纸基过氯乙烯树脂微流控亚硝酸根离子检测片的研制

基于滤纸上过氯乙烯树脂栏选择性通过亚硝酸根离子, 结合微流控分析装置设计, 研制成纸基过氯乙烯树脂微流控亚硝酸根离子检测芯片. 采用该微流控亚硝酸根离子检测芯片测定了亚硝酸盐样品, 线性范围和检测限分别为70～1500 μmol/L 和48 μmol/L. 该微流控亚硝酸根离子检测芯片已成功应用于水样和食品中亚硝酸盐测定, 结果满意.     

Lab-on-paper-based devices using chemiluminescence and electrogenerated chemiluminescence detection

As an analytical support, paper, being low cost, highly abundant, of high porosity, disposable or biodegradable, and easy to use, store, transport, and print, has excellent chemical compatibility with many applications. Since the first microfluidic paper-based analytical device (μ-PAD or lab-on-paper) was proposed, the paper-based assay has never attracted as much attention as it does now. There has recently been rapidly increasing interest in using sensitive luminescence methods, for example chemiluminescence (CL) and electrogenerated chemiluminescence (ECL), as the detection strategy for lab-on-paper devices. Because of their intrinsic characteristics, CL and ECL provide outstanding performance while retaining the simplicity, low cost, multifunctionality, versatility, flexibility, and disposability of μ-PADs. The objective of this review is to cover the development of lab-on-paper-based devices using CL and ECL detection, including fabrication of paper devices, construction of sensing interfaces, signal amplification strategies, external instruments used, and applications. We believe that lab-on-paper devices with CL and ECL detection methods will meet the diverse requirements of point-of-care diagnosis.     

Paper-based electrochemiluminescent 3D immunodevice for lab-on-paper, specific, and sensitive point-of-care testing

Recent research on microfluidic paper-based analytical devices (μPADs) has shown that paper has great potential for the fabrication of low-cost diagnostic devices for healthcare and environmental monitoring applications. Herein, electrochemiluminescence (ECL) was introduced for the first time into μPADs that were based on screen-printed paper-electrodes. To further perform high-specificity, high-performance, and high-sensitivity ECL on μPADs for point-of-care testing (POCT), ECL immunoassay capabilities were introduced into a wax-patterned 3D paper-based ECL device, which was characterized by SEM, contact-angle measurement, and electrochemical impedance spectroscopy. With the aid of a home-made device-holder, the ECL reaction was triggered at room temperature. By using a typical tris(bipyridine)ruthenium-tri-n-propylamine ECL system, this paper-based ECL 3D immunodevice was applied to the diagnosis of carcinoembryonic antigens in real clinical serum samples. This contribution further expands the number of sensitive and specific detection modes of μPADs.     

微流控纸芯片在环境分析检测中的应用

近年来,微流控纸芯片由于低成本、便携化、检测快等优点,在需要快速检测的环境分析领域中展现出了巨大的应用前景.该综述从微流控纸芯片在环境分析中的应用角度,总结归纳了微流控纸芯片在环境分析中的最新研究进展,并展望了其在未来的发展趋势与挑战.论文内容引用150余篇源于科学引文索引(SCI)与中文核心期刊中的相关论文.该综述包...     

Biomolecule immobilization techniques for bioactive paper fabrication

Research into paper-based sensors or functional materials that can perform analytical functions with active recognition capabilities is rapidly expanding, and significant research effort has been made into the design and fabrication of bioactive paper at the biosensor level to detect potential health hazards. A key step in the fabrication of bioactive paper is the design of the experimental and operational procedures for the immobilization of biomolecules such as antibodies, enzymes, phages, cells, proteins, synthetic polymers and DNA aptamers on a suitably prepared paper membrane. The immobilization methods are concisely categorized into physical absorption, bioactive ink entrapment, bioaffinity attachment and covalent chemical bonding immobilization. Each method has individual immobilization characteristics. Although every biomolecule–paper combination has to be optimized before use, the bioactive ink entrapment method is the most commonly used approach owing to its general applicability and biocompatibility. Currently, there are four common applications of bioactive paper: (1) paper-based bioassay or paper-based analytical devices for sample conditioning; (2) counterfeiting and countertempering in the packaging and construction industries; (3) pathogen detection for food and water quality monitoring; and (4) deactivation of pathogenic bacteria using antimicrobial paper. This article reviews and compares the different biomolecule immobilization techniques and discusses current trends. Current, emerging and future applications of bioactive paper are also discussed.     

Anomalous diffusion in an electrolyte saturated paper matrix

Diffusion of colored dye on water saturated paper substrates has been traditionally exploited with great skill by renowned water color artists. The same physics finds more recent practical applications in paper-based diagnostic devices deploying chemicals that react with a bodily fluid yielding colorimetric signals for disease detection. During spontaneous imbibition through the tortuous pathways of a porous electrolyte saturated paper matrix, a dye molecule undergoes diffusion in a complex network of pores. The advancing front forms a strongly correlated interface that propagates diffusively but with an enhanced effective diffusivity. We measure this effective diffusivity and show that it is several orders of magnitude greater than the free solution diffusivity and has a significant dependence on the solution pH and salt concentration in the background electrolyte. We attribute this to electrically mediated interfacial interactions between the ionic species in the liquid dye and spontaneous surface charges developed at porous interfaces, and introduce a simple theory to explain this phenomenon.     

Paper-based fluorescent devices for multifunctional assays: Biomarkers detection,inhibitors screening and chiral recognition

The development of a single analytical platform with different functions is highly desirable but remains a challenge at present. Here, a paper-based device based on fluorescent carbon dots (CDs) functionalized paper/MnO₂ nanosheets (MnO₂ NS) hybrid devices (PCD/NS) was proposed for single-device multi-function applications. MnO₂ NS functioned as a fluorescence quencher of CDs and recognizer of H₂O₂ released from the oxidase catalyzed system. Fluorescence recovery would occur after the decomposition of MnO₂ NS induced by H₂O₂, by which a simple and effective strategy could be developed for fluorescence monitoring multiplex biological events. Xanthine (XA) sensing, xanthine oxidase (XOD) inhibitors screening analysis and chiral recognition of glucose enantiomers were performed on PCD/NS to investigate the multifunctional application of the paper-based device. By means of PCD/NS, XA could be determined in the range of 0.1–40 µmol/L with a low detection of limit of 0.06 µmol/L. The IC₅₀ value of allopurinol, the model inhibitor of XOD, was sensitively detected to be 7.4 µmol/L. Glucose enantiomers were also recognized in terms of the specific fluorescence response to d-glucose. This work firstly presented a paper-based device capable of biomarkers detection, inhibitors screening and chiral recognition, which enlightened a promising strategy for the construction of multifunctional devices and hold the great potential application in clinical diagnosis and drug discovery.     

Electrochemical sensing of bisphenol A on single-walled carbon nanotube paper electrodes

The electrochemical detection of BPA often requires modification of electrodes to overcome BPA′s slower kinetics and higher oxidation potential. This work reports a modification-free, paper electrode based on vacuum-filtered SWCNT thin film. The prepared electrode does not need to be polished or transferred into the conducting substrates. The linear sweep voltammetric detection showed a linear response from 0.5–10 μM and 25–100 μM with the experimental LOD of 1.0 μM (S/N=3). The interference study and good recovery percentage (93–105 %) in real water samples demonstrated the method‘s selectivity. The sensor can be promising for developing a simple, low-cost, portable, and paper-based BPA monitoring system.     

Enhancement of sensitivity of paper-based sensor array for the identification of heavy-metal ions

Paper-based microfluidic devices have been widely investigated in recent years. Among various detection techniques, colorimetric method plays a very important role in paper-based microfluidic devices. The limitation, however, is also clear: they generally require highly sensitive indicators. In this work, we have developed a novel enrichment-based paper test for the discrimination of heavy-metal ions. Comparing to regular paper-based microfluidic devices, enrichment-based technique showed largely improved sensitivity. Combining with eight pyridylazo compounds and array technologies-based pattern-recognition, we have obtained the discrimination capability of eight different heavy-metal ions at same concentration as low as 50 μM using our enrichment-based pyridylazo compounds array paper. Identification of the heavy-metal ions was readily achieved using a standard chemometric approach. This method can be, of course, used for other analytes as well.     

Electro-kinetically driven route for highly sensitive blood pathology on a paper-based device

Enhancing the sensitivity of colorimetric detection in paper-devices is a quintessential step in achieving frugal diagnosis. Here, we demonstrate an effective way of improving the detection sensitivity of paper-based devices, as mediated by electro-kinetic mechanisms. By directly employing blood plasma, we investigate the electro-kinetic clustering of glucose, a neutral molecule in paper devices. Under the influence of uniform electric field, dispersed glucose gets accumulated in the paper strips. Due to the combination of EOF and electrophoretic migration, we achieve twofold increase in the colour intensity for both normal and diabetic samples. This approach is robust and possesses better sensitivity than conventional colorimetric assays and can be easily extended to other body fluid based diagnosis. These results may turn out to be of profound importance in improving the quality of pathological diagnosis in low-cost paper-based point-of-care devices deployed in resource-limited settings.     

Development of Paper Actuators Based on Carbon-Nanotube-Composite Paper

We propose a unique soft actuator—a paper actuator—based on carbon-nanotube-composite paper (CNT-composite paper), which is a composite of carbon nanotubes (CNTs) and paper. CNT-composite paper has highly efficient properties because of the contained CNTs, such as high electrical conductivity and semiconducting properties. We are considering using CNT-composite paper for various devices. In this study, we successfully developed a paper actuator. We determined the structure of the paper actuator by referencing that of bucky-gel actuators. The actuator operates using the force generated by the movement of ions. In addition to making the paper actuator, we also attempted to improve its performance, using pressure as an index and an electronic scale to measure the pressure. We investigated the optimal dispersant for use in paper actuators, expecting the residual dispersant on the CNT-composite paper to affect the performance differently depending on the type of dispersant. Referring to research on bucky-gel actuators, we also found that the addition of carbon powder to the electrode layers is effective in improving the pressure for paper actuators. We believe that the paper actuator could be used in various situations due to its ease of processing.     

Fabrication of paper-based microfluidic sensors by printing

A novel method for the fabrication of paper-based microfluidic diagnostic devices is reported; it consists of selectively hydrophobizing paper using cellulose reactive hydrophobization agents. The hydrophilic–hydrophobic contrast of patterns so created has excellent ability to control capillary penetration of aqueous liquids in paper channels. Incorporating this idea with digital ink jet printing techniques, a new fabrication method of paper-based microfluidic devices is established. Ink jet printing can deliver biomolecules and indicator reagents with precision into the microfluidic patterns to form bio-chemical sensing zones within the device. This method thus allows the complete sensor, i.e. channel patterns and the detecting chemistries, to be fabricated only by two printing steps. This fabrication method can be scaled up and adapted to use high speed, high volume and low cost commercial printing technology. Sensors can be fabricated for specific tests, or they can be made as general devices to perform on-demand quantitative analytical tasks by incorporating the required detection chemistries for the required tasks.     

Roughness effects of cellulose and paper substrates on water drop impact and recoil

The impact dynamics of water drops on sized and unsized smooth cellulose films and paper surfaces with controlled roughness levels were studied. The objective was to better understand the effect of roughness on the liquid drop impact dynamics on paper surfaces, isolating from the effect chemical heterogeneity. Drop impact in the first few milliseconds were recorded using high-speed CCD camera and the three-phase contact line movement of the water drop was analyzed. Smooth cellulose film surface and rough paper surface showed similar impact dynamics, suggesting that the surface energy plays a more dominant role than surface roughness. Significantly different dynamic contact angles of water drop on the sized and unsized surfaces were observed during drop impact. The Laplace pressure of the curved spreading front pointing to the centre of a spreading drop on these sized cellulose and paper surfaces reduces the three-phase contact line movement, and leads to smaller maximum spreading diameter. Our results suggest that the water drop spreads on the rough surface is most likely via a “roll-over” action rather than “stick and jump” movements.     

Paper-based enzyme-free immunoassay for rapid detection and subtyping of influenza A H1N1 and H3N2 viruses

Development of rapid screening in the ambulatory environment is the most pressing needs for the control of spread of infectious disease. Despite there are many methods to detect the immunoassay results, quantitative measurement in rapid disease screening is still a great challenge for point-of-care applications. In this work, based on the internal structural protein, i.e., nucleoprotein (NP), and outer surface glycoproteins, i.e., H1 and H3, of the influenza viruses, specific and sensitive immunoassay on paper-based platform was evaluated and confirmed. Detection and subtyping of influenza A H1N1 and H3N2 viruses found in people were demonstrated by colorimetric paper-based sandwich immunoassay. Concentration-dependent response to influenza viruses was shown and the detection limits could achieve 2.7 × 10³ pfu/assay for H1 detection and 2.7 × 10⁴ pfu/assay for H3 detection, which are within the clinical relevant level. Moreover, detection of influenza virus from infected cell lysate and clinical samples was demonstrated to further confirm the reliability of the paper-based immunoassay. The use of paper for the development of diagnostic devices has the advantages of lightweight, ease-of-use, and low cost and paper-based immunoassay is appropriate to apply for rapid screening in point-of-care applications.     

Progress in patterned paper sizing for fabrication of paper-based microfluidic sensors

In this paper, we report the progress in using paper sizing chemistry to fabricate patterned paper for chemical and biological sensing applications. Patterned paper sizing uses paper sizing agents to selectively hydrophobize certain area of a sheet. The hydrophilic-hydrophobic contrast of the pattern so created has an excellent ability to control capillary penetration of aqueous liquids in channels of the pattern. Incorporating this idea with digital ink jet printing technique, a new fabrication method of paper-based microfluidic devices is established. Ink jet printing can deliver biomolecules and chemicals with precision into the microfluidic patterns to form biological/chemical sensing sites within the patterns, forming the complete sensing devices. This study shows the potential of combining paper sizing chemistry and ink jet printing to produce paper-based sensors at low cost and at commercial volume.     

Determination of nitrite in saliva using microfluidic paper-based analytical devices

Point-of-care platforms can provide fast responses, decrease the overall cost of the treatment, allow for in-home determinations with or without a trained specialist, and improve the success of the treatment. This is especially true for microfluidic paper-based analytical devices (μPAD), which can enable the development of highly efficient and versatile analytical tools with applications in a variety of biomedical fields. The objective of this work was the development of μPADs to identify and quantify levels of nitrite in saliva, which has been proposed as a potential marker of periodontitis. The devices were fabricated by wax printing and allowed the detection of nitrite by a colorimetric reaction based on a modified version of the Griess reaction. The presented modifications, along with the implementation of a paper-based platform, address many of the common drawbacks (color development, stability, etc.) associated with the Griess reaction and are supported by results related to the design, characterization, and application of the proposed devices. Under the optimized conditions, the proposed devices enable the determination of nitrite in the 10–1000 μmol L⁻¹ range with a limit of detection of 10 μmol L⁻¹ and a sensitivity of 47.5 AU [log (μmol L⁻¹)]⁻¹. In order to demonstrate the potential impact of this technology in the healthcare industry, the devices were applied to the analysis of a series of real samples, covering the relevant clinical range.     

Disposable and Flexible Electrochemical Paper-based Analytical Devices Using Low-cost Conductive Ink

In this work, a simple procedure for construction of disposable electrochemical paper-based analytical devices (ePADs) by screen-printing using low-cost materials and a home craft electronic printer is proposed. The devices were constructed using liner paper as a substrate and carbon ink prepared with graphite powder and wood glue. The ePAD was evaluated as an electrochemical sensor and biosensor. The proposed conductive carbon-based ink can be easily prepared and is an eco-friendly and non-toxic material. The developed ePAD was simple to produce and can be used as a low-cost electrochemical sensor, at less than US $0.20 per device.     

Supramolecular edifices and switches based on metals

Our studies allowed to unravel at least partially, the “so-called” spontaneous self-assembly processes of supramolecular edifices based on metals. The formation of a tricuprous double-stranded helix in solution was found to be driven by thermodynamics via highly distorted intermediates. Dinuclear europium(III) triple-stranded helices were built in solution via alternative “braiding” and “keystone” mechanism. The overall process was also dominated by thermodynamics. Moreover, multipodal ligand with the appropriate binding sites can operate as Cu(II)/Cu(I) molecular switches. Recently, we examined ligands with neighboring binding functionalities (N,N) and (N,O) which confer to the corresponding divalent metal complexes new properties. They could operate as proton-driven multistage molecular switching devices based on region-selective metal binding.     

Recent development in nanomaterials fabricated paper-based colorimetric and fluorescent sensors: A review

The paper-based sensing devices have drawn a broad interest in analytical chemistry for colorimetric and fluorescent-based analysis of biological, environmental, clinical, and food samples. It is due to the simple, rapid, biodegradable, user-friendly, less expensive, and low waste generation into the environment. Here, the recent development of paper-based sensors fabricated with different noble metal nanoparticles (NPs) and semiconductor and carbon quantum dots (QDs) is demonstrated to analyze several chemical substances from various samples. User-friendly and portable recording devices such as digital cameras, smartphones, scanners, etc. along with color detecting softwares are employed to measure the color intensity of nanomaterials fabricated paper devices after the deposition of a sample solution containing various chemical substances. The advantages and disadvantages of incorporating nanomaterials in the paper substrate (direct deposition, inkjet printing, screen printing and wax printing) are illustrated. The mechanism for colorimetric, fluorescence, phosphorescence, and chemiluminescence sensing using noble metal NPs (Ag, Cu, and Au), semiconductors, and carbon QDs for the determination of metal ions, anions, pesticides, biomolecules, and other toxic chemical substances are discussed. Thus, this review article would be highly useful for scientists and researchers to design colorimetric sensors to monitor chemical toxicants in clinical, environment, foods, and many other related samples.     

Polyimidazolyl acetate ionic liquid grafted on cellulose filter paper as thin-film extraction phase for extraction of non-steroidal anti-inflammatory drugs from water

Recently, pharmaceuticals and personal care products in the water environment exhibited potential risks to both human and aquatic organisms. In order to improve the sensitivity and accuracy of pharmaceutical detection, the polyimidazolyl acetate ionic liquid was synthesized by Radziszewski reaction and coated on cellulose filter papers as a thin-film extraction phase for extraction of non-steroidal anti-inflammatory drugs from water. The attenuated total reflection-infrared spectrometry, thermogravimetric analysis, and scanning electron microscope analyses demonstrated that the polyimidazolyl acetate ionic liquid was successfully prepared and attached to the surface of the cellulose filter paper through chemical bonding. The adsorption capacity of the homemade thin-film extraction material for the four non-steroidal anti-inflammatory drugs was greater than 8898 ng/cm² under the optimum conditions, and the desorption rate was over 90%. Then, a paper-based thin-film extraction phase-high-performance liquid chromatography-tandem mass spectrometry method was established for the extraction of non-steroidal anti-inflammatory drugs in water. This method provided limits of detection and limits of quantification were in the range of 0.02–0.15 and 0.17–0.50 μg/L, respectively. Hence, the obtained thin-film extraction phase showed excellent recovery and reproducibility for the target non-steroidal anti-inflammatory drugs with carboxyl groups from water.