Flexible time–temperature indicator: a versatile platform for laminated paper-based analytical devices

  • Ali Turab Jafry
  • Hosub Lim
  • Won-Kee Sung
  • Jinkee Lee
Research Paper


Time–temperature indicators are devices employed for monitoring thermal history of perishable food products from storage to consumption. As the food industry has opted for intelligent packaging, which also involves thin foldable wrappings, a requirement arises for a flexible device capable of attaching and sensing on a curved product surface. In this study, we have fabricated a distance-based flexible time–temperature indicator (FTTI) by employing electronic cutting machine and through press lamination of thermoplastic films; we have incorporated the FTTI with a unique starting actuation switch made of thin (150 μm) cover glass. Flow profile in 0.45 μm nitrocellulose membrane is measured for oleic, octanoic, and decanoic acids representing test temperatures of 5, 15 and 30 °C, respectively. Results demonstrate the sensor to be robust and flexible with precise responsiveness to oscillating temperature conditions. Further improvement in time-scale is achieved by employing a series of fan-shaped cut channels. This two-dimensional flow increases the device time by 170% in comparison with straight channel and improves scale readability by achieving a linear distance-time relation in the porous membrane. The advantages of low cost, simple design, freedom from equipment, robustness, and flexibility render the FTTI a versatile platform for distance-based diagnostics, food quality control, and environmental monitoring devices.


Time–temperature indicator Laminated paper-based device Food quality control Fan-shaped channel 



We appreciate the support provided by the High Value-added Food Technology Development Program by the Ministry of Agriculture, Food, and Rural Affairs (313023-3), Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, Information and Communications Technology (ICT) & Future Planning (2014R1A1A1037730) and the project titled ‘Development of Freshness Maintenance System Using Slightly Acidic Hypochlorous Seawater Ice’, funded by the Ministry of Oceans and Fisheries, Korea (No. 20150494).


  1. Benner EM, Petsev DN (2013) Potential flow in the presence of a sudden expansion: application to capillary driven transport in porous media. Phys Rev E 87:033008CrossRefGoogle Scholar
  2. Berli CLA, Kler PA (2016) A quantitative model for lateral flow assays. Microfluid Nanofluid 20:104CrossRefGoogle Scholar
  3. Bruzewicz DA, Reches M, Whitesides GM (2008) Low-cost printing of poly(dimethylsiloxane) barriers to define microchannels in paper. Anal Chem 80:3387–3392CrossRefGoogle Scholar
  4. Cai L, Xu C, Lin S, Luo J, Wu M, Yang F (2014) A simple paper-based sensor fabricated by selective wet etching of silanized filter paper using a paper mask. Biomicrofluidics 8:056504CrossRefGoogle Scholar
  5. Carrilho E, Martinez AW, Whitesides GM (2009) Understanding wax printing: a simple micropatterning process for paper-based microfluidics. Anal Chem 81:7091–7095CrossRefGoogle Scholar
  6. Cassano CL, Fan ZH (2013) Laminated paper-based analytical devices (LPAD): fabrication, characterization, and assays. Microfluid Nanofluid 15:173–181CrossRefGoogle Scholar
  7. Chumpitaz LDA, Coutinho LF, Meirelles AJA (1999) Surface tension of fatty acids and triglycerides. J Am Oil Chem Soc 76:379–382CrossRefGoogle Scholar
  8. Dullien FA (1979) Porous media: fluid transport and pore structure. Academic press, New York, pp 170–174Google Scholar
  9. Dungchai W, Chailapakul O, Henry CS (2011) A low-cost, simple, and rapid fabrication method for paper-based microfluidics using wax screen-printing. Analyst 136:77–82CrossRefGoogle Scholar
  10. Ellouze M, Augustin JC (2010) Applicability of biological time temperature integrators as quality and safety indicators for meat products. Int J Food Microbiol 138:119–129CrossRefGoogle Scholar
  11. Fenton EM, Mascarenas MR, López GP, Sibbett SS (2009) Multiplex lateral-flow test strips fabricated by two-dimensional shaping. ACS Appl Mater Interfaces 1:124–129CrossRefGoogle Scholar
  12. Fu E, Lutz B, Kauffman P, Yager P (2010) Controlled reagent transport in disposable 2D paper networks. Lab Chip 10:918–920CrossRefGoogle Scholar
  13. Fu E, Ramsey SA, Kauffman P, Lutz B, Yager P (2011) Transport in two-dimensional paper networks. Microfluid Nanofluid 10:29–35CrossRefGoogle Scholar
  14. Fu E, Liang T, Spicar-Mihalic P, Houghtaling J, Ramachandran S, Yager P (2012) Two-dimensional paper network format that enables simple multistep assays for use in low-resource settings in the context of malaria antigen detection. Anal Chem 84:4574–4579CrossRefGoogle Scholar
  15. Galagan Y, Su WF (2008) Fadable ink for time–temperature control of food freshness: novel new time–temperature indicator. Food Res Int 41:653–657CrossRefGoogle Scholar
  16. Gao X et al (2014) Dual-scaled porous nitrocellulose membranes with underwater superoleophobicity for highly efficient oil/water separation. Adv Mater 26:1771–1775CrossRefGoogle Scholar
  17. Gliński J, Przybylski J, Chavepeyer G, Platten J-K (2001) Untypical surface properties of the system caprylic Acid + n-Propyl acetate. J Solution Chem 30:925–936CrossRefGoogle Scholar
  18. Gou M et al (2010) Time–temperature chromatic sensor based on polydiacetylene (PDA) vesicle and amphiphilic copolymer. Sens Actuators, B-Chem 150:406–411CrossRefGoogle Scholar
  19. Guiavarc’h Y, Van Loey A, Zuber F, Hendrickx M (2004) Bacillus licheniformis α-amylase immobilized on glass beads and equilibrated at low moisture content: potentials as a Time-Temperature Integrator for sterilisation processes. Innov Food Sci Emerg 5:317–325CrossRefGoogle Scholar
  20. He Y, Wu Y, Fu J-Z, Wu W-B (2015) Fabrication of paper-based microfluidic analysis devices: a review. RSC Adv 5:78109–78127CrossRefGoogle Scholar
  21. Hong S, Kim W (2015) Dynamics of water imbibition through paper channels with wax boundaries. Microfluid Nanofluid 19:845–853CrossRefGoogle Scholar
  22. Jafry AT, Lim H, Kang SI, Suk JW, Lee J (2016) A comparative study of paper-based microfluidic devices with respect to channel geometry. Colloids Surf A 492:190–198CrossRefGoogle Scholar
  23. Jahanshahi-Anbuhi S et al (2012) Creating fast flow channels in paper fluidic devices to control timing of sequential reactions. Lab Chip 12:5079–5085CrossRefGoogle Scholar
  24. Jang I, Song S (2015) Facile and precise flow control for a paper-based microfluidic device through varying paper permeability. Lab Chip 15:3405–3412CrossRefGoogle Scholar
  25. Jiang X, Fan ZH (2016) Fabrication and operation of paper-based analytical devices. Annu Rev Anal Chem 9:203–222CrossRefGoogle Scholar
  26. Kauffman P, Fu E, Lutz B, Yager P (2010) Visualization and measurement of flow in two-dimensional paper networks. Lab Chip 10:2614–2617CrossRefGoogle Scholar
  27. Kiesvaara J, Yliruusi J (1993) The use of the Washburn method in determining the contact angles of lactose powder. Int J Pharm 92:81–88CrossRefGoogle Scholar
  28. Kim K, Kim E, Lee SJ (2012) New enzymatic time–temperature integrator (TTI) that uses laccase. J Food Eng 113:118–123CrossRefGoogle Scholar
  29. Kirk-Othmer (1993) The Kirk-Othmer Encyclopedia of chemical technology, vol 1. Wiley, Hoboken, pp 147–168Google Scholar
  30. Kokalj T, Park Y, Vencelj M, Jenko M, Lee LP (2014) Self-powered imbibing microfluidic pump by liquid encapsulation: SIMPLE. Lab Chip 14:4329–4333CrossRefGoogle Scholar
  31. Lee SJ, Jung SW (2013) Time-temperature indicator, method for manufacturing the time-temperature indicator, quality guarantee system using the time-temperature indicator, and quality guarantee method using the quality guarantee system. WO 2013002552 A3Google Scholar
  32. Li X, Tian J, Nguyen T, Shen W (2008) Paper-based microfluidic devices by plasma treatment. Anal Chem 80:9131–9134CrossRefGoogle Scholar
  33. Lim S, Gunasekaran S, Imm J-Y (2012) Gelatin-templated gold nanoparticles as novel time-temperature indicator. J Food Sci 77:N45–N49CrossRefGoogle Scholar
  34. Määttänen A, Fors D, Wang S, Valtakari D, Ihalainen P, Peltonen J (2011) Paper-based planar reaction arrays for printed diagnostics. Sens Actuators, B-Chem 160:1404–1412CrossRefGoogle Scholar
  35. Manske WJ (1976) Selected time interval indicating device. US 3954011 AGoogle Scholar
  36. Martinez AW, Phillips ST, Butte MJ, Whitesides GM (2007) Patterned paper as a platform for inexpensive, low-volume, portable bioassays. Angew Chem Int Ed 46:1318–1320CrossRefGoogle Scholar
  37. Martinez AW, Phillips ST, Whitesides GM, Carrilho E (2010) Diagnostics for the developing world: microfluidic paper-based analytical devices. Anal Chem 82:3–10CrossRefGoogle Scholar
  38. MatWeb L (2017) Flexural strength testing of plastics. http://www.matweb.com/reference/flexuralstrength.aspx. Accessed 01 Feb 2017
  39. Mendez S et al (2010) Imbibition in porous membranes of complex shape: quasi-stationary flow in thin rectangular segments. Langmuir 26:1380–1385CrossRefGoogle Scholar
  40. Mu X, Zhang L, Chang S, Cui W, Zheng Z (2014) Multiplex microfluidic paper-based immunoassay for the diagnosis of hepatitis c virus infection. Anal Chem 86:5338–5344CrossRefGoogle Scholar
  41. Nie J, Zhang Y, Lin L, Zhou C, Li S, Zhang L, Li J (2012) Low-cost fabrication of paper-based microfluidic devices by one-step plotting. Anal Chem 84:6331–6335CrossRefGoogle Scholar
  42. Noh H, Phillips ST (2010) Metering the capillary-driven flow of fluids in paper-based microfluidic devices. Anal Chem 82:4181–4187CrossRefGoogle Scholar
  43. Norrby H, Nygårdh M (2011) Label having a temperature-monitoring function, a package for goods provided with a label, as well as a method and equipment for the application of labels to packages for goods. US 7878410 B2Google Scholar
  44. Park J, Shin J, Park J-K (2016) Experimental analysis of porosity and permeability in pressed paper. Micromachines 7:48CrossRefGoogle Scholar
  45. Sameenoi Y, Nongkai PN, Nouanthavong S, Henry CS, Nacapricha D (2014) One-step polymer screen-printing for microfluidic paper-based analytical device (μPAD) fabrication. Analyst 139:6580–6588CrossRefGoogle Scholar
  46. Starov VM, Velarde MG, Radke CJ (2007) Wetting and Spreading Dynamics vol 138. Surfactant science series. Taylor & Francis Group, Boca Raton, FloridaMATHGoogle Scholar
  47. Timestrip® (2016) Timestrip PLUS. http://timestrip.com/products/timestrip-plus/. Accessed 15 Nov 2016
  48. Toley BJ, McKenzie B, Liang T, Buser JR, Yager P, Fu E (2013) Tunable-delay shunts for paper microfluidic devices. Anal Chem 85:11545–11552CrossRefGoogle Scholar
  49. Vanderroost M, Ragaert P, Devlieghere F, De Meulenaer B (2014) Intelligent food packaging: the next generation. Trends Food Sci Tech 39:47–62CrossRefGoogle Scholar
  50. Wang X, Hagen JA, Papautsky I (2013) Paper pump for passive and programmable transport. Biomicrofluidics 7:014107CrossRefGoogle Scholar
  51. Wang S, Liu X, Yang M, Zhang Y, Xiang K, Tang R (2015) Review of time temperature indicators as quality monitors in food packaging. Packag Technol Sci 28:839–867CrossRefGoogle Scholar
  52. Washburn EW (1921) The dynamics of capillary flow. Phys Rev 17:273–283CrossRefGoogle Scholar
  53. Wei X et al (2016) Microfluidic distance readout sweet hydrogel integrated paper-based analytical device (μDiSH-PAD) for visual quantitative point-of-care testing. Anal Chem 88:2345–2352CrossRefGoogle Scholar
  54. Whitesides GM (2006) The origins and the future of microfluidics. Nature 442:368–373CrossRefGoogle Scholar
  55. Zhang C et al (2013) Time–Temperature indicator for perishable products based on kinetically programmable Ag overgrowth on Au nanorods. ACS Nano 7:4561–4568CrossRefGoogle Scholar
  56. Zweben C, Smith W, Wardle M (1979) Test methods for fiber tensile strength, composite flexural modulus, and properties of fabric-reinforced laminates. In: Composite Materials: Testing and Design (Fifth Conference), 1979. ASTM InternationalGoogle Scholar
  57. Zweig SE (2005) Electronic time-temperature indicator. US 6950028 B2Google Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2017

Authors and Affiliations

  • Ali Turab Jafry
    • 1
  • Hosub Lim
    • 1
  • Won-Kee Sung
    • 2
  • Jinkee Lee
    • 1
  1. 1.School of Mechanical EngineeringSungkyunkwan UniversitySuwonRepublic of Korea
  2. 2.EzLabYongin-siRepublic of Korea

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