Electrode Surface Research Articles

Highly Efficient Acidic Electrosynthesis of Hydrogen Peroxide at Industrial-Level Current Densities Promoted by Alkali Metal Cations.

Acidic H2O2 synthesis through electrocatalytic 2e- oxygen reduction presents a sustainable alternative to the energy-intensive anthraquinone oxidation technology. Nevertheless, acidic H2O2 electrosynthesis suffers from low H2O2 Faradaic efficiencies primarily due to the competing reactions of 4e- oxygen reduction to H2O and hydrogen evolution in environments with high H+ concentrations. Here, we demonstrate the significant effect of alkali metal cations, acting as competing ions with H+, in promoting acidic H2O2 electrosynthesis at industrial-level currents, resulting in an effective current densities of 50-421 mA cm-2 with 84-100 % Faradaic efficiency and a production rate of 856-7842 μmol cm-2 h-1 that far exceeds the performance observed in pure acidic electrolytes or low-current electrolysis. Finite-element simulations indicate that high interfacial pH near the electrode surface formed at high currents is crucial for activating the promotional effect of K+. In situ attenuated total reflection Fourier transform infrared spectroscopy and ab initio molecular dynamics simulations reveal the central role of alkali metal cations in stabilizing the key *OOH intermediate to suppress 4e- oxygen reduction through interacting with coordinated H2O.

Highly Efficient Acidic Electrosynthesis of Hydrogen Peroxide at Industrial‐Level Current Densities Promoted by Alkali Metal Cations

AbstractAcidic H2O2 synthesis through electrocatalytic 2e− oxygen reduction presents a sustainable alternative to the energy‐intensive anthraquinone oxidation technology. Nevertheless, acidic H2O2 electrosynthesis suffers from low H2O2 Faradaic efficiencies primarily due to the competing reactions of 4e− oxygen reduction to H2O and hydrogen evolution in environments with high H+ concentrations. Here, we demonstrate the significant effect of alkali metal cations, acting as competing ions with H+, in promoting acidic H2O2 electrosynthesis at industrial‐level currents, resulting in an effective current densities of 50–421 mA cm−2 with 84–100 % Faradaic efficiency and a production rate of 856–7842 μmol cm−2 h−1 that far exceeds the performance observed in pure acidic electrolytes or low‐current electrolysis. Finite‐element simulations indicate that high interfacial pH near the electrode surface formed at high currents is crucial for activating the promotional effect of K+. In situ attenuated total reflection Fourier transform infrared spectroscopy and ab initio molecular dynamics simulations reveal the central role of alkali metal cations in stabilizing the key *OOH intermediate to suppress 4e− oxygen reduction through interacting with coordinated H2O.

Improved Compatibility of α-NaMnO2 Cathodes at the Interface with Safer and more Reliable Electrolytes.

The behaviour and compatibility of monoclinic sodium manganite, α-NaMnO2, cathodes at the interface with electrolytes based on the 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EMIFSI) and N-trimethyl-N-butylammonium bis(fluorosulfonyl)imide (N1114FSI) ionic liquids is presented and discussed. The Na+ insertion process was analysed through cyclic voltammetry tests combined with impedance spectroscopy measurements and the cell performance was tested by charge-discharge cycles. XPS and FIB-SEM measurements allowed analysis of the surface composition and the morphology of post-mortem cathodes. Overall, the α-NaMnO2 cathode showed high reversibility in N1114FSI-based electrolyte, delivering 60 % of the initial capacity after 1200 cycles in conjunction with a Coulombic efficiency above 99%. To our knowledge, these very promising results are the best result obtained till now for monolithic α-NaMnO2 cathodes, are ascribable to the formation of a stable passive layer onto the electrode surface, as confirmed by spectroscopic analysis.

Cathode|Electrolyte Interface Engineering by a Hydrogel Polymer Electrolyte for a 3D Porous High-Voltage Cathode Material in a Quasi-Solid-State Zinc Metal Battery by In Situ Polymerization.

This work highlights the development of a superior cathode|electrolyte interface for the quasi solid-state rechargeable zinc metal battery (QSS-RZMB) by a novel hydrogel polymer electrolyte using an ultraviolet (UV) light-assisted in situ polymerization strategy. By integrating the cathode with a thin layer of the hydrogel polymer electrolyte, this technique produces an integrated interface that ensures quick Zn2+ ion conduction. The coexistence of nanowires for direct electron routes and the enhanced electrolyte ion infiltration and diffusion by the 3D porous flower structure with a wide open surface of the Zn-MnO electrode complements the interface formation during the in situ polymerization process. The QSS-RZMB configured with an integrated cathode (i-Zn-MnO) and the hydrogel polymer electrolyte (PHPZ-30) as the separator yields a comparable specific energy density of 214.14Whkg-1 with that of its liquid counterpart (240.38Whkg-1, 0.5MZn(CF3SO3)2 aqueous electrolyte). Other noteworthy features of the presented QSS-RZMB system include its superior cycle life of over 1000 charge-discharge cycles and 85% capacity retention with 99% coulombic efficiency at the current density of 1.0Ag-1, compared to only 60% capacity retention over 500 charge-discharge cycles displayed by the liquid-state system under the same operating conditions.

Porous Prussian blue nanolayers formed in situ on Fe-MOFs-modified electrode surfaces by electrochemically triggered dual-templating effect for ultrasensitive detection of lead ions and Staphylococcus aureus

In this study, introducing Fe-MOFs as reactants to the electrode surface creates a novel mode for modulating interface performance that can lead to rapid enrichment of reactants in the proximity of electrodes by electrochemical-induced confinement effect. A facile, controllable, and room temperature electrochemical approach utilizes Fe-MOFs as nanotemplates to produce porous Prussian blue (PB) nanolayers on the electrode surfaces. Unlike conventional chemical conversion that needs a supply of exogenous acid regents, the electrochemical method creates a solid acidic condition in the oxygen evolution reaction cycle to release Fe3+ from the Fe-MOFs, improving conversion efficiency and electrochemical activity of PB. Furthermore, small oxygen bubbles generated by splitting H2O near the electrodes are also good templates, promoting the formation of porous structures that can increase effective surface area and mass-transfer efficiency. As a conceptional application, using Fe-MOFs as self-sacrificial tags, an ultrasensitive electrochemical platform with triple amplification is developed to detect Pb2+ and S. aureus based on DNAzyme-CHA cascade reaction. The designed platform shows low detection limits of 8.5 fM and 1 CFU/mL for Pb2+ and S. aureus, respectively. Moreover, the platform has high selectivity, stability and reproducibility, and also shows satisfactory recovery rates when validated using actual samples.

Electrogenerated chemiluminescence from luminol-labelled microbeads triggered by in situ generation of hydrogen peroxide.

We developed a sensing strategy that mimics the bead-based electrogenerated chemiluminescence immunoassay. However, instead of the most common metal complexes, such as Ru or Ir, the luminophore is luminol. The electrogenerated chemiluminescence of luminol was promoted by in situ electrochemical generation of hydrogen peroxide at a boron-doped diamond electrode. The electrochemical production of hydrogen peroxide was achieved in a carbonate solution by an oxidation reaction, while at the same time, microbeads labelled with luminol were deposited on the electrode surface. For the first time, we proved that was possible to obtain light emission from luminol without its direct oxidation at the electrode. This new emission mechanism is obtained at higher potentials than the usual luminol electrogenerated chemiluminescence at 0.3-0.5V, in conjunction with hydrogen peroxide production on boron-doped diamond at around 2-2.5V (vs Ag/AgCl).

MXene@MnIn2S4‐Gated Organic Photoelectrochemical Transistors with Nanozyme‐Mediated Multiple Quenching Effects for Ultrasensitive Detection of Okadaic Acid

AbstractOrganic optoelectronics have attracted widespread interdisciplinary research interest but lags far behind in the application in marine environmental detection. The organic photoelectrochemical transistor (OPECT) shows promise as a powerful tool for comprehensive monitoring and early warning of marine conditions, which can be further enhanced by the valuable signal amplification strategy of nanozyme‐mediated catalytic precipitation. Herein, OPECT technology is integrated with nanozyme‐mediated catalytic precipitation for the first time, establishing an ultrasensitive detection platform for okadaic acid (OA). Specifically, MXene@MnIn2S4 (MXMnIS) hybrid composed of Schottky‐junction is synthesized via a hydrothermal method, which can efficiently modulate the device with high current gain. Linking with a sandwich immunoassay, the Ru‐C3N4 nanozyme with peroxidase‐mimicking activity can catalyze the oxidation of 4‐chloro‐1‐naphthol (4‐CN) to form an insoluble precipitate on the electrode surface, resulting in a decrease in the photocurrent and altering the transistor response. Importantly, the proposed OPECT biosensor presented an excellent sensitivity and a low detection limit (32.5 pM), fully satisfying the fundamental requirements for the quantitative detection of intracellular and extracellular OA in the practical culture media of Prorocentrum lima at different growth stages. This OPECT platform based on the nanozyme‐mediated quenching effect is significant for effectively monitoring the safety of the marine ecological environment and food safety.

Intermolecular Interaction Mediated Potassium Ion Intercalation Chemistry in Ether‐Based Electrolyte for Potassium‐Ion Batteries

AbstractElectrolyte design is indeed a highly effective strategy to improve battery performance. However, identifying the intermolecular interaction in electrolyte solvation structure is rarely reported in potassium‐ion batteries. Herein, it is discovered that a solvent‐solvent intermolecular interaction can be formed when introducing the cyclopentylmethyl ether (CPME) solvent into the commonly used 1,2‐dimethoxyethane (DME)‐based electrolytes. Such interaction is not only analyzed by 2D 1H‐1H correlation spectroscopy for the first time but also found that it can weaken the K+‐DME interaction significantly, consequently enabling a reversible K+ (de‐)intercalation within the graphite. By employing this strategy without using any fluorine‐based solvent, a new fluorine‐free and low‐concentration ether‐based electrolyte is designed, which is not only compatible with graphite but also facilitates the design of high‐energy‐density and safe potassium ion sulfur batteries. A novel molecular interfacial model is further presented to analyze the interfacial behaviors of K+‐solvent‐anion complexes on the electrode surface that are affected by intermolecular interactions, elucidating the reasons behind the superior electrolyte compatibility and graphite electrode performance at the molecular scale. This work sheds some light on the critical role of solvent–solvent interactions in electrolyte design for potassium‐ion batteries and provides valuable insights for engineering and enhancing the performance of electrolytes and batteries.

Highly Sensitive and Selective Detection of L-Tryptophan by ECL Using Boron-Doped Diamond Electrodes.

L-tryptophan is an amino acid that is essential to the metabolism of humans. Therefore, there is a high interest for its detection in biological fluids including blood, urine, and saliva for medical studies, but also in food products. Towards this goal, we report on a new electrochemiluminescence (ECL) method for L-tryptophan detection involving the in situ production of hydrogen peroxide at the surface of boron-doped diamond (BDD) electrodes. We demonstrate that the ECL response efficiency is directly related to H2O2 production at the electrode surface and propose a mechanism for the ECL emission of L-tryptophan. After optimizing the analytical conditions, we show that the ECL response to L-tryptophan is directly linear with concentration in the range of 0.005 to 1 µM. We achieved a limit of detection of 0.4 nM and limit of quantification of 1.4 nM in phosphate buffer saline (PBS, pH 7.4). Good selectivity against other indolic compounds (serotonin, 3-methylindole, tryptamine, indole) potentially found in biological fluids was observed, thus making this approach highly promising for quantifying L-tryptophan in a broad range of aqueous matrices of interest.

Long-Term Stable Cycling of Dendrite-Free Lithium Metal Batteries Using ZIF-90@PP Composite Separator.

Lithium metal batteries (LMBs) are anticipated to meet the demand for high energy density, but the growth of lithium dendrites seriously hinders its practical application. Herein, we constructed a kind of composite separator (ZIF-90@PP) consisting of zeolite imidazole framework-90 (ZIF-90) and polypropylene (PP) to promote the uniform deposition of Li+ and inhibit the growth of lithium dendrites. The aldehyde groups interacting with TFSI- and the nitrogen-containing negative groups attracting Li+ of ZIF-90 can facilitate the dissociation of LiTFSI to release more Li+, thus alleviating the influence of space charge near the electrode surface and accelerating the transfer of Li+. Not only does the excellent electrolyte wettability of ZIF-90 enhance the electrolyte retention capacity of the separator, but the orderly nano-channels in ZIF-90 also restrict the free migration of anions and homogenize the distribution of Li+. Consequently, the functional separator achieves a long-term stable Li plating/stripping cycling for over 780 h at 2 mA cm-2. Moreover, an impressive average coulombic efficiency of 98.67% at 0.5 C after 300 cycles is realized by Li || LFP full cells based on ZIF-90@PP with a capacity retention rate of 71.22%. The high-rate and long cycling performance of the modified Li || LFP cells further demonstrates the advantages of the ZIF-90@PP composite separator.

Effect of Alkali Metal Cations and Trace Metal Impurities on Cathodic Corrosion of Gold Electrode Surfaces

AbstractIn this work, we comprehensively studied the cathodic corrosion of Au electrodes as a function of the identity of alkali metal hydroxides at different concentrations and various negative potentials. We reveal that the ratio of free water and water bound in hydration shells controls the overall cathodic corrosion behavior, alongside the specific adsorption of alkali metal cations. Moreover, we highlight the crucial role of electrolyte cleanliness, particularly regarding the presence of trace metal impurities. Interestingly, the presence of trace amounts of nickel and iron in as‐received CsOH suppresses cathodic corrosion by their deposition onto Au surfaces. In contrast, after purification the polarization of Au surfaces in 10 M CsOH leads to the formation of nanoporous surfaces with high electrochemically active surface area, in which the degree of porosity can be tuned by varying the polarization time at −1.6 V vs. RHE.

Development of electrochemical sensors based on silver nanoparticles electrodeposited on gold screen-printed electrodes: application to nitrate trace analysis in water

Abstract. A simple, reusable and sensitive electrochemical sensor based on a gold screen-printed electrode modified with silver nanoparticles has been developed for the detection of nitrate in water. Scanning electron microscopy, square wave voltammetry and electrochemical impedance spectroscopy were used to characterize the modification of the electrode surface. The modified electrode with different silver nanoparticle loadings was also tested, as well as the influence of scan rate on the reduction of nitrate. The sensor exhibited a wide linear response to nitrate from 100 to 1500 µM and a detection limit of 7.7 µM, which is significantly less than the maximum contaminant level admitted in drinking water (800 µM). The reproducibility, repeatability and selectivity of the sensor have also been examined. The suitability of the proposed sensor for real sample detection was successfully demonstrated via recovery studies performed in spiked tap water samples. The proposed approach was used to determine nitrate in freshwater, and the results were in good agreement with those obtained from a commercial nitrate sensor. These advantages make the developed sensor a promising alternative approach for integration into an online monitoring system for water monitoring.

Mass Transfer Limitation within Molecular Crowding Electrolyte Reorienting (100) and (101) Texture for Dendrite‐Free Zinc Metal Batteries

Aqueous zinc metal batteries are emerging as a promising alternative for energy storage due to their high safety and low cost. However, their development is hindered by the formation of Zn dendrites and side reactions. Herein, a macromolecular crowding electrolyte (MCE40) is prepared by incorporating polyvinylpyrrolidone (PVP) into the aqueous solutions, exhibiting an enlarged electrochemical stability window and anti‐freezing properties. Notably, through electrochemical measurements and characterizations, it is discovered that the mass transfer limitation near the electrode surface within the MCE40 electrolyte inhibits the (002) facets. This leads to the crystallographic reorientation of Zn deposition to expose the (100) and (101) textures, which undergo a “nucleation‐merge‐growth” process to form a uniform and compact Zn deposition. Consequently, the MCE40 enables highly reversible and stable Zn plating/stripping in Zn/Cu half cells over 600 cycles and in Zn/Zn symmetric cells for over 3000 hours at 1 mA cm−2. Furthermore, Na0.33V2O5/Zn and MnO2/Zn full cells display promising capacity and sustained stability over 500 cycles at room and sub‐zero temperatures. This study highlights a novel electrochemical mechanism for achieving preferential Zn deposition, introducing a unique strategy for fabricating dendrite‐free zinc metal batteries.

Mass Transfer Limitation within Molecular Crowding Electrolyte Reorienting (100) and (101) Texture for Dendrite-Free Zinc Metal Batteries.

Aqueous zinc metal batteries are emerging as a promising alternative for energy storage due to their high safety and low cost. However, their development is hindered by the formation of Zn dendrites and side reactions. Herein, a macromolecular crowding electrolyte (MCE40) is prepared by incorporating polyvinylpyrrolidone (PVP) into the aqueous solutions, exhibiting an enlarged electrochemical stability window and anti-freezing properties. Notably, through electrochemical measurements and characterizations, it is discovered that the mass transfer limitation near the electrode surface within the MCE40 electrolyte inhibits the (002) facets. This leads to the crystallographic reorientation of Zn deposition to expose the (100) and (101) textures, which undergo a "nucleation-merge-growth" process to form a uniform and compact Zn deposition. Consequently, the MCE40 enables highly reversible and stable Zn plating/stripping in Zn/Cu half cells over 600 cycles and in Zn/Zn symmetric cells for over 3000 hours at 1 mA cm-2. Furthermore, Na0.33V2O5/Zn and MnO2/Zn full cells display promising capacity and sustained stability over 500 cycles at room and sub-zero temperatures. This study highlights a novel electrochemical mechanism for achieving preferential Zn deposition, introducing a unique strategy for fabricating dendrite-free zinc metal batteries.

Synthetic Mn3Ce2O5-Cluster Mimicking the Oxygen-Evolving Center in Photosynthesis.

The photosynthetic oxygen-evolving center (OEC) is a unique Mn4CaO5-cluster that catalyzes water splitting into electrons, protons, and dioxygen. Precisely structural and functional mimicking of the OEC is a long-standing challenge and pressingly needed for understanding the structure-function relationship and catalytic mechanism of O-O bond formation. Herein we report two simple and robust artificial Mn3Ce2O5-complexes that display a remarkable structural similarity to the OEC in regarding of the ten-atom core (five metal ions and five oxygen bridges) and the alkyl carboxylate peripheral ligands. This Mn3Ce2O5-cluster can catalyze the water-splitting reaction on the surface of ITO electrode. These results clearly show that cerium can structurally and functionally replace both calcium and manganese in the cluster. Mass spectroscopic measurements demonstrate that the oxide bridges in the cluster are exchangeable and can be rapidly replaced by the isotopic oxygen of H218O in acetonitrile solution, which supports that the oxide bridge(s) may serve as the active site for the formation of O-O bond during the water-splitting reaction. These results would contribute to our understanding of the structure-reactivity relationship of both natural and artificial clusters and shed new light on the development of efficient water-splitting catalysts in artificial photosynthesis.

Utilization of Spontaneous Alkyne-Gold Self-Assembly Chemistry as an Alternative Method for Fabricating Electrochemical Aptamer-Based Sensors.

Electrochemical aptamer-based (E-AB) sensors are a promising class of biosensors which use structure-switching redox-labeled oligonucleotides (aptamers) codeposited with passivating alkanethiol monolayers on electrode surfaces to specifically bind and detect target analytes. Signaling in E-AB sensors is an outcome of aptamer conformational changes upon target binding, with the sequence of the aptamer imparting specificity toward the analyte of interest. The change in conformation translates to a change in electron transfer between the redox label attached to the aptamer and the underlying electrode and is related to analyte concentration, allowing specific electrochemical detection of nonelectroactive analytes. E-AB sensor measurements are reagentless with time resolutions of seconds or less and may be miniaturized into the submicron range. Traditionally these sensors are fabricated using thiol-on-gold chemistry. Here we present an alternate immobilization chemistry, gold-alkyne binding, which results in an increase in sensor lifetimes under ideal conditions by up to ∼100%. We find that gold-alkyne binding is spontaneous and supports efficient E-AB sensor signaling with analytical performance characteristics similar to those of thiol generated monolayers. The surface modification differs from gold-thiol binding only in the time and aptamer concentration required to achieve similar aptamer surface coverages. In addition, alkynated aptamers differ from their thiolated analogues only by their chemical handle for surface attachment, so any existing aptamers can be easily adapted to utilize this attachment strategy.

Understanding Performance Limitation of Liquid Alkaline Water Electrolyzers

Liquid alkaline water electrolyzers (LAWEs), being the most commercially mature electrolysis technology, play a pivotal role in large-scale hydrogen production. However, LAWEs suffer from low operational efficiency, primarily due to un-optimized electrode structure and chemical compositions. Thus, we investigated how various electrode configurations could impact LAWE performance. Our results show that Ni felt electrodes outperform the conventional Ni foam thanks to improved electrochemical active surface area (ECSA) and preferred electrode surface structure that minimizes the micro-gaps in between the electrode and separator. By comparing the stainless steel (SS) felt electrodes with Ni felt electrodes, SS not only shows better oxygen evolution reaction activity but also improved hydrogen evolution reaction activity, which is less studied in the literature. We also show that a bilayer structure with small pore radius facing the separator could further improve LAWE performance by further optimizing interfacial contact between electrode and separator. These findings enable LAWEs to sustain 2 A cm−2 at 2.2 V and operate steadily at 1 A cm−2 for nearly 600 h with negligible performance decay. Our studies establish criteria for selecting electrodes to achieve high-performance LAWE and, in turn, expedite the adoption of LAWEs in hydrogen production and the transition towards low-carbon economies.

A portable microfluidic electrochemical sensor with nonlinear fit strategy for wide-range uric acid detection

In this work, we have developed a portable electrochemical sensing device controlled by a smartphone through Bluetooth, which was applied for regular uric acid (UA) monitoring in prevention and healthcare management. On the core lies a nonlinear fitting model (I = k·(N − exp(−K·cbulk + b))) which is proposed for the first time and given from the differential equation based on the theoretical analysis. We believe this model can reflect the intrinsic relationship between the obtained current and the bulk analyte concentration, therefore leading to an expanding UA detection range (10-fold) compared to the widely used linear standard curve model and reducing the requirements for the modification of the electrode materials. Besides, the integration of the microfluidic chip promoted the removal of UA oxidation products at the electrode surface, yielding excellent sensing stability with a relative standard deviation (RSD) lower than 1 % during 10 consecutive runs. Consequently, we acquired the relationship between Square Wave Voltammetry (SWV) current and UA concentration (I = 15.27*(2.05 − exp(−0.00108*(cbulk − 663.5))), R2 = 0.9999) in the range of 5 to 1000 μM with a limit of detection (LoD) of 2.4 μM using a completely unmodified screen-printed carbon electrode (SPCE). Proof of concept experiments using 25× diluted human urine spiked with UA yielded a recovery rate of 87.5–101.4 % and a satisfactory selectivity result, which is within the value expected for clinical use, indicating the potential of the developed instrument and nonlinear fitting model for urinary UA detection.

Structure and properties of electrochemical interfaces with grafting polyelectrolyte: A fluid density functional theory study

The structure of the electrode/electrolyte interface directly determines electrochemical performance. One effective method for controlling this interface structure is by grafting polyelectrolyte onto the electrode surface, which can significantly alter the double layer structure and enhance electrochemical performance. This study focuses on the graft modification of polyelectrolytes at the electrochemical interface and investigates the impact of the length and density of the grafted polyelectrolyte chain on the structure and capacitance of the electrode/ionic liquid interface using fluid density functional theory (FDFT). The findings indicate that the grafted polymerbrush disrupts the alternating layer of anions and cations at the conventional interface and exerts an additional adsorption effect on counter ions, thereby reducing the density of freely movable co-ions. Consequently, this process increases the effective charge and capacitance of the interface. The results of this investigation contribute to a deeper comprehension of polyelectrolyte solutions at solid–liquid interfaces and guide the regulation of electrochemical interface properties.

Multiplexed electrochemical nucleic acid sensor based on visible light-mediated metal-free thiol-yne click reaction for simultaneous detection of different nucleic acid targets

Simultaneous detection of multiple tumor biomarkers with a simple and low-cost assay is crucial for early cancer detection and diagnosis. Herein, we presented a low-cost and simple assay for multiplexed detection of tumor biomarkers using a spatially separated electrodes strategy. The sensor is fabricated based on a metal-free thiol-yne click reaction, which is mediated by visible light, on commercially available indium tin oxide (ITO) electrodes. Four biomarkers, including p53 DNA, Brca2 DNA, K-ras DNA, and MicroRNA-204 RNA, were used as model analytes, and the corresponding oligonucleotide probes were modified on the desired electrode units sequentially with 530 nm irradiation light in the presence of photosensitizer Eosin Y. By this visible light-mediated coupling reaction, oligonucleotide probe densities of up to 9.2 ± 0.7 × 1010 molecules/cm2 were readily obtained on the ITO electrode surface. The proposed multiplexed E-NA sensor could detect four different nucleic acid targets concurrently without crosstalk among adjacent electrodes and was also successfully applied for detecting targets in a 20% fetal calf serum sample. The detection limits for p53 DNA, Brca2 DNA, K-ras DNA, and MicroRNA-204 RNA were 0.72 nM, 0.97 nM, 2.15 nM, and 1.73 nM, respectively. The developed approach not only has a great potential for developing cost-effective biosensors on affordable substrates for nucleic acid target detection, but also be easily extended to detect other targets by modifying the specific oligonucleotide probes anchored on the electrode.