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J. Earth Syst. Sci. (2021) 130:88 Ó Indian Academy of Sciences https://doi.org/10.1007/s12040-021-01570-w (0123456789().,-volV)( 0123456789().,-vol V) Heavy metal contamination and provenance of sediments recovered at the Grijalva River delta, southern Gulf of Mexico 1 2, MARTHA PATRICIA AYALA-PEREZ ,JOHN SARMSTRONG-ALTRIN * 2 and MARIA LUISA MACHAIN-CASTILLO 1Posgrado en Ciencias del Mar y Limnologıa, Universidad Nacional Autonoma de Mexico, Ciudad Universitaria, 04510 Mexico City, CDMX, Mexico. 2Unidad de Procesos Oceanicos y Costeros, Instituto de Ciencias del Mar y Limnologıa, Universidad Nacional Autonoma de Mexico, Ciudad Universitaria, 04510 Mexico City, CDMX, Mexico. *Corresponding author. e-mail: [email protected] john˙[email protected] MS received 19 November 2020; revised 5 January 2021; accepted 6 January 2021 This study examines textural characteristics, carbonate, organic carbon and chemical composition of sediment samples recovered in the nearshore region (*3–19 m water depth) at the Grijalva River mouth, southern Gulf of Mexico. The aim of this study is to assess the heavy metal contamination and prove- nance variations in sediments between the dry and northers (rainy) seasons. The proportion of sand, carbonate, and organic carbon contents were abundant at sites located near to the Grijalva River mouth, principally in northers season. Silt content is dominant in the dry season, especially in the sites located away from the Grijalva River mouth. The Chemical Index (CIX) values obtained for the dry (*76–84) and northers (*75–87) seasons indicated a moderate to high intensity of weathering and a humid climate in the source area. The low K2O/Al2O3 ratio values (\0.5) in the dry and northers seasons indicated a higher proportion of aluminosilicates than detrital minerals, due to moderate-to-high intensity of weathering. The correlation among elemental concentrations revealed the association of Cr, Nb, Zr, Hf, Y, and rare earth elements (REE) with detrital minerals rather than aluminosilicates. The major element concentrations, Th/Sc, La/Sc, Co/Th, and Cr/Ni elemental ratios indicated the derivation of sediments from intermediate and maBc igneous rocks. A similarity in the North American Shale Composite (NASC) normalized rare earth element (REE) patterns and Eu anomaly between the dry and northers seasons suggested that the variations in sediment input played a less significant role and the provenance of sediments remained constant. The enrichment factor (EF) showed moderate to severe enrichment for Cr, Ni, and Sb (EF = *2.63–7.57), highest in the northers season, especially at the Grijalva River mouth, although the index of geo-accumulation (Igeo) for these elements suggested as moderately polluted (Igeo = 0.34–2.0). The slightly elevated EF values for Cr, Ni, and Sb during northers season were probably due to an increase in sediment discharge into the sea during the northers season. We inferred that the enrich- ment of Cr, Ni, and Sb in sediments was due to both lithogenic and anthropogenic origins. The sediments were inCuenced by the intermediate and basic igneous rocks of the Chiapas Massif Complex, and the waste generated by the urban areas located within the Grijalva River drainage basin. Keywords. Contamination; enrichment factor; geochemistry; sediment texture; nearshore; Grijalva. 88 Page 2 of 23 J. Earth Syst. Sci. (2021) 130:88 1. Introduction Rosales-Hoz et al. 2015; Celis-Hernandez et al. 2017; Machain-Castillo et al. 2020). As, Ba and Cu Urbanization and industrialization of coastal areas have been found to exceed threshold eAect level in the last decade have increased the stress of the and Cd, Cr, and Ni probable eAect level bench- people living in the coastal and marine environ- marks in the sGOM (Machain-Castillo et al. 2019). ments. Land-use changes due to settlements, Machain-Castillo et al. (2020) documented that the agriculture, cattle raising, oil and mining indus- Grijalva River is an important contributor of tries increase erosion and associated heavy metal heavy metals, pesticides, and hydrocarbons to the contaminants carried by the rivers, that ulti- SW Gulf of Mexico. mately discharge into the marine environment Other studies investigated the provenance of (El-Baz and Khalil 2018; Swiercz and Zaje˛cka coastal and deep sea sediments of the Gulf of Mexico 2018; Maftei et al. 2019). These contaminants based on the mineralogy, textural, and geochemistry incorporated into the marine sediments could pose data (Kasper-Zubillaga et al. 1999; Carranza-Ed- toxic eAects in the local biota, therefore, it is wards et al. 2015; Armstrong-Altrin and Machain- important to determine the concentration of Castillo 2016; Ramos-Vazquez et al. 2017; Tapia- heavy metals in sediments and to assess their level Fernandez et al. 2017; Anaya-Gregorio et al. 2018; of toxicity for the biota and marine sediments Armstrong-Altrin et al. 2018, 2019, 2020; Ramos- (Kurt 2018; Alexandrowicz 2019; Celis-Hernandez Vazquez and Armstrong-Altrin 2019; Machain- et al. 2020; Wang et al. 2020). Castillo et al. 2020). The major and trace element concentrations of The above-mentioned studies were concentrated terrigenous sediments are useful to infer the within or far away from the coastline, where the provenance and intensity of weathering in the sediment deposition and mixing processes are dif- source area (Cullers 2000; Bansal et al. 2018; ferent from the nearshore environment. Neverthe- Greggio et al. 2018;Huet al. 2019; Al-Kaaby and less, knowledge on nearshore sediments is Albadran 2020; Armstrong-Altrin et al. 2020). The important, because it covers the river discharge immobile elements like Al2O3, TiO2, Th, Zr, Co, area as well as the characteristics of the catchment Nb, Sc and REE are the best indicators of parent area. In fact, the provenance and heavy metal rocks, which is due to their low mobility during contamination of sediments in the shallow water transport and short residence time in seawater depth or nearshore environment in the Gulf of (Wang et al. 2018, 2019a, b; Men et al. 2019; Mexico were less investigated. Hence, to fulBll this Chaudhuri et al. 2020). Also, REE has a little gap, this study examines the geochemistry of sed- geochemical fractionating during weathering, and iments recovered in the nearshore environment Eu anomaly can provide information regarding the during the dry and northers seasons in front of the type of source rocks (Tapia-Fernandez et al. 2017; Grijalva River mouth, sGOM. The aim of this Carranza-Edwards et al. 2019; Madhavaraju et al. study is to investigate the status of heavy metal 2019; Balaram 2020). contamination in sediments in the Grijalva River Heavy metal concentrations in beach sediments discharge area and to recognize its hazard to the were analyzed in various studies around the world marine environment and biota. In addition, based and these studies utilized techniques like enrich- on the geochemistry data, we investigated the ment factor (EF) and geochemical index (Igeo) to intensity of weathering and provenance of assess the contamination degree (El-Baz and Khalil sediments. 2018; Lazo et al. 2018; Varga et al. 2018; Damian et al. 2019; Horasan and Arik 2019). In the Gulf of Mexico, the coastal processes like littoral currents, eddies, tidal, and wind directions were addressed 2. Study area by various researchers (Monreal-Gomez et al. 1992; Salas de Leon et al. 2004, 2005; Salas-Perez et al. The study area is part of the Grijalva–Usumacinta 2008; Exposito-D ıaz et al. 2009). Similarly, trace River system (GURS), which is considered as the element concentrations in the coastal and near- longest river in Mexico, its drainage basin consists shore sediments from the southern Gulf of Mexico of 85,553 km2 (Day et al. 2003). The Grijalva River (sGOM) were studied by various authors, partic- (1521 km length) originates from the northwestern ularly their historical trends and heavy metal Guatemala and Chiapas State, Mexico and dis- contamination (Ruiz-Fernandez et al. 2012, 2019; charges into the sGOM, Tabasco State. The annual J. Earth Syst. Sci. (2021) 130:88 Page 3 of 23 88 Figure 1. Map showing the sample locations in the Grijalva River delta, southern Gulf of Mexico (source: Carta Geologica; scale 1:1,000,000; map modiBed after Armstrong-Altrin 2015). water discharge of GURS Cuvial system in the Gulf and hydrocarbons in the nearshore environment of Mexico is *2678 m3 sÀ1 yr À1 (Hudson et al. (Rosales-Hoz et al. 2015). 2005). The samples were collected in the nearshore zone 2.1 Climate at the Grijalva River mouth, in the sGOM, Tabasco State, within the physiographic province The climate is warm and humid with an average of the Bay of Campeche (Bgure 1;92°410–92°270W annual temperature above 268C (Garcıa and longitude and 18°360–18°390N latitude). The Gri- Vidal 1990). Rainfall is almost throughout the jalva River is joined at its lower course with an arm year, but it is more abundant in summer and fall of the Usumacinta River with a length of approx- seasons. The average annual precipitation is 2000 imately 40 km from where the Usumacinta changes mm and occasionally it is [3000 mm/year its course to join with the Grijalva River with a (Yan˜ez-Arancibia et al. 2009). The prevailing Cow of 1700 m3/s (Ortiz-Perez 1992). The devel- winds are east-northeast direction, with an aver- opment of industry along the GURS basin has age speed of 4–6 m/s and they are inCuenced by propitiated the availability of metals, pesticides northers, which are cold air masses from the 88 Page 4 of 23 J. Earth Syst. Sci. (2021) 130:88 north, in addition to tropical storms and hurri- Table 1. Location of surface sediment samples retrieved at the canes. The northers generate winds of greater Grijalva River delta, southern Gulf of Mexico.

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