journal article·2018-04Open access

Naked-eye point-of-care testing platform based on a pH-responsive superwetting surface: toward the non-invasive detection of glucose

Zhong Feng Gao, Ei Ei Sann, Xiaoding Lou, Renyi Liu, Jun Dai, Xiaolei Zuo, Fan Xia, Lei Jiang

NPG Asia Materials· Volume 10· Issue 4

Abstract

Herein, we demonstrate a contact angle (CA)-based naked-eye point-of-care testing platform with rapid pH-responsive superwettability that can switch between superhydrophilic and superhydrophobic properties for quantitative biosensing. The CA of the droplet on the pH-responsive surface approached ~0° at pH 1 and conversely reached 161.4° ± 6.2° at pH 13. We realized the sensitive detection of the pH, urea, and glucose by monitoring the changes in the CA. The traditional invasive diagnosis of diabetes causes pain and brings the risk of infections, such as acquired immune deficiency syndrome (AIDS), hepatitis B, hepatitis C, and syphilis, to the user. To address this issue, we implemented a method for the non-invasive diagnosis of diabetes in human saliva and urine, which avoided the significant drawbacks mentioned above. The accuracy of this method was demonstrated by comparing the results with those from commercial glucometers and theoretical calculations. Interestingly, we successfully monitored glucose levels in sweat before, during, and after cycling. The sensing performance was barely influenced by the temperature, elevation, and droplet color, illustrating promise for expansion to hundreds of millions of potential customers, especially those with color blindness or color weakness. Given its low cost, lack of instruments, and rapid response (within 1 s), this strategy might overcome the limitations of the mechanical stability and durability of superwettable materials and thus might extend the industrial-scale application of bioinspired superwettable systems. Nanostructured surfaces developed by researchers in China enable patients to visualize approximate blood glucose levels for point-of-care diagnostics. The contact angle between the edge of a liquid droplet and the surface on which it sits depends on the interaction between the droplet and the surface. Fan Xia and Jun Dai from the Huazhong University of Science and Technology and their co-workers now harness this concept to develop a simple blood glucose test. The team made a surface by coating a glass substrate with silicon nanoparticles. Acidic droplets or those with low urea or high glucose levels had a small contact angle, giving the droplet a very flat shape. Lower levels of glucose, higher levels of urea or less acidic samples resulted in a more spherical shape. These surfaces could help test for diabetes. A pH-responsive superwetting surface is fabricated and applied as a point-of-care testing platform for naked eye biosensing. Because of the outstanding switching between superhydrophilicity and superhydrophobicity, contact angle based biosensing method is developed for pH, urea, and glucose detection. Especially, non-invasive detection of glucose is achieved for diabetes diagnosis and exercise monitoring. Given to its low cost, instrument-free, disposable, and rapid response (within 1 s), this strategy not only provides a universal platform of point-of-care testing but also extends the industrial-scale application of bioinspired superwettability systems.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Biosensors and Analytical Detection · Advanced Sensor and Energy Harvesting Materials · Surface Modification and Superhydrophobicity

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (50)

Show source-provided references
1. Liu, M., Wang, S. & Jiang, L. Nature-inspired superwettability systems. Nat. Rev. Mater. 2, 17036 (2017).10.1038/natrevmats.2017.36 ↗
2. Cape, J. N. Contact angles of water droplets on needles of Scots pine (Pinus sylvestris) growing in polluted atmospheres. New Phytol. 93, 293–299 (1983).10.1111/j.1469-8137.1983.tb03432.x ↗
3. Percy, K. E. & Baker, E. A. Effects of simulated acid rain on leaf wettability, rain retention and uptake of some inorganic ions. New Phytol. 108, 75–82 (1988).10.1111/j.1469-8137.1988.tb00206.x ↗
4. Nagase, K. et al. Effects of graft densities and chain lengths on separation of bioactive compounds by nanolayered thermoresponsive polymer brush surfaces. Langmuir 24, 511–517 (2008).10.1021/la701839s ↗
5. Kahn, J. S., Hu, Y. & Willner, I. Stimuli-responsive DNA-based hydrogels: from basic principles to applications. Acc. Chem. Res. 50, 680–690 (2017).10.1021/acs.accounts.6b00542 ↗
6. Lu, Y., Aimetti, A. A., Langer, R. & Gu, Z. Bioresponsive materials. Nat. Rev. Mater. 1, 16075 (2016).10.1038/natrevmats.2016.19 ↗
7. Zhang, W. et al. Microfluidics separation reveals the stem-cell-like deformability of tumor-initiating cells. Proc. Natl Acad. Sci. 109, 18707–18712 (2012).10.1073/pnas.1209893109 ↗
8. Zhou, J., Lu, X., Hu, J. & Li, J. Reversible immobilization and direct electron transfer of cytochrome c on pH sensitive polymer interface. Chem. Eur. J. 13, 2847–2853 (2007).10.1002/chem.200601335 ↗
9. Zhou, J., Wang, G., Hu, J., Lu, X. & Li, J. Temperature, ionic strength and pH induced electrochemical switch of smart polymer interfaces, Chem. Commun. 0, 4820–4822 (2006)
10. Stuart, M. A. C. et al. Emerging applications of stimuli-responsive polymer materials. Nat. Mater. 9, 101–113 (2010).10.1038/nmat2614 ↗
11. Verho, T. et al. Reversible switching between superhydrophobic states on a hierarchically structured surface. Proc. Natl Acad. Sci. 109, 10210–10213 (2012).10.1073/pnas.1204328109 ↗
12. Lafuma, A. & Quéré, D. Superhydrophobic states. Nat. Mater. 2, 457–460 (2003).10.1038/nmat924 ↗
13. Krumpfer, J. W. & McCarthy, T. J. Dip-coating crystallization on a superhydrophobic surface: a million mounted crystals in a 1 cm2 array. J. Am. Chem. Soc. 133, 5764–5766 (2011).10.1021/ja2011548 ↗
14. Cheng, M. et al. Bell-shaped superhydrophilic—superhydrophobic—superhydrophilic double transformation on a pH-responsive smart surface. Adv. Mater. 26, 306–310 (2014).10.1002/adma.201302187 ↗
15. Ganesh, V. A., Raut, H. K., Nair, A. S. & Ramakrishna, S. A review on self-cleaning coatings. J. Mater. Chem. 21, 16304 (2011).10.1039/c1jm12523k ↗
16. Kreder, M. J., Alvarenga, J., Kim, P. & Aizenberg, J. Design of anti-icing surfaces: smooth, textured or slippery? Nat. Rev. Mater. 1, 15003 (2016).10.1038/natrevmats.2015.3 ↗
17. Pinchasik, B. E., Kappl, M. & Butt, H. J. Small structures, big droplets: the role of nanoscience in fog harvesting. ACS Nano 10, 10627–10630 (2016).10.1021/acsnano.6b07535 ↗
18. Tian, D., Song, Y. & Jiang, L. Patterning of controllable surface wettability for printing techniques. Chem. Soc. Rev. 42, 5184 (2013).10.1039/c3cs35501b ↗
19. Wang, B., Liang, W., Guo, Z. & Liu, W. Biomimetic super-lyophobic and super-lyophilic materials applied for oil/water separation: a new strategy beyond nature. Chem. Soc. Rev. 44, 336–361 (2015).10.1039/C4CS00220B ↗
20. Huang, X., Liu, Y., Yung, B., Xiong, Y. & Chen, X. Nanotechnology-enhanced no-wash biosensors for in vitro diagnostics of cancer. ACS Nano 11, 5238–5292 (2017).10.1021/acsnano.7b02618 ↗
21. Martinez, A. W., Phillips, S. T., Butte, M. J. & Whitesides, G. M. Patterned paper as a platform for inexpensive, low-volume, portable. Angew. Chem. Int. Ed. 46, 1318–1320 (2010).10.1002/anie.200603817 ↗
22. Liu, M. et al. Target-induced and equipment-free DNA amplification with a simple paper device. Angew. Chem. Int. Ed. 55, 2709–2713 (2016).10.1002/anie.201509389 ↗
23. Elghanian, R. Selective colorimetric detection of polynucleotides based on the distance-dependent optical properties of gold nanoparticles. Science 277, 1078–1081 (1997).10.1126/science.277.5329.1078 ↗
24. Chapman, R. et al. Multivalent nanoparticle networks enable point-of-care detection of human phospholipase-A2 in serum. ACS Nano 9, 2565–2573 (2015).10.1021/nn5057595 ↗
25. Pardee, K. et al. Paper-based synthetic gene networks. Cell 159, 940–954 (2014).10.1016/j.cell.2014.10.004 ↗
26. Hsieh, K., Ferguson, B. S., Eisenstein, M., Plaxco, K. W. & Soh, H. T. Integrated electrochemical microsystems for genetic detection of pathogens at the point of care. Acc. Chem. Res. 48, 911–920 (2015).10.1021/ar500456w ↗
27. Labib, M., Sargent, E. H. & Kelley, S. O. Electrochemical methods for the analysis of clinically relevant biomolecules. Chem. Rev. 116, 9001–9090 (2016).10.1021/acs.chemrev.6b00220 ↗
28. Zheng, G., Patolsky, F., Cui, Y., Wang, W. U. & Lieber, C. M. Multiplexed electrical detection of cancer markers with nanowire sensor arrays. Nat. Biotechnol. 23, 1294–1301 (2005).10.1038/nbt1138 ↗
29. Imani, S. et al. Wearable chemical–electrophysiological hybrid biosensing system for real-time health and fitness monitoring. Nat. Commun. 7, 11650 (2016).10.1038/ncomms11650 ↗
30. Zhu, Z. et al. Translating molecular recognition into a pressure signal to enable rapid, sensitive, and portable biomedical analysis. Angew. Chem. Int. Ed. 54, 10448–10453 (2015).10.1002/anie.201503963 ↗
31. Xiang, Y. & Lu, Y. Using personal glucose meters and functional DNA sensors to quantify a variety of analytical targets. Nat. Chem. 3, 697–703 (2011).10.1038/nchem.1092 ↗
32. Chen, Y. et al. Double-enzymes-mediated bioluminescent sensor for quantitative and ultrasensitive point-of-care testing. Anal. Chem. 89, 5422–5427 (2017).10.1021/acs.analchem.7b00239 ↗
33. Wei, Q. et al. Detection and spatial mapping of mercury contamination in water samples using a smart-phone. ACS Nano 8, 1121–1129 (2014).10.1021/nn406571t ↗
34. Wong, B. Color blindness. Nat. Methods 8, 441-441 (2011).10.1038/nmeth.1618 ↗
35. Lin, L., Yan, J. & Li, J. Small-molecule triggered cascade enzy-matic catalysis in hour-glass shaped nanochannel reactor for glucose monitoring. Anal. Chem. 86, 10546–10551 (2014).10.1021/ac501983a ↗
36. Wen, Z., Ci, S. & Li, J. Pt nanoparticles inserting in carbon nanotubes arrays nanocomposites for glucose biosensors. J. Phys. Chem. C 113, 13482–13487 (2009).10.1021/jp902830z ↗
37. Deng, X., Mammen, L., Butt, H. J. & Vollmer, D. Candle soot as a template for a transparent robust superamphiphobic coating. Science 335, 67–70 (2012).10.1126/science.1207115 ↗
38. Tuteja, A. et al. Designing superoleophobic surfaces. Science 318, 1618–1622 (2007).10.1126/science.1148326 ↗
39. Huang, J., Cheng, F., Binks, B. P. & Yang, H. PH-responsive gas-water-solid interface for multiphase catalysis. J. Am. Chem. Soc. 137, 15015–15025 (2015).10.1021/jacs.5b09790 ↗
40. Grosso, E. D., Dallaire, A. M., Vallée-Bélisle, A. & Ricci, F. Enzyme-operated DNA-based nanodevices. Nano Lett. 15, 8407–8411 (2015).10.1021/acs.nanolett.5b04566 ↗
41. You, M. et al. Photon-regulated DNA-enzymatic nanostructures by molecular assembly. ACS Nano 5, 10090–10095 (2011).10.1021/nn204007y ↗
42. Liu, B., Sun, Z., Huang, P. J. J. & Liu, J. Hydrogen peroxide displacing DNA from nanoceria: Mechanism and detection of glucose in serum. J. Am. Chem. Soc. 137, 1290–1295 (2015).10.1021/ja511444e ↗
43. Nakamura, B. S. & Ogura, Y. Action mechanism of gucose oxidase of aspergillus niger. J. Biochem. 63, 308–316 (1968).10.1093/oxfordjournals.jbchem.a128747 ↗
44. Lee, H. et al. Wearable/disposable sweat-based glucose monitoring device with multistage transdermal drug delivery module. Sci. Adv. 3, 1–9 (2017).
45. Liu, C. et al. A glucose oxidase-coupled DNAzyme sensor for glucose detection in tears and saliva. Biosens. Bioelectron. 70, 455–461 (2015).10.1016/j.bios.2015.03.070 ↗
46. Zhang, Z., Chen, Z., Cheng, F., Zhang, Y. & Chen, L. Highly se-nsitive on-site detection of glucose in human urine with naked eye based on enzymatic-like reaction mediated etching of gold nanorods. Biosens. Bioelectron. 89, 932–936 (2017).10.1016/j.bios.2016.09.090 ↗
47. Ruud, J., Steculorum, S. M. & Bru, J. C. Neuronal control of peripheral insulin sensitivity and glucose metabolism. Nat. Commun. 8, 15259 (2017).10.1038/ncomms15259 ↗
48. Riddell, M. & Perkins, B. A. Exercise and glucose metabolism in persons with diabetes mellitus: Perspectives on the role for continuous glucose monitoring. J. Diabetes Sci. Technol. 3, 914–923 (2009).10.1177/193229680900300439 ↗
49. Gao, W. et al. Fully integrated wearable sensor arrays for multiplexed in situ perspiration analysis. Nature 529, 509–514 (2016).10.1038/nature16521 ↗
50. Sonner, Z. et al. The microfluidics of the eccrine sweat gland, including biomarker partitioning, transport, and biosensing implications. Biomicrofluidics 9, 031301 (2015).10.1063/1.4921039 ↗