Modulus-tunable multifunctional hydrogel ink with nanofillers for 3D-Printed soft electronics.

Seamless integration and conformal contact of soft electronics with tissue surfaces have emerged as major challenges in realizing accurate monitoring of biological signals. However, the mechanical mismatch between the electronics and biological tissues impedes the conformal interfacing between them. Attempts have been made to utilize soft hydrogels as the bioelectronic materials to realize tissue-comfortable bioelectronics. However, hydrogels have several limitations in terms of their electrical and mechanical properties. In this study, we present the development of a 3D-printable modulus-tunable hydrogel with multiple functionalities. The hydrogel has a cross-linked double network, which greatly improves its mechanical properties. Functional fillers such as XLG or functionalized carbon nanotubes (fCNT) can be incorporated into the hydrogel to provide tunable mechanics (Young's modulus of 10-300 kPa) and electrical conductivity (electrical conductivity of ∼20 S/m). The developed hydrogel exhibits stretchability (∼1000% strain), self-healing ability (within 5 min), toughness (400-731 kJ/m3) viscoelasticity, tissue conformability, and biocompatibility. Upon examining the rheological properties in the modulated region, hydrogels can be 3D printed to customize the shape and design of the bioelectronics. These hydrogels can be fabricated into ring-shaped strain sensors for wearable sensor applications.

Recent trends in core/shell nanoparticles: their enzyme-based electrochemical biosensor applications.

Improving novel and efficient biosensors for determining organic/inorganic compounds is a challenge in analytical chemistry for clinical diagnosis and research in biomedical sciences. Electrochemical enzyme-based biosensors are one of the commercially successful groups of biosensors that make them highly appealing because of their low cost, high selectivity, and sensitivity. Core/shell nanoparticles have emerged as versatile platforms for developing enzyme-based electrochemical biosensors due to their unique physicochemical properties and tunable surface characteristics. This study provides a comprehensive review of recent trends and advancements in the utilization of core/shell nanoparticles for the development of enzyme-based electrochemical biosensors. Moreover, a statistical evaluation of the studies carried out in this field between 2007 and 2023 is made according to the preferred electrochemical techniques. The recent applications of core/shell nanoparticles in enzyme-based electrochemical biosensors were summarized to quantify environmental pollutants, food contaminants, and clinical biomarkers. Additionally, the review highlights recent innovations and strategies to improve the performance of enzyme-based electrochemical biosensors using core/shell nanoparticles. These include the integration of nanomaterials with specific functions such as hydrophilic character, chemical and thermal stability, conductivity, biocompatibility, and catalytic activity, as well as the development of new hybrid nanostructures and multifunctional nanocomposites.

Progress and Perspective in harnessing MXene-carbon-based composites (0-3D): Synthesis, performance, and applications.

MXene is recognized as a promising catalyst for versatile applications due to its abundant metal sites, physicochemical properties, and structural formation. This comprehensive review offers an in-depth analysis of the incorporation of carbon into MXene, resulting in the formation of MXene-carbon-based composites (MCCs). Pristine MXene exhibits numerous outstanding characteristics, such as its atomically thin 2D structure, hydrophilic surface nature, metallic electrical conductivity, and substantial specific surface area. The introduction of carbon guides the assembly of MCCs through electrostatic self-assembly, pairing positively charged carbon with negatively charged MXene. These interactions result in increased interlayer spacing, reduced ion/electron transport distances, and enhanced surface hydrophilicity. Subsequent sections delve into the synthesis methods for MCCs, focusing on MXene integrated with various carbon structures, including 0D, 1D, 2D, and 3D carbon. Comprehensive discussions explore the distinctive properties of MCCs and the unique advantages they offer in each application domain, emphasizing the contributions and advancements they bring to specific fields. Furthermore, this comprehensive review addresses the challenges encountered by MCCs across different applications. Through these analyses, the review promotes a deeper understanding of exceptional characteristics and potential applications of MCCs. Insights derived from this review can serve as guidance for future research and development efforts, promoting the widespread utilization of MCCs across a broad spectrum of disciplines and spurring future innovations.

Electrical Transport and Dynamics of Confined DNA through Highly Conductive 2D Graphene Nanochannels.

Confining DNA in nanochannels is an important approach to studying its structure and transportation dynamics. Graphene nanochannels are particularly attractive for studying DNA confinement due to their atomic flatness, precise height control, and excellent mechanical strength. Here, using femtosecond laser etching and wetting transfer, we fabricate graphene nanochannels down to less than 4.3 nm in height, with the length-to-height ratios up to 103. These channels exhibit high stability, low noise, and self-cleaning ability during the long-term ionic current recording. We report a clear linear relationship between DNA length and the residence time in the channel and further utilize this relationship to differentiate DNA fragments based on their lengths, ranging widely from 200 bps to 48.5 kbps. The graphene nanochannel presented here provides a potential platform for label-free analyses and reveals fundamental insights into the conformational dynamics of DNA and proteins in confined space.

Intelligent perceptual textiles based on ionic-conductive and strong silk fibers.

Endowing textiles with perceptual function, similar to human skin, is crucial for the development of next-generation smart wearables. To date, the creation of perceptual textiles capable of sensing potential dangers and accurately pinpointing finger touch remains elusive. In this study, we present the design and fabrication of intelligent perceptual textiles capable of electrically responding to external dangers and precisely detecting human touch, based on conductive silk fibroin-based ionic hydrogel (SIH) fibers. These fibers possess excellent fracture strength (55 MPa), extensibility (530%), stable and good conductivity (0.45 S·m-1) due to oriented structures and ionic incorporation. We fabricated SIH fiber-based protective textiles that can respond to fire, water, and sharp objects, protecting robots from potential injuries. Additionally, we designed perceptual textiles that can specifically pinpoint finger touch, serving as convenient human-machine interfaces. Our work sheds new light on the design of next-generation smart wearables and the reshaping of human-machine interfaces.

One-dimensional proximity superconductivity in the quantum Hall regime.

Extensive efforts have been undertaken to combine superconductivity and the quantum Hall effect so that Cooper-pair transport between superconducting electrodes in Josephson junctions is mediated by one-dimensional edge states1-6. This interest has been motivated by prospects of finding new physics, including topologically protected quasiparticles7-9, but also extends into metrology and device applications10-13. So far it has proven challenging to achieve detectable supercurrents through quantum Hall conductors2,3,6. Here we show that domain walls in minimally twisted bilayer graphene14-18 support exceptionally robust proximity superconductivity in the quantum Hall regime, allowing Josephson junctions to operate in fields close to the upper critical field of superconducting electrodes. The critical current is found to be non-oscillatory and practically unchanging over the entire range of quantizing fields, with its value being limited by the quantum conductance of ballistic, strictly one-dimensional, electronic channels residing within the domain walls. The system described is unique in its ability to support Andreev bound states at quantizing fields and offers many interesting directions for further exploration.

Sensitivity volume as figure-of-merit for maximizing data importance in electrical impedance tomography.

Objective.Electrical impedance tomography (EIT) is a noninvasive imaging method whereby electrical measurements on the periphery of a heterogeneous conductor are inverted to map its internal conductivity. The EIT method proposed here aims to improve computational speed and noise tolerance by introducing sensitivity volume as a figure-of-merit for comparing EIT measurement protocols.Approach.Each measurement is shown to correspond to a sensitivity vector in model space, such that the set of measurements, in turn, corresponds to a set of vectors that subtend a sensitivity volume in model space. A maximal sensitivity volume identifies the measurement protocol with the greatest sensitivity and greatest mutual orthogonality. A distinguishability criterion is generalized to quantify the increased noise tolerance of high sensitivity measurements.Main result.The sensitivity volume method allows the model space dimension to be minimized to match that of the data space, and the data importance to be increased within an expanded space of measurements defined by an increased number of contacts.Significance.The reduction in model space dimension is shown to increasecomputational efficiency, accelerating tomographic inversion by several orders of magnitude, while the enhanced sensitivitytolerates higher noiselevels up to several orders of magnitude larger than standard methods.

Exploring the electrical robustness of conductive textile fasteners for wearable devices in different human motion conditions.

Conventional snap fasteners used in clothing are often used as electrical connectors in e-textile and wearable applications for signal transmission due to their wide availability and ease of use. Nonetheless, limited research exists on the validation of these fasteners, regarding the impact of contact-induced high-amplitude artefacts, especially under motion conditions. In this work, three types of fasteners were used as electromechanical connectors, establishing the interface between a regular sock and an acquisition device. The tested fasteners have different shapes and sizes, as well as have different mechanisms of attachment between the plug and receptacle counterparts. Experimental evaluation was performed under static conditions, slow walking, and rope jumping at a high cadence. The tests were also performed with a test mass of 140 g. Magnetic fasteners presented excellent electromechanical robustness under highly dynamic human movement with and without the additional mass. On the other hand, it was demonstrated that the Spring snap buttons (with a spring-based engaging mechanism) presented a sub-optimal performance under high motion and load conditions, followed by the Prong snap fasteners (without spring), which revealed a high susceptibility to artefacts. Overall, this work provides further evidence on the importance and reliability of clothing fasteners as electrical connectors in wearable systems.

Low-impedance tissue-device interface using homogeneously conductive hydrogels chemically bonded to stretchable bioelectronics.

Stretchable bioelectronics has notably contributed to the advancement of continuous health monitoring and point-of-care type health care. However, microscale nonconformal contact and locally dehydrated interface limit performance, especially in dynamic environments. Therefore, hydrogels can be a promising interfacial material for the stretchable bioelectronics due to their unique advantages including tissue-like softness, water-rich property, and biocompatibility. However, there are still practical challenges in terms of their electrical performance, material homogeneity, and monolithic integration with stretchable devices. Here, we report the synthesis of a homogeneously conductive polyacrylamide hydrogel with an exceptionally low impedance (~21 ohms) and a reasonably high conductivity (~24 S/cm) by incorporating polyaniline-decorated poly(3,4-ethylenedioxythiophene:polystyrene). We also establish robust adhesion (interfacial toughness: ~296.7 J/m2) and reliable integration between the conductive hydrogel and the stretchable device through on-device polymerization as well as covalent and hydrogen bonding. These strategies enable the fabrication of a stretchable multichannel sensor array for the high-quality on-skin impedance and pH measurements under in vitro and in vivo circumstances.

Nanocellulose-mediated conductive hydrogels with NIR photoresponse and fatigue resistance for multifunctional wearable sensors.

The rapid development of hydrogels has garnered significant attention in health monitoring and human motion sensing. However, the synthesis of multifunctional conductive hydrogels with excellent strain/pressure sensing and photoresponsiveness remains a challenge. Herein, the conductive hydrogels (BPTP) with excellent mechanical properties, fatigue resistance and photoresponsive behavior composed of polyacrylamide (PAM) matrix, 2,2,6,6-tetramethylpiperidin-1-yloxy-oxidized cellulose nanofibers (TOCNs) reinforcement and polydopamine-modified black phosphorus (BP@PDA) photosensitizer are prepared through a facile free-radical polymerization approach. The PDA adhered to the BP surface by π-π stacking promotes the optical properties of BP while also preventing BP oxidation from water. Through hydrogen bonding interactions, TOCNs improve the homogeneous dispersion of BP@PDA nanosheets and the mechanical toughness of BPTP. Benefiting from the synergistic effect of PDA and TOCNs, the conductive BPTP integrates superior mechanical performances, excellent photoelectric response and photothermal conversion capability. The BPTP-based sensor with high cycling stability demonstrates superior strain sensitivity (GF = 6.0) and pressure sensing capability (S = 0.13 kPa-1) to monitor various human activities. Therefore, this work delivers an alternative construction strategy for generating high-performance conductive hydrogels as multifunctional wearable sensors.

Study on the effect of different high-voltage electric field polarization process parameters on the vitality of dried chili pepper seeds.

To study the effect of different high-voltage electric field polarisation treatment process parameters on the viability of seeds of dried chili peppers. In this study, a high-voltage electrostatic polarisation treatment system was constructed to carry out experiments on the effects of different high-voltage electric field polarisation treatment process parameters on the viability of dried chili seeds. Conduct one-way tests to determine the preferred polarisation method and the preferred interval for output voltage and polarisation time. Two-factor, five-level central combination test with output voltage and polarization time as test factors and seed conductivity as a response indicator. Determining the better combination of parameters for output voltage and polarization time; Conducting seed germination trials to validate the effectiveness of the polarisation process. The results of the one-way test showed that: Negative-voltage polarisation was more effective than positive-voltage polarisation and alternating positive-negative-voltage polarisation in promoting seed vigor, with a better output voltage in the range of 10-14 kV, and a better polarisation time in the range of 20-40 s; The results of orthogonal tests showed that: Under the condition of negative voltage polarisation treatment, the output voltage of 12.08 kV and polarisation time of 30.32 s was the better parameter combination, at which the seed conductivity was minimum 159.87 uS/(cm g). Analyzing the function of cell membrane selective semi-permeability by seed conductivity change and revealing the mechanism of seed viability enhancement by high voltage electric field polarisation treatment; In the seed germination test, compared with the control group, seed germination potential increased by 9.09%, germination rate increased by 20.45%, germination index increased by 3.49, and vigor index increased by 41.66 under high-voltage electrostatic polarisation treatment, and all vigor indexes were significantly improved. The results of this study can provide a basis for the selection of processes and parameters for subsequent high-voltage electric field polarisation treatment of crop seeds.

Highly elastic, fatigue-resistant, antibacterial, conductive, and nanocellulose-enhanced hydrogels with selenium nanoparticles loading as strain sensors.

The fabrication of highly elastic, fatigue-resistant and conductive hydrogels with antibacterial properties is highly desirable in the field of wearable devices. However, it remains challenging to simultaneously realize the above properties within one hydrogel without compromising excellent sensing ability. Herein, we fabricated a highly elastic, fatigue-resistant, conductive, antibacterial and cellulose nanocrystal (CNC) enhanced hydrogel as a sensitive strain sensor by the synergistic effect of biosynthesized selenium nanoparticles (BioSeNPs), MXene and nanocellulose. The structure and potential mechanism to generate biologically synthesized SeNPs (BioSeNPs) were systematically investigated, and the role of protease A (PrA) in enhancing the adsorption between proteins and SeNPs was demonstrated. Additionally, owing to the incorporation of BioSeNPs, CNC and MXene, the synthesized hydrogels showed high elasticity, excellent fatigue resistance and antibacterial properties. More importantly, the sensitivity of hydrogels determined by the gauge factor was as high as 6.24 when a high strain was applied (400-700 %). This study provides a new horizon to synthesize high-performance antibacterial and conductive hydrogels for soft electronics applications.

Casein-based hydrogels: Advances and prospects.

Casein-based hydrogels (Casein Gels) possess advantageous properties, including mechanical strength, stability, biocompatibility, and even adhesion, conductivity, sensing capabilities, as well as controlled-releasing behavior of drugs. These features are attributed to their gelation methods and functionalization with various polymers. Casein Gels is an important protein-based material in the food industry, in terms of dairy and functional foods, biological and medicine, in terms of carrier for bioactive and sensitive drugs, wound healing, and flexible sensors and wearable devices. Herein, this review aims to highlight the importance of the features mentioned above via a comprehensive investigation of Casein Gels through multiple directions and dimensional applications. Firstly, the composition, structure, and properties of casein, along with the gelation methods employed to create Casein Gels are elaborated, which serves as a foundation for further exploration. Then, the application progresses of Casein Gels in dairy products, functional foods, medicine, flexible sensors and wearable devices, are thoroughly discussed to provide insights into the diverse fields where Casein Gels have shown promise and utility. Lastly, the existing challenges and future research trends are highlighted from an interdisciplinary perspective. We present the latest research advances of Casein Gels and provide references for the development of multifunctional biomass-based hydrogels.

Fabrication of a tailor-made conductive polyaniline/ascorbic acid-coated nanofibrous mat as a conductive and antioxidant cell-free cardiac patch.

Polyaniline (PANI) wasin-situpolymerized on nanofibrous polycaprolactone mats as cell-free antioxidant cardiac patches (CPs), providing electrical conductivity and antioxidant properties. The fabricated CPs took advantage of intrinsic and additive antioxidant properties in the presence of PANI backbone and ascorbic acid as a biocompatible dopant of PANI. The antioxidant nature of CPs may reduce the serious repercussions of oxidative stress, produced during the ischemia-reperfusion (I/R) process following myocardial infarction. The polymerization parameters were considered as aniline (60 mM, 90 mM, and 120 mM), ascorbic acid concentrations ([aniline]:[ascorbic acid] = 3:0, 3:0.5, 3:1, 3:3), and polymerization time (1 h and 3 h). Mainly, the more aniline concentrations and polymerization time, the less sheet resistance was obtained. 1,1 diphenyl-2-picrylhydrazyl (DPPH) assay confirmed the dual antioxidant properties of prepared samples. The advantage of the employedin-situpolymerization was confirmed by the de-doping/re-doping process. Non-desirable groups were excluded based on their electrical conductivity, antioxidant properties, and biocompatibility. The remained groups protected H9c2 cells against oxidative stress and hypoxia conditions. Selected CPs reduced the intracellular reactive oxygen species content and mRNA level of caspase-3 while the Bcl-2 mRNA level was improved. Also, the selected cardiac patch could attenuate the hypertrophic impact of hydrogen peroxide on H9c2 cells. Thein vivoresults of the skin flap model confirmed the CP potency to attenuate the harmful impact of I/R.

In situ fast self-assembled preparation of dandelion-like Cu(OH)2@Cu3(HHTP)2 with core-shell heterostructure arrays for electrochemical sensing of formaldehyde in food samples.

Formaldehyde is known to harm the respiratory, nervous, and digestive systems of people. In this paper, a novel dandelion-like electrocatalyst with core-shell heterostructure arrays were fast self-assembled prepared in situ using copper foam (CF) as support substrate and 2,3,6,7,10,11 hexahydroxy-triphenyl (HHTP) as ligand (Cu(OH)2@Cu3(HHTP)2/CF) by a simple two-step hydrothermal reaction. The 1D Cu(OH)2 nanorods "core" and the 2D π-conjugated conducting metal-organic frameworks (Cu3(HHTP)2cMOF) "shell" with remote delocalized electrons give the dandelion-like heterogeneous catalysts excellent electrochemical activity such as a large specific surface area, high conductivity and a fast electron transfer rate. The Cu(OH)2@Cu3(HHTP)2/CF exhibited excellent electrocatalytic performance for formaldehyde under alkaline conditions with a linear range of 0.2 µmol/L - 125 µmol/L and 125 µmol/L - 8 mmol/L, a detection limit as low as 15.9 nmol/L (S/N = 3), as well as good accuracy, consistency, and durability, and it effectively identified FA in food.

First-principles study of LiFePO4 modified by graphene and defective graphene oxide.

The energy stability and electronic structural of graphene and defective graphene oxide (GO) parallel to the surface of LiFePO4 (010) were theoretically investigated by using first-principles density functional theory calculations within the DFT + U framework. The calculated formation energy shows that GO coating on the surface of LiFePO4 (010) is energetically favorable and has higher bond strength compared to graphene. The calculation of the electronic structure indicates that the emergence of band in-gap states originates from graphene coating, with adsorbed O atoms contributing significantly above the Fermi level. Electron density difference indicate that GO stands on the LFP (010) surface through C-O and Fe-O bonds, rather than relying on van der Waals forces placed parallel to the LFP crystal, with the chemical bond at the LFP/GO interface (Fe-O-C) both anchoring the coated carbon layer and promoting electron conductivity at the interface. In addition, LFP/GO shows superior electrochemical performance, Atomic Populations suggests that the average Fe-O bonding on the surface of LiFePO4 (010) was clearly changed after graphene or GO coating, which led to the expansion of Li+ channels and favored the migration insertion and extraction of Li+.

Electrochemical Doping Effect on the Conductivity of Melanin-Inspired Materials.

Eumelanin is a natural pigment that can be particularly valuable for sustainable bioelectronic devices due to its inherent biocompatibility and hydration-dependent conductivity. However, the low conductivity of eumelanin limits its technological development. In this research, electrochemical doping was proposed as an alternative route to increase the electronic conductivity of synthetic eumelanin derivatives. Thin films of sulfonated eumelanin were deposited on platinum interdigitated electrodes and electrochemically treated by using cyclic voltammetry and chronoamperometry treatments. X-ray photoelectron spectroscopy analysis confirmed ion doping in sulfonated melanin. Current-voltage, current-time, and electrochemical impedance measurements were used to investigate the effect of different aqueous electrolytes (including KCl and LiClO4) treatments on the charge transport of sulfonated eumelanin. We show that the conductivity depends on the type and size of the anion used and can reach 10-3 S·cm-1. Additionally, depending on the electrolyte, there is a change in charge transport from mixed ionic/electronic to a predominantly electronic-only conduction. Our results show that the chemical nature of the ion plays an important role in the electrochemical doping and, consequently, in the charge transport of eumelanin. These insights serve as inspiration to explore the use of alternative electrolytes with different compositions further and develop eumelanin-based devices with tunable conductivities.

An overview of electrochemical biosensors used for COVID-19 detection.

This short review presents the latest advances in the field of electrochemical biosensors, focusing particularly on impedimetric biosensors for the direct measurement of analytes. As a source of study we have chosen to describe these advances in the latest global health crisis originated from the COVID-19 pandemic, initiated by the SARS-CoV-2 virus. In this period, the necessity for swift and precise detection methods has grown rapidly due to an imminent need for the development of an analytical method to identify and isolate infected patients as an attempt to control the spreading of the disease. Traditional approaches such as the enzyme-linked immunosorbent assay (ELISA), were extensively used during the SARS-CoV-2 pandemic, but their drawbacks, including slow response time, became evident. In this context, the potential of electrochemical biosensors as an alternative for COVID-19 detection was emphasized. These biosensors merge electrochemical technology with bioreceptors, offering benefits such as rapidity, accuracy, portability, and real-time result provision. Additionally, we present instances of electrochemical biosensors modified with conductive polymers, eliminating the necessity for an electrochemical probe. The adaptability of the developed materials and devices facilitated the prompt production of electrochemical biosensors during the pandemic, creating opportunities for broader applications in infectious disease diagnosis.

A microdosimetry analysis of reversible electroporation in scattered, overlapping, and cancerous cervical cells.

We present a numerical method for studying reversible electroporation on normal and cancerous cervical cells. This microdosimetry analysis builds on a unique approach for extracting contours of free and overlapping cervical cells in the cluster from the Extended Depth of Field (EDF) images. The algorithm used for extracting the contours is a joint optimization of multiple-level set function along with the Gaussian mixture model and Maximally Stable Extremal Regions. These contours are then exported to a multi-physics domain solver, where a variable frequency pulsed electric field is applied. The trans-Membrane voltage (TMV) developed across the cell membrane is computed using the Maxwell equation coupled with a statistical approach, employing the asymptotic Smoluchowski equation. The numerical model was validated by successful replication of existing experimental configurations that employed low-frequency uni-polar pulses on the overlapping cells to obtain reversible electroporation, wherein, several overlapping clumps of cervical cells were targeted. For high-frequency calculation, a combination of normal and cancerous cells is introduced to the computational domain. The cells are assumed to be dispersive and the Debye dispersion equation is used for further calculations. We also present the resulting strength-duration relationship for achieving the threshold value of electroporation between the normal and cancerous cervical cells due to their size and conductivity differences. The dye uptake modulation during the high-frequency electric field electroporation is further advocated by a mathematical model.

Conductive and capacitive network for enriching the exoelectrogens and enhancing the extracellular electron transfer in microbial fuel cells.

Although lots of nanomaterials modified anodes have been reported to improve the bacterial attachment and extracellular electron transfer (EET) in microbial fuel cells (MFCs), the lack of a three dimensional (3D) conductive and capacitive network severely limited MFCs performance. In this work, 3D conductive networks derived from mucor mycelia were grown on carbon cloth (CC), and capacitive FeMn phosphides/oxides were further anchored on these 3D networks by electrochemical deposition (denoted as FeMn/CMM@CC) to simultaneously address the above challenges. As a result, the multivalent metal active sites were evenly distributed on 3D conductive network, which favored the enrichment of exoelectrogens, mass transport and EET. Consequently, the as-prepared FeMn/CMM@CC anode displayed accumulated charge of 131.4C/m2, higher than bare CC. Meanwhile, FeMn/CMM@CC anode substantially promoted flavin excretion and the amounts of nano conduits. The abundance of Geobacter was 63 % on bare CC, and greatly increased to 83 % on FeMn/CMM@CC. MFCs equipped by FeMn/CMM@CC anode presented the power density of 3.06 W/m2 and coulombic efficiency (29.9 %), evidently higher than bare CC (1.29 W/m2, 7.3 %), and the daily chemical oxygen demand (COD) removal amount also increased to 92.6 mg/L/d. This work developed a facile method to optimize the abiotic-biotic interface by introducing 3D conductive and capacitive network, which was proved to be a promising strategy to modify macro-porous electrodes.