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Geochemistry of Pyritic Mudstones from the Singa Formation, Malaysia: Insights Into Gold Potential, Source of Sulfur and Organic Matter

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Geochemistry of Pyritic Mudstones from the Singa Formation, Malaysia: Insights Into Gold Potential, Source of Sulfur and Organic Matter geosciences Article Geochemistry of Pyritic Mudstones from the Singa Formation, Malaysia: Insights into Gold Potential, Source of Sulfur and Organic Matter Charles Makoundi 1,* , Zakaria Endut 2,*, Ross R. Large 1, Khin Zaw 1, Elena Lounejeva 1, Mohd Shafeea Leman 3,4, Kamal Roslan Mohamed 3,4 and Mohd Basril Iswadi Basori 3 1 Centre for Ore Deposit and Earth Science, University of Tasmania, Private Bag 126, Hobart, TAS 7001, Australia; [email protected] (R.R.L.); [email protected] (K.Z.); [email protected] (E.L.) 2 School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, Nibong Tebal 14300, Penang, Malaysia 3 Geology Programme, School of Environment and Nature Resource Sciences, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, Bangi 43600, Selangor, Malaysia; [email protected] (M.S.L.); [email protected] (K.R.M.); [email protected] (M.B.I.B.) 4 Langkawi Research Centre, Institute for Environment and Development (Lestari), Jalan Teluk Yu, Kampung Kok, Langkawi 07000, Kedah, Malaysia * Correspondence: [email protected] (C.M.); [email protected] (Z.E.); Tel.: +61-36-226-2472 (C.M.); +60-19-982-8334 (Z.E.) Citation: Makoundi, C.; Endut, Z.; Abstract: Major trace element analyses, including pyrite chemistry of pyritic mudstones of shallow- Large, R.R.; Zaw, K.; Lounejeva, E.; marine Singa Formation of Pennsylvanian–Early Permian age have been carried out to assess gold Leman, M.S.; Mohamed, K.R.; Basori, potential, the source of sulfur and organic matter. Regionally, Singa Formation spatially correlates M.B.I. Geochemistry of Pyritic with the Bohorok Formation (Sumatra, Indonesia), the Kaeng Krachang group (Thailand), and the Mudstones from the Singa Formation, Lebyin group (Burma or Myanmar). In Southeast Asia, this formation is important because it has Malaysia: Insights into Gold a record of glacial processes that occurred along the northern margin of Gondwana in the Late Potential, Source of Sulfur and Paleozoic age. This study has revealed that mudstones of the Singa Formation, which contain Organic Matter. Geosciences 2021, 11, lonestones of glacial origin, deposited under suboxic–oxic conditions in shallow marine environment 279. https://doi.org/10.3390/ during Pennsylvanian–Early Permian time. The black mudstones contain total organic carbon which geosciences11070279 ranges from 0.1 to 0.7 wt.%, and gold content varying from 40 to 62 ppb, making them gold source Academic Editors: Marco Viccaro and rocks. This study has revealed diagenetic gold presence in the early pyrite generations (pyrites 1, 2, Jesus Martinez-Frias and 3) in these mudstones with gold content ranging up to 1.6 ppm Au which is indicative of early enrichment of gold. Conversely, late generations of pyrite (pyrites 4, 5, and 6) in these mudstones Received: 10 May 2021 record low gold content up to 0.5 ppm Au. The δ34S values for pyrite grains range from −24.6‰ Accepted: 29 June 2021 to +6.2‰ likely indicate a combination of magmatic and biogenic source of sulfur. Organic carbon Published: 2 July 2021 isotope composition of the pebbly mudstone samples shows a wide range from −23.9‰ to −5.8‰ indicating a mixed terrestrial and marine source. Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in Keywords: gold; source rock; X-ray fluorescence analysis; geochemistry; Malaysia published maps and institutional affil- iations. 1. Introduction Fine-grained sedimentary sequences host several trace elements, including Zn, Pb, Cu, Copyright: © 2021 by the authors. Mo, Se, V, U, Ni, As, Ag, Sb, Cr, and Au [1–4]. Black shales (commonly metamorphosed Licensee MDPI, Basel, Switzerland. to greenschist facies) are host to significant gold deposits in certain regions in the world This article is an open access article such as the Chuniespoort Group of the Late Archean–Early Proterozoic Transvaal Sequence distributed under the terms and (South Africa), the Central Gold Belt (Malaysia), and the Sepon Mineral District (Laos), the conditions of the Creative Commons Mathinna Turbidite deformed sequence in Northeast Tasmania (Australia), Upper Devo- Attribution (CC BY) license (https:// nian black shale series of the Xikuangshan Sb deposit in Hunan (China) [5–9]. Paleozoic creativecommons.org/licenses/by/ 4.0/). glacial deposits are cropping out in Southeast Asia [10]. Geosciences 2021, 11, 279. https://doi.org/10.3390/geosciences11070279 https://www.mdpi.com/journal/geosciences Geosciences 2021, 11, 279 2 of 22 Tasmania (Australia), Upper Devonian black shale series of the Xikuangshan Sb deposit in Hunan (China) [5–9]. Paleozoic glacial deposits are cropping out in Southeast Asia [10]. ThisThis study study focuses focuses on onthe theLate Late Carboniferous Carboniferous (Pennsylvanian (Pennsylvanian)–Early)–Early Permian Permian Singa Singa FormationFormation (Figure (Figure 1),1 which), which was was deposited deposited during during Late Late Paleozoic Paleozoic glacial glacial times times [11] and [ 11 ] and priorprior to to the the Pangea Pangea break break-up-up [ [1212]].. Argillaceous Argillaceous sequences sequences including including black black or or dark mud- mudstostonesnes are are distributed distributed in in the the Langkawi Langkawi Islands. Islands These. These mudstones mudstones have have never never been been investi- investigatedgated for their for tracetheir elementtrace element content. content It begs. It the begs question the question whether whether the black the mudstones black can mudstonesbe source can rocks be forsource metals rocks in for the metals district. in Thethe district. element The of strongelement interest of strong is the interest proximity is of thethe proximity Singa Formation of the Singa to theFormation locally exposedto the locally granitic exposed outcrops granitic (which outcrops is a possible (which is source a of possiblemagmatic source fluids), of magmatic and its connectionfluids), and with its con othernection formations with other across formations the region. across the region. FigureFigure 1. 1.GeologicalGeological sketch sketch map map of Langkawi of Langkawi Islands, Islands, Malaysia Malaysia (modified (modified after afterChe et Che al., et2008) al., 2008)[11]. [11]. In Inthis this study study,, we we report report the themetal metal content content of black of black mudstones mudstones for the for Singa the SingaFormation Formation evaluatedevaluated from from both both pyrite pyrite trace trace element chemistry and wholewhole rockrock analyses.analyses.The The signifi- significancecance of this of this study study lies lies in understanding in understanding the the redox redox conditions conditions over over the the deposition deposition of these ofmudstones these mudstones in the in Gondwanaland the Gondwanaland Sea and Sea toand also to accountalso account forgold for gold source source rock rock potential. potential.The reason The beingreason is being thatin is manythat in orogenic many orogenic gold systems, gold systems, mudstones mudstones or shales or shales were found wereto contain found to early contain enrichment early enrichment of gold in of their gold first in generationtheir first generation of sedimentary of sedimentary pyrite followed pyriteby later followed remobilization by later remobilization of gold to concentrate of gold to in concentrate structural trapsin structural during traps basin during inversion or basinsubsequent inversion tectonic or subsequent deformation. tectonic This deformation study investigated. This study whether investigate sedimentaryd whether pyrites sedimentaryexisting in pyrites the Singa exist mudstonesing in the containSinga mudstones gold and tracecontain elements gold and that trace would element warrants that further wouldmetallogenic warrant further research. metallogenic research. TheThe Central Central Gold Gold Belt Belt of of Peninsular Malaysia is knownknown toto containcontain mudstones mudstones associ- associatedated with with significant significant gold-enriched gold-enriched structures structures which which have ha beenve been in the in verythe very core core of economic of economicgeology geology research, research, mineral mineral exploration, exploration, and mining and mining in Malaysia. in Malaysia In. this In this study, study, the trace theelement trace element content content of these of mudstonesthese mudstones is compared is compared to that to ofthat carbonaceous of carbonaceous shales shales which are which are widely known to be best gold source rocks [1–4]. widely known to be best gold source rocks [1–4]. In addition, knowing the origin and isotopic signature of the organic carbon and sulfur is important as mudstones or shales in orogenic gold systems often have elevated2 Geosciences 2021, 11, 279 3 of 22 content of organic carbon and sulfur reflecting the redox conditions (oxic to euxinic) of the ocean during their deposition. The source of organic carbon and sulfur of these black or dark mudstones is an important contribution in understanding the origin of organic matter and sulfur from these clast-bearing mudstones in the Sibumasu Terrane. 2. Geological Setting Paleozoic sedimentary rocks and granite crop out on the Langkawi Islands [13]. The distribution of these rocks is shown in Figure1. The oldest Paleozoic sequence is the Machinchang Formation, which consists mainly of three Members. The oldest Hulur Member, which is a coarsening upward sequence that contains interbedded graded silt- stone, grey shale, and clayey sandstone, is interpreted
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