AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
Powered by AMiner. Clicking this button will take you away from SciOpen.
Home Nano Research Article
PDF (35.6 MB)
Cite
EndNote(RIS) BibTeX
Collect
Submit Manuscript AI Chat Paper
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article | Open Access

Amalgamated gold-nanoalloys with enhanced catalytic activity for the detection of mercury ions (Hg2+) in seawater samples

Natasha Logan1, Claire McVey1, Christopher Elliott1, Cuong Cao1,2( )
Institute for Global Food Security, School of Biological Sciences, Queen’s University Belfast, 19 Chlorine Gardens, Belfast, BT9 5DL, UK
Material and Advanced Technologies for Healthcare, Queen’s University Belfast, 18-30 Malone Road, Belfast, BT9 5BN, UK
Show Author Information

Graphical Abstract

Abstract

Mercury (Hg) is extremely toxic, and continues to cause major threats to aquatic life, human health and the environment. Hg2+ mainly derives from seawater as a product of atmospheric deposition, therefore there is great demand for sensing approaches that can detect Hg2+ in seawater samples. Herein, we demonstrate that the peroxidase-mimicking activity of gold nanoparticles (AuNPs) or so-called nanozymes, can be exploited for the detection of Hg2+ ions in various water samples. In a high electrolyte environment, the catalytic activity for the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) was significantly diminished due to poor stability of the bare-AuNPs. This activity was reduced by ~ 73.7% when the NaCl concentration was higher than 1.168%, which is much lower than that of seawater (~ 3.5%), thus presenting its unsuitability for detecting Hg2+ in harsh water matrices. To overcome this limitation, AuNPs were first functionalized with oligo-ethylene glycol (OEG), of which their colloidal form presented high stability in NaCl concentrations up to 20% and across a wide range of pHs from 1-14. Interestingly, the catalytic activity of OEG-AuNPs for the oxidation of TMB was strongly suppressed by the coating, but enhanced upon formation of Au-Hg amalgamation. This novel finding underlies a straightforward, sensitive, and highly selective detection platform for Hg2+ in water samples. The approach could detect the exposure limit level for Hg2+ in drinking water (i.e., 2 ppb for tap and bottled water) as set by the United States Environmental Protection Agency (EPA) and the World Health Organization (WHO). When Hg2+ was spiked into a 3.5% saline solution and a coastal seawater certified reference material (CRM), the detection limits were found to be 10 and 13 ppb, respectively, which exceed the Hg2+ concentrations commonly found within seawater (~ 60-80 ppb). The whole procedure takes less than 45 min to conduct, providing a highly innovative, rapid and low-cost approach for detecting Hg2+ in complex water matrices.

Keywords

gold nanoparticlesnanozymeperoxidase-likemercury detectionwater samplesseawater

Electronic Supplementary Material

Download File(s)
12274_2020_2731_MOESM1_ESM.pdf (3.8 MB)

References

[1]
Schuster, P. F.; Schaefer, K. M.; Aiken, G. R.; Antweiler, R. C.; Dewild, J. F.; Gryziec, J. D.; Gusmeroli, A.; Hugelius, G.; Jafarov, E.; Krabbenhoft, D. P. et al. Permafrost stores a globally significant amount of mercury. Geophys. Res. Lett. 2018, 45, 1463-1471.
Crossref Google Scholar
[2]
Poornima, V.; Alexandar, V.; Iswariya, S.; Perumal, P. T.; Uma, T. S. Gold nanoparticle-based nanosystems for the colorimetric detection of Hg2+ ion contamination in the environment. RSC Adv. 2016, 6, 46711-46722.
Crossref Google Scholar
[3]
United States Environmental Protection Agency (EPA). National Primary Drinking Water Regulations [Online]. https://www.epa.gov/ground-water-and-drinking-water/national-primary-drinking-water-regulations (accessed Mar 05, 2020).
Crossref
[4]
World Health Organization (WHO). Guidelines for Drinking-Water Quality Third Edition. Geneva, World Health Organization[Online]. http://www.who.int/water_sanitation_health/dwq/GDWQ2004web.pdf (accessed Sep 14, 2019).
Crossref
[5]
Lamborg, C. H.; Hammerschmidt, C. R.; Bowman, K. L.; Swarr, G. J.; Munson, K. M.; Ohnemus, D. C.; Lam, P. J.; Heimburger, L. E.; Rijkenberg, M. J.; Saito, M. A. A global ocean inventory of anthropogenic mercury based on water column measurements. Nature 2014, 512, 65-68.
Crossref Google Scholar
[6]
Bloxham, M. J.; Hill, S. J.; Worsfold, P. J. Determination of trace metals in sea-water and the on-line removal of matrix interferences by flow injection with inductively coupled plasma mass spectrometric detection. J. Anal. At. Spectrom. 1994, 9, 935-938.
Crossref Google Scholar
[7]
Wang, C. I.; Huang, C. C.; Lin, Y. W.; Chen, W. T.; Chang, H. T. Catalytic gold nanoparticles for fluorescent detection of mercury(II) and lead(II) ions. Anal. Chim. Acta 2012, 745, 124-130.
Crossref Google Scholar
[8]
Zhou, Q. X.; Lei, M.; Liu, Y. L.; Wu, Y. L.; Yuan, Y. Y. Simultaneous determination of cadmium, lead and mercury ions at trace level by magnetic solid phase extraction with Fe@Ag@Dimercaptobenzene coupled to high performance liquid chromatography. Talanta 2017, 175, 194-199.
Crossref Google Scholar
[9]
Sharma, R.; Ragavan, K. V.; Thakur, M. S.; Raghavarao, K. S. M. S. Recent advances in nanoparticle based aptasensors for food contaminants. Biosens. Bioelectron. 2015, 74, 612-627.
Crossref Google Scholar
[10]
Lee, J. S.; Han, M. S.; Mirkin, C. A. Colorimetric detection of mercuric ion (Hg2+) in aqueous media using DNA-functionalized gold nanoparticles. Angew. Chem., Int. Ed. 2007, 46, 4093-4096.
Crossref Google Scholar
[11]
Li, D.; Wieckowska, A.; Willner, I. Optical analysis of Hg2+ ions by oligonucleotide-gold-nanoparticle hybrids and DNA-based machines. Angew. Chem. 2008, 120, 3991-3995.
Crossref Google Scholar
[12]
Liu, C. W.; Hsieh, Y. T.; Huang, C. C.; Lin, Z. H.; Chang, H. T. Detection of mercury(II) based on Hg2+-DNA complexes inducing the aggregation of gold nanoparticles. Chem. Commun. 2008, 2242-2244.
Crossref Google Scholar
[13]
Ma, Y. J.; Jiang, L.; Mei, Y. J.; Song, R. B.; Tian, D. B.; Huang, H. Colorimetric sensing strategy for mercury(II) and melamine utilizing cysteamine-modified gold nanoparticles. Analyst 2013, 138, 5338-5343.
Crossref Google Scholar
[14]
Lin, C. Y.; Yu, C. J.; Lin, Y. H.; Tseng, W. L. Colorimetric sensing of silver(I) and mercury(II) ions based on an assembly of tween 20-stabilized gold nanoparticles. Anal. Chem. 2010, 82, 6830-6837.
Crossref Google Scholar
[15]
Guo, Y. M.; Wang, Z.; Qu, W. S.; Shao, H. W.; Jiang, X. Y. Colorimetric detection of mercury, lead and copper ions simultaneously using protein-functionalized gold nanoparticles. Biosens. Bioelectron. 2011, 26, 4064-4069.
Crossref Google Scholar
[16]
Su, D. Y.; Yang, X.; Xia, Q. D.; Chai, F.; Wang, C. G.; Qu, F. Y. Colorimetric detection of Hg2+ using thioctic acid functionalized gold nanoparticles. RSC Adv. 2013, 3, 24618-24624.
Crossref Google Scholar
[17]
McVey, C.; Logan, N.; Thanh, N. T. K.; Elliott, C.; Cao, C. Unusual switchable peroxidase-mimicking nanozyme for the determination of proteolytic biomarker. Nano Res. 2019, 12, 509-516.
Crossref Google Scholar
[18]
Luo, W. J.; Zhu, C. F.; Su, S.; Li, D.; He, Y.; Huang, Q.; Fan, C. H. Self-catalyzed, self-limiting growth of glucose oxidase-mimicking gold nanoparticles. ACS Nano 2010, 4, 7451-7458.
Crossref Google Scholar
[19]
Zheng, X. X.; Liu, Q.; Jing, C.; Li, Y.; Li, D.; Luo, W. J.; Wen, Y. Q.; He, Y.; Huang, Q.; Long, Y. T. et al. Catalytic gold nanoparticles for nanoplasmonic detection of DNA hybridization. Angew. Chem., Int. Ed. 2011, 50, 11994-11998.
Crossref Google Scholar
[20]
Shin, H. Y.; Cho, S.; Kim, M. I. Enzyme-free colorimetric detection of glucose using a composite entrapping gold and magnetic nanoparticles within an agarose gel matrix. J. Nanosci. Nanotechnol. 2017, 17, 7971-7977.
Crossref Google Scholar
[21]
He, W. W.; Zhou, Y. T.; Wamer, W. G.; Hu, X. N.; Wu, X. C.; Zheng, Z.; Boudreau, M. D.; Yin, J. J. Intrinsic catalytic activity of Au nanoparticles with respect to hydrogen peroxide decomposition and superoxide scavenging. Biomaterials 2013, 34, 765-773.
Crossref Google Scholar
[22]
Liang, H.; Wu, Y.; Qu, X. Y.; Li, J. Y.; Li, J. Au@Pt nanoparticles as catalase mimics to attenuate tumor hypoxia and enhance immune cell-mediated cytotoxicity. Nanotechnology 2017, 28, 465702.
Crossref Google Scholar
[23]
Lin Y. W.; Huang, C. C.; Chang, H. T. Gold nanoparticle probes for the detection of mercury, lead and copper ions. Analyst 2011, 136, 863-871.
Crossref Google Scholar
[24]
Lien, C. W.; Tseng, Y. T.; Huang, C. C.; Chang, H. T. Logic control of enzyme-like gold nanoparticles for selective detection of lead and mercury ions. Anal. Chem. 2014, 86, 2065-2072.
Crossref Google Scholar
[25]
Chen, Z. B.; Tan, L. L.; Wang, S. X.; Zhang, Y. M.; Li, Y. H. Sensitive colorimetric detection of K(I) using catalytically active gold nanoparticles triggered signal amplification. Biosens. Bioelectron. 2016, 79, 749-757.
Crossref Google Scholar
[26]
Jv, Y.; Li, B. X.; Cao, R. Positively-charged gold nanoparticles as peroxidiase mimic and their application in hydrogen peroxide and glucose detection. Chem. Commun. 2010, 46, 8017-8019.
Crossref Google Scholar
[27]
Tseng, C. W.; Chang, H. Y.; Chang, J. Y.; Huang, C. C. Detection of mercury ions based on mercury-induced switching of enzyme-like activity of platinum/gold nanoparticles. Nanoscale 2012, 4, 6823-6830.
Crossref Google Scholar
[28]
Wang, G. L.; Xu, X. F.; Cao, L. H.; He, C. H.; Li, Z. J.; Zhang, C. Mercury(II)-stimulated oxidase mimetic activity of silver nanoparticles as a sensitive and selective mercury(II) sensor. RSC Adv. 2014, 4, 5867-5872.
Crossref Google Scholar
[29]
Sui, N.; Liu, F. Y.; Wang, K.; Xie, F. X.; Wang, L. N.; Tang, J. J.; Liu, M. H.; Yu, W. W. Nano Au-Hg amalgam for Hg2+ and H2O2 detection. Sens. Actuators B Chem. 2017, 252, 1010-1015.
Crossref Google Scholar
[30]
Long, Y. J.; Li, Y. F.; Liu, Y.; Zheng, J. J.; Tang, J.; Huang, C. Z. Visual observation of the mercury-stimulated peroxidase mimetic activity of gold nanoparticles. Chem. Commun. 2011, 47, 11939-11941.
Crossref Google Scholar
[31]
Yan, L. X.; Chen, Z. P.; Zhang, Z. Y.; Qu, C. L.; Chen, L. X.; Shen, D. Z. Fluorescent sensing of mercury(II) based on formation of catalytic gold nanoparticles. Analyst 2013, 138, 4280-4283.
Crossref Google Scholar
[32]
Chen, Z. B.; Zhang, C. M.; Gao, Q. G.; Wang, G.; Tan, L. L.; Liao, Q. Colorimetric signal amplification assay for mercury ions based on the catalysis of gold amalgam. Anal. Chem. 2015, 87, 10963-10968.
Crossref Google Scholar
[33]
Han, K. N.; Choi, J. S.; Kwon, J. Gold nanozyme-based paper chip for colorimetric detection of mercury ions. Sci. Rep. 2017, 7, 2806.
Crossref Google Scholar
[34]
Wu, L. L.; Wang, L. Y.; Xie, Z. J.; Xue, F.; Peng, C. F. Colorimetric detection of Hg2+ based on inhibiting the peroxidase-like activity of DNA-Ag/Pt nanoclusters. RSC Adv. 2016, 6, 75384-75389.
Crossref Google Scholar
[35]
Yang, H. G.; Xiong, Y. H.; Zhang, P.; Su, L. J.; Ye, F. G. Colorimetric detection of mercury ions using MnO2 nanorods as enzyme mimics. Anal. Methods 2015, 7, 4596-4601.
Crossref Google Scholar
[36]
Wei, H.; Wang, E. K. Nanomaterials with enzyme-like characteristics (nanozymes): Next-generation artificial enzymes. Chem. Soc. Rev. 2013, 42, 6060-6093.
Crossref Google Scholar
[37]
Lin, Y. H.; Ren, J. S.; Qu, X. G. Nano-gold as artificial enzymes: Hidden talents. Adv. Mater. 2014, 26, 4200-4217.
Crossref Google Scholar
[38]
Gao, L. Z.; Yan, X. Y. Nanozymes: An emerging field bridging nanotechnology and biology. Sci. China Life Sci. 2016, 59, 400-402.
Crossref Google Scholar
[39]
Zhou, X. C.; Xu, W. L.; Liu, G. K.; Panda, D.; Chen, P. Size-dependent catalytic activity and dynamics of gold nanoparticles at the single-molecule level. J. Am. Chem. Soc. 2010, 132, 138-146.
Crossref Google Scholar
[40]
Li, W.; Chen, B.; Zhang, H. X.; Sun, Y. H.; Wang, J.; Zhang, J. L.; Fu, Y. BSA-stabilized Pt nanozyme for peroxidase mimetics and its application on colorimetric detection of mercury(II) ions. Biosens. Bioelectron. 2015, 66, 251-258.
Crossref Google Scholar
[41]
Huang, Y. Q.; Fu, S.; Wang, Y. S.; Xue, J. H.; Xiao, X. L.; Chen, S. H.; Zhou, B. Protamine-gold nanoclusters as peroxidase mimics and the selective enhancement of their activity by mercury ions for highly sensitive colorimetric assay of Hg(II). Anal. Bioanal. Chem. 2018, 410, 7385-7394.
Crossref Google Scholar
[42]
Park, K. S.; Kim, M. I.; Cho, D. Y.; Park, H. G. Label-free colorimetric detection of nucleic acids based on target-induced shielding against the peroxidase-mimicking activity of magnetic nanoparticles. Small 2011, 7, 1521-1525.
Crossref Google Scholar
[43]
Kim, H.; Lee, J. U.; Song, S.; Kim, S.; Sim, S. J. A shape-code nanoplasmonic biosensor for multiplex detection of Alzheimer’s disease biomarkers. Biosens. Bioelectron. 2018, 101, 96-102.
Crossref Google Scholar
[44]
Kim, H.; Lee, J. U.; Kim, S.; Song, S.; Sim, S. J. A nanoplasmonic biosensor for ultrasensitive detection of Alzheimer’s disease biomarker using a chaotropic agent. ACS Sens. 2019, 4, 595-602.
Crossref Google Scholar
[45]
Cao, C.; Sim, S. J. Preparation of highly stable oligo(ethylene glycol) derivatives-functionalized gold nanoparticles and their application in LSPR-based detection of PSA/ACT complex. J. Nanosci. Nanotechnol. 2007, 7, 3754-3757.
Crossref Google Scholar
[46]
Cao, C.; Sim, S. J. Resonant Rayleigh light scattering response of individual Au nanoparticles to antigen-antibody interaction. Lab Chip 2009, 9, 1836-1839.
Crossref Google Scholar
[47]
Cao, C.; Gontard, L. C.; Tram, L. L. T.; Wolff, A.; Bang, D. D. Dual enlargement of gold nanoparticles: From mechanism to scanometric detection of pathogenic bacteria. Small 2011, 7, 1701-1708.
Crossref Google Scholar
[48]
Haiss, W.; Thanh, N. T. K.; Aveyard, J.; Fernig, D. G. Determination of size and concentration of gold nanoparticles from UV-vis spectra. Anal. Chem. 2007, 79, 4215-4221.
Crossref Google Scholar
[49]
Gao, M.; Lyalin, A.; Taketsugu, T. Role of the support effects on the catalytic activity of gold clusters: A density functional theory study. Catalysts 2011, 1, 18-39.
Crossref Google Scholar
[50]
Wang, S.; Chen, W.; Liu, A. L.; Hong, L.; Deng, H. H.; Lin, X. H. Comparison of the peroxidase-like activity of unmodified, amino-modified, and citrate-capped gold nanoparticles. ChemPhysChem 2012, 13, 1199-1204.
Crossref Google Scholar
[51]
Lim, S. H.; Ahn, E. Y.; Park, Y. Green synthesis and catalytic activity of gold nanoparticles synthesized by Artemisia capillaris water extract. Nanoscale Res. Lett. 2016, 11, 474.
Crossref Google Scholar
[52]
Qi, G. H.; Fu, C. C.; Chen, G.; Xu, S. P.; Xu, W. Q. Highly sensitive SERS sensor for mercury ions based on the catalytic reaction of mercury ion decorated Ag nanoparticles. RSC Adv. 2015, 5, 49759-49764.
Crossref Google Scholar
[53]
Drozd, M.; Pietrzak, M.; Parzuchowski, P. G.; Malinowska, E. Pitfalls and capabilities of various hydrogen donors in evaluation of peroxidase-like activity of gold nanoparticles. Anal. Bioanal. Chem. 2016, 408, 8505-8513.
Google Scholar
[54]
Food and Drug Administration (FDA). Mercury Levels in Commercial Fish and Shellfish (1990-2012)[Online]. https://www.fda.gov/food/foodborneillnesscontaminants/metals/ucm115644.htm. (accessed Sep 14, 2019).
Nano Research
Volume 13 Issue 4,
April 2020
Pages 989-998
DOI: 10.1007/s12274-020-2731-y
Cite this article:
Logan N, McVey C, Elliott C, et al. Amalgamated gold-nanoalloys with enhanced catalytic activity for the detection of mercury ions (Hg2+) in seawater samples. Nano Research, 2020, 13(4): 989-998. https://doi.org/10.1007/s12274-020-2731-y
Topics:
Binary alloysCatalyst activityCatalytic oxidation Chlorine compoundsElectrolytesFiber optic sensorsGold alloysGold nanoparticlesHealth risksMetal nanoparticlesMetalsSols

1044

Views

38

Downloads

53

Crossref

N/A

Web of Science

54

Scopus

0

CSCD

Altmetrics
Received: 19 December 2019
Revised: 20 February 2020
Accepted: 23 February 2020
Published: 14 March 2020
© The Author(s) 2020

This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/ licenses/by/4.0/.
Return