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Front. Environ. Sci. Eng.    2023, Vol. 17 Issue (5) : 57    https://doi.org/10.1007/s11783-023-1657-5
REVIEW ARTICLE
Surface-enhanced Raman spectroscopy for emerging contaminant analysis in drinking water
Seo Won Cho1,2, Haoran Wei1,2()
1. Environmental Chemistry and Technology Program, University of Wisconsin–Madison, Madison, WI 53706, USA
2. Department of Civil and Environmental Engineering, University of Wisconsin–Madison, Madison, WI 53706, USA
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Abstract

● Definition of emerging contaminants in drinking water is introduced.

● SERS and standard methods for emerging contaminant analysis are compared.

● Enhancement factor and accessibility of SERS hot spots are equally important.

● SERS sensors should be tailored according to emerging contaminant properties.

● Challenges to meet drinking water regulatory guidelines are discussed.

Emerging contaminants (ECs) in drinking water pose threats to public health due to their environmental prevalence and potential toxicity. The occurrence of ECs in our drinking water supplies depends on their physicochemical properties, discharging rate, and susceptibility to removal by water treatment processes. Uncertain health effects of long-term exposure to ECs justify their regular monitoring in drinking water supplies. In this review article, we will summarize the current status and future opportunities of surface-enhanced Raman spectroscopy (SERS) for EC analysis in drinking water. Working principles of SERS are first introduced and a comparison of SERS and liquid chromatography-tandem mass spectrometry in terms of cost, time, sensitivity, and availability is made. Subsequently, we discuss the strategies for designing effective SERS sensors for EC analysis based on five categories—per- and polyfluoroalkyl substances, novel pesticides, pharmaceuticals, endocrine-disrupting chemicals, and microplastics. In addition to maximizing the intrinsic enhancement factors of SERS substrates, strategies to improve hot spot accessibilities to the targeting ECs are equally important. This is a review article focusing on SERS analysis of ECs in drinking water. The discussions are not only guided by numerous endeavors to advance SERS technology but also by the drinking water regulatory policy.
Keywords Emerging contaminant      Surface-enhanced Raman spectroscopy      Drinking water monitoring      Sensor      Regulatory policy     
Corresponding Author(s): Haoran Wei   
Issue Date: 30 November 2022
 Cite this article:   
Seo Won Cho,Haoran Wei. Surface-enhanced Raman spectroscopy for emerging contaminant analysis in drinking water[J]. Front. Environ. Sci. Eng., 2023, 17(5): 57.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1657-5
https://academic.hep.com.cn/fese/EN/Y2023/V17/I5/57
Fig.1  Schematic illustrating the definition of emerging contaminants in drinking water.
Analytical method Advantages Disadvantages
SERS • Simple sample pretreatment• Rapid and non-destructive sample analysis• Field deployable• Lower measurement cost (~5–10 $/h)• Lower instrumental cost (~10–30 k$) • Higher LOD (> 1 μg/L for direct SERS; down to sub-ng/L level for indirect SERS)• Limited to analytes with high affinity to plasmonic nanoparticles• Mediocre reproducibility• Interference by complex water matrices
LC-MS/MS • Lower LOD (down to sub-ng/L level)• High precision• Standard methods published by the environmental regulatory authorities • Time-consuming sample pretreatment & analysis• Requiring well-trained personnel• Higher measurement cost (~50–80$/h)• Higher instrumental cost (~500 k$)
Tab.1  A summary of the advantages and disadvantages of SERS and LC-MS/MS
Fig.2  Schematic of the working principle of a typical SERS sensor for EC analysis.
EC categories ECs SERS substrates/labels Water matrices LOD (μg/L) Regulations/Advisories Ref.
PFAS PFOA, PFOS, and 6:2 FTS AgNP-graphene oxide/ethyl violet Groundwater 50 U.S. EPA HAL: PFOA 0.004 ng/L and PFOS 0.02 ng/L in drinking water Fang et al. (2016)
PFOA Ag nanoclusters on silica microspheres/crystal violet DI water 11 Bai et al. (2022)
Novel pesticides Acetamiprid Au and Ag nanostructures covered on SiO2 DI water 9 U.S. EPA DWLOC: 80 μg/L (chronic exposure for children 1–6 years old) Atanasov et al. (2020a)
AuNPs on Ti3C2/SiO2/PDMS surface DI water 2×10–6 Gao et al. (2021)
Colloidal AuNPs Acetone 10 Dowgiallo and Guenther (2019)
Clothianidin Ag layer on nanostructured PVDF film Methanol-DI water (1:1) 1 Minnesota Department of Health guidance: 200 μg/L Creedon et al. (2020)
AuNPs on Ti3C2/SiO2/PDMS surface DI Water 2×10–6 Gao et al. (2021)
Colloidal AuNPs Methanol 103 Dowgiallo and Guenther (2019)
Silver dendrite/electropolymerized molecular identifier/AgNP sandwich hybrids Ethanol 0.03 Zhao et al. (2020)
Imidacloprid Ag layer on nanostructured PVDF film Methanol-DI water (1:1) 1 Minnesota Department of Health guidance: 2 μg/L Creedon et al. (2020)
Citrate-coated AuNP colloid Methanol-DI Water (1:1) 5 Hou et al. (2015)
AuNPs on Ti3C2/SiO2/PDMS surface DI water 1×10–6 Gao et al. (2021)
Colloidal AuNP Acetone 100 Dowgiallo and Guenther (2019)
Nitenpyram Fern-like Ag dendrites on filter paper Apple surface 0.3 None Wang et al. (2019)
Ag nanospheres and nanocubes Acetone 3×105 Puente et al. (2022)
Thiacloprid Ag and Au nanostructures on alumina ceramic DI water 105 U.S. EPA DWLOC: 38 μg/L Atanasov et al. (2020b)
Cysteamine-modified silver-coated gold nanoparticles Liquid milk 23 Hussain et al. (2020)
Thiamethoxam AuNPs on Ti3C2/SiO2/PDMS surface DI water 2×10–6 Minnesota Department of Health guidance: 200 μg/L Gao et al. (2021)
Colloidal AuNP Acetone 100 Dowgiallo and Guenther (2019)
Pharmaceuticals Sulfamethoxazole Sepiolite/chitosan/AgNPs DI water 20 Minnesota Department of Health guidance: 100 μg/L Hu et al. (2022)
Ag layer on a nanostructured quartz wafer DI water/lake, river, tap water 0.05/0.6 Patze et al. (2017)
Hydroxylamine-coated AgNP colloid Human urine 2×103 Markina et al. (2020)
Diclofenac Thiocholine-functionalized AgNP colloid DI water 6×103 None Stewart et al. (2015)
Au nanogrid DI water 3×10–4 Cho et al. (2020)
Carbamazepine AuNPs within bacterial cellulose mat DI water 2 Minnesota Department of Health guidance: 40 μg/L Wei and Vikesland (2015)
Au@Ag core-shell NP colloid Saliva 0.3 Chen et al. (2021)
Endocrine-disrupting chemicals 17β-estradiol Au@Ag core-shell NP colloid/Cy3 DI water 3×10–4 Japan MRC: 0.08 μg/L (E2) and 0.02 μg/L (17α-ethinylestradiol) Pu et al. (2019)
AuNPs on a magnetic bead/MGITC Human serum 7×10–4 Wang et al. (2016)
Total steroid estrogens Au@Ag core-shell NP colloid/4-MBA Multiple surface waters 10–3 Liu et al. (2019)
Micro- and nanoplastics PS micro- and nanoplastics (50–1,000 nm) Ag nanowires KI solution 0.1 California SDWA Yang et al. (2022)
PS and PMMA micro- and nanoplastics (360–5,000 nm) Klarite DI water 2.625×104 Xu et al. (2020a)
PS, PE, and PP micro- and nanoplastics (100 nm) AgNPs Pure water and sea water 4×104 Lv et al. (2020)
PET, PE, PVC, PP, PS, and PC microplastics (80–150 µm) Sponge supported AuNPs Ultrapure water, sea water, rainwater, river water, snow water, and tap water 1×103 Yin et al. (2021)
PET microplastics AuNP doped filter paper water 105 Xu et al. (2022)
PS sub-micro- (161 nm) and nanoplastics (33 nm) AuNPs (46 nm and 14 nm) SDS and KPS solution (solution obtained from milling) 104/2 × 104 Caldwell et al. (2021)
PS and PMMA microspheres AuNPs@V-shaped anodized aluminum oxide (AAO) substrate DI water 5×107 Liu et al. (2022)
PS nanoplastics (~50 nm) AgNPs River water 5×103 Zhou et al. (2021)
PS sub-microplastics (600 nm) Au nanourchins DI water 1–5 particles Lee and Fang (2022)
PS nanoplastics (500 nm) Ag nanowire membrane Seafood market water and seawater 1 Yang et al. (2022)
Tab.2  A summary of SERS-based sensors for emerging contaminant analysis
Fig.3  SERS spectra of clothianidin and imidacloprid that were collected after deposition of their methanol-water solutions (1 μg/L) onto the Ag film@PVDF SERS substrate. Reprinted (adapted) with permission from Creedon et al. (2020). Highly sensitive SERS detection of neonicotinoid pesticides. Complete Raman spectral assignment of clothianidin and imidacloprid. Journal of Physical Chemistry A, 124(36): 7238–7247. Copyright 2020 American Chemical Society.
Fig.4  Raman spectra of carbamazepine collected from an AuNP/bacterial cellulose SERS substrate under pH of 2.0, 3.0, and 6.0 (Wei and Vikesland, 2015). This is an open access article distributed under the terms of the Creative Commons CC BY license, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Fig.5  Schematics of (a) aptamer functionalization on a gold nanogrid SERS substrate and (b) strategy for labeled SERS analysis of 17β-estradiol (Pu et al., 2019; Cho et al., 2020). Reprinted with permission from (Yeon Sik Jung, et al. 2020). Selective, quantitative, and multiplexed surface-enhanced Raman spectroscopy using aptamer-functionalized monolithic plasmonic nanogrids derived from cross-point nano-welding. Advanced Functional Materials, 30: 2000612. Copyright 2020 John Wiley and Sons. Reprinted with permission from Hongbin Pu, Xiaohui Xie, Dawen Sun, et al. (2019). Double-strand DNA functionalized Au@Ag NPs for ultrasensitive detection of 17β-estradiol using surface-enhanced Raman spectroscopy. Talanta, 195: 419–425. Copyright 2019 Elsevier.
Fig.6  Schematics of (a) Klarite and (b) a bifunctional silver nanowire membrane. Reprinted (adapted) with permission from Yang Q, Zhang S, Su J, Li S, Lv X, Chen J, Lai Y, Zhan J (2022). Identification of Trace Polystyrene Nanoplastics Down to 50 nm by the Hyphenated Method of Filtration and Surface-Enhanced Raman Spectroscopy Based on Silver Nanowire Membranes. Environmental Science & Technology, 56(15): 10818–10828. Copyright 2022 American Chemical Society. Reprinted (adapted) with permission from Xu G, Cheng H, Jones R, Feng Y, Gong K, Li K, Fang X, Tahir M A, Valev V K, Zhang L (2020). Surface-Enhanced Raman Spectroscopy Facilitates the Detection of Microplastics < 1 μm in the Environment. Environmental Science & Technology, 54(24): 15594–15603. Copyright 2020 American Chemical Society.
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