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In this work, three different dyes have been tested for the determination of gaseous ammonia. This gas is one of the products of microbial degradation and therefore its presence is an indicator of deterioration and could be used as a food freshness indicator. Three different sensors have been prepared and tested, two of them using the natural pigments curcumin and anthocyanin and the other one using bromothymol blue. All of them are biocompatible and therefore allowed to use in contact with food. Different compositions, materials for deposition, stability and reversibility for ammonia gas detection have been studied under high humidity conditions simulating real packaged food conditions. Colorimetry is the technique used to obtain the analytical parameter, the H coordinate of the HSV colour space, simply using a camera, avoiding the use of complex instrumentation. Sensibility, toxicity grade and stability found show that the sensor could be implemented in packaged food and form the basis of a freshness indicator for the food industry.

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Concerns about food safety and environmental impact from chemical surfactants have prompted interest in natural lignocellulosic materials as alternatives. In this study, we combined hydrated deep eutectic solvent (DES) pretreatment with ultrasound treatment to prepare lignocellulosic nanofibrils (LCNF) from bamboo shoot shells with appropriate surface properties for stabilizing Pickering emulsions. The pretreatment intensity effectively modulated the surface characteristics of LCNF, achieving desirable wettability through lignin retention and in-situ esterification. The resulting LCNF/curcumin Pickering emulsion (CPE) demonstrated curcumin protection and pH-responsive color changes, while the ensuing CPE/PVA composite film exhibited ultraviolet shielding, mechanical strength, oxygen barrier, and antioxidant properties. Furthermore, the CPE/PVA film showed promise as a real-time indicator for monitoring shrimp freshness, maintaining sensitivity to spoilage even after six months of storage. These findings advance the advancement of green LCNF technologies, providing eco-friendly solutions for valorizing bamboo shoot shells and enhancing the application of LCNF in Pickering emulsions.

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Smart packaging material capable of real-time monitoring of food freshness is essential for ensuring food safe. At present, colorimetric ammonia-sensing smart film often possesses issues with complicated production, high cost, and inferior long-term colour stability. Herein, Zinc­copper bimetallic organic framework (ZnCu-BTC, BTC = 1,3,5-benzenetricarboxylate acid) nanorods with colorimetric ammonia-responsiveness were synthesized by adopting facile aqueous solution method, which were then explored as nano inclusions in potato starch/polyvinyl alcohol (PS/PVA) composite film towards developing high-performance smart packaging material. The results demonstrated that the introduction of ZnCu-BTC nanorods within PS/PVA brought about remarkable improvement in blend compatibility, accompanied by a boost in tensile strength to 47.2 MPa, as well as enhanced ultraviolet (UV) blocking efficacy (over 95.0 %). Additionally, the barrier properties of PS/PVA film against water vapor and oxygen were fortified due to the addition of ZnCu-BTC. More importantly, the developed PS/PVA/ZnCu-BTC nanocomposite film displayed satisfactory antibacterial activity (over 99 %) against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), favorable colorimetric ammonia-sensing ability, and long-term colour stability. The ZnCu-BTC incorporated PS/PVA nanocomposite film could grant real-time detection of prawn freshness decline via remarkable colour change, indicating vast promise for smart food packaging applications.

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A novel type of colorimetric/fluorescent nanopaper indicator has been developed from the melt-extruded poly (vinyl alcohol-co-ethylene) nanofibers with surface anchored metal-organic frameworks (MOFs) by an interfacial coordination strategy. Specifically, the fluorescein isothiocyanate molecules could be anchored to the nanofiber surface by nickel ions and co-assembled into a hydrophilic nanocoating via a dynamic water/alcohol solvent evaporation method. Interestingly, this hydrophilic surface enables fast adsorption of moistures and interaction with biological amine vapors, resulting a saffron cake-layer of MOF nanocrystals with ultra-sensitive colorimetric/fluorescent responses based on an alkaline pH/ammonia induced competitive coordination mechanism. Finally, these porous nanofibrous matrix and active nanocoating make the nano-paper an ultra-sensitive optical platform for in-situ monitoring of the shrimp freshness from mins to weeks. Therefore, this composite film shows great potential into advanced paper-based indicators for food quality control and safety in processing industry.

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With an increasing emphasis on food safety and public health, there is an ongoing effort to develop reliable, non-invasive methods to assess the freshness of diverse food products. Chitosan-based food freshness indicators, leveraging properties such as biocompatibility, biodegradability, non-toxicity, and high stability, offer an innovative approach for real-time monitoring of food quality during storage and transportation. This review introduces intelligent food freshness indicators, specifically those utilizing pH-sensitive dyes like anthocyanins, curcumin, alizarin, shikonin, and betacyanin. It highlights the benefits of chitosan-based intelligent food freshness indicators, emphasizing improvements in barrier and mechanical properties, antibacterial activity, and composite film solubility. The application of these indicators in the food industry is then explored, alongside a concise overview of chitosan's limitations. The paper concludes by discussing the challenges and potential areas for future research in the development of intelligent food freshness indicators using chitosan. Thus, chitosan-based smart food preservation indicators represent an innovative approach to providing real-time data for monitoring food quality, offering valuable insights to both customers and retailers, and playing a pivotal role in advancing the food industry.

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Increasing concern over the safety of consumable products, particularly aquatic products, due to freshness issues, has become a pressing issue. Therefore, ensuring the quality and safety of aquatic products is paramount. To address this, a dual-mode colorimetric-fluorescence sensor utilizing Ce-MOF as a mimic peroxidase to detect H2S was developed. Ce-MOF was prepared by a conventional solvothermal synthesis method. Ce-MOF catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) by hydrogen peroxide (H2O2) to produce blue oxidized TMB (oxTMB). When dissolved, hydrogen sulfide (H2S) was present in the solution, and it inhibited the catalytic effect of Ce-MOF and caused the color of the solution to fade from blue to colorless. This change provided an intuitive indication for the detection of H2S. Through steady-state dynamic analysis, the working mechanism of this sensor was elucidated. The sensor exhibited pronounced color changes from blue to colorless, accompanied by a shift in fluorescence from none to light blue. Additionally, UV-vis absorption demonstrated a linear correlation with the H2S concentration, ranging from 200 to 2300 µM, with high sensitivity (limit of detection, LOD = 0.262 µM). Fluorescence intensity also showed a linear correlation, ranging from 16 to 320 µM, with high selectivity and sensitivity (LOD = 0.156 µM). These results underscore the sensor's effectiveness in detecting H2S. Furthermore, the sensor enhanced the accuracy of H2S detection and fulfilled the requirements for assessing food freshness and safety.

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In this study, the ß-cyclodextrin encapsulated betanin (BET@ß-CD) with improved thermal stability and retention as well as the berberine (BBR) with aggregate induced luminescence effect were incorporated into corn amylose (CA) biomatrix to develop colorimetric/fluorescent dual-channel smart film. Results shown that the added functional components were uniformly distributed in the film matrix. The high tensile strength (78.87%), low water solubility (31.15%) and water vapor permeability (1.24 × 10-10 g Pa-1 s-1 m-1) of the film predicted its acceptable stability. It was worth mentioning that the film displayed excellent responsiveness to volatile ammonia (0.025-25 mg/mL) with at least 4 times recyclability. Application experiment demonstrated that the film can achieve macroscopic dynamic monitoring of the freshness of shrimps stored at 25 °C, 4 °C, -20 °C under daylight (red to yellow) and UV light (yellow-green to blue-green). Thus, the study suggests an attractive and effective strategy for constructing dual-mode smart packaging materials for food freshness detection.

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Herein, the nanolignin-containing cellulose nanofibrils (LCNF)-enabled ratiometric fluorescent bio-nanocomposite film is developed. Interestingly, the inclusion of LCNF in the cellulose-based film enhances the detecting performance of food freshness, such as high sensitivity to biogenic amines (BAs) (limit of detection (LOD) of up to 1.83 ppm) and ultrahigh discernible fluorescence color difference (ΔE = 113.11). The underlying mechanisms are the fluorescence resonance energy transfer (FRET), π - π interaction, and cation - π interaction between LCNF and fluorescein isothiocyanate (FITC), as well as the increased hydrophobicity due to lignin, which increases the interactions of amines with FITC. Its color stability (up to 28 days) and mechanical property (49.4 Mpa) are simultaneously improved. Furthermore, a smartphone based detecting platform is developed to achieve access to food safety. This work presents a novel technology, which can have a great potential in the field of food packaging and safety.

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A spindle-like Cu-based framework (Cu-Trp, Trp = L-Tryptophan) nanocrystal with ammonia-responsiveness was fabricated via simple aqueous solution approach, and it was subsequently explored as a functional compatibilizer of carboxymethyl starch/polyvinyl alcohol (CMS/PVA) blend toward constructing high-performance intelligent packaging films. The results showed that incorporation of Cu-Trp nanocrystal into CMS/PVA blend resulted in significant promotions regarding to the compatibility, mechanical strength (42.92 MPa), UV-blocking (with UV transmittance of only 2.4%), and water vapor barrier effectiveness of the blend film. Besides, the constructed CMS/PVA/Cu-Trp nanocomposite film exhibited superb long-term color stability, favorable antibacterial capacity (over 98.0%) toward both E. coli and S. aureus bacteria, as well as color change ability under ammonia environment. Importantly, the application trial confirmed that the CMS/PVA/Cu-Trp nanocomposite film is capable of visually monitoring shrimp spoilage during storage. These results implied that the CMS/PVA/Cu-Trp nanocomposite film holds tremendous potential as an intelligent active packaging material.

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Rapid and sensitive monitoring of pH and histamine is crucial for bridging biological and food systems and identifying corresponding abnormal situations. Herein, N-doped carbon dots (CDs) are fabricated by a hydrothermal method employing dipicolinic acid and o-phenylenediamine as precursors. The CDs exhibit colorimetric and fluorescent dual-mode responses to track pH and histamine variations in living cells and food freshness, respectively. The aggregation-induced emission enhancement and intramolecular charge transfer result in a decrease in absorbance and an increase in fluorescence, which become readily apparent as the pH changes from acidic to neutral. This property enables precise differentiation between normal and cancerous cells. Furthermore, given the intrinsic basicity of histamine, pH-responsive CDs are advantageous for additional colorimetric and fluorescent monitoring of histamine in food freshness, achieving linearities of 25-1000 µM and 30-1000 µM, respectively, which are broader than those of alternative nanoprobes. Interestingly, the smartphone-integrated sensing platform can portably and visually evaluate pH and histamine changes due to sensitive color changes. Therefore, the sensor not only establishes a dynamic connection between pH and histamine for the purposes of biological and food monitoring, but also presents a novel approach for developing a multifunctional biosensor that can accomplish environmental monitoring and biosensing simultaneously.

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Intelligent packaging embedded with food freshness indicators can monitor food quality and be deployed for food safety and cutting food waste. The innovative nano-inks for dynamic shelf-life printing based on natural food colorant with application in real-time monitoring of shrimp freshness were prepared. Co-assembly of saffron petal anthocyanin (SPA) with hydrophobic curcumin (Cur) into chitin nano-scaffold (particle sizes around 26 ± 8 nm) could deliver hindering SPA leaching, confirmed by FT-IR, FE-SEM, AFM, and color stability test. The best response to pH-sensitivity was found in a ratio of (1:4) Cur/SPA (30% (v/w) in ChNFs that was correlated with the chemical and microbial changes of shrimp during shrimp freshness. However, smart screen-printed inks signified higher responsiveness to pH changes than FFI films. Therefore, smart-printed indicators introduced the excellent potential for a short response time, easy, cost-effective, eco-friendly, co-assembly, great color stabilities, and lifetime for nondestructively freshness monitoring foods and supplements.

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Food packaging detection devices have attracted attention to optimize storage situations and reduce food spoilage. However, low-cost and highly sensitive multifunctional sensors for detecting both food freshness and packaging pressure are still lacking. In this study, a multifunctional sensor was developed consisting of a MXene coated alcohol-soluble polyurethane fiber network (MXene/APU) and composite biohydrogel films made of konjac glucomannan, chitosan, and blueberry anthocyanin (KCB). Based on the pressure sensitivity of MXene/APU and the color changes of KCB in response to pH values, the sensor can detect internal package bulging, external squeezing, and food deterioration. The pressure sensor shows a sensitivity of 1.16 kPa-1, a response time of 200 ms, a wide strain range of 1092%, and stability over multiple loops. The pressure sensor could detect human motion and identify surface morphologies. The excellent sensor performance was attributed to the porous structure and large specific surface area of microfiber networks, conductivity of MXene nanosheets, and protective effect of KCB films coated on the conductive membrane. Besides, the microfluidic blow-spinning method used to prepare microfiber networks showed the advantages of low energy consumption and high production efficiency. Based on the color changes of blueberry anthocyanin loaded in KCB films in response to pH, the sensor realized sensitive spoilage detection of food containing protein. This study provides a new multifunctional food packaging sensing device and a greater understanding of the optimization and application of related devices.

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This study developed an innovative approach that combines a colourimetric sensor array (CSA) composed of twelve pH-response dyes with advanced algorithms, aiming to detect amine gases and assess the freshness of chilled beef. With the assistance of multivariate statistical analysis, the sensor array can effectively distinguish five amine gases and enable rapid quantification of trimethylamine vapour with a limit of detection (LOD) of 8.02 ppb and visually monitor the fresh levels of chilled beef. Moreover, the utilization of deep learning models (ResNet34, VGG16, and GoogleNet) for chilled beef freshness evaluation achieved an overall accuracy of 98.0 %. Furthermore, t-distributed stochastic neighbour embedding (t-SNE) visualized the feature extraction process and provided explanations to understand the classification process of deep learning. The results demonstrated that applying deep learning techniques in the process of pattern recognition of CSA can help in realizing the rapid, robust, and accurate assessment of chilled beef freshness.

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Comprehensive attention should be paid to the potential food spoilage in food transport. However, there is a problem of freshness destruction by repeated freezing and thawing during the cold chain transport. Herein, a fluorescent hydrogel with N-doped green-emitting carbon dots (N-GCDs), bovine serum albumin-gold nanoclusters (BSA-AuNCs) as fluorescent probes and polyvinyl alcohol-sodium alginate hydrogel as carrier matrix was developed to continuously detect temperature and freshness. Due to the solvatochromic effect of N-GCDs, when the temperature surpassed the threshold, the mixture of water and dimethyl sulfoxide underwent a phase transition and melted into the gel, changing the fluorescence color to realize the temperature monitoring. Then, due to the pH effect of BSA-AuNCs, the gel could respond to pH changes in food deterioration to monitor the food freshness. Thus, the changes of both fluorescence color and intensity of the hydrogel provides a new method for visual and portable authenticity of food freshness.

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pH-responsive intelligent films for food freshness monitoring have attracted great attentions recently. In this study, several intelligent films based on chitosan (CS), polyvinyl alcohol (PVA), and grape skin anthocyanin (GSA) were prepared, and the effect of film-forming solution pH on the properties of intelligent films was investigated. The results of SEM, FTIR, XRD and TGA displayed that the hydrogen bond between CS and GSA was strong at strong acidic conditions (2.0-2.5), and it weakened at weak acidic conditions (3.0-4.5). Meanwhile, the hydrogen bond between PVA and GSA was negligible under strong acidic conditions, and it appeared under weak acidic conditions. Consequently, the films fabricated under weak acidic conditions displayed lower water solubility, lower water vapor permeability, and higher elongation at break. The tensile strength of films increased firstly and subsequently decreased with pH increasing, reaching a maximum value of 31.44 MPa at pH 3.5. Additionally, the films prepared at pH 2.5 and 4.0 showed the best color responsiveness to ammonia and acetic acid, respectively. Overall, the intelligent films prepared under variant pH have the potential to realize the goal of monitoring the freshness of different types of food, thereby expanding the application subject of anthocyanins-based intelligent films.

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The real-time monitoring of food freshness in refrigerators is of significant importance in detecting potential food spoiling and preventing serious health issues. One method that is commonly reported and has received substantial attention is the discrimination of food freshness via the tracking of volatile molecules. Nevertheless, the ambient environment of low temperature (normally below 4 °C) and high humidity (90% R.H.), as well as poor selectivity in sensing gas species remain the challenge. In this research, an integrated smart gas-tracking device is designed and fabricated. By applying pump voltage on the yttria-stabilized zirconia (YSZ) membrane, the oxygen concentration in the testing chamber can be manually tailored. Due to the working principle of the sensor following the mixed potential behavior, distinct differences in sensitivity and selectivity are observed for the sensor that operated at different oxygen concentrations. Typically, the sensor gives satisfactory selectivity to H2S, NH3, and C2H5OH at the oxygen concentrations of 10%, 30%, and 40%, respectively. In addition, an acceptable response/recovery rate (within 24 s) is also confirmed. Finally, a refrigerator prototype that includes the smart gas sensor is built, and satisfactory performance in discriminating food freshness status of fresh or semi-fresh is verified for the proposed refrigerator prototype. In conclusion, these aforementioned promising results suggest that the proposed integrated smart gas sensor could be a potential candidate for alarming food spoilage.

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With the increasing concerns of food safety and public health, tremendous efforts have been concentrated on the development of effective, reliable, nondestructive methods to evaluate the freshness level of different kinds of food. Natural colorants-based intelligent colorimetric indicators which are typically constructed with natural colorants and polymer matrices has been regarded as an innovative approach to notify the customers and retailers of the food quality during the storage and transportation procedure in real-time. This review briefly elucidates the mechanism of natural colorants used for intelligent colorimetric indicators and fabrication methodologies of natural colorants-based food freshness indicators. Subsequently, their multifunctional applications in intelligent food packaging systems like antioxidant packaging, antimicrobial packaging, biodegradable packaging, UV-blocking packaging and inkless packaging are well introduced. This paper also summarizes several optimizing strategies for the practical application of this advanced technology from different perspectives. Strategies like adopting a hydrophobic matrix, constructing double-layer film and encapsulation have been developed to improve the stability of the indicators. Co-pigmentation, metal ion complexation, pigment-mixing and using substrates with high surface area are proved to be effective to enhance the sensitivity of the indicators. Approaches include multi-index evaluation, machine learning and smartphone-assisted evaluation have been proven to improve the accuracy of the intelligent food freshness indicators. Finally, future research opportunities and challenges are proposed. Based on the fundamental understanding of natural colorants-based intelligent colorimetric food freshness indicators, and the latest research and findings from literature, this review article will help to develop better, lower cost and more reliable food freshness evaluation technique for modern food industry.

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Food safety is a pressing concern for human society, as it directly impacts people's lives, while food freshness serves as one of the most crucial indicators in ensuring food safety. There exist diverse techniques for monitoring food freshness, among which intelligent packaging based on artificial intelligence technology boasts the advantages of low cost, high efficiency, fast speed and wide applicability; however, it is currently underutilized. By analyzing the current research status of intelligent packaging both domestically and internationally, this paper provides a clear classification of intelligent packaging technology. Additionally, it outlines the advantages and disadvantages of using intelligent packaging technology for food freshness detection methods, while summarizing the latest research progress in applying artificial intelligence-based technologies to food freshness detection through intelligent packaging. Finally, the author points out the limitations of the current research, and anticipates future developments in artificial intelligence technology for assisting freshness detection in intelligent packaging. This will provide valuable insights for the future development of intelligent packaging in the field of food freshness detection.

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To combat food freshness fraud, it is urgent to develop a method which could realize the detection of biogenic amines (BAs) present in food. In our study, we developed a colorimetric and ratiometric fluorescence dual-mode sensor which integrated with silver metallization-based response system of AIE liposome + OPD + RSM + Ag+ toward BAs in foods for fighting freshness fraud. With the hydrolysis from the alkaline of BAs to resorcinol monoacetate (RSM), the production resorcinol (RS) could metallize silver ion (Ag+) to silver atoms (Ag0) which could lead to a BAs concentration-dependent decrease of the oxidation product 2,3-diaminophenothiazine (DAP) of Ag+ to o-phenylenediamine (OPD). As a result, the dual-mode sensor has a low detection limit and wide linear range in the spiked detection of soy products, pork and milk samples for BAs. Thus, providing a reliable method for food safety and forestalling food freshness fraud.

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Biogenic amines (BAs), which naturally occur as chemicals in seafood, are indicators of food freshness and quality. High concentrations of BAs can cause an undesirable inflammatory response. However, traditional detection methods cannot meet the needs of rapid analysis nowadays. It is essential to explore a simple and valid method to monitor the food quality. Herein, we design and prepare a nanoclay-based turn on fluorescent material with BAs response, which could be used for the real-time and visual detection of raw fish freshness. As the concentration of BAs increase, the sensor of the fluorescence signal is significantly enhanced. The sensor demonstrated wonderful response and sensitivity which showed a detection limit of 0.935 mg/L for typical BAs histamine within a linear range of 2-14 mg/L in an aqueous solution. More importantly, we developed a responsive BAs device by doping the sensor into polyvinyl alcohol (PVA), which is well applied as a rapid-responsive fluorescent marker for visual monitoring the freshness of raw fish.

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