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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Green Chemistry".

Deadline for manuscript submissions: closed (15 September 2021) | Viewed by 33037

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Prof. Dr. Albert Lebedev

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Department of Organic Chemistry, Lomonosov Moscow State University, Moscow, Russia
Interests: organic mass spectrometry; environmental chemistry; peptide sequencing; disinfection by-products

Special Issue Information

Dear Colleagues,

An enormous number of various compounds—from the vapors of heavy metals and inorganic gases to the most complex organic and bioorganic compounds, including entire microorganisms—enters the Earth’s atmosphere and water reservoirs every day. The number of known priority pollutants and emerging contaminants of environmental concern currently exceeds several thousand (US EPA Part 423, US EPA Part 401). It grows every day as new pollutants enter the environment (NORMAN List of Emerging Substances). This expanding list can also include their metabolites and degradation products, as well as reaction products occurring due to numerous atmospheric and aquatic reactions. In some cases, these products may even be more toxic than their parent compounds. Therefore, it becomes more and more challenging to conduct comprehensive screening for known and emerging environmental contaminants. Today, various laboratories all over the world work on the identification and quantification of environmental pollutants and contaminants using more and more powerful approaches and analytical tools. In the majority of these studies, a targeted approach is used, when the investigators know, a priori, what they are trying to detect. An alternative, non-targeted approach involves attempts to identify all the chemical compounds in the samples. The latter represents a challenging task, although it allows the establishment of novel contaminants and the finding of peculiarities of the pollution in certain territories of the planet. On the basis of these studies, local lists of priority pollutants can be created, followed by the establishment of the sources of these pollutants and development of adequate policies to address those sources.

The proposed Special Issue of Molecules will cover the results of studies of environmental pollution with various compounds, from the Arctic to Antarctic, with modern analytical tools. Besides those of direct air samples, the results of analyses of snow, rain, fog, cloud water etc.—indirectly revealing atmospheric pollution—as well as studies on water and soil contamination are welcomed

Prof. Dr. Albert Lebedev
Guest Editor

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Keywords

environmental pollution
priority pollutants
organic pollutants
POPs
organohalogen compounds
pesticides
emerging contaminants
GC-MS, LC-MS
instrumental methods of analysis
targeted analysis
non targeted analysis

Published Papers (12 papers)

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Editorial

Jump to: Research, Review

5 pages, 206 KiB

Open AccessEditorial

Planet Contamination with Chemical Compounds

by Albert T. Lebedev and Susan D. Richardson

Molecules 2022, 27(5), 1621; https://doi.org/10.3390/molecules27051621 - 1 Mar 2022

Cited by 1 | Viewed by 1447

Abstract

The number of known priority pollutants and emerging contaminants of environmental concern currently exceeds several thousand (US EPA Part 423, US EPA Part 401) [...] Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

Research

Jump to: Editorial, Review

14 pages, 1383 KiB

Open AccessArticle

Volatiles Emission by Crotalaria nitens after Insect Attack

by Fausto Prada, Elena E. Stashenko and Jairo René Martínez

Molecules 2021, 26(22), 6941; https://doi.org/10.3390/molecules26226941 - 17 Nov 2021

Cited by 3 | Viewed by 2189

Abstract

Plants are known to increase the emission of volatile organic compounds upon the damage of phytophagous insects. However, very little is known about the composition and temporal dynamics of volatiles released by wild plants of the genus Crotalaria (Fabaceae) attacked with the specialist lepidopteran caterpillar Utetheisa ornatrix (Linnaeus) (Erebidae). In this work, the herbivore-induced plant volatiles (HIPV) emitted by Crotalaria nitens Kunth plants were isolated with solid phase micro-extraction and the conventional purge and trap technique, and their identification was carried out by GC/MS. The poly-dimethylsiloxane/divinylbenzene fiber showed higher affinity for the extraction of apolar compounds (e.g., trans-β-caryophyllene) compared to the Porapak™-Q adsorbent from the purge & trap method that extracted more polar compounds (e.g., trans-nerolidol and indole). The compounds emitted by C. nitens were mainly green leaf volatile substances, terpenoids, aromatics, and aldoximes (isobutyraldoxime and 2-methylbutyraldoxime), whose maximum emission was six hours after the attack. The attack by caterpillars significantly increased the volatile compounds emission in the C. nitens leaves compared to those subjected to mechanical damage. This result indicated that the U. ornatrix caterpillar is responsible for generating a specific response in C. nitens plants. It was demonstrated that HIPVs repelled conspecific moths from attacked plants and favored oviposition in those without damage. The results showed the importance of volatiles in plant–insect interactions, as well as the choice of appropriate extraction and analytical methods for their study. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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29 pages, 3908 KiB

Open AccessArticle

Determination of Metallic Impurities by ICP-MS Technique in Eyeshadows Purchased in Poland. Part I

by Aleksandra Pawlaczyk, Magdalena Gajek, Martyna Balcerek and Małgorzata I. Szynkowska-Jóźwik

Molecules 2021, 26(21), 6753; https://doi.org/10.3390/molecules26216753 - 8 Nov 2021

Cited by 6 | Viewed by 2526

Abstract

Eye shadows, which are products willingly and frequently used by women and even children, have been reported in literature to contain toxic metals. In this work, a total of 94 eye shadows samples available on the Polish market were collected. Eye shadow products have been selected in order to include several parameters important from the point of view of the typical consumer such as: product type (mat/pearl), consumer group (for adults and children), price range (very cheap, medium price, expensive and very expensive), color (twelve different colors were tested), manufacturer (eight brands were investigated) or country of production (four countries were included). The concentration of selected metals (Ag, Ba, Bi, Cd, Pb, Sr, Tl) was determined by ICP-MS technique after the sample extraction with a mixture of nitric acid and hydrogen peroxide in a microwave closed system. For Ag, Cd and Tl, some results were below the established limit of quantification for the employed technique. The presence of strontium, barium, lead and bismuth was confirmed in all studied samples. The obtained results for analyzed elements were, in general, quite comparable with the data reported by other authors. A small number of samples exceeding the permissible values (two samples were beyond the limit value for Cd of 0.5 mg/kg and one exceed the acceptable concentration for Pb of 10 mg/kg) also proves a relatively good condition of the Polish cosmetics market and suggests insubstantial risk for the potential consumers. The results gathered for some of the eye shadows intended for children turned out to be alarmingly high, in particular for elements such as Cd. The highest concentration of Cd reached almost 4 mg/kg, while of Pb amounted to 16 mg/kg. The presence of the statistically significant differences was confirmed for all included parameters with an exception of the color of the eye shadow. Considering the results acquired only for Cd and Pb with respect to the country of origin, the least contaminated cosmetics by metallic impurities seem to be the one produced in Canada, while the ones presenting the highest health risk among all studied eye shadows are make-up cosmetics originating from Poland and Italy. Multivariate analysis of a large data set using CA methods and PCA provided valuable information on dependencies between variables and objects. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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13 pages, 1120 KiB

Open AccessArticle

Gas Chromatography–Mass Spectrometry Quantification of 1,1-Dimethylhydrazine Transformation Products in Aqueous Solutions: Accelerated Water Sample Preparation

by Mark S. Popov, Nikolay V. Ul’yanovskii and Dmitry S. Kosyakov

Molecules 2021, 26(19), 5743; https://doi.org/10.3390/molecules26195743 - 22 Sep 2021

Cited by 5 | Viewed by 2139

Abstract

The use of highly toxic rocket fuel based on 1,1-dimethylhydrazine (UDMH) in many types of carrier rockets poses a threat to environment and human health associated with an ingress of UDMH into wastewater and natural reservoirs and its transformation with the formation of numerous toxic nitrogen-containing products. Their GC-MS quantification in aqueous samples requires matrix change and is challenging due to high polarity of analytes. To overcome this problem, accelerated water sample preparation (AWASP) based on the complete removal of water with anhydrous sodium sulfate and transferring analytes into dichloromethane was used. Twenty-nine UDMH transformation products including both the acyclic and heterocyclic compounds of various classes were chosen as target analytes. AWASP ensured attaining near quantitative extraction of 23 compounds with sample preparation procedure duration of no more than 5 min. Combination of AWASP with gas chromatography–mass spectrometry and using pyridine-d₅ as an internal standard allowed for developing the rapid, simple, and low-cost method for simultaneous quantification of UDMH transformation products with detection limits of 1–5 μg L⁻¹ and linear concentration range covering 4 orders of magnitude. The method has been validated and successfully tested in the analysis of aqueous solutions of rocket fuel subjected to oxidation with atmospheric oxygen, as well as pyrolytic gasification in supercritical water modelling wastewater from carrier rockets launch sites. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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19 pages, 2663 KiB

Open AccessArticle

Sulfamethoxazole Leaching from Manure-Amended Sandy Loam Soil as Affected by the Application of Jujube Wood Waste-Derived Biochar

by Mohammad I. Al-Wabel, Munir Ahmad, Muhammad I. Rafique, Mutair A. Akanji, Adel R. A. Usman and Abdullah S. F. Al-Farraj

Molecules 2021, 26(15), 4674; https://doi.org/10.3390/molecules26154674 - 2 Aug 2021

Cited by 6 | Viewed by 1978

Abstract

Vertical translocation/leaching of sulfamethoxazole (SMZ) through manure-amended sandy loam soil and significance of biochar application on SMZ retention were investigated in this study. Soil was filled in columns and amended with manure spiked with 13.75 mg kg⁻¹ (S1), 27.5 mg kg⁻¹ (S2), and 55 mg kg⁻¹ (S3) of SMZ. Jujube (Ziziphus jujube L.) wood waste was transformed into biochar and mixed with S3 at 0.5% (S3-B1), 1.0% (S3-B2), and 2.0% (S3-B3) ratio. Cumulative SMZ leaching was lowest at pH 3.0, which increased by 16% and 34% at pH 5.0 and 7.0, respectively. A quicker release and translocation of SMZ from manure occurred during the initial 40 h, which gradually reduced over time. Intraparticle diffusion and Elovich kinetic models were the best fitted to leaching data. S3 exhibited the highest release and vertical translocation of SMZ, followed by S2, and S1; however, SMZ leaching was reduced by more than twofold in S3-B3. At pH 3.0, 2.0% biochar resulted in 99% reduction in SMZ leaching within 72 h, while 1.0% and 0.5% biochar applications reduced SMZ leaching to 99% within 120 and 144 h, respectively, in S3. The higher SMZ retention onto biochar could be due to electrostatic interactions, H-bonding, and π-π electron donor acceptor interactions. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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10 pages, 8412 KiB

Open AccessArticle

Statistics of the Popularity of Chemical Compounds in Relation to the Non-Target Analysis

by Boris L. Milman and Inna K. Zhurkovich

Molecules 2021, 26(8), 2394; https://doi.org/10.3390/molecules26082394 - 20 Apr 2021

Cited by 3 | Viewed by 2387

Abstract

The idea of popularity/abundance of chemical compounds is widely used in non-target chemical analysis involving environmental studies. To have a clear quantitative basis for this idea, frequency distributions of chemical compounds over indicators of their popularity/abundance are obtained and discussed. Popularity indicators are the number of information sources, the number of chemical vendors, counts of data records, and other variables assessed from two large databases, namely ChemSpider and PubChem. Distributions are approximated by power functions, special cases of Zipf distributions, which are characteristic of the results of human/social activity. Relatively small group of the most popular compounds has been denoted, conventionally accounting for a few percent (several million) of compounds. These compounds are most often explored in scientific research and are practically used. Accordingly, popular compounds have been taken into account as first analyte candidates for identification in non-target analysis. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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18 pages, 2619 KiB

Open AccessFeature PaperArticle

Monitoring and Statistical Analysis of Formation of Organochlorine and Organobromine Compounds in Drinking Water of Different Water Intakes

by Margarita Yu. Vozhdaeva, Alfiya R. Kholova, Igor A. Melnitskiy, Ilya I. Beloliptsev, Yulia S. Vozhdaeva, Evgeniy A. Kantor and Albert T. Lebedev

Molecules 2021, 26(7), 1852; https://doi.org/10.3390/molecules26071852 - 25 Mar 2021

Cited by 9 | Viewed by 2300

Abstract

The main drawback of drinking water chlorination involves the formation of quite hazardous disinfection by-products (DBPs), represented mainly by halogenated species. Based on the authors’ monitoring data since 2002, the prevalence of chlorine over bromine in the composition of volatile DBPs was shown for the drinking water in Ufa (Russia). However, the situation was completely reversed in the case of semi-volatile DBPs. The principal goal of the present study involved rationalization of the results of the long-term monitoring. Gas chromatography–mass spectrometry (GC-MS) was used for the qualitative and quantitative analysis of volatile DBPs. Identification of semi-volatile compounds was carried out with GC-MS, while gas chromatography with an atomic emission detector (GC-AED) was used for their quantification. A significant contribution of oxygen to the composition of semi-volatile compounds proves the decisive role of the dissolved organic matter oxidative destructive processes. Statistical analysis revealed notable linear correlations for trihalomethane and haloacetic acid formation vs. chlorine dose. On the contrary, halogenated semi-volatile products do not demonstrate any correlations with the water quality parameters or chlorine dose. Principal component analysis (PCA) placed them into separate groups. The results allow for proposing that formation of the organohalogenated species involved the fast penetration of bromine into the humic matter molecules and, further, their oxidative destruction by active chlorine. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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17 pages, 4159 KiB

Open AccessArticle

Simply Applicable Method for Microplastics Determination in Environmental Samples

by Urška Šunta, Polonca Trebše and Mojca Bavcon Kralj

Molecules 2021, 26(7), 1840; https://doi.org/10.3390/molecules26071840 - 25 Mar 2021

Cited by 13 | Viewed by 3742

Abstract

Microplastics (MPs) have gained significant attention in the last two decades and have been widely researched in the marine environment. There are, however, less studies on their presence, routes of entry, and impacts on the biota in the soil environment. One of the main issues in the study of MPs is a lack of standardized methods for their identification in environmental samples. Currently the most commonly used techniques are thermal desorption gas chromatography–mass spectrometry (GC–MS) methods and pyrolysis followed by GC–MS. In this study, headspace-solid phase microextraction followed by GC–MS is proposed as a simple and widely applicable method for the determination of commonly present polymer MPs (polyethylene terephthalate, polystyrene, polyvinyl chloride, polyethylene, and polypropylene) in environmental samples, for analytical laboratories with basic equipment worldwide. The proposed method is based on the identification of compounds, which are formed during the well-controlled melting process of specific coarse (1–5 mm) and fine fraction (1 mm–100 μm) MPs. The method was upgraded for the identification of individual polymer type in blends and in complex environmental matrices (soil and algae biomass). The successful application of the method in complex matrices makes it especially suitable for widescale use. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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16 pages, 306 KiB

Open AccessArticle

Determination of Pharmaceuticals, Heavy Metals, and Oxysterols in Fish Muscle

by Barbara Bobrowska-Korczak, Agnieszka Stawarska, Arkadiusz Szterk, Karol Ofiara, Małgorzata Czerwonka and Joanna Giebułtowicz

Molecules 2021, 26(5), 1229; https://doi.org/10.3390/molecules26051229 - 25 Feb 2021

Cited by 14 | Viewed by 2398

Abstract

The present study aimed to assess the levels of 98 multi-class pharmaceuticals including cardiovascular drugs, antidepressants, hypnotics, antibiotics, and sulfonamides occurring in the muscle tissue of fish caught in the Baltic Sea. The following fish species were collected: perch (Perca fluviatilis); flounder (Platichthys flesus); turbot (Scophthalmus maximus); plaice (Pleuronectes platessa); cod (Gadus morhua callarias); bream (Abramis brama); crucian (Carassius carassius). Additionally, in the examined fish muscle the levels of heavy metals and trace elements were determined (As; Ag; Au; Ba; Cd; Co; Cr; Cu; Hg; Li; Mo; Ni; Pb; Sb; Se; Sn; Tl; V) as well as the levels of cholesterol and its 5 derivatives (7-ketocholesterol; 7α-hydroxycholesterol; 7β-hydroxycholesterol; 5β,6β-epoxy-cholesterol; 5α,6α-epoxycholesterol). In the performed studies 11 out of 98 examined pharmaceuticals were detected in fish muscle. The levels of pharmaceuticals in fish muscle varied depending on the species. In the tissues of bream and crucian, no pharmaceuticals were found. Mercury, lead and arsenic were detected in the muscles of all examined fish. Based on the hazard factor for Hg, Pb, Cd, Ni (target hazard quotient, THQ < 1), it was found that the consumption of the studied fish does not constitute a health risk. However, the THQ for As remained >1 indicated possible risk from those metals. In the examined fish muscle the total cholesterol oxidation products (COPs) level of oxysterols were, respectively: 6.90 (cod) μg/g–4.18 μg/g (perch), which corresponded to 0.7–1.5% of cholesterol. The main COPs evaluated were 7-ketocholesterol (0.78 ± 0.14–1.79 ± 0.06 μg/g), 7β-hydroxycholesterol (0.50 ± 0.04–3.20 ± 2.95 μg/g) and 5β,6β-epoxycholesterol (0.66 ± 0.03–1.53 ± 0.66 μg/g). The assessment of health hazards due to contaminations is necessary, which may help to introduce national legislation and global standards aimed at reducing or even eliminating the exposure to contaminants. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

19 pages, 2711 KiB

Open AccessArticle

Environmental Risk Assessment Resulting from Sediment Contamination with Perfluoroalkyl Substances

by Grażyna Gałęzowska, Justyna Rogowska, Ewa Olkowska, Wojciech Ratajczyk and Lidia Wolska

Molecules 2021, 26(1), 116; https://doi.org/10.3390/molecules26010116 - 29 Dec 2020

Cited by 5 | Viewed by 2687

Abstract

Due to wide use of perfluoroalkyl substances (PFASs) (e.g., in metal-plating, in fire-fighting foam, lubricants) and their resistance to degradation, they occur widely in the environment. The aim of this study was to estimate the environmental risk resulting from the presence of PFASs in the Gulf of Gdansk. Therefore, 17 PFASs concentrations were determined using ultra performance liquid chromatography with tandem mass spectrometry detection (UPLC-MS/MS). Additionally, sediment ecotoxicity was investigated. The results of the chemical analysis were used to asses environmental risk of PFASs. In samples collected around discharge collectors from a wastewater treatment plant and the Vistula mouth, Σ17PFASs values were 0.00403 ÷ 40.6 and 0.509 ÷ 614 ng/g d.w., respectively. In samples collected around discharge collectors, PFHxA, PFPeA, PFHpA, and PFOA were dominating, while at the Vistula River mouth, PFHxS, PFDS, and PFBS were prevalent. For most sediments, no toxic effect was observed in the toxicity tests with Heterocypris inconguens and Aliivibrio ficsheri. There was no observed correlation between the PFASs level and their ecotoxicity. Generally, the results of environmental risk assessment indicate that the PFASs would not generate high impact on the aquatic life (five water samples have shown medium risk related to PFBS and PFDoA). Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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16 pages, 3440 KiB

Open AccessArticle

The Influence of Non-Engineered Municipal Landfills on Groundwater Chemistry and Quality in Bloemfontein, South Africa

by Rinae Makhadi, Saheed A. Oke and Olusola O. Ololade

Molecules 2020, 25(23), 5599; https://doi.org/10.3390/molecules25235599 - 28 Nov 2020

Cited by 4 | Viewed by 2381

Abstract

This study assessed the groundwater quality around two municipal solid waste landfill sites, in the city of Bloemfontein, Free State Province, South Africa. The two landfill sites are located in two contrasting geological terrains, with both lacking some basic facilities found in a well-designed landfill. A total of eight groundwater samples were collected from pollution monitoring boreholes near the two landfill sites, with five samples representing the northern landfill site and three samples representing the southern landfill site. The samples were collected in the autumn and winter seasons to assess any possible seasonal variations. They were analysed for physicochemical (pH, electrical conductivity (EC), total dissolve solids (TDS), chemical oxygen demand (COD) and total organic carbon (TOC)) and microbiological parameters (Escherichia coli, total coliform). The results of the analysis showed that the waters from both landfills were generally dominated by Ca, Mg, SO4, and HCO3 ions. Some of the major anions and cations in the water samples were above the South African National Standard (SANS241:2015) and World Health Organisation (WHO) permissible limits for drinking water. Majority of the boreholes had total dissolved solids and electrical conductivity values exceeding the SANS 241:2015 and WHO permissible limits. Piper trilinear plots for the two landfill sites showed that Ca(Mg)HCO3 water type predominates, but Ca(Mg)SO4 and Ca(Mg)Cl were also found. These water types were further confirmed with expanded Durov diagrams, indicating that that the boreholes represented a water type that is seldom found which is undergoing ion exchange, typical of sulphate contamination. From the SAR diagrams, boreholes in the northern landfill site had a high salinity hazard with only one borehole in the southern landfill site having a high salinity hazard. The geology was found to play a significant role in the distribution of contaminants into the groundwater systems in the study area. The study concluded that the northern landfill site had a poorer water quality in comparison to the southern landfill site based on the analysed physicochemical parameters. However, the southern landfill site showed significant microbial contamination, due to the elevated amount of E. coli and total coliform concentrations. The high permeability of the weathered dolerites in the northern landfill site might have enabled the percolation of contaminants into the groundwater resulting in the poorer water quality. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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Review

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32 pages, 1385 KiB

Open AccessReview

Interactions between Humic Substances and Microorganisms and Their Implications for Nature-like Bioremediation Technologies

by Natalia A. Kulikova and Irina V. Perminova

Molecules 2021, 26(9), 2706; https://doi.org/10.3390/molecules26092706 - 5 May 2021

Cited by 57 | Viewed by 5786

Abstract

The state of the art of the reported data on interactions between microorganisms and HSs is presented herein. The properties of HSs are discussed in terms of microbial utilization, degradation, and transformation. The data on biologically active individual compounds found in HSs are summarized. Bacteria of the phylum Proteobacteria and fungi of the phyla Basidiomycota and Ascomycota were found to be the main HS degraders, while Proteobacteria, Actinobacteria, Bacteroidetes, and Firmicutes were found to be the predominant phyla in humic-reducing microorganisms (HRMs). Some promising aspects of interactions between microorganisms and HSs are discussed as a feasible basis for nature-like biotechnologies, including the production of enzymes capable of catalyzing the oxidative binding of organic pollutants to HSs, while electron shuttling through the utilization of HSs by HRMs as electron shuttles may be used for the enhancement of organic pollutant biodegradation or lowering bioavailability of some metals. Utilization of HSs by HRMs as terminal electron acceptors may suppress electron transfer to CO₂, reducing the formation of CH₄ in temporarily anoxic systems. The data reported so far are mostly related to the use of HSs as redox compounds. HSs are capable of altering the composition of the microbial community, and there are environmental conditions that determine the efficiency of HSs. To facilitate the development of HS-based technologies, complex studies addressing these factors are in demand. Full article

(This article belongs to the Special Issue Planet Contamination with Chemical Compounds)

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