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1. Engineering a point-of-care paper-microfluidic electrochemical device applied to the multiplexed quantitative detection of biomarkers in sputum

Author

Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, Universitat Politècnica de Catalunya. GBMI - Grup de Biotecnologia Molecular i Industrial, Gutierrez Capitan, Manuel, Sanchís Villariz, Ana, Carvalho, Estela, Baldi Coll, Antonio, Vilaplana Holgado, Lluïsa, Cardoso, Vanessa, Calleja Navalpotro, Álvaro, Wei, Mingxing, de la Rica, Roberto, Hoyo Pérez, Javier, Bassegoda Puigdomenech, Arnau, Tzanov, Tzanko, Marco Colas, María Pilar, Lanceros Méndez, Senentxu, Fernandez Sanchez, Cesar, Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, Universitat Politècnica de Catalunya. GBMI - Grup de Biotecnologia Molecular i Industrial, Gutierrez Capitan, Manuel, Sanchís Villariz, Ana, Carvalho, Estela, Baldi Coll, Antonio, Vilaplana Holgado, Lluïsa, Cardoso, Vanessa, Calleja Navalpotro, Álvaro, Wei, Mingxing, de la Rica, Roberto, Hoyo Pérez, Javier, Bassegoda Puigdomenech, Arnau, Tzanov, Tzanko, Marco Colas, María Pilar, Lanceros Méndez, Senentxu, and Fernandez Sanchez, Cesar

Abstract

Health initiatives worldwide demand affordable point- of-care devices to aid in the reduction of morbidity and mortality rates of high-incidence infectious and noncommunicable diseases. However, the production of robust and reliable easy-to-use diagnostic platforms showing the ability to quantitatively measure several biomarkers in physiological fluids and that could in turn be decentralized to reach any relevant environment remains a challenge. Here, we show the particular combination of paper-microfluidic technology, electro- chemical transduction, and magnetic nanoparticle-based immunoassay approaches to produce a unique, compact, and easily deployable multiplex device to simultaneously measure interleukin-8, tumor necrosis factor-a, and myeloperoxidase biomarkers in sputum, developed with the aim of facilitating the timely detection of acute exacerbations of chronic obstructive pulmonary disease. The device incorporates an on-chip electrochemical cell array and a multichannel paper component, engineered to be easily aligned into a polymeric cartridge and exchanged if necessary. Calibration curves at clinically relevant biomarker concentration ranges are produced in buffer and artificial sputum. The analysis of sputum samples of healthy individuals and acutely exacerbated patients produces statistically significant biomarker concentration differences between the two studied groups. The device can be mass-produced at a low cost, being an easily adaptable platform for measuring other disease-related target biomarkers., This research was funded by the Spanish Ministry of Economy and Competitiveness (MINECO) grants PCIN-2016-052 and PCIN-2016-134 and by Portuguese Fundação para a Ciência e a Technologia grant ENMed/0049/2016, through the ERA-NET EuroNanoMed II initiative (LungCheck project). This research was also funded by the European Commision-NextGenerationEU (Regulation EU 2020/2094), through CSIC’s Global Health Platform (PTI). This work used the Spanish ICTS Network MICRONANOFABS and was partly supported by the Spanish Ministry of Science and Innovation., Peer Reviewed, Postprint (published version)

Published
2023

2. Highly Ductile Cellulose-Rich Papers Obtained by Ultrasonication-Assisted Incorporation of Low Molecular Weight Plasticizers

Author

Eliasson, Adrian, Hedenqvist, Mikael S., Brolin, Anders, Wågberg, Lars, Malmström, Eva, Eliasson, Adrian, Hedenqvist, Mikael S., Brolin, Anders, Wågberg, Lars, and Malmström, Eva

Abstract

Ultrasonication was used as a mean toincorporate glycerolor urea, yielding paper films with a ductility of up to 35%. Fiber-based materials are attractive sustainable alternativestofossil-based plastics, however, the lack of ductility (i.e., brittleness)limits their applicability in complex shapes as are often utilizedfor plastics. In this study, we hypothesize that it is possible toenhance the ductility of a cellulose-rich material by the incorporationof low molecular weight plasticizers (glycerol, urea, citric acid,and tannic acid). However, no significant effects could be observedafter swelling in the presence of plasticizers. To enhance any potentialeffect, it was decided to employ ultrasonication to mechanically disintegratethe fiber and aid the sorption of plasticizer prior to formation ofsheets from the treated fibers. Glycerol or urea in combination withultrasonication resulted in both internal and external fibrillationof the fibers, and it could be observed that the resulting fines createa film at the surface of the fibers in the formed sheets. Tensiletesting shows that this gives rise to a 100% increase in ductilitycompared to sheets from untreated fibers. The use of citric or tannicacid has the opposite effect, reducing ductility to a third of thatof the reference sheet. This is suggested to be due to the formationof covalent cross-links in the treated fibers, which also leads todifferent internal and external fibrillation mechanisms, as observedby scanning electron microscopy. The exceptionally high improvementof the strain-at-break for sheets from the glycerol- and urea-treatedfibers suggests that low molecular weight plasticizers affect theinternal properties of the fiber wall as well as the interactionsbetween the fine material forming in-between the fibers. The findingsfrom the current study suggest that the proposed approach to obtainductile cellulose-rich materials holds promise for the future, butit is also clear that more in-depth research is req, QC 20230630

Published
2023
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3. Printable and Versatile Superhydrophobic Paper via Scalable Nonsolvent Armor Strategy

Author

Liu, Shanqiu, Chen, Kangwei; https://orcid.org/0000-0002-2977-2464, Salim, Alma, Li, Jingguo, Bottone, Davide; https://orcid.org/0000-0002-6133-5088, Seeger, Stefan; https://orcid.org/0000-0003-2892-7468, Liu, Shanqiu, Chen, Kangwei; https://orcid.org/0000-0002-2977-2464, Salim, Alma, Li, Jingguo, Bottone, Davide; https://orcid.org/0000-0002-6133-5088, and Seeger, Stefan; https://orcid.org/0000-0003-2892-7468

Abstract

Despite great scientific and industrial interest in waterproof cellulosic paper, its real world application is hindered by complicated and costly fabrication processes, limitations in scale-up production, and use of organic solvents. Furthermore, simultaneously achieving nonwetting properties and printability on paper surfaces still remains a technical and chemical challenge. Herein, we demonstrate a nonsolvent strategy for scalable and fast fabrication of waterproofing paper through in situ surface engineering with polysilsesquioxane nanorods (PSNR). Excellent superhydrophobicity is attained on the functionalized paper surface with water contact angle above 160˚. Notably, the engineered paper features outstanding printability and writability, as well as greatly enhanced strength and integrity upon prolonged exposure to water (tensile strength ≈ 9.0 MPa). Additionally, the PSNR concurrently armors paper-based printed items and artwork with waterproofing, self-cleaning and antimicrobial functionalities without compromising their appearance, readability and mechanical properties. We also demonstrate that the engineered paper holds the additional advantages of easy processing, low cost and mechanochemical robustness, which makes it particularly promising for real world applications.

Published
2022

49. Rapid Assembly of Cellulose Microfibers into Translucent and Flexible Microfluidic Paper-Based Analytical Devices via Wettability Patterning

Author

Peng Ma, Shanshan Wang, Jie Wang, Yu Wang, Yue Dong, Shunji Li, Huiying Su, Peng Chen, Xiaojun Feng, Yiwei Li, Wei Du, and Bi-Feng Liu

Subjects
Paper, Glucose, Lab-On-A-Chip Devices, Microfluidics, Wettability, Humans, Microfluidic Analytical Techniques, Cellulose, Analytical Chemistry
Abstract

Microfluidic paper-based analytical devices (μPADs) are emerging as powerful analytical platforms in clinical diagnostics, food safety, and environmental protection because of their low cost and favorable substrate properties for biosensing. However, the existing top-down fabrication methods of paper-based chips suffer from low resolution (200 μm). Additionally, papers have limitations in their physical properties (e.g., thickness, transmittance, and mechanical flexibility). Here, we demonstrate a bottom-up approach for the rapid fabrication of heterogeneously controlled paper-based chip arrays. We simply print a wax-patterned microchip with wettability contrasts, enabling automatic and selective assembly of cellulose microfibers to construct predefined paper-based microchip arrays with controllable thickness. This paper-based microchip printing technology is feasible for various substrate materials ranging from inorganic glass to organic polymers, providing a versatile platform for the full range of applications including transparent devices and flexible health monitoring. Our bottom-up printing technology using cellulose microfibers as the starting material provides a lateral resolution down to 42 ± 3 μm and achieves the narrowest channel barrier down to 33 ± 2 μm. As a proof-of-concept demonstration, a flexible paper-based glucose monitor is built for human health care, requiring only 0.3 μL of sample for testing.

Published
2022
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50. Paper Device Combining CRISPR/Cas12a and Reverse-Transcription Loop-Mediated Isothermal Amplification for SARS-CoV-2 Detection in Wastewater

Author

Haorui Cao, Kang Mao, Fang Ran, Pengqi Xu, Yirong Zhao, Xiangyan Zhang, Hourong Zhou, Zhugen Yang, Hua Zhang, and Guibin Jiang

Subjects
SARS-CoV-2, Biotin, CRISPR/Cas12a, General Chemistry, Wastewater, Fluoresceins, Sensitivity and Specificity, RNA, Viral, Environmental Chemistry, CRISPR-Cas Systems, Nucleic Acid Amplification Techniques, Pandemics, wastewater, RT-LAMP, paper device
Abstract

Wastewater-based surveillance of the COVID-19 pandemic holds great promise; however, a point-of-use detection method for SARS-CoV-2 in wastewater is lacking. Here, a portable paper device based on CRISPR/Cas12a and reverse-transcription loop-mediated isothermal amplification (RT-LAMP) with excellent sensitivity and specificity was developed for SARS-CoV-2 detection in wastewater. Three primer sets of RT-LAMP and guide RNAs (gRNAs) that could lead Cas12a to recognize target genes via base pairing were used to perform the high-fidelity RT-LAMP to detect the N, E, and S genes of SARS-CoV-2. Due to the trans-cleavage activity of CRISPR/Cas12a after high-fidelity amplicon recognition, carboxyfluorescein-ssDNA-Black Hole Quencher-1 and carboxyfluorescein-ssDNA-biotin probes were adopted to realize different visualization pathways via a fluorescence or lateral flow analysis, respectively. The reactions were integrated into a paper device for simultaneously detecting the N, E, and S genes with limits of detection (LODs) of 25, 310, and 10 copies/mL, respectively. The device achieved a semiquantitative analysis from 0 to 310 copies/mL due to the different LODs of the three genes. Blind experiments demonstrated that the device was suitable for wastewater analysis with 97.7% sensitivity and 82% semiquantitative accuracy. This is the first semiquantitative endpoint detection of SARS-CoV-2 in wastewater via different LODs, demonstrating a promising point-of-use method for wastewater-based surveillance.

Published
2022
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