. The comple-mentary nature of the gradient-and surrogate-based tools is demonstrated by establishing proper bounds and constraints with the surrogate model, and then obtaining accurate optimized solutions with the gradient-based optimizer. These optimal solutions enable the quantification of the tradeoffs between energy and power density, and the effect of optimizing the electrode thickness and porosity. In conjunction with known guidelines, the numerical optimization frame-work developed herein can be applied directly to cell and pack design.

Water-induced electrode poisoning and the mitigation strategy for high temperature polymer electrolyte membrane fuel cells

Engineering failure of membrane electrode assembly caused by increasingly fuel poisoning in the high temperature polymer electrolyte membrane fuel cells fed with humidified reformate gases is firstly demonstrated herein this work. Based on the results of the in-situ environmental scanning electron microscope, electrochemical analyses, and limiting current method, a water-induced phosphoric acid invasion model is constructed in the porous electrode to elucidate the failure causations of the hindered hydrogen mass transport and the enhanced carbon monoxide poisoning. To optimize the phosphoric acid distribution under the inevitably humidified circumstance, a facile and effective strategy of constructing acid-proofed electrode is proposed and demonstrates outstanding stability with highly humidified reformate gases as anode fuel. This work discusses a potential defect that was rarely studied previously under practical working circumstance for high temperature polymer electrolyte membrane fuel cells, providing an alternative opinion of electrode design based on the fundamental aspects towards the engineering problems.

Performance and mechanism of Prussian blue (PB) modified carbon felt electrode

Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order to distinguish the mechanism of the PB modified carbon felt electrode, the electrochemical quartz crystal microbalance (EQCM) was employed. The results of cyclic voltammetry show that the modification can improve the reversibility and the suitable PB deposition is the amount of 10 circles deposition. PB modified carbon felt electrode can effectively decrease the charge transfer resistance. The voltage efficiency of VRB employing PB modified carbon felt electrode can be increased by 12%. The mass change of the PB modified Pt crystal electrode in the process of the potential scan is obvious. The reaction of substitution of VO2+ for high-spin Fe ion in PB is probable to happen and the possible reaction equation is given. The preliminary exploration shows that PB modified carbon felt is electrochemically promising for redox flow battery.

Mesoporous molybdenum carbide for greatly enhanced hydrogen evolution at high current density and its mechanism studies

Currently the catalysis of hydrogen evolution reaction(HER)is mainly focused on the inherent electrocatalytic activity at relatively lower current densities while scarce at high current densities.Nevertheless,the latter is highly demanding in efficient mass-production of hydrogen.A SiO_(2) nanospheres template-synthesis is used to prepare mesoporous molybdenum carbide nanocrystals-embedded nitrogen-doped carbon foams(mp-Mo_(2)C/NC).The material shows much more excellent catalytic activity than the non-etched Mo_(2)C/NC toward hydrogen evolution reaction(HER)in acidic medium.More interestingly mp-Mo_(2)C/NC still has larger overpotential than Pt/C at lower current densities,but possess remarkably smaller overpotential than the latter at higher current densities for much better electrocatalytic performance.An approach is developed to investigate the electrode kinetics by Tafel plots,especially with eliminating the diffusion effect,indicating that Pt/C and mp-Mo_(2)C/NC display different reaction mechanisms.At low current densities the former presents reversible reaction,while the latter shows mixed electrochemical polarization/reversible electrode process.In the region of higher current densities,the former becomes totally gas-diffusion controlled with large overpotential,while the latter can still retain an electrode polarization process for much lower overpotential at the same current density.Result endorses that the meso-porously structured mp-Mo_(2)C/NC plays a critical role in avoiding gas diffusion control-resulting large overpotential at high current densities.This work holds great potential for an inexpensive catalyst better than Pt/C in practical applications of mass-production hydrogen at high current densities,while clearly shedding fundamental lights on designs of rational HER catalysts for the uses at high current densities.

Laser-induced graphene-coated wearable smart textile electrodes for biopotentials signal monitoring

This paper describes how to produce a wearable dry electrode at a reasonable cost and how to use it for the monitoring of biopotentials in electrocardiography.Smart textiles in wearable technologies have made a great advancement in the health care management and living standards of humans.Graphene was manufactured using the low-cost single-step process,laser ablation of polyimide,a commercial polymer.Graphene dispersions were made using solvent isopropyl alcohol which has low boiling point,nontoxicity,and environmental friendliness.After successive coating of the graphene dispersion on the cotton fabric to make it conductive,the sheet resistance of the resulting fabric dropped to 3% of its initial value.The laser-induced graphene(LIG)cotton dry electrodes thus manufactured are comparable to Ag/AgCl wet electrodes in terms of the skin-to-electrode impedance,measuring between 78.0 and 7.2 kΩ for the frequency between 40 Hz and 1 kHz.The LIG cotton electrode displayed a signal-to-noise ratio of 20.17 dB.Due to its comfort,simplicity,and good performance over a longer period of time,the textile electrode appears suited for medical applications.

Insights into Nano-and Micro-Structured Scaffolds for Advanced Electrochemical Energy Storage

Adopting a nano-and micro-structuring approach to fully unleashing the genuine potential of electrode active material benefits in-depth understandings and research progress toward higher energy density electrochemical energy stor-age devices at all technology readiness levels.Due to various challenging issues,especially limited stability,nano-and micro-structured(NMS)electrodes undergo fast electrochemical performance degradation.The emerging NMS scaffold design is a pivotal aspect of many electrodes as it endows them with both robustness and electrochemical performance enhancement,even though it only occupies comple-mentary and facilitating components for the main mechanism.However,extensive efforts are urgently needed toward optimizing the stereoscopic geometrical design of NMS scaffolds to minimize the volume ratio and maximize their functionality to fulfill the ever-increasing dependency and desire for energy power source supplies.This review will aim at highlighting these NMS scaffold design strategies,summariz-ing their corresponding strengths and challenges,and thereby outlining the potential solutions to resolve these challenges,design principles,and key perspectives for future research in this field.Therefore,this review will be one of the earliest reviews from this viewpoint.

Decouple charge transfer reactions in the Li-ion battery

In the development of Li-ion batteries(LIBs)with high energy/power density,long cycle-life,fast charging,and high safety,an insight into charge transfer reactions is required.Although electrochemical impedance spectroscopy(EIS)is regarded as a powerful diagnosis tool,it is not a direct but an indirect measurement.With respect to this,some critical questions need to be answered:(i)why EIS can reflect the kinetics of charge transfer reactions;(ii)what the inherent logical relationship between impedance models under different physical scenes is;(iii)how charge transfer reactions compete with each other at multiple scales.This work aims at answering these questions via developing a theory framework so as to mitigate the blindness and uncertainty in unveiling charge transfer reactions in LIBs.To systematically answer the above questions,this article is organized into a three-in-one(review,tutorial,and research)type and the following contributions are made:(i)a brief review is given for impedance model development of the LIBs over the past half century;(ii)an open source code toolbox is developed based on the unified impedance model;(iii)the competive mechanisms of charge transfer reactions are unveiled based on the developed EIS-Toolbox@LIB.This work not only clarifies theoretical fundamentals,but also provides an easy-to-use open source code for EIS-Toolbox@LIB to optimize fast charge/discharge,mitigate cycle aging,and improve energy/power density.

Fabricating sustainable lignin-derived porous carbon as electrode for high-performance supercapacitors

Lignocellulosic biomass such as plants and agricultural waste are ideal to tackle the current energy crisis and energy-related environmental issues.Carbon-rich lignin is abundant in lignocellulosic biomass,whose high-value transformation and utilization has been the most urgent problem to be solved.Herein,we propose a method for the preparation of porous carbon from lignin employing an H_(3)PO_(4)-assisted hydrothermal method.We characterize the as-prepared lignin-derived porous carbon and investigate its potential for energy storage.After assisted hydrothermal treatment followed by carbonization at 800℃,the lignin-derived porous carbon displays a high specific capacitance(223.6 F·g^(–1) at 0.1 A·g^(–1))and excellent cycling ability with good capacitance retention.In this present study,the resultant lignin-derived porous carbon was used as the electrode of a supercapacitor,illustrating yet another potential high-value use for lignin,namely as a candidate for the sustainable fabrication of main supercapacitor components.

Quick fabrication of evenly porous PbO_(2) through potential linear increase electrodeposition

Anodic oxidation electrodeposition is the primary way to prepare lead dioxide anode. The regulation of the external circuit for the reaction is a unique advantage of electrocatalytic reaction, which can regulate crystallization and accelerate the reaction process. In this study, lead dioxide coatings with uniform pore size distribution were quickly prepared on three different substrates by potential linear increase electrodeposition(PLIED). Morphology and structure analysis shows that the prepared electrodes have uniform porous morphology, and Ti/SnO_(2)/PLIED has the smallest grain size. Three electrodes all display well degradation performance to azophloxine and diclofenac sodium. Ti/PLIED, and Ti/SnO_(2)/PLIED are appreciated for degrading organics with a simple structure in low concentrations. At the same time,Ti/SnO_(2)/PLIED is more suitable for complex organics in high concentrations. Electrochemical activity tests indicate the different mechanisms of the PLIED electrodes that build the other degradation performance.Three PLIED electrodes show excellent electrical and electrochemical stability during the cycle degradation process. The results provide a reference for the subsequent anodic oxidation electrodeposition research and the regulating effect of the external circuit on coating properties.