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Applied Geochemistry This article was published in an Elsevier journal. The attached copy is furnished to the author for non-commercial research and education use, including for instruction at the author’s institution, sharing with colleagues and providing to institution administration. Other uses, including reproduction and distribution, or selling or licensing copies, or posting to personal, institutional or third party websites are prohibited. In most cases authors are permitted to post their version of the article (e.g. in Word or Tex form) to their personal website or institutional repository. Authors requiring further information regarding Elsevier’s archiving and manuscript policies are encouraged to visit: http://www.elsevier.com/copyright Author's personal copy Applied Geochemistry Applied Geochemistry 22 (2007) 1970–1993 www.elsevier.com/locate/apgeochem Arsenic and presumed resistate trace element geochemistry of the Lincolnshire (UK) sedimentary ironstones, as revealed by a regional geochemical survey using soil, water and stream sediment sampling Neil Breward British Geological Survey, Keyworth, Nottingham NG12, 5GG, UK Received 31 October 2006; accepted 8 March 2007 Editorial handling by C. Reimann Available online 10 May 2007 Abstract A regional geochemical survey using soils, stream sediment and stream water sampling revealed multi-element geochem- ical anomalies, though of low environmental mobility, associated with Mesozoic sedimentary ironstones in Lincolnshire, UK. The most prominent of these anomalies were of As and V in soils and sediments, but elevated levels of elements such as Cr, La, Ce and Th were also observed. These were initially thought to be part of a residual resistate element or heavy- mineral suite, but careful examination suggests that these too may be primarily associated with the process of Fe oxide precipitation during the initial formation of the ironstones. Crown Copyright Ó 2007 Published by Elsevier Ltd. All rights reserved. 1. Introduction The English county of Lincolnshire hosts several Mesozoic sedimentary ironstone formations, nota- During the preparation of the Regional Geo- bly the Frodingham ironstone at Scunthorpe, the chemical Atlas of the Humber-Trent region (British Marlstone Rock in the south near Grantham, and Geological Survey, 2007) for the British Geological the Claxby ironstone which runs below the escarp- Survey’s Geochemical Baseline Survey of the Envi- ment of the Wolds from Spilsby north to Caistor ronment (G-BASE) project, a series of strong and (Fig. 1). The former are of Lower Jurassic age, the distinctive geochemical patterns for a number of ele- latter is of Lower Cretaceous age, but all show some ments were observed over sedimentary ironstone interesting geochemical characteristics. Each of outcrops in Lincolnshire, U.K., and are worthy of these named ‘ironstone formations’ contain ferrugi- special attention. Possible explanations for the pat- nous sandstones, limestones and mudstones in addi- terns observed are given and examined. tion to beds of true ironstones which generally contain greater than 30% by weight Fe oxides. Sed- imentary ironstones, other than the more problem- E-mail address: [email protected] atic banded iron formations, are mainly lagoonal 0883-2927/$ - see front matter Crown Copyright Ó 2007 Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.apgeochem.2007.03.058 Author's personal copy N. Breward / Applied Geochemistry 22 (2007) 1970–1993 1971 Fig. 1. Sketch map of the ‘solid’ geology of Lincolnshire, and location within the UK. or shallow-water marine deposits where conditions ganic phosphate with Fe(III) as hydroxide to give allow movement of free reduced Fe in solution as the highly insoluble FePO4–Fe(OH)3 additive com- 2þ (III) Æ FeðaqÞ or as colloidal Fe complexes and its precip- plex. Strengite (FePO4 2H2O) and ferrihydrite (II) (III) itation in a variety of insoluble Fe and Fe (Fe(OH)3) can be considered to be the nominal compounds, minerals such as goethite, limonite, sid- end-members of this complex reaction series. One erite, vivianite and chamosite being the most com- additional feature of this sorption reaction is that 3À mon forms. The content of sulphides such as arsenate, AsO4 , can behave very similarly to phos- 3À pyrite is variable, depending largely on the original phate, PO4 , under these conditions (cf. Dixit and organic-matter content of the lagoonal sediments Hering, 2003), and is also strongly sorbed to Fe and the O2 fugacity during sedimentation and pre- hydroxide precipitates, resulting in elevated As lev- cipitation, but is generally low in the ironstones els in many sedimentary ironstones. Scorodite under consideration here. This is significant, as pyr- (FeAsO4 Æ2H2O) is analogous to strengite and simi- ite can be an important carrier mineral for As, and larly forms a complex reaction series with ferrihy- such a readily-oxidised mineral would make the drite, though the pure scorodite end-member is a high As levels noted in this study much more mobile rare mineral, which is only formed under strongly and potentially hazardous. A comprehensive expla- acidic conditions (e.g., in precipitates from acid nation of sedimentary ironstone geochemistry can mine drainage waters) and is not especially resistant be found in Maynard (1983), and Young and Taylor to weathering. The peculiar sources and deposi- (1989). Elevated levels of other elements are often tional environment of sedimentary ironstones may found in sedimentary ironstones, notably Ca (as also lead to elevated levels of other trace elements, many are impure limestones) and P, due to the reac- notably those which are commonly believed to have tion and sorption of solubilised organic and inor- a ‘resistate’ mineral host, such as Cr, V, Th and the Author's personal copy 1972 N. Breward / Applied Geochemistry 22 (2007) 1970–1993 Fig. 1 (continued) lanthanide elements Ce and La. Resistate elements from the late Triassic (Mercia Mudstone Group) are generally those whose host minerals are highly to the Upper Cretaceous (Chalk). The Quaternary resistant to both chemical and physical weathering geological map (Fig. 2) shows a variety of coverings and hence have a very long residence time in soils of till and fluvioglacial sands and gravels, lacustrine, and sediments. They are not necessarily the same river and marine alluvium, peat and patches of as ‘heavy minerals’, though some heavy minerals blown sand. Holocene beach and Fen deposits, with are resistate. smaller areas of anthropogenic ‘made ground’, com- plete the sequence. The stratigraphic relationships 2. Topography and geological background are shown in Figs. 3 and 4. Of the three major iron- stones present, the Frodingham and Claxby beds Much of Lincolnshire is relatively low-lying, but are restricted to this area, while the Marlstone rock with ridges of higher ground formed by a number of bed is more strongly developed to the south, notably resistant geological formations, notably the Frod- in Leicestershire and Oxfordshire, and only crops ingham and Marlstone Rock Bed ironstones, the out in the south of the area shown. The Frodingham Lincolnshire Limestone, and the Chalk, which rises ironstone provided rich Fe ores and was extensively to over 160 m O.D. in the Wolds. A map of the mined until recently, forming the basis for the steel ‘solid’ (Pre-Quaternary) geology is shown in industry of Scunthorpe. The Claxby ironstone has a Fig. 1, and shows a broadly north–south to NW– narrow outcrop at the base of the Chalk escarpment SE pattern of Mesozoic sedimentary rocks ranging and was worked on a much smaller scale, e.g., at Author's personal copy N. Breward / Applied Geochemistry 22 (2007) 1970–1993 1973 Fig. 2. Sketch map of the Quaternary geology of Lincolnshire. Nettleton [NGR 511, 400] near Caistor, 20 km west landmass, and is described in detail in several pub- of Grimsby, though the last mine here closed in lications (Johnson and Breward, 2004; Johnson 1969. The Marlstone rock bed was not worked in et al., 2005). When sampling commenced in the the area of interest, but was formerly mined in the late 1960s the work was stimulated by mineral area immediately to the south, for example between exploration, but this high-resolution survey has Grantham and Melton Mowbray. Other much thin- evolved continuously and now has many environ- ner and impersistent ironstones are locally present mental applications. The geochemical mapping, at some other horizons within the Lias and Lower originally based on the collection of wet-sieved Cretaceous (e.g., within the Hundleby and Tealby sub-150 lm drainage sediments at a target sam- Clays), but naturally show less prominent geochem- pling density of one stream sediment sample per ical features at outcrop. km2, has expanded to include the sampling and analysis of stream waters and soils (sub-2 mm) 3. The G-BASE regional geochemical survey project and now also includes the systematic sampling of urban soils (Fordyce et al., 2005). Solid materials The Geochemical Baseline Survey of the Envi- are analysed for some 38 elements by X-ray fluo- ronment (G-BASE) is a long-established, high-res- rescence spectrometry (XRFS), and filtered stream olution regional geochemical mapping project run waters (0.45 lm) are analysed mainly by induc- by the British Geological Survey, aimed at making tively-coupled plasma atomic emission spectrome- a complete geochemical survey for the whole UK try (ICP–AES) and inductively-coupled plasma Author's personal copy 1974 N. Breward / Applied Geochemistry 22 (2007) 1970–1993 Fig. 3. Outline stratigraphy of the Lower Jurassic (Lias Group) in Lincolnshire. Fig. 4. Outline stratigraphy of the Upper Jurassic and Lower Cretaceous in Lincolnshire. mass spectrometry (ICP–MS) for up to 35 ele- high resolution survey and wide range of elements, ments, plus parameters such as pH and conductiv- the project database now contains data for some ity by other methods. Consequentially, with such a five million individual element determinations. Author's personal copy N.
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