A Novel DNA Biosensor Using a Ferrocenyl Intercalator Applied to the Potential Detection of Human Population Biomarkers in Wastewater

Yang, Zhugen; d’Auriac, Marc Anglès; Goggins, Sean; Kasprzyk-Hordern, Barbara; Thomas, Kevin V.; Frost, Christopher G.; Estrela, Pedro

doi:10.1021/acs.est.5b00637

Cited by 46 publications

(28 citation statements)

References 43 publications

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“…The number of endogenous biomarkers excreted by humans that were successfully quantified in wastewater is very limited94041. Furthermore, only one of those focused on an endogenous biomarker as an indicator for the overall health of population (8-iso-PGF 2α )9 while another two studies investigated the use of endogenous biomarkers for estimating population size (5-hydroxyindoleacetic acid40 and DNA41).…”

Section: Discussionmentioning

confidence: 99%

“…Furthermore, only one of those focused on an endogenous biomarker as an indicator for the overall health of population (8-iso-PGF 2α )9 while another two studies investigated the use of endogenous biomarkers for estimating population size (5-hydroxyindoleacetic acid40 and DNA41). The development and validation of endogenous biomarkers for the assessment of public health through WBE is indeed complicated since there are a limited number of validated endogenous urinary biomarkers for routine clinical use.…”

Section: Discussionmentioning

confidence: 99%

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Increased levels of the oxidative stress biomarker 8-iso-prostaglandin F2α in wastewater associated with tobacco use

Ryu

Gracia-Lor

Bade

et al. 2016

Sci Rep

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Wastewater analysis has been demonstrated to be a complementary approach for assessing the overall patterns of drug use by a population while the full potential of wastewater-based epidemiology has yet to be explored. F2-isoprostanes are a prototype wastewater biomarker to study the cumulative oxidative stress at a community level. In this work, 8-iso-prostaglandin F2α (8-iso-PGF2α) was analysed in raw 24 h-composite wastewater samples collected from 4 Norwegian and 7 other European cities in 2014 and 2015. Using the same samples, biomarkers of alcohol (ethyl sulfate) and tobacco (trans-3′-hydroxycotinine) use were also analysed to investigate any possible correlation between 8-iso-PGF2α and the consumption of the two drugs. The estimated per capita daily loads of 8-iso-PGF2α in the 11 cities ranged between 2.5 and 9.9 mg/day/1000 inhabitants with a population-weighted mean of 4.8 mg/day/1000 inhabitants. There were no temporal trends observed in the levels of 8-iso-PGF2α, however, spatial differences were found at the inter-city level correlating to the degree of urbanisation. The 8-iso-PGF2α mass load was found to be strongly associated with that of trans-3′-hydroxycotinine while it showed no correlation with ethyl sulfate. The present study shows the potential for 8-iso-PGF2α as a wastewater biomarker for the assessment of community public health.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Increased levels of the oxidative stress biomarker 8-iso-prostaglandin F2α in wastewater associated with tobacco use

Ryu

Gracia-Lor

Bade

et al. 2016

Sci Rep

Self Cite

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“…This data can be achieved with biosensors . Biosensors have already been applied in WBE to screen PSA, prostate cancer biomarker (Yang et al, ), DNA (Yang et al, ), and cocaine (Yang et al, ). There are, however, several issues that need to be addressed; mainly the relatively low sensitivity of biosensors and most probably low selectivity.…”

Section: General Summary and Perspectivesmentioning

confidence: 99%

Mass spectrometric strategies for the investigation of biomarkers of illicit drug use in wastewater

Hernández

Castiglioni

Covaci

et al. 2016

Mass Spectrometry Reviews

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The analysis of illicit drugs in urban wastewater is the basis of wastewater‐based epidemiology (WBE), and has received much scientific attention because the concentrations measured can be used as a new non‐intrusive tool to provide evidence‐based and real‐time estimates of community‐wide drug consumption. Moreover, WBE allows monitoring patterns and spatial and temporal trends of drug use. Although information and expertise from other disciplines is required to refine and effectively apply WBE, analytical chemistry is the fundamental driver in this field. The use of advanced analytical techniques, commonly based on combined chromatography—mass spectrometry, is mandatory because the very low analyte concentration and the complexity of samples (raw wastewater) make quantification and identification/confirmation of illicit drug biomarkers (IDBs) troublesome. We review the most‐recent literature available (mostly from the last 5 years) on the determination of IDBs in wastewater with particular emphasis on the different analytical strategies applied. The predominance of liquid chromatography coupled to tandem mass spectrometry to quantify target IDBs and the essence to produce reliable and comparable results is illustrated. Accordingly, the importance to perform inter‐laboratory exercises and the need to analyze appropriate quality controls in each sample sequence is highlighted. Other crucial steps in WBE, such as sample collection and sample pre‐treatment, are briefly and carefully discussed. The article further focuses on the potential of high‐resolution mass spectrometry. Different approaches for target and non‐target analysis are discussed, and the interest to perform experiments under laboratory‐controlled conditions, as a complementary tool to investigate related compounds (e.g., minor metabolites and/or transformation products in wastewater) is treated. The article ends up with the trends and future perspectives in this field from the authors’ point of view. © 2016 by The Authors. Mass Spectrometry Reviews published by Wiley Periodicals, Inc. Mass Spec Rev 37:258–280, 2018

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“…Thus, such devices are of particular interest in the area of personal diagnostics, for example, forp oint-of-care devices and on-site monitoring. [4] An example of al abel-free approach is the use of compounds that are able to intercalate into the DNA double helix. One of the main advantages of using intercalating compounds is the fact that these molecules can interactw ith any given DNA sequence.…”

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confidence: 99%

“…Synthesis of af errocene-labeled intercalating compound for the detection of double-stranded DNA (dsDNA) was recent-ly reported. [4] However, this strategy is limited by the oxidation of the 1e À redox species,t hat is, the ferrocene derivative, which in the case of low dsDNA coverage leads to low currents. In contrast, redoxe nzymes conjugated to intercalation compounds offer much higher efficiency at low dsDNAc overage because of the amplification of the amperometrics ignal based on the catalytic redox conversion of as pecific substrate.…”

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Amperometric Detection of dsDNA using an Acridine‐Orange‐Modified Glucose Oxidase

et al. 2017

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What is the most significant result of this study?We created an alternative DNA post-hybridization labeling strategy based on as pecific intercalating compound that was covalently bound to ah ighly active redox enzyme providing the basis for electrochemical readout. In contrast to the widely applied biotinstreptavidin chemistry,where abiotin-labeled signal DNA sequence binds to as treptavidin-conjugated enzyme or vice versa, the great advantage of our approach is the possibility of sequence-independent post-labeling. This eliminates the need of having au nique label for each target DNA sequence and generalizes the suggested approach to any double-stranded DNA sequence. Moreover,t he labeling is done in as ingle step, which further simplifies the electrochemical DNA detection protocol. What was the biggest challenge?The biggest challenge on the way to the results presented in this article was the synthesis of as uitable intercalating compound which has exclusive selectivity for double-stranded DNA and can be linked in as pecific reaction to the surface of the chosen redox enzyme. Starting with the widely used proflavine resulted in many hours of frustrating synthesis owing to the unpredictable chemistry of this aromatic diamine. Finally,c hanging to acridine orange allowed for as uccessful synthesis and defined covalent attachment of the intercalator to glucose oxidase by using well-known alkylation and amination chemistries. What future opportunities do you see?Owing to the general sequence-independent strategy we anticipate that the proposed concept can be easily coupled with other amplification techniques to achieve highly sensitive DNA analysis. We are currently focusing on coupling of the acridine orangebased glucose oxidase system with additional isothermal amplification techniques, while keeping simplicity and speed as the main priorities. AcknowledgementsWe thank the Ruhr University Bochum and BMBF for the funding within af ramework of the project InnoEMat "eDx" (FKZ: 13XP5007C).Invited for this month'sc over is the group of Prof. Dr.W olfgang Schuhmann, Dr.D aliborka Jambrec and Dr.A drianR uff at Ruhr-Universitäti nB ochum, Germany.T he cover picture shows an ovel procedure for the preferential post-hybridizationl abeling of double-strandedD NA based on the intercalating compound acridineo range, which was covalently bound to glucose oxidase. Labelingw ith ah ighly active biocatalyst allows for as imple and sequence-independent amplificationo ft he signal proportional to the amount of hybridizedD NA thatm ay be coupled with other amplification strategies. Read the full text of the article at

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A Novel DNA Biosensor Using a Ferrocenyl Intercalator Applied to the Potential Detection of Human Population Biomarkers in Wastewater

Cited by 46 publications

References 43 publications

Increased levels of the oxidative stress biomarker 8-iso-prostaglandin F2α in wastewater associated with tobacco use

Increased levels of the oxidative stress biomarker 8-iso-prostaglandin F2α in wastewater associated with tobacco use

Mass spectrometric strategies for the investigation of biomarkers of illicit drug use in wastewater

Amperometric Detection of dsDNA using an Acridine‐Orange‐Modified Glucose Oxidase

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