Design and synthesis of target-responsive hydrogel for portable visual quantitative detection of uranium with a microfluidic distance-based readout device.

Due to uranium's increasing exploitation in nuclear energy and its toxicity to human health, it is of great significance to detect uranium contamination. In particular, development of a rapid, sensitive and portable method is important for personal health care for those who frequently come into contact with uranium ore mining or who investigate leaks at nuclear power plants. The most stable form of uranium in water is uranyl ion (UO2(2+)). In this work, a UO2(2+) responsive smart hydrogel was designed and synthesized for rapid, portable, sensitive detection of UO2(2+). A UO2(2+) dependent DNAzyme complex composed of substrate strand and enzyme strand was utilized to crosslink DNA-grafted polyacrylamide chains to form a DNA hydrogel. Colorimetric analysis was achieved by encapsulating gold nanoparticles (AuNPs) in the DNAzyme-crosslinked hydrogel to indicate the concentration of UO2(2+). Without UO2(2+), the enzyme strand is not active. The presence of UO2(2+) in the sample activates the enzyme strand and triggers the cleavage of the substrate strand from the enzyme strand, thereby decreasing the density of crosslinkers and destabilizing the hydrogel, which then releases the encapsulated AuNPs. As low as 100nM UO2(2+) was visually detected by the naked eye. The target-responsive hydrogel was also demonstrated to be applicable in natural water spiked with UO2(2+). Furthermore, to avoid the visual errors caused by naked eye observation, a previously developed volumetric bar-chart chip (V-Chip) was used to quantitatively detect UO2(2+) concentrations in water by encapsulating Au-Pt nanoparticles in the hydrogel. The UO2(2+) concentrations were visually quantified from the travelling distance of ink-bar on the V-Chip. The method can be used for portable and quantitative detection of uranium in field applications without skilled operators and sophisticated instruments.

[1]  Xiaoling Zhang,et al.  An aptamer cross-linked hydrogel as a colorimetric platform for visual detection. , 2010, Angewandte Chemie.

[2]  Xi‐lin Xiao,et al.  A label-free electrochemical biosensor for trace uranium based on DNAzymes and gold nanoparticles , 2014, Journal of Radioanalytical and Nuclear Chemistry.

[3]  G. Shen,et al.  DNAzyme-based biosensors and nanodevices. , 2015, Chemical communications.

[4]  J. Milojković,et al.  Influence of Soil Type and Physical–Chemical Properties on Uranium Sorption and Bioavailability , 2011, Water, Air, & Soil Pollution.

[5]  M. Aschner,et al.  Toxicity Studies on Depleted Uranium in Primary Rat Cortical Neurons and in Caenorhabditis Elegans: What Have We Learned? , 2009, Journal of toxicology and environmental health. Part B, Critical reviews.

[6]  Yi Lu New transition-metal-dependent DNAzymes as efficient endonucleases and as selective metal biosensors. , 2002, Chemistry.

[7]  Jian-hui Jiang,et al.  Aptamer-conjugated nanomaterials and their applications. , 2011, Advanced drug delivery reviews.

[8]  C. Ruan,et al.  Surface-enhanced Raman spectroscopy for uranium detection and analysis in environmental samples. , 2007, Analytica chimica acta.

[9]  Srinivasa Rao,et al.  Fluorescent uranyl ion lidded cucurbit[5]uril capsule. , 2012, Inorganic chemistry.

[10]  I. Willner,et al.  Fluorescent DNA hydrogels composed of nucleic acid-stabilized silver nanoclusters. , 2013, Small.

[11]  N. Khashab,et al.  Colorimetric peroxidase mimetic assay for uranyl detection in sea water. , 2015, ACS applied materials & interfaces.

[12]  Yi Lu,et al.  A catalytic beacon sensor for uranium with parts-per-trillion sensitivity and millionfold selectivity , 2007, Proceedings of the National Academy of Sciences.

[13]  Bing Xu,et al.  A biocompatible method of decorporation: bisphosphonate-modified magnetite nanoparticles to remove uranyl ions from blood. , 2006, Journal of the American Chemical Society.

[14]  Yi Lu,et al.  Highly sensitive and selective colorimetric sensors for uranyl (UO2(2+)): development and comparison of labeled and label-free DNAzyme-gold nanoparticle systems. , 2008, Journal of the American Chemical Society.

[15]  K. B. Gongalsky Impact of Pollution Caused by Uranium Production on Soil Macrofauna , 2003, Environmental monitoring and assessment.

[16]  Y. Sugitani,et al.  A Photoacoustic and Fluorescent Spectroscopic Study of Uranyl Compounds , 1980 .

[17]  Xiaoxue Zeng,et al.  A turn-off fluorescent biosensor for the rapid and sensitive detection of uranyl ion based on molybdenum disulfide nanosheets and specific DNAzyme. , 2015, Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy.

[18]  Zhi Zhu,et al.  Target-responsive "sweet" hydrogel with glucometer readout for portable and quantitative detection of non-glucose targets. , 2013, Journal of the American Chemical Society.

[19]  Zhi Zhu,et al.  Target-responsive DNAzyme cross-linked hydrogel for visual quantitative detection of lead. , 2014, Analytical chemistry.

[20]  D. Mandler,et al.  Electrochemical determination of low levels of uranyl by a vibrating gold microelectrode. , 2015, Analytical chemistry.

[21]  Zhi Zhu,et al.  Au@Pt nanoparticle encapsulated target-responsive hydrogel with volumetric bar-chart chip readout for quantitative point-of-care testing. , 2014, Angewandte Chemie.

[22]  J. Domingo,et al.  Reproductive and developmental toxicity of natural and depleted uranium: a review. , 2001, Reproductive toxicology.

[23]  M. R. Jamali,et al.  Synthesis of salicylaldehyde-modified mesoporous silica and its application as a new sorbent for separation, preconcentration and determination of uranium by inductively coupled plasma atomic emission spectrometry. , 2006, Analytica chimica acta.

[24]  Itamar Willner,et al.  DNAzymes for sensing, nanobiotechnology and logic gate applications. , 2008, Chemical Society reviews.

[25]  Chaoyong James Yang,et al.  DNAzyme crosslinked hydrogel: a new platform for visual detection of metal ions. , 2011, Chemical communications.

[26]  Yi Lu,et al.  A DNAzyme-gold nanoparticle probe for uranyl ion in living cells. , 2013, Journal of the American Chemical Society.

[27]  Yi Lu,et al.  Metal-ion-dependent folding of a uranyl-specific DNAzyme: insight into function from fluorescence resonance energy transfer studies. , 2011, Chemistry.

[28]  Hai-Zhu Yu,et al.  Fluorescent recognition of uranyl ions by a phosphorylated cyclic peptide. , 2015, Chemical communications.

[29]  S. Aggarwal,et al.  Determination of low atomic number elements at trace levels in uranium matrix using vacuum chamber total reflection X-ray fluorescence , 2010 .

[30]  D. Brugge,et al.  Exposure Pathways and Health Effects Associated with Chemical and Radiological Toxicity of Natural Uranium: A Review , 2005, Reviews on environmental health.