In this paper, the characterization and application of a chemically reduced graphene oxide modified glassy carbon (CR-GO/GC) electrode, a novel electrode system, for the preparation of electrochemical sensing and biosensing platform are proposed. Different kinds of important inorganic and organic electroactive compounds (i.e., probe molecule (potassium ferricyanide), free bases of DNA (guanine (G), adenine (A), thymine (T), and cytosine (C)), oxidase/dehydrogenase-related molecules (hydrogen peroxide (H2O2)/beta-nicotinamide adenine dinucleotide (NADH)), neurotransmitters (dopamine (DA)), and other biological molecules (ascorbic acid (AA), uric acid (UA), and acetaminophen (APAP)) were employed to study their electrochemical responses at the CR-GO/GC electrode, which shows more favorable electron transfer kinetics than graphite modified glassy carbon (graphite/GC) and glassy carbon (GC) electrodes. The greatly enhanced electrochemical reactivity of the four free bases of DNA at the CR-GO/GC electrode compared with that at graphite/GC and GC electrodes makes the CR-GO/GC electrode a better choice for the electrochemical biosensing of four DNA bases in both the single-stranded DNA (ssDNA) and double-stranded DNA (dsDNA) at physiological pH without a prehydrolysis step. This allows us to detect a single-nucleotide polymorphism (SNP) site for short oligomers with a particular sequence at the CR-GO/GC electrode without any hybridization or labeling processes in this work, suggesting the potential applications of CR-GO in the label-free electrochemical detection of DNA hybridization or DNA damage for further research. Based on the greatly enhanced electrochemical reactivity of H2O2 and NADH at the CR-GO/GC electrode, CR-GO/GC electrode-based bioelectrodes (in connection with glucose oxidase (GOD) and alcohol dehydrogenase (ADH)) show a better analytical performance for the detection of glucose and ethanol compared with graphite/GC- or GC-based bioelectrodes. By comparing the electrochemical performance of CR-GO with that of the conventional graphite and GC, we reveal that CR-GO with the nature of a single sheet showing favorable electrochemical activity should be a kind of more robust and advanced carbon electrode material which may hold great promise for electrochemical sensors and biosensors design.

Have you seen the film? Coupling a spray‐coating technique with a facile, low‐cost, efficient and environmentally friendly electrochemical method may realize the controllable synthesis of large‐area and patterned electrochemically reduced graphene oxide films on various conductive and insulating substrates with thicknesses ranging from a single monolayer to several microns (see figure).

One of the critical issues in the industrial development of fuel cells (e.g., proton exchange membrane fuel cells, direct methanol fuel cells and biofuel cells) is the high cost, serious intermediate tolerance, anode crossover, sluggish kinetics, and poor stability of the platinum (Pt) as the preferred electrocatalysts for the oxygen reduction reaction (ORR) at the cathode. The development of novel noble-metal-free electrocatalysts with low cost, high activity and practical durability for ORR has been considered as one of the most active and competitive fields in chemistry and materials science. In this critical review, we will summarize recent advances on engineering advanced carbon nanomaterials with different dimensions for the rational design and synthesis of noble-metal-free oxygen reduction electrocatalysts including heteroatom-doped carbon nanomaterials, transition metal-based nanoparticle (NP)-carbon nanomaterial composites and especially the stable iron carbide (Fe3C)-based NP-carbon nanomaterial composites. Introducing advanced carbon nanomaterials with high specific surface area and stable structure into the noble-metal-free ORR field has not only led to a maximized electrocatalyst surface area for the electron transfer but also resulted in enhanced electrocatalyst stability for long-term operation. Therefore, the rational design and synthesis of noble-metal-free electrocatalysts based on heteroatoms, transition metal-based NPs and Fe3C-based NP functionalized carbon nanomaterials are of special relevance for their ORR applications, and represents a rapidly growing branch of research. The demonstrated examples in this review will open new directions on designing and optimizing advanced carbon nanomaterials for the development of extremely active and durable earth-abundant cathodic catalysts for fuel cell applications.

In this paper, the electrochemical behavior of L-cysteine (CySH) was investigated thoroughly at an ordered mesoporous carbon-modified glassy carbon (OMC/GC) electrode. The voltammetric studies showed there were three anodic peaks for the electrooxidation of CySH in the pH range of 2.00-5.00; however, one peak disappeared above pH 5.00. This behavior has never been reported before. Through the studies of the effect of pH on the distribution fractions (delta) of the four chemical species of CySH, we conclude only CySH2+ (H3A+) and CyS- (HA-) are the electroactive substances and should be responsible for the electrooxidation of CySH. And for the first time, we successfully established the exact and systemic mechanisms based on the electroactive species to explain CySH oxidation at different pH values. On the other hand, a sensitive CySH sensor was developed based on an OMC/GC electrode, which shows a large determination range (18-2500 micromol L(-1)), a high sensitivity (23.6 microA mmol L(-1)), and a remarkably low detection limit (2.0 nmol L(-1), which is the lowest value ever reported for direct CySH determination on the electrodes) at pH 2.00. At pH 7.00, the modified electrode can be still used to readily detect CySH in the range of the physiological levels. These make OMC/GC electrode a promising candidate for efficient electrochemical sensors for the detection of CySH.

Over the past decade, researchers have devoted considerable attention to the integration of living organisms with electronic elements to yield bioelectronic devices. Not only is the integration of DNA, enzymes, or whole cells with electronics of scientific interest, but it has many versatile potential applications. Researchers are using these ideas to fabricate biosensors for analytical applications and to assemble biofuel cells (BFCs) and biomolecule-based devices. Other research efforts include the development of biocomputing systems for information processing. In this Account, we focus on our recent progress in engineering at the bioelectrochemical interface (BECI) for the rational design and construction of important bioelectronic devices, ranging from electrochemical (EC-) biosensors to BFCs, and self-powered logic biosensors. Hydrogels and sol-gels provide attractive materials for the immobilization of enzymes because they make EC-enzyme biosensors stable and even functional in extreme environments. We use a layer-by-layer (LBL) self-assembly technique to fabricate multicomponent thin films on the BECI at the nanometer scale. Additionally, we demonstrate how carbon nanomaterials have paved the way for new and improved EC-enzyme biosensors. In addition to the widely reported BECI-based electrochemical impedance spectroscopy (EIS)-type aptasensors, we integrate the LBL technique with our previously developed "solid-state probe" technique for redox probes immobilization on electrode surfaces to design and fabricate BECI-based differential pulse voltammetry (DPV)-type aptasensors. BFCs can directly harvest energy from ambient biofuels as green energy sources, which could lead to their application as simple, flexible, and portable power sources. Porous materials provide favorable microenvironments for enzyme immobilization, which can enhance BFC power output. Furthermore, by introducing aptamer-based logic systems to BFCs, such systems could be applied as self-powered and intelligent aptasensors for the logic detection. We have developed biocomputing keypad lock security systems which can be also used for intelligent medical diagnostics. BECI engineering provides a simple but effective approach toward the design and fabrication of EC-biosensors, BFCs, and self-powered logic biosensors, which will make essential contributions in the development of creative and practical bioelectronic devices. The exploration of novel interface engineering applications and the creation of new fabrication concepts or methods merit further attention.

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This article reviews recent advances and progress in developing electrochemical (EC) biosensing and logic biosensing systems based on self-powered biofuel cells (BFCs). BFCs that exploit enzymes and microbes have attracted a considerable recent interest owing to their unique ability to provide sustainable energy from renewable fuel source under mild conditions. This review focuses on recently introduced novel concepts for using BFCs as the basic element for EC-biosensing and especially EC-logic biosensing applications. The fabrication and design of such selfpowered EC-biosensing and EC-logic biosensing are described along and different new approaches for BFCs-based EC-biosensing and EC-logic biosensing involving substrate effects, inhibition effects, blocking effects and gene regulation effects. Latest advances in coupling a self-powered diagnostic operation with logic-activated drug release functionality are discussed. We conclude with the implications of the new self-powered biosensing/logic-biosensing platforms along with future prospects and challenges.

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