Plant Residues as Direct and Indirect Sources of Hydrocarbons in


Plant Residues as Direct and Indirect Sources of Hydrocarbons in...

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Plant residues as direct and indirect sources of hydrocarbons in soils: current issues and legal implications. Marco Vecchiato, Tiziano Bonato, Andrea Bertin, Elena Argiriadis, Carlo Barbante, and Rossano Piazza Environ. Sci. Technol. Lett., Just Accepted Manuscript • DOI: 10.1021/acs.estlett.7b00464 • Publication Date (Web): 10 Nov 2017 Downloaded from http://pubs.acs.org on November 13, 2017

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Plant Residues as Direct and Indirect Sources of Hydrocarbons in Soils:

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Current Issues and Legal Implications.

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Marco Vecchiato a*, Tiziano Bonato Rossano Piazza

a,c

a,b

, Andrea Bertin b, Elena Argiriadis a, Carlo Barbante

a,c

,

.

7 8 9 10

a

Department of Environmental Sciences, Informatics and Statistics (DAIS), Ca’ Foscari University of

Venice, Via Torino 155, 30172 Venezia-Mestre, Venice, Italy.

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b

Società Estense Servizi Ambientali (S.E.S.A. S.p.A.), Via Comuna 5/B, 35042, Este, PD, Italy.

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c

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Venezia-Mestre, Venice, Italy.

Institute for the Dynamics of Environmental Processes (IDPA-CNR), Via Torino 155, 30172

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*Corresponding author: Marco Vecchiato

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e-mail: [email protected]

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phone: +39 0412348545

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Keywords: Soil; Total petroleum hydrocarbons (TPH); n-Alkanes; leaf waxes; amendments.

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Abstract

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Plant residues are the main source of organic matter in soil: this process takes place naturally in

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forests and with organic amendments in farmlands. Terrestrial plants also synthesize

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hydrocarbons: typically, angiosperms contain hundreds to thousands mg kg-1 of long-chain n-

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alkanes in leaf waxes. However, petroleum pollution is a worldwide issue and different national

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regulations set at 50 mg kg-1 the guideline limit for petroleum hydrocarbons in green areas.

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Focusing on the Italian legislation as a case study, we hypothesized that direct or indirect high

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inputs of plant residues could lead the soil to exceed this limit, resulting in a false positive

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petroleum contamination. Therefore, we investigated the occurrence of hydrocarbons in soils with

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different inputs of natural or farming biomasses. The highest total petroleum hydrocarbons (TPH)

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concentrations were found in background soils from protected woodlands, remarkably with most

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samples resulting above the guideline limit. Similarly, TPH in agricultural soils amended with

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compost and digestate resulted higher than in soil samples where only chemical fertilizers were

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used. n-Alkanes Carbon Preference Indices (CPIs) underlined the role of plant residues as source of

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hydrocarbons in these samples, clearly distinguishing spiked petrogenic contamination. Possible

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revisions of the regulatory and analytical methods were later discussed.

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Introduction

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Terrestrial plants produce hydrocarbons as components of the epicuticular waxes to protect plant

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tissues from the external environment1. When plant residues are incorporated in soil, these

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contribute to the soil organic matter2, both naturally in woodlands and forests or artificially from

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crop residues or manure in agricultural lands. The input of biomasses and the fertilization with

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amendments, as compost and digestate, have positive effects on the biological, physical, and

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chemical soil properties, reducing dumping of wastes in landfill sites3–5. Moreover, the organic

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matter in agricultural soils is considered one potential sink for sequestration of atmospheric

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carbon dioxide2,6.

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On the other hand, petroleum hydrocarbons are some of the most widespread soil pollutants

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worldwide and hydrocarbon contamination of soil is an issue widely studied in the scientific

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literature. However, one of the main analytical and legal issues is how to distinguish between

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actual petrogenic contamination from naturally occurring hydrocarbons and biogenic 2 ACS Paragon Plus Environment

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interferences, since these could potentially lead to unnecessary remediation costs7. However,

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although many parameters (reported in the SI) have been proposed and used to identify the

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environmental contamination due to petroleum hydrocarbons8–11, none of them is unique and

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effective for the different petroleum-derived products, probably except total petroleum

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hydrocarbons (TPH). This parameter, despite its selectivity drawbacks7, is generally adopted to

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assess the soil contamination from the different petroleum products. The analytical determination

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of TPH includes a large family of different hydrocarbons, regardless of their toxicity, origin and

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composition (linear, branched, cyclic and aromatic compounds)12,13. Italian legislation (Legislative

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Decree 152/2006, Part IV, Title V, Annex 5) sets the limit for heavy hydrocarbons (with a number

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of carbon atoms higher than 12) in public, private, residential green areas and agricultural land at

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50 mg kg-1 d.w.; those sites found to exceed these limits should be remediated or a site-specific

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risk analysis should prove the absence of human health risks. The parameter C>12 is substantially

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corresponding to TPH, defining a slight modification of the normed analytical method ISO

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16703:2004 changing the application range from C10-C40 to C12-C40 13.

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The limit at 50 mg kg-1 d.w. is not based on hydrocarbon toxicity, which is highly dependent on the

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speciation and the availability of the hydrocarbons, but it was selected because it was considered

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to be high enough to avoid false positives14. Consequently this value was chosen as target value

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for soil quality standards in different European countries12,14. However, the various national

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regulations result in very different procedures and intervention guidelines for remediation of

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contamination episodes of agricultural soil. For example, there is a wide discrepancy of two orders

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of magnitude between the Italian and Dutch intervention values for remediation of hydrocarbons

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in soil, being the limits set at 50 mg kg-1 and 5000 mg kg-1 (VROM 2012), respectively12. This clearly

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shows the need for the harmonization of national procedures for contaminated sites in the

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European Union14. Outside from Europe, a similar situation is present also in the USA, with

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significant variability of methods, action and clean-up levels for hydrocarbons in contaminated

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soils among the different states, in a framework of increasing complexity15. The Canadian

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legislation specifies different carbon ranges to analyze the total hydrocarbons in soil7. Notably the

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method does not include a purification step, therefore also polar biogenic compounds such as

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plant waxes, fatty acids and sterols are considered as petroleum hydrocarbon contaminants, even

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when naturally exceeding the regulatory levels16.

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Plant-derived n-alkanes

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Terrestrial plants typically synthesize long chain n-alkanes as part of the epicuticular leaf wax,

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contributing to the hydrophobic properties and protecting the leaf from the external environment.

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Leaf n-alkanes are commonly produced with a strong odd-over-even predominance (OEP), and,

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lacking functional groups, are especially long-lived molecules1. For these reasons n-alkanes are

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widely used as biomarkers to reconstruct environmental changes in modern and paleoecological

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studies1,17. The abundance and distribution of the n-alkanes in leaves depend on the plant species,

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the growing season and the environmental conditions (e.g. temperature, moisture, nutrient

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availability, soil properties), varying even within an individual tree1,18. Typically, angiosperms

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produce hundreds to thousands mg of n-alkanes per kg of dry leaf matter, while gymnosperms are

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at orders of magnitude lower. n-C27, n-C29 and n-C31 are the dominant n-alkanes in graminoids and

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woody angiosperms in variable relative abundances1. The Carbon Preference Index (CPI) is a

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definitive measure of biologically synthesized compounds, defining the degree to which odd

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carbon number n-alkanes dominate over even carbon numbers, being the ratio of the sums of

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concentrations of odd and even n-alkane homologues in a given carbon number range19. Mean CPI

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values in leaves of the large majority of modern plant are around 10 although with very large

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variations, being in few cases close or lower than 1, which is the typical CPI value of petrogenic

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inputs1,20. Another parameter is the weighted average of the various carbon chain lengths of the n-

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alkanes, usually defined as the Average Chain Length (ACL=∑(Cnxn)/∑Cn), where Cn is the

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concentration of each n-alkane with n carbon atoms1. Leaf surface waxes can be sources of n-

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alkanes to soil both in woodland and grassland21,22, as well as directly from crop residues in

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agricultural land 23. Other tissues of higher plants (e.g. beech and spruce roots) are characterized

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