Dipstick and lateral-flow formats have dominated rapid diagnostics over the last three decades. These formats gained popularity in the consumer markets due to their compactness, portability and facile interpretation without external instrumentation. However, lack of quantitation in measurements has challenged the demand of existing assay formats in consumer markets. Recently, paper-based microfluidics has emerged as a multiplexable point-of-care platform which might transcend the capabilities of existing assays in resource-limited settings. However, paper-based microfluidics can enable fluid handling and quantitative analysis for potential applications in healthcare, veterinary medicine, environmental monitoring and food safety. Currently, in its early development stages, paper-based microfluidics is considered a low-cost, lightweight, and disposable technology. The aim of this review is to discuss: (1) fabrication of paper-based microfluidic devices, (2) functionalisation of microfluidic components to increase the capabilities and the performance, (3) introduction of existing detection techniques to the paper platform and (4) exploration of extracting quantitative readouts via handheld devices and camera phones. Additionally, this review includes challenges to scaling up, commercialisation and regulatory issues. The factors which limit paper-based microfluidic devices to become real world products and future directions are also identified.

Paper-based microfluidic point-of-care diagnostic devices

Supercapacitors are electrochemical energy storage devices that operate on the simple mechanism of adsorption of ions from an electrolyte on a high-surface-area electrode. Over the past decade, the performance of supercapacitors has greatly improved, as electrode materials have been tuned at the nanoscale and electrolytes have gained an active role, enabling more efficient storage mechanisms. In porous carbon materials with subnanometre pores, the desolvation of the ions leads to surprisingly high capacitances. Oxide materials store charge by surface redox reactions, leading to the pseudocapacitive effect. Understanding the physical mechanisms underlying charge storage in these materials is important for further development of supercapacitors. Here we review recent progress, from both in situ experiments and advanced simulation techniques, in understanding the charge storage mechanism in carbon- and oxide-based supercapacitors. We also discuss the challenges that still need to be addressed for building better supercapacitors.

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Efficient storage mechanisms for building better supercapacitors

The utility of metal–organic frameworks (MOFs) as functional materials in electronic devices has been limited to date by a lack of MOFs that display high electrical conductivity. Here, we report the synthesis of a new electrically conductive 2D MOF, Cu3(HITP)2 (HITP=2,3,6,7,10,11-hexaiminotriphenylene), which displays a bulk conductivity of 0.2 S cm−1 (pellet, two-point-probe). Devices synthesized by simple drop casting of Cu3(HITP)2 dispersions function as reversible chemiresistive sensors, capable of detecting sub-ppm levels of ammonia vapor. Comparison with the isostructural 2D MOF Ni3(HITP)2 shows that the copper sites are critical for ammonia sensing, indicating that rational design/synthesis can be used to tune the functional properties of conductive MOFs.

Cu3(hexaiminotriphenylene)2: An Electrically Conductive 2D Metal–Organic Framework for Chemiresistive Sensing

Carbon nanotubes (CNTs) promise to advance a number of real-world technologies. Of these applications, they are particularly attractive for uses in chemical sensors for environmental and health monitoring. However, chemical sensors based on CNTs are often lacking in selectivity, and the elucidation of their sensing mechanisms remains challenging. This review is a comprehensive description of the parameters that give rise to the sensing capabilities of CNT-based sensors and the application of CNT-based devices in chemical sensing. This review begins with the discussion of the sensing mechanisms in CNT-based devices, the chemical methods of CNT functionalization, architectures of sensors, performance parameters, and theoretical models used to describe CNT sensors. It then discusses the expansive applications of CNT-based sensors to multiple areas including environmental monitoring, food and agriculture applications, biological sensors, and national security. The discussion of each analyte focuses on the strategies used to impart selectivity and the molecular interactions between the selector and the analyte. Finally, the review concludes with a brief outlook over future developments in the field of chemical sensors and their prospects for commercialization.

Carbon Nanotube Chemical Sensors

A comprehensive review on the development and state of the art of colorimetric and fluorometric sensor arrays is presented Chemical sensing aims to detect subtle changes in the chemical environment by transforming relevant chemical or physical properties of molecular or ionic species (ie, analytes) into an analytically useful output Optical arrays based on chemoresponsive colorants (dyes and nanoporous pigments) probe the chemical reactivity of analytes, rather than their physical properties (eg, mass) The chemical specificity of the olfactory system does not come from specific receptors for specific analytes (eg, the traditional lock-and-key model of substrate-enzyme interactions), but rather olfaction makes use of pattern recognition of the combined response of several hundred olfactory receptors In a similar fashion, arrays of chemoresponsive colorants provide high-dimensional data from the color or fluorescence changes of the dyes in these arrays as they are exposed to analytes This provides chemical sensing with high sensitivity (often down to parts per billion levels), impressive discrimination among very similar analytes, and exquisite fingerprinting of extremely similar mixtures over a wide range of analyte types, in both the gas and liquid phases Design of both sensor arrays and instrumentation for their analysis are discussed In addition, the various chemometric and statistical analyses of high-dimensional data (including hierarchical cluster analysis (HCA), principal component analysis (PCA), linear discriminant analysis (LDA), support vector machines (SVMs), and artificial neural networks (ANNs)) are presented and critiqued in reference to their use in chemical sensing A variety of applications are also discussed, including personal dosimetry of toxic industrial chemical, detection of explosives or accelerants, quality control of foods and beverages, biosensing intracellularly, identification of bacteria and fungi, and detection of cancer and disease biomarkers

The Optoelectronic Nose: Colorimetric and Fluorometric Sensor Arrays.

Chemiresistive sensors are becoming increasingly important as they offer an inexpensive option to conventional analytical instrumentation, they can be readily integrated into electronic devices, and they have low power requirements. Nanowires (NWs) are a major theme in chemosensor development. High surface area, interwire junctions, and restricted conduction pathways give intrinsically high sensitivity and new mechanisms to transduce the binding or action of analytes. This Review details the status of NW chemosensors with selected examples from the literature. We begin by proposing a principle for understanding electrical transport and transduction mechanisms in NW sensors. Next, we offer the reader a review of device performance parameters. Then, we consider the different NW types followed by a summary of NW assembly and different device platform architectures. Subsequently, we discuss NW functionalization strategies. Finally, we propose future developments in NW sensing to address selectivity, sensor drift, sensitivity, response analysis, and emerging applications.

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Nanowire Chemical/Biological Sensors: Status and a Roadmap for the Future.

This communication describes a simple solvent-free method for fabricating chemoresistive gas sensors on the surface of paper. The method involves mechanical abrasion of compressed powders of sensing materials on the fibers of cellulose. We illustrate this approach by depositing conductive layers of several forms of carbon (e.g., single-walled carbon nanotubes [SWCNTs], multi-walled carbon nanotubes, and graphite) on the surface of different papers (Figure 1, Figure S1). The resulting sensors based on SWCNTs are capable of detecting NH3 gas at concentrations as low as 0.5 part-per-million.

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Mechanical Drawing of Gas Sensors on Paper

Chemically functionalized carbon nanotubes (CNTs) are promising materials for sensing of gases and volatile organic compounds. However, the poor solubility of carbon nanotubes hinders their chemical functionalization and the subsequent integration of these materials into devices. This manuscript describes a solvent-free procedure for rapid prototyping of selective chemiresistors from CNTs and graphite on the surface of paper. This procedure enables fabrication of functional gas sensors from commercially available starting materials in less than 15 min. The first step of this procedure involves the generation of solid composites of CNTs or graphite with small molecule selectors—designed to interact with specific classes of gaseous analytes—by solvent-free mechanical mixing in a ball mill and subsequent compression. The second step involves deposition of chemiresistive sensors by mechanical abrasion of these solid composites onto the surface of paper. Parallel fabrication of multiple chemiresistors from diverse composites rapidly generates cross-reactive arrays capable of sensing and differentiating gases and volatile organic compounds at part-per-million and part-per-thousand concentrations.

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Rapid prototyping of carbon-based chemiresistive gas sensors on paper

The threat of chemical warfare agents (CWAs) necessitates the development of functional materials that not only quickly detect the presence of CWAs but also actively protect against their toxicity. We have synthesized responsive units that exhibit colorimetric responses upon exposure to CWAs and incorporated them into a versatile detection platform based on copolymers prepared by ring-opening metathesis polymerization (ROMP). The theoretical detection limits for CWA simulants in solution for these polymers are as low as 1 ppm. By incorporating hydrogel-promoting units as pendant chains, we are able to obtain polymers that instantly respond to CWA vapors and are easy to regenerate to the deactivated state by simple treatment with ammonium hydroxide vapor. We further demonstrate a collapse of the polymer gels in response to trifluoroacetic acid (TFA), a strong acid that produces a more fully ionized state as a result of its more caustic nature.

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Colorimetric Stimuli-Responsive Hydrogel Polymers for the Detection of Nerve Agent Surrogates

We report the synthesis of dithienobenzotropone-based conjugated alternating copolymers by direct arylation polycondensation. Postpolymerization modification by hydride reduction yields cross-conjugated, reactive hydroxyl-containing copolymers that undergo phosphorylation and ionization upon exposure to the chemical warfare agent mimic diethylchlorophosphate (DCP). The resulting conjugated, cationic copolymer is highly colored and facilitates the spectroscopic and colorimetric detection of DCP in both solution and thin-film measurements.

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Jonathan G. Weis

Papers

Nanowire Chemical/Biological Sensors: Status and a Roadmap for the Future.

Mechanical Drawing of Gas Sensors on Paper

Rapid prototyping of carbon-based chemiresistive gas sensors on paper

Colorimetric Stimuli-Responsive Hydrogel Polymers for the Detection of Nerve Agent Surrogates

Thiophene-Fused Tropones as Chemical Warfare Agent-Responsive Building Blocks