A Step Towards Miniaturized Milk Adulteration Detection System: Smartphone-Based Accurate pH Sensing Using Electrospun Halochromic Nanofibers

Development of an economical miniaturized platform for monitoring inherent biophysical properties of milk is imperative for tamper-proof milk adulteration detection. Towards this, herein, we demonstrate synthesis and evaluation of a paper-based scalable pH sensor derived from electrospun halochromic nanofibers. The sensor manifests into three unique color-signatures corresponding to pure (6.6 ≤ pH ≤ 6.9), acidic (pH < 6.6), and basic (pH > 6.9) milk samples, enabling a colorimetric detection mechanism. In a practical prototype, color transitions on the sensor strips are captured using smartphone camera and subsequently assigned to one of the three pH ranges using an image-based classifier. Specifically, we implemented three well-known machine learning algorithms and compared their classification performances. For a standard training-to-test ratio of 80:20, support vector machines achieved nearly perfect classification with average accuracy of 99.71%.

[1]  Chunyan Sun,et al.  Visual detection of melamine in raw milk by label-free silver nanoparticles , 2012 .

[2]  R. Marshall,et al.  Microbiological Spoilage of Dairy Products , 2009 .

[3]  Tong Boon Tang,et al.  Electronic tongue for fresh milk assessment A revisit of using pH as indicator , 2013, 2013 IEEE International Conference on Circuits and Systems (ICCAS).

[4]  Gary D. Christian,et al.  Single fibre optic fluorescence pH probe , 1987 .

[5]  Yu Chen,et al.  Paper based platform for colorimetric sensing of dissolved NH3 and CO2. , 2015, Biosensors & bioelectronics.

[6]  Iline Steyaert,et al.  Polycaprolactone and polycaprolactone/chitosan nanofibres functionalised with the pH-sensitive dye Nitrazine Yellow. , 2013, Carbohydrate polymers.

[7]  S. Marzouk,et al.  Improved electrodeposited iridium oxide pH sensor fabricated on etched titanium substrates. , 2003, Analytical chemistry.

[8]  Anatoly V. Zherdev,et al.  Quantum dot-based lateral flow immunoassay for detection of chloramphenicol in milk , 2013, Analytical and Bioanalytical Chemistry.

[9]  Peter E. Hart,et al.  Nearest neighbor pattern classification , 1967, IEEE Trans. Inf. Theory.

[10]  Shovan K. Majumder,et al.  Detection of Urea Adulteration in Milk Using Near-Infrared Raman Spectroscopy , 2014, Food Analytical Methods.

[11]  D. Reneker,et al.  Nanometre diameter fibres of polymer, produced by electrospinning , 1996 .

[12]  Jun-shi Chen,et al.  A worldwide food safety concern in 2008--melamine-contaminated infant formula in China caused urinary tract stone in 290,000 children in China. , 2009, Chinese medical journal.

[13]  Tianlu Chen,et al.  Phenol red immobilized PVA membrane for an optical pH sensor with two determination ranges and long-term stability , 2005 .

[14]  Douglas G. Dalgleish,et al.  Effect of temperature and pH on the interactions of whey proteins with casein micelles in skim milk , 1996 .

[15]  Suryasnata Tripathy,et al.  Facile, low-cost, halochromic platform using electrospun nanofibers for milk adulteration detection , 2016, 2016 3rd International Conference on Emerging Electronics (ICEE).

[16]  Michael C. Petty,et al.  A novel technique for the detection of added water to full fat milk using single frequency admittance measurements , 2003 .

[17]  Sumaporn Kasemsumran,et al.  Feasibility of Near-Infrared Spectroscopy to Detect and to Quantify Adulterants in Cow Milk , 2007, Analytical sciences : the international journal of the Japan Society for Analytical Chemistry.

[18]  Georgia-Paraskevi Nikoleli,et al.  Construction of a simple optical sensor based on air stable lipid film with incorporated urease for the rapid detection of urea in milk. , 2010, Analytica chimica acta.

[19]  Nam Sun Wang,et al.  Milk Spoilage: Methods and Practices of Detecting Milk Quality , 2013 .

[20]  Karel Macek,et al.  Pareto Principle in Datamining: an Above-Average Fencing Algorithm , 2008 .

[21]  Corinna Cortes,et al.  Support-Vector Networks , 1995, Machine Learning.

[22]  Hüseyin Erdem,et al.  Relationships Between Milk Somatic Cell Count and pH in Dairy Cows , 2010 .

[23]  Zia Ullah Khokhar,et al.  Quantitation and Risk Assessment of Chemical Adulterants in Milk Using UHPLC Coupled to Photodiode Array and Differential Refractive Index Detectors , 2016, Food Analytical Methods.

[24]  Iline Steyaert,et al.  Dye Modification of Nanofibrous Silicon Oxide Membranes for Colorimetric HCl and NH3 Sensing , 2016 .

[25]  Banshi D Gupta,et al.  Surface plasmon resonance based fiber optic pH sensor utilizing Ag/ITO/Al/hydrogel layers. , 2013, The Analyst.

[26]  Katrina Campbell,et al.  Impacts of Milk Fraud on Food Safety and Nutrition with Special Emphasis on Developing Countries. , 2016, Comprehensive reviews in food science and food safety.

[27]  Yi-Zeng Liang,et al.  Monte Carlo cross validation , 2001 .

[28]  Suryasnata Tripathy,et al.  A comprehensive approach for milk adulteration detection using inherent bio-physical properties as 'Universal Markers': Towards a miniaturized adulteration detection platform. , 2017, Food chemistry.

[29]  Neeraj Gandhi,et al.  Milk Preservatives and Adulterants: Processing, Regulatory and Safety Issues , 2015 .

[30]  Grant Abernethy,et al.  Rapid detection of economic adulterants in fresh milk by liquid chromatography-tandem mass spectrometry. , 2013, Journal of chromatography. A.

[31]  P. Manzi,et al.  Melamine Detection in Milk and Dairy Products: Traditional Analytical Methods and Recent Developments , 2017, Food Analytical Methods.

[32]  P. Li,et al.  Melamine toxicity and the kidney. , 2009, Journal of the American Society of Nephrology : JASN.

[33]  Kurt Hornik,et al.  FEED FORWARD NETWORKS ARE UNIVERSAL APPROXIMATORS , 1989 .

[34]  Chun-Nan Kuo,et al.  Bromocresol Green/Mesoporous Silica Adsorbent for Ammonia Gas Sensing via an Optical Sensing Instrument , 2011, Sensors.

[35]  Zia Ullah Khokhar,et al.  Erratum to: Quantitation and Risk Assessment of Chemical Adulterants in Milk Using UHPLC Coupled to Photodiode Array and Differential Refractive Index Detectors , 2016, Food Analytical Methods.

[36]  L. Rodriguez-Saona,et al.  Rapid detection and quantification of milk adulteration using infrared microspectroscopy and chemometrics analysis. , 2013, Food chemistry.

[37]  Jens Lienig,et al.  Review on Hydrogel-based pH Sensors and Microsensors , 2008, Sensors.

[38]  Jianwei Qin,et al.  Simultaneous detection of multiple adulterants in dry milk using macro-scale Raman chemical imaging. , 2013, Food chemistry.

[39]  Colette McDonagh,et al.  Optical chemical pH sensors. , 2014, Analytical chemistry.

[40]  T. S. Natarajan,et al.  Development of universal pH sensing electrospun nanofibers , 2012 .

[41]  Radford M. Neal Pattern Recognition and Machine Learning , 2007, Technometrics.

[42]  M. Nielen,et al.  Comprehensive screening and quantification of veterinary drugs in milk using UPLC–ToF-MS , 2008, Analytical and bioanalytical chemistry.

[43]  Karen De Clerck,et al.  The development of polyamide 6.6 nanofibres with a pH-sensitive function by electrospinning , 2010 .

[44]  Royston Goodacre,et al.  Rapid and quantitative detection of the microbial spoilage in milk using Fourier transform infrared spectroscopy and chemometrics. , 2008, The Analyst.

[45]  Kinga Zor,et al.  Development and validation of a colorimetric sensor array for fish spoilage monitoring , 2016 .

[46]  A. Safavi,et al.  Novel optical pH sensor for high and low pH values , 2003 .