Reviewing the use of chitosan and polydopamine for electrochemical sensing

Biopolymers possess highly favorable properties for electrochemical biosensing such as their inherent biocompatibility, inexpensive nature, and strong interfacial adhesion. In this mini-review, we will focus on chitosan and polydopamine, two of the most commonly used biopolymers, for electrochemical sensing applications. Chitosan is a polysaccharide that exhibits high chemical resistance, offers straightforward modification and cross-linking, and possesses antibacterial properties and mucoadhesion. Polydopamine has the benefit of universal adhesion, in addition to the ability to form self-assembled structures. We will demonstrate how the unique structural and electrochemical features of these biopolymers can be used in a range of electrochemical biosensing platforms.     

基于金属纳米簇的荧光传感平台的最新研究进展

荧光纳米生物传感平台由于具有灵敏度高、选择性好、操作简单、成本低、实时监测等特点,吸引了广泛的关注。近年来,随着纳米技术的飞速发展,具有纳米结构的材料(纳米材料)在生物传感领域显示出独特的优势。与传统材料相比,纳米材料显示出独特的物化性质,如光学、电学、机械、催化和磁性等。金属(如Au、Ag、Cu及其合金)纳米簇(MNCs)是纳米科学和纳米技术领域中一种新颖的多功能纳米材料,其通常由几个到几十个金属原子组成,其核的尺寸通常小于2 nm。由于其发光能力强、易于合成和进行表面功能化、生物相容性好、尺寸超小、毒性低等优点,金属纳米簇在能源催化、医学诊断、电子器件、生物传感等领域得到了广泛的应用。此外,金属纳米簇的荧光性能极佳(如大的斯托克斯位移、可调节的荧光、高的光学稳定性和荧光量子产率等),因此被作为荧光纳米探针广泛应用于生物传感领域。该综述介绍了近年来基于不同构建机制的金属纳米簇基的传感平台的研究进展,及其在检测离子、生物分子、pH和温度传感等方面的应用。相信该综述能为从不同传感机理构建更具前景的生物传感器提供一些新见解和理论指导。     

Interferences from oxygen reduction reactions in bioelectroanalytical measurements: the case study of nitrate and nitrite biosensors

Bioelectroanalytical procedures based on cathodic processes are often subject to interference from dissolved oxygen. At the potentials applied for analyte detection, oxygen reduction may occur directly at the electrode or may be catalyzed by the electron mediators or the sensing enzyme of the biosensor. These processes affect the background current and may thus result in erroneous analyte quantification. In this review, current strategies to circumvent these oxygen interferences are presented and critically assessed with respect to their compatibility for on-site monitoring with amperometric biosensing devices operating at low potential. The main strategies consist in (1) use of oxygen scavenging systems to remove dissolved oxygen from the sample, (2) design of bioelectroanalytical approaches to shift the applied potential for analyte detection to more positive values, and (3) development of electrode materials to increase the overpotential for the oxygen reduction reaction. The latest developments in these approaches have recently led to the first biosensing devices based on reductases fully compatible with on-site monitoring requirements and this opens up possibilities for their widespread application.     

微生物燃料电池影响因素及作用机理探讨

以生活污水为初始接种体, 以醋酸钠水溶液为原料, 构建了一个无媒介体、无膜的单室微生物燃料电池, 考察了溶液的浓度、外电阻、温度和氧气的加入等因素对电池性能的影响, 监测了电池外电压和两极电极电势的变化过程, 分析了微生物燃料电池的运行机理. 研究结果表明: (1) 阳极吸附的微生物的活性是影响电池输出电压(输出功率)的关键因素. 营养液初始浓度越高, 微生物活性越高, 输出最大电压越高, 输出电压与浓度之间的关系符合MONOD方程; 溶液中溶氧的存在使微生物活性明显降低, 但溶氧浓度降低到一定程度后, 活性逐步恢复; 随着电池温度的升高, 微生物活性快速上升, 但温度突变到50 ℃后, 微生物活性明显降低; (2) 电池换水后, 由微生物活性所决定的阳极电势迅速达到平衡, 而阴极电势需要较长的时间才能达到极大值; (3) 随电流密度的变化, 两极电极电势相应发生变化, 其变化趋势符合原电池的基本规律; (4) 随外电阻的变化, 电池输出功率出现极大值, 即当外电阻为200 Ω时, 电池输出功率达到346 mW/m2.     

Detection of DNA hybridization on chemically modified graphene platforms

The increasing demand for simple, low-cost, rapid, sensitive and label-free methods for the detection of DNA sequences and the presence of single nucleotide polymorphisms (SNPs) has become an important issue in biomedical research. In this work, we studied the performances of several chemically modified graphene nanomaterials as sensing platforms by using the electrochemical impedance spectroscopy technique for the detection. We employed a hairpin DNA as a highly selective probe for the detection of SNP correlated to Alzheimer's disease. We believe that our findings may present a foundation for further research and development in graphene-based impedimetric biosensing.     

Nanomaterials Facilitating Conversion Efficiency Strategies for Microbial CO2 Reduction

Microbial electro- and photoelectrochemical CO₂ reduction represents an opportunity to tackle the environmental demand for sustainable fuel production. Nanomaterials critically impact the electricity- and solar-driven microbial CO₂ reduction processes. This minireview comprehensively summarizes the recent developments in the configuration and design of nanomaterials for enhancement of the bacterial adhesion and extracellular electron transfer (EET) processes, based on the modification technologies of improving chemical stability, electrochemical conductivity, biocompatibility, and surface area. Furthermore, the investigation of incorporating non-photosynthetic microorganisms using advanced light-harvesting nanostructured photoelectrodes for solar-to-chemical conversion, as well as the current understanding of EET mechanisms occurring at photosynthetic semiconductor nanomaterials-bacteria biohybrid interface is detailed. The crucial factors influencing the performance of microbial CO₂ reduction systems and future perspectives are discussed to provide guidance for the realization of their large-scale application.     

Preparation of Trace Fe2P Modified N,P Co-doped Carbon Materials and their Application to Hydrogen Peroxide Detection

The determination of hydrogen peroxide (H₂O₂) based on electrochemical sensors is highly attractive in the fields of environmental monitoring and biosensing, however development of non-precious metal-based electrocatalysts with high performances remains challenging. Here, a new non-enzymatic H₂O₂ sensor has been reported by using Fe₂P modified N,P co-doped carbon (Fe₂P/NP-C) materials as sensing materials. Fe₂P/NP-C materials were synthesized by pyrolysis of polydopamine coating Fe-based coordination polymer nanoparticles, which were obtained by direct mixing FeCl₃ and sodium hexametaphosphate at room temperature. The electrochemical tests display that Fe₂P/NP-C-based non-enzymatic H₂O₂ sensor exhibited detection limit of 60 μM and linear range from 0.1 mM to 1 mM, respectively. This work presents a new avenue to design of non-precious metal-based electrocatalysts for chemical sensing and biosensing applications.     

Recent Progress on the Development of Biofuel Cells for Self‐Powered Electrochemical Biosensing and Logic Biosensing: A Review

Biofuel cells (BFCs) based on enzymes and microorganisms have been recently received considerable attention because they are recognized as an attractive type of energy conversion technology. In addition to the research activities related to the application of BFCs as power source, we have witnessed recently a growing interest in using BFCs for self‐powered electrochemical biosensing and electrochemical logic biosensing applications. Compared with traditional biosensors, one of the most significant advantages of the BFCs‐based self‐powered electrochemical biosensors and logic biosensors is their ability to detect targets integrated with chemical‐to‐electrochemical energy transformation, thus obviating the requirement of external power sources. Following my previous review (Electroanalysis­ 2012 , 24, 197–209), the present review summarizes, discusses and updates the most recent progress and latest advances on the design and construction of BFCs‐based self‐powered electrochemical biosensors and logic biosensors. In addition to the traditional approaches based on substrate effect, inhibition effect, blocking effect and gene regulation effect for BFCs‐based self‐powered electrochemical biosensors and logic biosensors design, some new principles including enzyme effect, co‐stabilization effect, competition effect and hybrid effect are summarized and discussed by me in details. The outlook and recommendation of future directions of BFCs‐based self‐powered electrochemical biosensors and logic biosensors are discussed in the end.     

Optimization of double chamber microbial fuel cell for domestic wastewater treatment and electricity production

Microbial fuel cells (MFCs) represent a new approach for treating waste water along with electricity production. The present study addressed electricity production from domestic wastewater using a mediator-less double chamber MFC. The electricity production was monitored under different operational conditions for both summer and winter samples. Optimization of the anodic and cathodic chambers resulted in a maximal current of 0.784 and 0.645 mA with the maximal power intensity of 209 and 117 mW/m² in power duration of 24 h for the summer and winter samples, respectively. Scanning electron microscopy showed that the bacterial biofilm formation on the anode was denser for the summer sample than that when the winter sample was used, so was the total bacterial count. Therefore, samples taken during summer were considered better in electricity production and waste water treatment than those taken during winter basically because of the high microbial load during the hot season. In parallel, there was a decrease in both biological oxygen demand (BOD₅) and chemical oxygen demand (COD) values which reached 71.8% and 72.85%, respectively at the end of the operation process for the summer sample, while there was no evident decrease for the winter sample. Optimizing the operating conditions not only increased the potential of using domestic waste water in microbial fuel cells to produce electricity, but also improved the quality of the domestic waste water.     

Earth-Abundant Transition-Metal-Based Bifunctional Electrocatalysts for Overall Water Splitting in Alkaline Media

The depletion of fossil fuels has accelerated the search for clean, sustainable, scalable, and environmentally friendly alternative energy sources. Hydrogen is a potential energy carrier because of its advantageous properties, and the electrolysis of water is considered as an efficient method for its industrial production. However, the high-energy conversion efficiency of electrochemical water splitting requires cost-effective and highly active electrocatalysts. Therefore, researchers have aimed to develop high-performance electrode materials based on non-precious and abundant transition metals for conversion devices. Moreover, to further reduce the cost and complexity in real-world applications, bifunctional catalysts that can be simultaneously active on both the anodic (i.e., oxygen evolution reaction, OER) and cathodic (i.e., hydrogen evolution reaction, HER) sides are economically and technically desirable. This Minireview focuses on the recent progress in transition-metal-based materials as bifunctional electrocatalysts, including several promising strategies to promote electrocatalytic activities for overall water splitting in alkaline media, such as chemical doping, defect (vacancy) engineering, phase engineering, facet engineering, and structure engineering. Finally, the potential for further developments in rational electrode materials design is also discussed.     

微生物燃料电池在传感分析中的应用及研究进展

微生物燃料电池(Microbial fuel cell,MFC)是一种利用微生物将化学能直接转化为电能的装置.近年来,除改善微生物燃料电池的输出性能外,研究者也不断开发其在传感分析中的应用.基于微生物燃料电池的传感分析装置无需外加电源,具有操作简单、可连续检测等优点,是一种极具应用前景的传感分析技术.本文依据这些传感分析装置的用途进行分类,主要综述了微生物燃料电池在检测分析生化需氧量(BOD)、挥发性脂肪酸、毒性物质、微生物活性和数量以及其它方面的研究,并对其发展趋势和应用前景进行了展望.     

Electrochemical biosensors based on Ti3C2Tx MXene: future perspectives for on-site analysis

MXenes are recently developed two-dimensional layered materials composed of early transition metal carbides and/or nitrides that provide unique characteristics for biosensor applications. This review presents the recent progress made on the usage and applications of MXenes in the field of electrochemical biosensors, including microfluidic biosensors and wearable microfluidic biosensors, and highlights the challenges with possible solutions and future needs. The multilayered configuration and high conductivity make these materials as an immobilization matrix for the biomolecule immobilization with activity retention and to be explored in the fabrication of electrochemical sensors, respectively. First, how the MXene nanocomposite as an electrode modifier affects the sensing performance of the electrochemical biosensors based on enzymes, aptamer/DNA, and immunoassays is well described. Second, recent developments in MXene nanocomposites as wearable biosensing platforms for the biomolecule detection are highlighted. This review pointed out the future concerns and directions for the use of MXene nanocomposites to fabricate advanced electrochemical biosensors with high sensitivity and selectivity. Specifically, possibilities for developing microfluidic electrochemical sensors and wearable electrochemical microfluidic sensors with integrated biomolecule detection are emphasized.     

Linking glucose oxidation to luminol-based electrochemiluminescence using bipolar electrochemistry

The range of potential analytes for bipolar electrochemistry can be significantly extended by modification of bipolar electrodes with enzymatic biosensing layers. In this study, we employed a Prussian blue-based glucose detection system involving electrochemical reduction of enzymatically generated hydrogen peroxide at the cathodic pole. The concentration of glucose in solution can be correlated with oxidative luminol electrochemiluminescence at the opposite anodic pole, which was recorded with a photomultiplier tube. This opens a route for novel analytical systems using glucose oxidase as an amplification element for the reporter reaction.     

Printing polyaniline for sensor applications

In recent years, much research has focused on the development of low-cost, printed electrochemical sensor platforms for environmental monitoring and clinical diagnostics. Much effort in this area has been based on utilising the redox properties of conducting polymers, particularly polyaniline (PANI). In tackling the inherent lack of processability exhibited by these materials, several groups have examined various mass-amenable fabrication approaches to obtain suitable thin films of PANI for sensing applications. Specifically, the approaches investigated over the years include the in situ chemical synthesis of PANI, the use of sulphonated derivatives of PANI and the synthesis of aqueousbased nano-dispersions of PANI. Nano-dispersions have shown a great deal of promise for sensing applications, given that they are inkjet-printable, facilitating the patterning of conducting polymer directly to the substrate. We have shown that inkjet-printed films of PANI can be finely controlled in terms of their two-dimensional pattern, thickness, and conductivity, highlighting the level of precision achievable by inkjet printing. Utilising these nanomaterials as inkjet-printable inks opens novel, facile, and economical possibilities for conducting polymer-printed electronic applications in areas of sensing, but also many other application areas such as energy storage, displays, organic light-emitting diodes. Given that inkjet-printing is a scalable manufacturing technique, it renders possible the large-scale production of devices such as sensors for a range of applications. Several successes have emerged from our work and from the work of others in the area of applying PANI in low-cost sensor applications, which is the focus of this review.     

Microneedles-based electrochemical sensors: New tools for advanced biosensing

Electrochemical biosensors are used worldwide as analytical tools from laboratory applications to market products. The performance of electrochemical sensing can be boosted by adopting the microneedle (MN) geometry as an innovative configuration of standard electrodes. MNs can be miniaturized, easily functionalized, and properly designed for specific aim monitoring, but most of all, they allow a low invasive controlling tool for growth and for environment influence in plant and a painless door to human body fluids where target analytes can be detected, overcoming the natural barrier of the skin. In this review, the very recent developments in MN-based electrochemical biosensing published in the literature are summarized.     

显影抑制机理─—电化学探讨

显影抑制一直是人们感兴趣的问题,它不仅对降低显影灰雾,而且对获得高反差也有一定的作用.     

Electrochemical approach for monitoring the effect of anti tubulin drugs on breast cancer cells based on silicon nanograss electrodes

One of the most interested molecular research in the field of cancer detection is the mechanism of drug effect on cancer cells. Translating molecular evidence into electrochemical profiles would open new opportunities in cancer research. In this manner, applying nanostructures with anomalous physical and chemical properties as well as biocompatibility would be a suitable choice for the cell based electrochemical sensing. Silicon based nanostructure are the most interested nanomaterials used in electrochemical biosensors because of their compatibility with electronic fabrication process and well engineering in size and electrical properties. Here we apply silicon nanograss (SiNG) probing electrodes produced by reactive ion etching (RIE) on silicon wafer to electrochemically diagnose the effect of anticancer drugs on breast tumor cells. Paclitaxel (PTX) and mebendazole (MBZ) drugs have been used as polymerizing and depolymerizing agents of microtubules. PTX would perturb the anodic/cathodic responses of the cell-covered biosensor by binding phosphate groups to deformed proteins due to extracellular signal-regulated kinase (ERK^1/2) pathway. MBZ induces accumulation of Cytochrome C in cytoplasm. Reduction of the mentioned agents in cytosol would change the ionic state of the cells monitored by silicon nanograss working electrodes (SiNGWEs). By extending the contacts with cancer cells, SiNGWEs can detect minor signal transduction and bio recognition events, resulting in precise biosensing. Effects of MBZ and PTX drugs, (with the concentrations of 2 nM and 0.1 nM, respectively) on electrochemical activity of MCF-7 cells are successfully recorded which are corroborated by confocal and flow cytometry assays.     

2D Material Chemistry: Graphdiyne-based Biochemical Sensing

The modern internet-of-things era has witnessed an increasing growth in the demand for advanced sensors to collect precise information. To meet this demand, extensive efforts have been devoted to exploring competent materials and designing rational architectures for the fabrication of sensing devices. Graphdiyne represents a promising material due to the attractive electronic, optical and electrochemical properties deriving from its unique molecular structure. In this review, we firstly provide the points of view on the architectures and work principles of the graphdiyne-based sensing devices with respect to resistive, electrochemical, photoelectrochemical and fluorescent categories. Secondly, we present the promising applications on biochemical sensing, such as the detection of DNA, microRNA, and glucose. Finally, the challenges and prospects of graphdiyne-based biochemical sensing platforms are also discussed, in order to provide a cornerstone for understanding this rapidly developing area.     

Oxygen reduction kinetics on graphite cathodes in sediment microbial fuel cells

Sediment microbial fuel cells (SMFCs) have been used as renewable power sources for sensors in fresh and ocean waters. Organic compounds at the anode drive anodic reactions, while oxygen drives cathodic reactions. An understanding of oxygen reduction kinetics and the factors that determine graphite cathode performance is needed to predict cathodic current and potential losses, and eventually to estimate the power production of SMFCs. Our goals were to (1) experimentally quantify the dependence of oxygen reduction kinetics on temperature, electrode potential, and dissolved oxygen concentration for the graphite cathodes of SMFCs and (2) develop a mechanistic model. To accomplish this, we monitored current on polarized cathodes in river and ocean SMFCs. We found that (1) after oxygen reduction is initiated, the current density is linearly dependent on polarization potential for both SMFC types; (2) current density magnitude increases linearly with temperature in river SMFCs but remains constant with temperature in ocean SMFCs; (3) the standard heterogeneous rate constant controls the current density temperature dependence; (4) river and ocean SMFC graphite cathodes have large potential losses, estimated by the model to be 470 mV and 614 mV, respectively; and (5) the electrochemical potential available at the cathode is the primary factor controlling reduction kinetic rates. The mechanistic model based on thermodynamic and electrochemical principles successfully fit and predicted the data. The data, experimental system, and model can be used in future studies to guide SMFC design and deployment, assess SMFC current production, test cathode material performance, and predict cathode contamination.     

Combining metal-microbe and microbe-microbe dual direct electron transfer on Fe(0)-cathode of bio-electrochemical system to enhance anaerobic digestion of cellulose wastewater

Considering that cathode of microbial electrochemical system (MES) is a good electrons source for methane production via direct/indirect electron transfer to electroactive microorganisms, and that Fe(0) is also a confirmed electron donor for some electroactive microorganisms through metal-microbe direct electron transfer (DET), Fe(0)-cathode was equipped into an MES digester to enhance cathodic methane production. The results of this study indicated that the potential DET participator, Clostridium possibly obtained electrons directly from Fe(0)-cathode via metal-microbe electrons transfer, then transferred electrons directly to the definite DET participators, Methanosarcina/Methanothrix via microbe-microbe electrons transfer for CH₄ production. In addition, Methanobacterium is another specially enriched methanogen on Fe(0)-cathode, which might obtain electrons directly from Fe(0)-cathode to produce CH₄ via metal/electrode-microbe DET. The increment of conductivity of cathodic sludge in Fe(0)-cathode MES digester (R1) further confirmed the enrichment of electroactive microorganisms participating in DET process. As a consequence, a higher CH₄ production (1205–1508 mL/d) and chemical oxygen demand (COD) removal (79.0%-93.8%) were achieved in R1 compared with graphite-cathode MES digester (R2, 720–1090 mL/d and 63.6%-85.6%) and the conventional anaerobic digester (R3, 384–428 mL/d and 35.2%-41.0%). In addition, energy efficiency calculated indicated that the output energy of CH₄ production was 8.16 folds of electricity input in Fe(0)-cathode MES digester.