1. Introduction

2. Fundamentals of Paper Microfluidics

3. Classifications of Paper-Based Assays

4. Fabrication Techniques for Paper-Based Devices

4.9. Origami, Quilling, and Kirigami

Origami, quilling, and kirigami are innovative methods for fabricating paper-based devices, leveraging folding, quilling, and cutting principles to create intricate structures with diverse functionalities.

Origami, an ancient Japanese art form, involves precisely folding paper to create three-dimensional structures without cutting or adhesive. In paper device fabrication, origami provides an elegant means of constructing complex and functional designs. Researchers and engineers use origami techniques to fold paper into specific shapes, forming containers, channels, or dynamic components. The process typically begins with the design of a flat pattern that, when folded along predetermined lines, transforms into the desired 3D structure. The patterns are often created using computer-aided design (CAD) software. Origami-based paper devices have been developed for $\mu$PADS applications, such as creating fluidic channels and reservoirs through folding.

Quilling-based paper device fabrication involves creatively adapting quilling, a paper art form, to construct functional microfluidic devices [59]. This innovative approach utilizes the rolling, shaping, and arranging paper strips to create intricate structures, including microfluidic channels, reservoirs, and other components essential for analytical or diagnostic purposes. The process includes designing and planning the device layout, selecting suitable paper types, preparing quilling strips, employing quilling techniques to form desired shapes, assembling the components, and integrating functional elements. This method provides a cost-effective and customizable way to prototype simple microfluidic devices, offering accessibility and creativity in fabricating paper-based analytical tools for educational, research, or point-of-care applications.

Kirigami, an extension of origami, introduces the element of cutting into the folding process. This method allows for more intricate and flexible designs by strategically incorporating cuts and folds. In paper device fabrication, kirigami enables the creation of structures that can expand, contract, or exhibit specific movements. Designers use kirigami to craft patterns that, when folded and cut, resulting in functional and dynamic paper-based devices. This technique is particularly advantageous for applications requiring mechanical actuation or shape-changing capabilities. Kirigami-based devices have been found to be useful in flexible electronics and biomedical devices.

Figure 3(f-g) illustrates schematic representations of origami, quilling, and kirigami techniques employed in fabricating paper devices. These methods offer simplicity, low cost, and the ability to create complex structures without advanced equipment. However, precision in folding and cutting is crucial to achieving the intended functionalities. These methods have garnered attention for their potential to develop innovative and accessible solutions for various technological applications.

Table 1. Summary of fabrication techniques for paper-based sensors.

Table 1. Summary of fabrication techniques for paper-based sensors.

Fabrication techniques	Equipment and materials requirements	Advantages	Limitations	Ref.
Blade Cutting/Plotting	X-Y plotter, knife.	Provides sharp features, no chemical required.	Limited to 2D designs	[60,61]
Laser cutting	Laser cutter.	Precise, customizable designs, suitable for large-scale production, high resolution (∼60 $\mu$m)	Requires specialized equipment and polymer films to protect the paper device from damage, may generate debris.	[62,63,64,65,66]
Photolithography	UV light, heating plate, photomask, photoresists (positive/negative), mask aligner, chemicals, oxygen plasma.	High resolution (∼200 $\mu$m), well-established microfabrication technique	Equipment-intensive, may involve multiple complex steps and chances of channel contamination.	[54,67,68,69]
3D printing	3D printer, inks	Allows for complex, customized designs	Limited resolution compared to traditional microfabrication	[70,71,72,73,74,75,76]
Screen printing	Mesh screen, hot plate, transparency film, wax.	Low-cost, scalable for mass production	Resolution may vary, suitable for relatively simple designs, new screens are required for different patterns.	[77,78,79,80,81,82,83]
Wax printing	Hot plate, wax printer, solid wax.	Simple, rapid, cost-effective, and suitable for prototyping	Limited resolution (∼550 $\mu$m), wax spread, limited channel height control, temperature sensitivity	[84,85,86,87,88,89]
Inkjet printing	Customized inkjet printer, hydrophobic ink, hot plate, and chemicals.	Non-contact, suitable for rapid prototyping	Resolution may be lower than other techniques, requires multiple steps, and post-printing heating is required for some inks.	[90,91,92,93,94,95,96]
Embossing	Embossing tools, adhesives, silane.	Simple, flexible, suitable for rapid prototyping	Limited resolution, may affect paper integrity, susceptible to contamination.	[97,98,99,100]
Origami and Kirigami	Paper cutting and folding tools, adhesives.	Foldable Structures, flexible design, enhanced functionality, Scalability.	Precision challenges, design and assembly complexity, limited material compatibility.	[101,102,103,104,105,106,107,108]

5. Detection Techniques

5.5. Electrochemiluminescence

Electrochemiluminescence (ECL) represents a cutting-edge detection method seamlessly integrated into paper microfluidics-based sensors, providing a robust and precise analytical tool for detecting target analytes [118,119]. This innovative approach synergistically combines electrochemical and luminescent principles to achieve heightened sensitivity and selectivity.

In an Electrochemiluminescence-based paper microfluidic sensor, the device incorporates essential components such as electrodes and chemiluminescent reagents. The electrodes are pivotal in facilitating electrochemical reactions that generate species in excited states. These excited states subsequently release photons during relaxation, resulting in luminescence. The beauty of this method lies in its ability to leverage the controlled electrochemical reactions to induce luminescence, offering a precise and sensitive means of detecting analytes.

The detection mechanism within ECL-based paper microfluidic sensors revolves around measuring the emitted light. The intensity of the emitted light is directly correlated with the concentration of the target analyte present in the sample. This quantitative correlation enables precise analysis and quantification of analytes, making ECL-based sensors invaluable in various applications, including medical diagnostics, environmental monitoring, and bioanalytical research. Also, integrating electrochemiluminescence into paper microfluidics enhances the analytical capabilities of these sensors and contributes to the development of portable, cost-effective, and efficient platforms for on-site detection. The sensitivity and selectivity achieved through ECL make it a promising technology for advancing point-of-care diagnostics and real-time monitoring in diverse fields.

Figure 4(e) depicts the schematic of a Paper-Based Bipolar Electrode Electrochemiluminescence Platform designed to detect multiple targets, specifically miRNA-155 and miRNA-126. In this setup, the electron transfer process in each bipolar electrode is electrically coupled with the Electrochemiluminescence (ECL) reaction of each light-emitting probe due to the connection between the cathode and the anode. The DC power supply is connected to the parallel bipolar electrode sensing platform, executing the most suitable driving voltages for the two light-emitting probes (CdTe QDs and g-C${}_3$N${}_4$ NSs) with their co-reactants. Applying a driving voltage of 9 V to the co-reactant K${}_2$S${}_2$O${}_8$ in the hydrophilic unit, which is in close contact with the cathode region of the parallel bipolar electrode, induces an excitation–radiative transition process with the emission of the light signal. Simultaneously, an oxidation reaction occurs at the anode when in contact with the solution containing H${}_2$O${}_2$, resulting in the bipolar electrode facilitating the electron transfer between the cathode and anode path.

Figure 4. (a) Paper-based lateral flow assay for colorimetric sensing of Dengue NS1. Reprinted with permission from Kumar et al. [109], Biomicrofluidics 2018, 12, 034104. ©2018 AIP Publishing LLC. (b) Paper-Based Electrochemical Sensors for glucose sensing, Reprinted with permission from Valentine et al. [120], ACS Appl. Mater. Interfaces 2020, 12, 30680–30685. ©2020 American Chemical Society. (c) Schematic diagram of the paper-based fluorescent sensor for rapid early screening of oral squamous cell carcinoma. Reprinted with permission from He et al. [121], ACS Appl. Mater. Interfaces 2023, 15, 20, 24913-24922. ©2023 American Chemical Society. (d) Paper-based Chemiluminescence sensing of antioxidants (dopamine, CT, Cys, GSH, and TA): CL spectra (top) and CL images (bottom). Reprinted with permission from Li et al. [122], Sens. Actuators B Chem. 2023, 393, 134166. ©2023 Elsevier B.V. (e) Illustration of a conceptual paper-based bipolar electrode electrochemiluminescence platform for detecting multiple miRNAs. Reprinted with permission from Wang et al. [123], Anal. Chem. 2020, 93, 1702–170. ©2020 American Chemical Society.

Figure 4. (a) Paper-based lateral flow assay for colorimetric sensing of Dengue NS1. Reprinted with permission from Kumar et al. [109], Biomicrofluidics 2018, 12, 034104. ©2018 AIP Publishing LLC. (b) Paper-Based Electrochemical Sensors for glucose sensing, Reprinted with permission from Valentine et al. [120], ACS Appl. Mater. Interfaces 2020, 12, 30680–30685. ©2020 American Chemical Society. (c) Schematic diagram of the paper-based fluorescent sensor for rapid early screening of oral squamous cell carcinoma. Reprinted with permission from He et al. [121], ACS Appl. Mater. Interfaces 2023, 15, 20, 24913-24922. ©2023 American Chemical Society. (d) Paper-based Chemiluminescence sensing of antioxidants (dopamine, CT, Cys, GSH, and TA): CL spectra (top) and CL images (bottom). Reprinted with permission from Li et al. [122], Sens. Actuators B Chem. 2023, 393, 134166. ©2023 Elsevier B.V. (e) Illustration of a conceptual paper-based bipolar electrode electrochemiluminescence platform for detecting multiple miRNAs. Reprinted with permission from Wang et al. [123], Anal. Chem. 2020, 93, 1702–170. ©2020 American Chemical Society.

6. Applications in Health Sensing

6.1. Diagnostic Assays for Infectious Diseases and Others Analytes

Paper-based point-of-care (POC) diagnostic devices have garnered significant attention due to their portability, cost-effectiveness, biodegradability, and ease of use [124]. These devices leverage the unique properties of paper substrates to perform various diagnostic assays, making them promising tools, especially in resource-limited settings, which fulfill the World Health Organisation’s POC device development guidelines. Paper-based diagnostics typically involve using paper strips or cards that can wick biological samples, such as blood, saliva, or urine, through channels or zones containing reagents for specific assays [125].

Paper-based microfluidic devices have been used for point-of-care testing of vector-borne and flavivirus families such as Malaria [126,127], Dengue virus [128,129,130], Zika virus [131,132]. For example, Suvanasuthi et al. [133] introduced a paper-based colorimetric biosensor for detecting dengue virus serotypes (DENV1-4). The paper substrate’s hydrophobic barriers were fabricated using 3D printing with polylactic acid (PLA) and wax filaments. The developed prototype demonstrated the ability to differentiate between dengue virus serotypes based on subtle nucleotide sequence variations. Figure 5(a) illustrates the schematics of device assembly and provides photographs showing the visual color changes corresponding to different dengue virus serotypes. Karlikow et al. [134] introduced a paper-based diagnostic platform for detecting Zika and chikungunya viruses in serum samples. The tests achieved high accuracy and sensitivity by utilizing a cell-free expression system, isothermal amplification, toehold-switch reactions, and a custom portable reader and computer vision-enabled image analysis software. Figure 5(b) depicts the detection mechanism schematics of the paper-based device. In suspected infection cases, the tests demonstrated accuracies of 98.5% for both Zika (95% confidence interval, 96.2–99.6%, 268 serum samples) and chikungunya (95% confidence interval, 91.7–100%, 65 serum samples) viruses, with sensitivities ranging from 2 aM to 5 fM, falling within clinically relevant concentrations. The prototype’s performance was successfully validated in field conditions.

Moreover, paper-based devices have been employed to diagnose other diseases and analytes, including influenza virus H5N1 [135], Neisseria meningitides [136], nucleic acid detection [137,138], non-communicable diseases [139], cancer diagnosis [57,140,141], chronic obstructive pulmonary disease (COPD) biomarkers [142], HIV [143,144], pregnancy, infertility [145,146], and bioanalytes (uric acid, glucose, H${}_2$O${}_2$, Cholesterol) [147,148,149], etc. In a recent study, Bezdekova et al. [150] introduced a proof-of-concept paper-based device for diagnosing prostate cancer (CaP) from urine samples. Initially, urine samples underwent UV irradiation to induce the formation of fluorescent clusters. Subsequently, a selective molecularly imprinted polymeric layer was prepared on a paper substrate, allowing for the specific capture of these UV-induced fluorescent clusters within the urine sample to be diagnosed. Figure 5(c) illustrates the process of formation, capture, and detection of CaP-specific clusters in UV-irradiated urine samples. These clusters, captured using molecular imprinting technology, are then quantified using fluorescence spectroscopy.

Chaiyo et al. [151] introduced a novel 3D electrochemical paper-based analytical device (3D-ePAD) coupled with near-field communication (NFC) potentiostat for the nonenzymatic detection of cholesterol. Figure 5(d) illustrates the design of the paper device and the strategies employed for cholesterol detection. This integrated platform comprises an origami PAD (oPAD) and an inset PAD (iPAD). $\beta$-Cyclodextrin ($\beta$-CD) immobilized on the oPAD is the specific material for cholesterol detection without enzymes. The device seamlessly integrates cholesterol detection with a battery-free NFC potentiostat on a smartphone. Cholesterol concentration is assessed through a [Fe(CN)${}_6$]${}^{3-/4-}$ current signal, a redox indicator stored in the detection section of the iPAD. The 3D-ePAD/NFC system demonstrates a linear detection range of 1–500 $\mu$M and a maximum detection limit of 0.3 $\mu$M for cholesterol. Furthermore, the sensor effectively measures cholesterol levels in real human serum samples, yielding results consistent with those obtained from a commercial cholesterol meter.

Most recently, during the COVID-19 pandemic, $\mu$PADs have played a pivotal role in point-of-care initial disease screening [152,153,154,155,156,157,158]. One such example, Lee et al. [159] developed a colorimetric lateral flow immunoassay (LFIA) using a recombinant protein linker CBP31-BC to immobilize antibodies on a cellulose membrane in an oriented manner. Figure 5(e) shows the schematic of the CBP31-BC-based LFIA for detecting SARS-CoV-2. This LFIA demonstrated sensitive detection of cultured SARS-CoV-2 in 15 minutes, with a low detection limit of $5\times {10}^4$ copies/mL. Clinical evaluation using 19 samples validated by reverse transcription-polymerase chain reaction (RT-PCR) revealed 100% accuracy in detecting positive and negative samples, even those with low viral loads.

These POC devices have been instrumental in enabling rapid and real-time testing for the SARS-CoV-2 virus, facilitating early identification and containment of infections. Their ease of use, cost-effectiveness, and portability have made them particularly valuable in various settings, including clinics, airports, and resource-limited areas.

Figure 5. (a) Schematics of device assembly and photographs of visual color changes for different dengue virus serotypes. Reprinted with permission from Suvanasuthi et al. [133], Talanta 2022, 237, 122962. ©2021 Elsevier B.V.; (b) Schematics of paper-based platforms for detecting the Zika and chikungunya viruses in serum samples. Reprinted with permission from Karlikow et al. [134], Nat. Biomed. Eng. 2022, 6, 246–256. licensed under a Creative Commons Attribution 4.0 International License, ©2022 The Author(s); (c) Illustration of a paper-based analytical device for detecting prostate cancer using UV-irradiated urine samples. Reprinted with permission from Bezdekova et al. [150], Sensors and Actuators B: Chemical 2024, 403, 135146. ©2023 Elsevier B.V.; (d) The design concept of the 3D-ePAD, incorporating origami PAD (oPAD) and insert PAD (iPAD), and the detection mechanism for cholesterol across different concentrations. Reprint with permission from Chaiyo et al. [151], ACS Meas. Sci. Au 2024. licensed under CC-BY-NC-ND 4.0., ACS Meas. Sci. Au 2024. ©2024 The Authors.; (e) Schematic of the CBP31-BC-based LFIA for detecting SARS-CoV-2. Reprinted with permission from Lee et al. [159], Sens. Actuators B: Chem. 2023, 379, 133245. ©2022 Elsevier B.V.

Figure 5. (a) Schematics of device assembly and photographs of visual color changes for different dengue virus serotypes. Reprinted with permission from Suvanasuthi et al. [133], Talanta 2022, 237, 122962. ©2021 Elsevier B.V.; (b) Schematics of paper-based platforms for detecting the Zika and chikungunya viruses in serum samples. Reprinted with permission from Karlikow et al. [134], Nat. Biomed. Eng. 2022, 6, 246–256. licensed under a Creative Commons Attribution 4.0 International License, ©2022 The Author(s); (c) Illustration of a paper-based analytical device for detecting prostate cancer using UV-irradiated urine samples. Reprinted with permission from Bezdekova et al. [150], Sensors and Actuators B: Chemical 2024, 403, 135146. ©2023 Elsevier B.V.; (d) The design concept of the 3D-ePAD, incorporating origami PAD (oPAD) and insert PAD (iPAD), and the detection mechanism for cholesterol across different concentrations. Reprint with permission from Chaiyo et al. [151], ACS Meas. Sci. Au 2024. licensed under CC-BY-NC-ND 4.0., ACS Meas. Sci. Au 2024. ©2024 The Authors.; (e) Schematic of the CBP31-BC-based LFIA for detecting SARS-CoV-2. Reprinted with permission from Lee et al. [159], Sens. Actuators B: Chem. 2023, 379, 133245. ©2022 Elsevier B.V.

7. Environmental Monitoring/Sensing

7.1. Detection of Soil Contaminants

Soil contaminants significantly threaten environmental ecosystems and human health, necessitating efficient early detection and mitigation monitoring systems. Paper-based microfluidic devices have emerged as promising tools in soil contaminant monitoring due to their cost-effectiveness, simplicity, and portability. These devices leverage the capillary action of paper to facilitate the flow of liquids through microchannels, allowing for the detection of various contaminants. They are well-suited for applications in resource-limited settings where sophisticated laboratory equipment may be impractical. These paper-based systems can be designed to detect a range of soil contaminants, including heavy metals, pesticides, and organic pollutants.

Suo et al.[177] developed a high-throughput paper-based fluorescence resonance energy transfer (FRET) aptasensor for the sensitive detection of low concentrations of Pb${}^{2+}$. Figure 7(a) illustrates detection methodology. Fabricated on the Whatman No.1 chromatographic paper, the device demonstrated the capability to detect Pb${}^{2+}$ in a concentration range spanning from 0.01 to 10 $\mu$M, with an impressive limit of detection (LOD) of 6.1 nM. This innovative strategy successfully analyzed various real samples, including water, soil, and food, showcasing its applicability in practical scenarios for environmental and food safety assessments. Integrating FRET technology into a paper-based platform enhances the efficiency and throughput of the aptasensor, offering a versatile and sensitive tool for rapid detection in diverse sample matrices. Yu et al. [178] introduced a fiber-made filter paper-based device for the real-time monitoring of Cd${}^{2+}$ in water, rice, and rice soil (see Figure 7(b)). The developed test paper exhibited highly sensitive and visible sensing capabilities for Cd${}^{2+}$ in water, rice supernatants, and rice soil supernatants. The LODs in these real samples were remarkably low, measuring at 0.0112 ppb for water, 1.1240 ppb for rice supernatants, and 0.1124 ppb for rice soil supernatants. These LODs were found to be lower than the national standards for food safety in China (GB 2762-2022), underscoring the device’s potential for precise and reliable detection, with implications for ensuring compliance with stringent safety regulations in diverse environmental and agricultural settings.

Furthermore, pesticides, vital for ensuring food security by controlling pests, weeds, and plant diseases, have significantly increased food availability over the past 50 years. However, their widespread use has led to environmental pollution, adversely affecting ecosystems and human health [179,180]. Implementing efficient management practices and user-friendly point-source monitoring systems accessible to farmers can alleviate pesticides’ environmental and health impacts. In this context, paper microfluidics-based devices have played a significant role in pesticide detection [181]. Zhang et al. [182] developed an innovative paper-based colorimetric sensor for thiacloprid, a commonly used agricultural pesticide, with a low detection limit of 0.04 $\mu$M. Figure 7(c) shows the schematic representation of the principle behind the paper-based colorimetric sensor designed for the real-time monitoring of pesticides. The quantification of the sensor’s output was facilitated through RGB analysis, providing a simple and efficient method for detection. Notably, integrating a smartphone app for output reading enhances the accessibility and user-friendliness of the paper-based sensor, offering a promising solution for on-site and real-time monitoring of thiacloprid levels in agricultural settings. Ranveer et al. [183] designed a versatile paper-based dipstick assay for colorimetric detection of fungicides, organochlorines, organophosphates, carbamates, and herbicides in diverse matrices such as animal feed, water, milk, and soil. Figure 7(d) presents a schematic illustration depicting the detection of pesticides in dairy samples through the paper-based sensor.The developed dipstick demonstrated versatile applicability with impressive LOD for different pesticide groups. Specifically, the LOD values ranged from 1 to 10 $\mu g{L}^{-1}$ for fungicides, 1–50 $\mu g{L}^{-1}$ for organochlorines, 250–500 $\mu g{L}^{-1}$ for organophosphates, 1–50 $\mu g{L}^{-1}$ for carbamates, and 1 $\mu g{L}^{-1}$ for herbicides. This paper-based assay showcased sensitivity across a range of pesticide residues. It illustrated its potential as a rapid and cost-effective tool for assessing pesticide contamination in multiple environmental and food matrices. Caratelli et al. [184] introduced a 3D flower-like origami paper-based device designed for the electrochemical detection of pesticides, specifically paraoxon, 2,4-dichloro phenoxy acetic acid, and glyphosate, in the aerosol phase, catering to applications in precision agriculture. Figure 7(e) illustrates a schematic representation of the electrochemical biosensor for pesticide detection based on an origami-based paper device. The innovative device was seamlessly integrated with a smartphone for convenient output reading. Remarkably, this paper-based system demonstrated efficient detection of the three classes of pesticides in the aerosol phase, achieving impressive LODs equal to 30 ppb, 10 ppb, and 2 ppb for 2,4-D, glyphosate, and paraoxon, respectively. Integrating electrochemical sensing with a portable paper-based platform enhances accessibility and usability, offering a promising tool for real-time pesticide monitoring in agricultural settings with potential implications for sustainable and precise farming practices.

Paper-based sensors have been found to have a noteworthy application in detecting explosive residues in soil, presenting a valuable forensic-oriented environmental monitoring and security tool [185,186,187,188,189]. The unique attributes of paper microfluidic devices, such as their portability, simplicity, and cost-effectiveness, make them well-suited for on-site detection of explosive remnants. These sensors can be tailored to detect specific volatile compounds, offering a targeted and efficient approach to soil analysis. The detection mechanism often involves incorporating reactive agents or biomolecules onto the paper substrate, allowing for a rapid and selective response to the presence of explosive residues. This application is particularly crucial in areas where the remnants of explosives pose environmental and safety concerns, such as former military sites or regions affected by conflict. By leveraging the capabilities of paper-based sensors, ecological professionals and security personnel can conduct real-time, on-site assessments of soil contamination, facilitating prompt remediation efforts and contributing to a safer and more secure environment.

Figure 7. (a) Illustration of a high-throughput paper-based FRET aptasensor designed for the detection of Pb${}^{2+}$. Reprinted with permission from Suo et al.[177], Anal. Chim. Acta 2023, 1239, 340714. ©2022 Elsevier B.V.; (b) Schematics of fiber-made filter paper-based biosensors for the real-time monitoring of Cd${}^{2+}$ in water, rice, and rice soil. Reprinted with permission from Yu et al. [178], Inorg. Chem. 2023, 62, 6387–639. ©2023 American Chemical Society; (c) Principle illustration of the Paper-Based Colorimetric sensor for real-time monitoring of pesticides. Reprinted with permission from Zhang et al. [182], Chem. Eng. J. 2023, 451, 138928 ©2022 Elsevier B.V.; (d) Schematic illustration of pesticide detection in dairy samples using the paper-based sensor. Reprinted from Ranveer et al. [183], Curr. Res. Food Sci. 2023, 6, 100416. Under a Creative Commons license ©2022 Elsevier B.V.; (e) Schematic representation of the origami paper-based electrochemical biosensor for pesticide detection. Reprinted with permission from Caratelli et al. [184], Biosens. Bioelectron. 2022, 205, 114119. ©2022 Elsevier B.V.

Figure 7. (a) Illustration of a high-throughput paper-based FRET aptasensor designed for the detection of Pb${}^{2+}$. Reprinted with permission from Suo et al.[177], Anal. Chim. Acta 2023, 1239, 340714. ©2022 Elsevier B.V.; (b) Schematics of fiber-made filter paper-based biosensors for the real-time monitoring of Cd${}^{2+}$ in water, rice, and rice soil. Reprinted with permission from Yu et al. [178], Inorg. Chem. 2023, 62, 6387–639. ©2023 American Chemical Society; (c) Principle illustration of the Paper-Based Colorimetric sensor for real-time monitoring of pesticides. Reprinted with permission from Zhang et al. [182], Chem. Eng. J. 2023, 451, 138928 ©2022 Elsevier B.V.; (d) Schematic illustration of pesticide detection in dairy samples using the paper-based sensor. Reprinted from Ranveer et al. [183], Curr. Res. Food Sci. 2023, 6, 100416. Under a Creative Commons license ©2022 Elsevier B.V.; (e) Schematic representation of the origami paper-based electrochemical biosensor for pesticide detection. Reprinted with permission from Caratelli et al. [184], Biosens. Bioelectron. 2022, 205, 114119. ©2022 Elsevier B.V.

7.3. Air Quality Monitoring/Gas Sensing

Air pollution poses a significant threat to public health and the environment. Conventional air quality monitoring systems are characterized by their high cost, limited portability, and dependency on sophisticated infrastructure. The emergence of paper-based microsystems presents a cost-effective and portable alternative, leveraging the inherent properties of paper substrates for efficient detection of air pollutants [207,208,209].

Colorimetric paper-based sensors offer an innovative approach to environmental monitoring, especially in detecting air pollutants. In their work, De Matteis et al. [210] designed a paper-based analytical device (PAD) capable of detecting contaminants such as Fe${}^{2+}$, Cu${}^{2+}$ ions in water, and NH${}_3$ and $C_2{H}_{4}O$ in the air, even at low concentrations. The researchers employed a wax pen to form a circular hydrophobic barrier on a Whatman filter paper substrate to create distinct sensing zones. These marked spots were utilized to detect the specified analytes at various concentrations. Figure 9(a) shows the schematics of detection mechanisms. Notably, the paper sensor displayed a colorimetric response directly correlated with the concentration of the identified pollutant species.

Bordbar et al. [211] developed a paper-based optical nose by depositing bimetallic silver and gold nanoparticles onto a paper substrate, synthesized using both natural and chemical reducing agents. This assay was evaluated for its capability to distinguish between gasoline and five ignitable liquids: diesel, ethanol, methanol, kerosene, and thinner. The interaction between the sensor and sample vapors led to nanoparticle aggregation, resulting in color changes captured by a scanner, producing distinct colorimetric maps for each analyte (Figure 9(b)). Visual observations were corroborated using multivariate statistical analyses, including principal component analysis and hierarchical clustering analysis. Additionally, partial least-squares regression aided in estimating the quantities of ignitable liquids present as counterfeit substances in gasoline samples, with root-mean-square errors for prediction ranging from 1.7% to 3.4%. Ultimately, the fabricated sensor demonstrated high efficiency for the onsite detection of pure industrial gasoline samples versus adulterated ones.

Moreover, paper-based devices are extensively utilized for electrochemical-based detection of air pollutants [212,213]. Mettakoonpitak et al.[214] introduced an innovative electrochemical paper-based device (ePAD) for the multiplexed detection of metals, specifically Cd, Pb, Cu, Fe, and Ni, from a single particulate matter sample. The paper-based device was designed with four independent channels and working electrodes, enabling the implementation of square-wave anodic stripping voltammetry (SWASV) and square-wave cathodic stripping voltammetry (SWCSV) for the simultaneous determination of multiple metals. Figure 9(c) shows an example of electrochemical-based paper sensors for air pollutant detection. Notably, the device exhibited impressive detection limits, ranging from 0.5 to 400.0 $\mu g{L}^{-1}$ for Cd(II), Pb(II), and Fe(II), 1.0 to 400.0 $\mu g{L}^{-1}$ for Cu(II), and 0.5 to 200.0 $\mu g{L}^{-1}$ for Ni(II). This multiplexed ePAD offers a versatile and efficient solution for sensitively detecting various metals in complex samples, showcasing its potential for environmental monitoring and analytical applications.

Davis et al. [215] engineered a flexible paper-based sensor for acetone detection at room temperature. The paper-based electrodes were crafted through the application of zinc oxide (ZnO)-polyaniline-based conductive inks (Figure 9(d)). These electrodes exhibited remarkable conductivity (80 S/m) and stability under rigorous mechanical and chemical conditions while demonstrating commendable flexibility (1000 bending cycles). The acetone sensor displayed notable sensitivity of 0.02/100 ppm and 0.6/10 $\mu$L, with a broad sensitivity range spanning from 260 to >1000 ppm under atmospheric conditions. Moreover, the sensors exhibited an impressive response time of 4 seconds and a recovery time of 15 seconds for acetone detection at room temperature without necessitating external heaters. The proposed paper device’s high sensitivity and long-term stability make it suitable for wearable biosensor applications.

Moreover, a cantilever-based paper-based sensor device has been demonstrated by Qin et al. [216]. They developed an inexpensive and lightweight hydrocarbon gas sensor utilizing a smartphone camera for readout. The sensor relies on paper-based milli-cantilever bending induced by polymer swelling. The sensing cantilever comprises three layers: a functional layer of polyethylene film, an adhesive layer of double-sided tape, and a weighing paper substrate. Figure 9(e) shows schematics of the milli-cantilever. The milli-fabricated sensing cantilever has dimensions of 8 mm length, 0.5 mm width, and 50 $\mu m$ thickness. The sensor’s response is measured as the displacement of the milli-cantilever-free end. Demonstrating its capabilities, the sensor exhibited a linear response to hydrocarbon concentrations, a broad detection range, low detection limits, and rapid response times. For instance, when exposed to xylene, the sensor displayed a detection range of 15–140 ppm, a low detection limit of 15 ppm, and a fast response time of 30 seconds.

Figure 9. (a) Colorimetric detection of Fe${}^{2+}$, Cu${}^{2+}$ ions, Reprinted with permission from De Matteis et al. [210], Sensors 2020, 20, 5502. under Creative Commons Attribution (CC BY) license. ©2020 The authors, published by MDPI; (b) Schematic representation of colorimetric detection process of gasoline utilizing a paper-based optical nose. Reprinted with permission from Bordbar et al. [211], ACS Appl. Mater. Interfaces 2022, 14, 6, 8333-8342. ©2022 American Chemical Society.; (c) Electrochemical detection of metals in aerosol samples using paper-based analytical device. Reprinted with permission from Mettakoonpitak et al. [214], Anal. Chem. 2020, 92, 1, 1439-1446. ©2019, American Chemical Society. ; (d) Schematics of the paper-based flexible sensors for detection of acetone at room temperature. Reprinted with permission from Davis et al. [215], ACS Appl. Mater. Interfaces 2023, 15, 21, 25734-25743. ©2023 American Chemical Society; (e) Sensing mechanism of the milli-cantilever. Reprinted with permission from Qin et al. [216], Anal. Chem. 2020, 92, 12, 8480-8486. ©2020 American Chemical Society.

Figure 9. (a) Colorimetric detection of Fe${}^{2+}$, Cu${}^{2+}$ ions, Reprinted with permission from De Matteis et al. [210], Sensors 2020, 20, 5502. under Creative Commons Attribution (CC BY) license. ©2020 The authors, published by MDPI; (b) Schematic representation of colorimetric detection process of gasoline utilizing a paper-based optical nose. Reprinted with permission from Bordbar et al. [211], ACS Appl. Mater. Interfaces 2022, 14, 6, 8333-8342. ©2022 American Chemical Society.; (c) Electrochemical detection of metals in aerosol samples using paper-based analytical device. Reprinted with permission from Mettakoonpitak et al. [214], Anal. Chem. 2020, 92, 1, 1439-1446. ©2019, American Chemical Society. ; (d) Schematics of the paper-based flexible sensors for detection of acetone at room temperature. Reprinted with permission from Davis et al. [215], ACS Appl. Mater. Interfaces 2023, 15, 21, 25734-25743. ©2023 American Chemical Society; (e) Sensing mechanism of the milli-cantilever. Reprinted with permission from Qin et al. [216], Anal. Chem. 2020, 92, 12, 8480-8486. ©2020 American Chemical Society.

8. Food Safety

Figure 10. (a) Illustration of the device schematics, operational steps, and a microscopic image of the S. typhi test zone, showcasing SERS mapping signals at 1075 cm${}^{-1}$, alongside the corresponding Raman spectrum. Reprinted with permission from Zhuang et al. [217], Biosens. Bioelectron. 2022, 207, 114167. ©2022 Elsevier B.V.; (b) Schematic representation of optical and electrochemical sensing platforms utilizing curcumin-immobilized paper substrates for ochratoxin A detection in grape juice and beer. Reprinted with permission from Dos Santos et al. [221], Sens. Actuators Rep. 2024, 7, 100184. Under a Creative Commons license, ©2023 The Author(s). Published by Elsevier B.V.; (c) Schematic Illustration of Microzone Paper-Based Mass Spectrometric Immunoassay for Detecting Food Allergens (peanut allergen Ara h1). Reprinted with permission from Lu et al. [228], Anal. Chem. 2024, 96, 6, 2387-2395. ©2024 American Chemical Society; (d) Schematics of 3D $\mu$PAD with colorimetric detection for iodine speciation in seaweed samples. Reprinted with permission from Placer et al. [231], Sens. Actuators B: Chem. 2023, 377, 133109. Under a Creative Commons license, ©2022 The Authors. Published by Elsevier B.V.; (e) The procedural steps of SMIPs-$\mu$PAD and actual images of the paper device before and after color development. Reprinted with permission from Wu et al. [237], Food Chem. 2024, 435, 137659. ©2023 Elsevier Ltd.

Figure 10. (a) Illustration of the device schematics, operational steps, and a microscopic image of the S. typhi test zone, showcasing SERS mapping signals at 1075 cm${}^{-1}$, alongside the corresponding Raman spectrum. Reprinted with permission from Zhuang et al. [217], Biosens. Bioelectron. 2022, 207, 114167. ©2022 Elsevier B.V.; (b) Schematic representation of optical and electrochemical sensing platforms utilizing curcumin-immobilized paper substrates for ochratoxin A detection in grape juice and beer. Reprinted with permission from Dos Santos et al. [221], Sens. Actuators Rep. 2024, 7, 100184. Under a Creative Commons license, ©2023 The Author(s). Published by Elsevier B.V.; (c) Schematic Illustration of Microzone Paper-Based Mass Spectrometric Immunoassay for Detecting Food Allergens (peanut allergen Ara h1). Reprinted with permission from Lu et al. [228], Anal. Chem. 2024, 96, 6, 2387-2395. ©2024 American Chemical Society; (d) Schematics of 3D $\mu$PAD with colorimetric detection for iodine speciation in seaweed samples. Reprinted with permission from Placer et al. [231], Sens. Actuators B: Chem. 2023, 377, 133109. Under a Creative Commons license, ©2022 The Authors. Published by Elsevier B.V.; (e) The procedural steps of SMIPs-$\mu$PAD and actual images of the paper device before and after color development. Reprinted with permission from Wu et al. [237], Food Chem. 2024, 435, 137659. ©2023 Elsevier Ltd.

Table 2. Summary of applications of paper-based sensors.

9. Biodegradability and Sustainability

10. Challenges and Future Perspectives

11. Conclusion

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