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Title
Abstract
Key Takeaways
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Introduction
Historical Review
Analytical Methods
Results and Discussion
Basic Data
GC-MS Analysis of C 15+ Alkanes
Conclusions
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Earth Sciences
Geochemistry and Petrology

The organic geochemistry of the Hasbeya asphalt (Lebanon): comparison with asphalts from the Dead Sea area and Iraq

Profile image of Arie NissenbaumArie NissenbaumProfile image of Jacques ConnanJacques Connan

2004, Organic Geochemistry

https://doi.org/10.1016/J.ORGGEOCHEM.2004.01.015
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15 pages

Abstract

The Hasbeya asphalt from Lebanon and the Mezar-1 asphalt from the Golan Heights were analyzed using current tools of petroleum geochemistry, namely isotopic analyses (dD, d 13 C, d 34 S) and molecular sterane and terpane parameters. The geochemical properties of these asphalts were compared to several other asphalts from Israel (floating blocks of the Dead Sea, Massada, Nahal Heimar, IPRG). All the asphalts belong to the same genetic family (e.g. high gammacerane and high steroid contents, no diasteranes) and originate from Senonian (Upper Cretaceous) organicmatter-rich carbonate source rocks deposited in an anoxic or dysoxic (perhaps hypersaline) palaeoenvironment. This family of asphalts is well differentiated from another famous asphalt from the Near East, the Hit-Abu Jir asphalt from Iraq. The Hasbeya asphalt is slightly biodegraded, whereas the Mezar-1 asphalt was affected by more severe biodegradation (occurrence of 25-nor-hopanes). Isotopic ratios of asphaltenes were found to be useful in allowing differentiation of asphalts from the same genetic family. This study completes the existing knowledge on Dead Sea asphalts by demonstrating that similar asphalts may be identified within a much larger geographic area, including the Golan Heights and Lebanon. These results raise the question of whether some of the archaeological asphalts that are found in the southern Fertile Crescent (Egypt, Israel, Syria, etc.) and which were assumed to be of Dead Sea origin, may actually have come from Hasbeya. #

Key takeaways
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  1. The Hasbeya asphalt shares a genetic family with Dead Sea asphalts, indicating regional geochemical similarities.
  2. Both Hasbeya and Dead Sea asphalts are derived from Senonian organic-matter-rich carbonate rocks in anoxic settings.
  3. Isotopic analyses (dD, d13C, d34S) effectively differentiate asphalts within the same genetic family.
  4. The Mezar-1 asphalt exhibits severe biodegradation, evidenced by the presence of 25-nor-hopanes.
  5. This study suggests that archaeological asphalts in the southern Fertile Crescent may originate from Hasbeya instead of the Dead Sea.
Figures (11)
Fig. 1. Location map of the Dead Sea and Lebanon area showing the various asphalt occurrences discussed in the pre- sent study. The Hasbeya asphalt mines are located in a relatively small area along the Hasbeya fault on the western flank of the Hermon anticline in southern Lebanon. This fault
Fig. 1. Location map of the Dead Sea and Lebanon area showing the various asphalt occurrences discussed in the pre- sent study. The Hasbeya asphalt mines are located in a relatively small area along the Hasbeya fault on the western flank of the Hermon anticline in southern Lebanon. This fault
wheel. The asphalt was hewed out of the rock, leaving behind some of the sediment as supporting columns. Asphalt pieces, which weighed about several rotels each (1 rotel= about 2.5 kg) were brought to the surface and sold by the local emir, who had a monopoly on asphalt production, to merchants in Damascus, Beirut and Aleppo. According to Burckhardt, most of the pits had been abandoned by the time of his visit, and the mining operation was restricted to one pit and worked only during the summer months (perhaps due to the frequent rains in the winter months). Anderson (1852), who was the scientist in Lieut. Lynch’s expedition to the Dead Sea in 1848, also mentioned the bitumen pits near Has- beya. This asphalt, he said, resembles Dead Sea asphalt, although it was “more metamorphosed’’. The pits were worked by 8-10 Arab and Kurd workmen and, accord- ing to the overseer, the proceeds barely covered the cost of labor (Anderson, 1852). In 1908, an anonymous author wrote that the asphalt in the Hasbeya deposit was found as impregnations in white Cretaceous soft rocks and that the deposits were of limited extent (Anonymous, 1908). According to Toll (1921), asphalt was mined in Hasbeya, where pure asphalt occurs in veins up to 4 m thick. Toll noted that the Hasbeya mines were quite rich and had been worked for many years. He wrote that in 1856, a group of Damascus merchants obtained a permit to mine asphalt in Has- Fig. 2. Isotopic data of asphaltenes from the different asphalts: plot of 8!3C (in %o/PDB) vs. 5D (in %o/SMOW) and 8!°C (in %o/PDB) vs. 5548 = 84S (in %o/CDT). Arrow indicates the location The Mezar-1 sample on the 5!3C scale since its 5D was not measured.
wheel. The asphalt was hewed out of the rock, leaving behind some of the sediment as supporting columns. Asphalt pieces, which weighed about several rotels each (1 rotel= about 2.5 kg) were brought to the surface and sold by the local emir, who had a monopoly on asphalt production, to merchants in Damascus, Beirut and Aleppo. According to Burckhardt, most of the pits had been abandoned by the time of his visit, and the mining operation was restricted to one pit and worked only during the summer months (perhaps due to the frequent rains in the winter months). Anderson (1852), who was the scientist in Lieut. Lynch’s expedition to the Dead Sea in 1848, also mentioned the bitumen pits near Has- beya. This asphalt, he said, resembles Dead Sea asphalt, although it was “more metamorphosed’’. The pits were worked by 8-10 Arab and Kurd workmen and, accord- ing to the overseer, the proceeds barely covered the cost of labor (Anderson, 1852). In 1908, an anonymous author wrote that the asphalt in the Hasbeya deposit was found as impregnations in white Cretaceous soft rocks and that the deposits were of limited extent (Anonymous, 1908). According to Toll (1921), asphalt was mined in Hasbeya, where pure asphalt occurs in veins up to 4 m thick. Toll noted that the Hasbeya mines were quite rich and had been worked for many years. He wrote that in 1856, a group of Damascus merchants obtained a permit to mine asphalt in Has- Fig. 2. Isotopic data of asphaltenes from the different asphalts: plot of 8!3C (in %o/PDB) vs. 5D (in %o/SMOW) and 8!°C (in %o/PDB) vs. 5548 = 84S (in %o/CDT). Arrow indicates the location The Mezar-1 sample on the 5!3C scale since its 5D was not measured.
During the drilling, hydrocarbon shows with a strong hydrogen sulfide smell were encountered at depths of 600-900 m. Asphalt was encountered in cavities and as fracture at filling in the Turonian dolomite, which con- tained water of low salinity with a dissolved organic matter content of 10-20 mg/l. The water temperature at the bottom of the borehole was around 60 °C, and the geothermal gradient was estimated to be 45 °C/km, a higher value than the geothermal gradient in most of Israel. The formation of asphalt from the oil shales in the area was studied by Tannenbaum (1983) and Tan- nenbaum and Aizenshtat (1985). The bitumen content of the oil shales was shown to be very high and geo- chemically very similar to the asphalt. They concluded that the asphalt was immature and that it had gone through short-range migration, accompanied by negli- gible fractionation, from the source rocks into the Tur- onian carbonates. Fig. 3. Gas Chromatogram of the C;5+ alkanes from the Hasbeya asphalt. Abbreviations: n-C,5=n-pentadecane, 30«8H = 17«,21B- hopane, 3lafpH S+R=17a,21B-homohopane 22S + 22R. The Mezar-1 borehole (previously known as the Ein- Said-1 borehole; Michelson, 1981; Tannenbaum, 1983) is located on the southern slopes of the Golan Heights, facing the Yarmouk River, about 4 km west of the Mukheibe dam and the Hammat-Gader (El-Hamma) hot springs (Fig. 1). The borehole was drilled in an attempt to gain access to the fresh water that drains underground from the Ajlun Heights of northern Jordan. The borehole
During the drilling, hydrocarbon shows with a strong hydrogen sulfide smell were encountered at depths of 600-900 m. Asphalt was encountered in cavities and as fracture at filling in the Turonian dolomite, which con- tained water of low salinity with a dissolved organic matter content of 10-20 mg/l. The water temperature at the bottom of the borehole was around 60 °C, and the geothermal gradient was estimated to be 45 °C/km, a higher value than the geothermal gradient in most of Israel. The formation of asphalt from the oil shales in the area was studied by Tannenbaum (1983) and Tan- nenbaum and Aizenshtat (1985). The bitumen content of the oil shales was shown to be very high and geo- chemically very similar to the asphalt. They concluded that the asphalt was immature and that it had gone through short-range migration, accompanied by negli- gible fractionation, from the source rocks into the Tur- onian carbonates. Fig. 3. Gas Chromatogram of the C;5+ alkanes from the Hasbeya asphalt. Abbreviations: n-C,5=n-pentadecane, 30«8H = 17«,21B- hopane, 3lafpH S+R=17a,21B-homohopane 22S + 22R. The Mezar-1 borehole (previously known as the Ein- Said-1 borehole; Michelson, 1981; Tannenbaum, 1983) is located on the southern slopes of the Golan Heights, facing the Yarmouk River, about 4 km west of the Mukheibe dam and the Hammat-Gader (El-Hamma) hot springs (Fig. 1). The borehole was drilled in an attempt to gain access to the fresh water that drains underground from the Ajlun Heights of northern Jordan. The borehole
Fig. 4. Gas chromatograms of the C;5; aromatics from the Hasbeya and the Nahal Heimar asphalt. (a) Nahal Heimar, no. 406, biodegraded, no n-alkanes. (b) Hasbeya, incipent biogradation, n-alkanes present. Identification and abbreviations of chemical struc- tures were done according to Riolo et al. (1986).
Fig. 4. Gas chromatograms of the C;5; aromatics from the Hasbeya and the Nahal Heimar asphalt. (a) Nahal Heimar, no. 406, biodegraded, no n-alkanes. (b) Hasbeya, incipent biogradation, n-alkanes present. Identification and abbreviations of chemical struc- tures were done according to Riolo et al. (1986).
Fig. 5. Distribution of some biomarker families in the C;5+ alkanes: comparison of the Mezar-1, Dead Sea and Abu Jir asphalts. The data are expressed as ppm of the C,5+ alkanes. J. Connan, A. Nissenbaum | Organic Geochemistry
Fig. 5. Distribution of some biomarker families in the C;5+ alkanes: comparison of the Mezar-1, Dead Sea and Abu Jir asphalts. The data are expressed as ppm of the C,5+ alkanes. J. Connan, A. Nissenbaum | Organic Geochemistry
Fig. 6. Distributions of terpanes (m/z 191) and steranes (m/z 217) from the Hasbeya and Dead Sea asphalts. Abbreviations: 23/3 = C3 tricyclopolyprenane, Ts=18a-22,29,30-trisnorneohopane, Tm=17a-22,29,30-trisnorhopane, 29%8H = 17o,218-30-norhopane, 30a8H = 17x,21B-hopane, 31aBHS = 17«,21B-22S-30-homohopane, 35aBHS = 17a,21B-22S-29-pentakishomohopane, GCR = gamma- cerane, 27St=27a0uR+S+270BBR+S, 27x0nnS =S5a,140,17x-20S-cholestane, 28a8BS = 5a,14B,17B-20S-24-methylcholestane, 29a BBR = 5a,14B,17B-20R-24-ethylcholestane, 215'=5a,148,17B-pregnane, 22St = 5a,14B,17B-20-methylpregnane. In order to enable a more comprehensive discussion of the results, reference was made to other asphalts from the Dead Sea Rift (Fig. 1): Dead Sea floating blocks, Nahal Heimar asphalts, Tamar-1 and IPRG asphalts (Rullk6tter et al., 1985; Connan et al., 1992) and Massada asphalt, and to the famous asphalt deposit of Hit-Abu Jir in Iraq (Connan, 1988; Connan et al., 1998). All samples were re-analyzed by the same techniques to provide directly comparable geochemical information. The soluble part of the sample is extracted with di- chloromethane or chloroform, and the emphasis is on the analysis of “saturated” and ‘aromatic hydro- carbon” fractions. The dichloromethane extract is frac- tionated into three classes of compounds (‘‘saturated hydrocarbons”, ‘aromatics hydrocarbons” and polars compounds) by the IATROSCAN Mk IV apparatus on Chromarods (5p silica SHI). The quantitative measure- ment of each fraction is carried out by a flame ionisation detector, to obtain a gross composition of the extract.
Fig. 6. Distributions of terpanes (m/z 191) and steranes (m/z 217) from the Hasbeya and Dead Sea asphalts. Abbreviations: 23/3 = C3 tricyclopolyprenane, Ts=18a-22,29,30-trisnorneohopane, Tm=17a-22,29,30-trisnorhopane, 29%8H = 17o,218-30-norhopane, 30a8H = 17x,21B-hopane, 31aBHS = 17«,21B-22S-30-homohopane, 35aBHS = 17a,21B-22S-29-pentakishomohopane, GCR = gamma- cerane, 27St=27a0uR+S+270BBR+S, 27x0nnS =S5a,140,17x-20S-cholestane, 28a8BS = 5a,14B,17B-20S-24-methylcholestane, 29a BBR = 5a,14B,17B-20R-24-ethylcholestane, 215'=5a,148,17B-pregnane, 22St = 5a,14B,17B-20-methylpregnane. In order to enable a more comprehensive discussion of the results, reference was made to other asphalts from the Dead Sea Rift (Fig. 1): Dead Sea floating blocks, Nahal Heimar asphalts, Tamar-1 and IPRG asphalts (Rullk6tter et al., 1985; Connan et al., 1992) and Massada asphalt, and to the famous asphalt deposit of Hit-Abu Jir in Iraq (Connan, 1988; Connan et al., 1998). All samples were re-analyzed by the same techniques to provide directly comparable geochemical information. The soluble part of the sample is extracted with di- chloromethane or chloroform, and the emphasis is on the analysis of “saturated” and ‘aromatic hydro- carbon” fractions. The dichloromethane extract is frac- tionated into three classes of compounds (‘‘saturated hydrocarbons”, ‘aromatics hydrocarbons” and polars compounds) by the IATROSCAN Mk IV apparatus on Chromarods (5p silica SHI). The quantitative measure- ment of each fraction is carried out by a flame ionisation detector, to obtain a gross composition of the extract.
After the precipitation of asphaltenes by n-hexane and their quantitative gravimetric measurement, an ali- quot of deasphalted extract (100 mg) was fractionated by MPLC (medium pressure liquid chromatography) on a LOBAR MERK column (300 mmx10 mm, Lichro- prep 30-60 jim), activated at 120 °C under N> for 30 min. The “saturated hydrocarbon’ fraction is eluted with n-hexane. Recovery of the “‘aromatic hydrocarbon” fraction was achieved with n-hexane using a back-flush step on both columns (pre-column and analytical column LOBAR-MERCK). This step may re-introduce some polar compounds (ketones, esters) into the so-called “aromatic hydrocarbon” fraction in case of archaeological samples (Connan, 2002). When dealing with asphalts as in the present study, the two “‘hydro- Gas chromatography—mass spectrometry (GC-MS) analysis of “saturated hydrocarbon” and ‘aromatic hydrocarbon” fractions was performed using a Hewlett- Packard 6890/5973 GC-MS instrument equipped with an on-column injector and operating at 70 eV with a mass range of m/z 50-550. A DBS fused silica capillary column was used (J&W, 60 mx0.25 mm, film thickness 0.1 um). The samples were injected at 75 °C, and the oven was programmed at 2 °C/min to 300 °C, where the temperature was held for 66 min. Fig. 7. Distribution of steranes (m/z 217) and terpanes (m/z 197) from the Mezar-1 asphalt. Abbreviations: 23/3 =C,; tricyclopoly- prenanes, 24/3=Cy,4 tricyclopolyprenane, 24/4=de-E-hopane, 26/3 =C2¢ tricyclopolyprenane, Ts = 18a-22,29,30-trisnorneohopane, Tm = 17a-22,29,30-trisnorhopane, 29DafH = 17a,21B-25-norhopanes, 29a8H =17«,21B-30-norhopane, 29Ts=, 300BH = 17«,21B- hopane, 30B0H=178,21a-hopane, 3lafSHS=170,21B-22S-30-homohopane, GCR=gammacerane, 32/6=C3. hexahy- drobenzohopane, 35aBHS=17«,21B-22S-29-pentakishomohopane, 21St=5a,14B8,17B-pregnane, 22St =5a,14B,17B-20-methyl- pregnane, 27diaS=diacholestane 20S, 27an0S=5a,140,17a-20S-cholestane, 28aBBS =5a,14B,17B-20S-24-methylcholestane, 29aBBR = 5a, 148,17B-20R-24-ethylcholestane. carbon” fractions are mainly C,5+ alkanes and Cis54+ aromatics. Finally the polar compounds are eluted with dichloromethane/methanol (85/15) in back-flush mode from the pre-column. Each recovered fraction is then weighed.
After the precipitation of asphaltenes by n-hexane and their quantitative gravimetric measurement, an ali- quot of deasphalted extract (100 mg) was fractionated by MPLC (medium pressure liquid chromatography) on a LOBAR MERK column (300 mmx10 mm, Lichro- prep 30-60 jim), activated at 120 °C under N> for 30 min. The “saturated hydrocarbon’ fraction is eluted with n-hexane. Recovery of the “‘aromatic hydrocarbon” fraction was achieved with n-hexane using a back-flush step on both columns (pre-column and analytical column LOBAR-MERCK). This step may re-introduce some polar compounds (ketones, esters) into the so-called “aromatic hydrocarbon” fraction in case of archaeological samples (Connan, 2002). When dealing with asphalts as in the present study, the two “‘hydro- Gas chromatography—mass spectrometry (GC-MS) analysis of “saturated hydrocarbon” and ‘aromatic hydrocarbon” fractions was performed using a Hewlett- Packard 6890/5973 GC-MS instrument equipped with an on-column injector and operating at 70 eV with a mass range of m/z 50-550. A DBS fused silica capillary column was used (J&W, 60 mx0.25 mm, film thickness 0.1 um). The samples were injected at 75 °C, and the oven was programmed at 2 °C/min to 300 °C, where the temperature was held for 66 min. Fig. 7. Distribution of steranes (m/z 217) and terpanes (m/z 197) from the Mezar-1 asphalt. Abbreviations: 23/3 =C,; tricyclopoly- prenanes, 24/3=Cy,4 tricyclopolyprenane, 24/4=de-E-hopane, 26/3 =C2¢ tricyclopolyprenane, Ts = 18a-22,29,30-trisnorneohopane, Tm = 17a-22,29,30-trisnorhopane, 29DafH = 17a,21B-25-norhopanes, 29a8H =17«,21B-30-norhopane, 29Ts=, 300BH = 17«,21B- hopane, 30B0H=178,21a-hopane, 3lafSHS=170,21B-22S-30-homohopane, GCR=gammacerane, 32/6=C3. hexahy- drobenzohopane, 35aBHS=17«,21B-22S-29-pentakishomohopane, 21St=5a,14B8,17B-pregnane, 22St =5a,14B,17B-20-methyl- pregnane, 27diaS=diacholestane 20S, 27an0S=5a,140,17a-20S-cholestane, 28aBBS =5a,14B,17B-20S-24-methylcholestane, 29aBBR = 5a, 148,17B-20R-24-ethylcholestane. carbon” fractions are mainly C,5+ alkanes and Cis54+ aromatics. Finally the polar compounds are eluted with dichloromethane/methanol (85/15) in back-flush mode from the pre-column. Each recovered fraction is then weighed.
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Abbreviations: 8'3C=8!3C (in %o/PDB), 5D = 8D (in %o/SMOW), 5*4S = 84S (in %o/CDT), Ts/Tm = 18«-22,29,30-trisnorneohopane/17«-22,29,30-trisnorhopane, 23/3 / 24/4 = C3 tricyclopolyprenane/C E-hopane, Tric/Pentac=Tricyclic terpanes/Pentacyclic terpanes, GCR/30«aBH =Gammacerane/17%,21B-hopane, m/z 191 / m/z 217=Terpanes/Steranes,% 27BBSt=% 5a,14B,17B-20R-chol ne + 5a,14B8,17B-20S-cholestane, 28BBSt=% 5a,14B,17B-20R-24-methylcholestane + 5a,148,17B-20S-24-methylcholestane, 29BBSt=% 5a,14B,17B-20R-24-ethylcholestane + 5a,14B,17B-20S-24-ethylch: tane. Alteration of steranes and terpanes comprises 16 degrees of alteration (Connan, unpublished), 0 corresponds to no alteration, 6-8 to changes in steranes with a significant loss of Cy7 and Co steran in Mezar-1 asphalts. Absolute quantitation ware carried out using deuterated standards (2,2,4,4-d4-5a-20R-24-ethylcholestane, 2,3-d2-17B,210-30-normoretane) for sterane and terpane measurements. Isotopic data of asphaltenes and molecular ratios of asphalts used in the study
Abbreviations: 8'3C=8!3C (in %o/PDB), 5D = 8D (in %o/SMOW), 5*4S = 84S (in %o/CDT), Ts/Tm = 18«-22,29,30-trisnorneohopane/17«-22,29,30-trisnorhopane, 23/3 / 24/4 = C3 tricyclopolyprenane/C E-hopane, Tric/Pentac=Tricyclic terpanes/Pentacyclic terpanes, GCR/30«aBH =Gammacerane/17%,21B-hopane, m/z 191 / m/z 217=Terpanes/Steranes,% 27BBSt=% 5a,14B,17B-20R-chol ne + 5a,14B8,17B-20S-cholestane, 28BBSt=% 5a,14B,17B-20R-24-methylcholestane + 5a,148,17B-20S-24-methylcholestane, 29BBSt=% 5a,14B,17B-20R-24-ethylcholestane + 5a,14B,17B-20S-24-ethylch: tane. Alteration of steranes and terpanes comprises 16 degrees of alteration (Connan, unpublished), 0 corresponds to no alteration, 6-8 to changes in steranes with a significant loss of Cy7 and Co steran in Mezar-1 asphalts. Absolute quantitation ware carried out using deuterated standards (2,2,4,4-d4-5a-20R-24-ethylcholestane, 2,3-d2-17B,210-30-normoretane) for sterane and terpane measurements. Isotopic data of asphaltenes and molecular ratios of asphalts used in the study
The gas chromatogram of the C,5+ aromatics of the Hasbeya asphalt are given in Fig. 4 with the corres- ponding gas chromatogram of the Nahal Heimar asphalt (sample 406). The Nahal Heimar asphalt, out- cropping at surface near the Dead Sea as a bitumen cementing rocks, has the same origin as the asphalt of the Dead Sea floating blocks. This surface asphalt is The gas chromatogram of C,5+ alkanes of Hasbeya asphalt (Fig. 3) reveals several diagnostic features. There is incipient biodegradation of n-alkanes which results in high pristane/n-C,7 and phytane/n-Cjg ratios of 2.0 and 3.7, respectively. Such a situation was not observed in the Dead Sea asphalt where the pristane/n- Fig. 8. Ternary diagram providing the composition of C27-Cr9aPBBsteranes (27aPBsteranes = 5a,14B,17B-20S-cholestane + 5a, 14B,17B- 20R-cholestane, 28aPPsteranes = 5x,14B,17B-20S-24-methylcholestane + 5a,14B,17B-20R-24-methylcholestane, 29aBBster- anes = 5a, 14B,17B-20S-24-ethylcholestane + 5a,14B,17B-20R-24-ethylcholestane) of the various asphalts: comparison of the Dead Sea family of asphalts to the famous asphalt deposit of Hit-Abu Jir in Iraq. Measurements of Cy7-Cro%BBsteranes were carried out with a deuterated standard (2,2,4,4,d4-5a,14B,17B-24-ethylcholestane) using the mass fragmentogram m/z 218 from which the% C27 (C27/ Co7+ Cog +Cr9),% Cog and% Cro are calculated.
The gas chromatogram of the C,5+ aromatics of the Hasbeya asphalt are given in Fig. 4 with the corres- ponding gas chromatogram of the Nahal Heimar asphalt (sample 406). The Nahal Heimar asphalt, out- cropping at surface near the Dead Sea as a bitumen cementing rocks, has the same origin as the asphalt of the Dead Sea floating blocks. This surface asphalt is The gas chromatogram of C,5+ alkanes of Hasbeya asphalt (Fig. 3) reveals several diagnostic features. There is incipient biodegradation of n-alkanes which results in high pristane/n-C,7 and phytane/n-Cjg ratios of 2.0 and 3.7, respectively. Such a situation was not observed in the Dead Sea asphalt where the pristane/n- Fig. 8. Ternary diagram providing the composition of C27-Cr9aPBBsteranes (27aPBsteranes = 5a,14B,17B-20S-cholestane + 5a, 14B,17B- 20R-cholestane, 28aPPsteranes = 5x,14B,17B-20S-24-methylcholestane + 5a,14B,17B-20R-24-methylcholestane, 29aBBster- anes = 5a, 14B,17B-20S-24-ethylcholestane + 5a,14B,17B-20R-24-ethylcholestane) of the various asphalts: comparison of the Dead Sea family of asphalts to the famous asphalt deposit of Hit-Abu Jir in Iraq. Measurements of Cy7-Cro%BBsteranes were carried out with a deuterated standard (2,2,4,4,d4-5a,14B,17B-24-ethylcholestane) using the mass fragmentogram m/z 218 from which the% C27 (C27/ Co7+ Cog +Cr9),% Cog and% Cro are calculated.
Fig. 9. Distribution of terpanes (m/z 191) and 25-norhopanes (m/z 177) in the Mezar-1 asphalt. Abbreviations: 29DaBH = 170,21 B-25- norhopanes (‘“demethylated hopanes”’), 294BH = 17a,218-30-norhopane,,.
Fig. 9. Distribution of terpanes (m/z 191) and 25-norhopanes (m/z 177) in the Mezar-1 asphalt. Abbreviations: 29DaBH = 170,21 B-25- norhopanes (‘“demethylated hopanes”’), 294BH = 17a,218-30-norhopane,,.

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Alaa Mostafa

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Molecular geochemical properties of crude oils and surface petroleum seeps from the southern part of the Gulf of Suez were evaluated. The characterizations of individual aliphatic, aromatic, and biomarker compounds were based on gas chromatography (GC) and gas chromatography/mass spectrometry (GC/MS) analyses. The results provided strong evidence for a close genetic association of these samples. The geochemical characteristics suggest an origin from Tertiary source rocks deposited in a normal marine environment that received continental runoff. The molecular signatures of the investigated samples were very similar to those of the Lower Miocene Rudeis Formation source rock in the southern Gulf of Suez. Further, biomarker fingerprints of the investigated oil seeps were compared with those of the Dead Sea asphalt, as well as the bitumen from some Egyptian mummies reported in the literature. The results demonstrate that oil seeps from the southern end of Gebel El Zeit were used by ancient Egyptians for embalming.

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The Evolution of the Dead Sea Floating Asphalt Blocks: Simulations by Pyrolysis
Amos Bein

Journal of Petroleum Geology, 1980

The asphalts found as floating blocks on the Dead Sea and deep-seated in wells diff'er from all other asphalts of the area, mostly by their more abundant and much betterpreserved n-alkanes. Since biodegradation was found to be the main alteration process through which crude oil was altered into aphalts, such well-preserved n-alkanes are unexpected. A hypothesis of secondary generation of these alkanes was tested by pyrolysis simulation of asphalt at 300OC duringperiods ranging up to 60 days. The abundance and distribution pattern of the n-alkanes in the simulated asphaltsafter 14 days of heating resembles that of the floating asphalt blocks and that found at a depth of 3,500 m. In addition to saturated hydrocarbons, aromatics and gases were also formed at the expense of resins and asphaltenes. The H/C ratio was balanced by the formation of pyrobitumen and by a gradual decrease of the HIC ratio in the residual resins and asphaltenes. The gas formed contained about 60 to 80% methane with an isotopic composition of-41 to 4Pha The hydrocarbon content of the simulated asphalt (gas and liquids) increased from about 15% at the starting material to about 60% after 60 days of heating. The recognition that asphalts in the Dead Sea basin are secondarily subjected to alteration upon burial might be of economic importance. Asphalts buried to a depth at which maturation conditionsare close to that reached in the pyrolysis simulation at 300OC after about 60 days may be counted on as source material for hydrocarbons.

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Tetrapyrroles and associated compounds in Dead Sea asphalts
Arie Nissenbaum

Chemical Geology, 1979

M*=tallo and free porphyrins (1000-1500 ppm) isolated from asphalts occurring as huge blocks Iloatmg m the northern part of the Dead Sea, have been analyzed by visible UV (V U V) spectrophotometry, and by mass spectrometry. The concentration o1" vanadyl porphyrins ,n the asphalts exceeds by far that of the Ni porphyrms, despite the I : 3 V/N, ratio found in the total asphalt 8ample The free porphyrins resemble those from the Umta Basin (U.S A) Rilsonite and contain a mixture of homologous Aetio and deoxyphyllo erythroaetioporphyrir=.~ (DPEP). The non porphyrm fraction of the asphalt showed an ,dentical aliphatw, hydrocarbon distribution with that of heavy, crude oil from the same area. The more polar fraction associated w,th the porphyrins was compared with the polar I'ract,on of the prev,ously described ozoker,te from the Dead Sea area. From high.

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The archaeological bitumens of Bahrain from the Early Dilmun period (c.2200 BC) to the sixteenth century AD: a problem of sources and trade
Robert Killick, Jacques Connan, Flemming Højlund

Arabian Archaeology and Epigraphy, 1998

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Bitumen from the Dead Sea in Early Iron Age Nubia
Kate Fulcher

Scientific Reports, 2020

Bitumen has been identified for the first time in Egyptian occupied Nubia, from within the town of Amara West, occupied from around 1300 to 1050 BC. The bitumen can be sourced to the Dead Sea using biomarkers, evidencing a trade in this material from the eastern Mediterranean to Nubia in the New Kingdom or its immediate aftermath. Two different end uses for bitumen were determined at the site. Ground bitumen was identified in several paint palettes, and in one case can be shown to have been mixed with plant gum, which indicates the use of bitumen as a ground pigment. Bitumen was also identified as a component of a friable black solid excavated from a tomb, and a black substance applied to the surface of a painted and plastered coffin fragment. Both contained plant resin, indicating that this substance was probably applied as a ritual funerary liquid, a practice identified from this time period in Egypt. The use of this ritual, at a far remove from the royal Egyptian burial sites at ...

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Asphalt from Horbat'En Ziq
Dr.jacques Connan
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A geochemical study on the bitumen from Dosariyah (Saudi-Arabia): tracking Neolithic-period bitumen in the Persian Gulf
PHILIPP DRECHSLER

Journal of Archaeological Science, 2015

This paper presents the results of a series of geochemical analysis conducted on 20 bitumen samples from the Neolithic site of Dosariyah (Eastern Province, Saudi Arabia). The aim of this study was to establish the geological origin of this bitumen in order to identify the bitumen seepage they were extracted from. The majority of the samples could be successfully related to bitumen seepages of northern Iraq. Two samples didn't match the bulk of the samples and probably came from the Burgan Hill seepage (Kuwait). Three samples were too badly degraded in order to deliver reliable data, and were removed from the dataset. These conclusions stand in contrast with H3/as-Sabiyah, da site culturally and geographically linked with Dosariyahd which bitumen came exclusively from the Burgan Hill. In this paper we argue that this difference may be explained by the difference in dating between the two sites, as H3/as-Sabiyah slightly predates Dosariyah.

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The bitumen imports at Tell Abraq : tracing the second millennium B.C. bitumen industry in south-east Arabia
Peter Magee

2017

Bitumen was widely traded throughout the Arabian Gulf in prehistory and its movement in the Neolithic and Early Bronze Age is well studied. This article presents the results of new geochemical work conducted on bitumen from the mid-second millennium BC at Tell Abraq (Emirate of Sharjah, UAE) to determine the geological origin of the samples. This study uses Stable Carbon Isotope Analysis (δ 13 C) on the asphaltenes fraction and Gas Chromatography-Mass Spectrometry (GC-MS) on the saturated hydrocarbon fraction. The Tell Abraq dataset offers a unique opportunity to understand trade and interaction as no bitumen from this period in southeastern Arabia has ever been investigated. The mid-second millennium BC is one of immense change in the region. It is widely considered that southeastern Arabia was disengaged from major economic interactions in the Arabian Gulf while Kassite influence in the central Gulf had drawn Bahrain (ancient Dilmun) into closer economic and political ties with Mesopotamia. The identification of Iranian bitumen at Tell Abraq illustrates that the situation in southeastern Arabia was more complex than previously thought.

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FAQs

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What differentiates Hasbeya asphalt from Dead Sea asphalt in terms of composition?add

The research reveals that both Hasbeya and Dead Sea asphalts exhibit similar bulk compositions, yet notable differences in their sterane distributions, particularly the predominance of C27 steranes in Hasbeya asphalt.

How does the biodegradation of Hasbeya asphalt compare to Dead Sea asphalt?add

Hasbeya asphalt exhibits incipient biodegradation with higher pristane/n-C17 and phytane/n-C18 ratios of 2.0 and 3.7, while Dead Sea asphalt shows significantly lower biodegradation indicators of 0.16 and 0.47, respectively.

What geological conditions contributed to the formation of Hasbeya asphalt?add

The Hasbeya asphalt is derived from immature organic-matter-rich limestone and chalk deposits of the Senonian age, formed under dysoxic or anoxic conditions, potentially in a hypersaline environment.

What historical significance does Hasbeya asphalt have?add

Historically, Hasbeya asphalt has been utilized since at least 1600 BC and maintained a production of approximately 400-500 tons annually, mostly exported for uses like varnishes.

What implications does the study have for understanding Middle Eastern asphalt sources?add

This study suggests that asphalts previously presumed to originate solely from the Dead Sea may also derive from Hasbeya, expanding the geographic understanding of ancient asphalt trade routes.

About the authors
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Arie Nissenbaum
Weizmann Institute of Science, Faculty Member
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Jacques Connan

Related papers

Molecular archaeology: Export of Dead Sea asphalt to Canaan and Egypt in the Chalcolithic-Early Bronze Age (4th-3rd millennium BC)
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The genesis of the asphalt in the Dead Sea area
Amos Bein

Journal of Geochemical Exploration, 1979

The hydrocarbon occurrences of asphalts, heavy oils and oil shales in the Dead Sea area and the possible genetic relation between them have been studied. The similarity in organochemical characteristics, i.e., the elemental composition of asphaltenes, the distribution pattern of the saturated hydrocarbons and the predominance of V (over Ni)porphyrins in both the oils and the asphalts indicate a close relation between them. On the other hand, dissimilarities in the same organochemical characteristics in both the asphalts and the oil shale exclude the hypotheses that asphalt was generated and expelled from the oil shales or that the shales were contaminated by oils. Water washing and biodegradation are considered to be the processes through which preferential depletion of hydrocarbons occurred, altering the oils to asphalts. The burial of the degraded asphalt to a relatively great depth resulted in a secondary generation of small amounts of light saturated hydrocarbons in these asphalts. The oils, which are thought to be the precursors of the asphalts, have either been flushed into the Dead Sea depression from the surrounding elevated areas or have seeped upwards from deep local accumulations in the graben.

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Asphalts, Oils, and Bituminous Rocks from the Dead Sea Area--A Geochemical Correlation Study
Baruch Spiro

AAPG Bulletin, 1983

Oils and asphalts (gilsonite) from the Dead Sea area, Israel, were characterized by bulk composition, specific C,j^ hydrocarbons (n-alkanes, isoprenoids, steranes, triterpanes), and aromatics including sulfur compounds and light hydrocarbons (Cj to C, molecular range). These indicators, complemented by literature data (sulfur content, sulfur isotope composition and distribution of petroporphyrins) define the oils and asphalts as belonging to a single geochemical province. The geochemical characteristics suggest a source material of bacterially reworked algae and a source rock poor in clay minerals, probably a calcareous rock. Calcareous bituminous rocks of the Campanian-Maestrichtian Ghareb Formation are exposed on the margin of the Dead Sea graben, on downwarped blocks, and they probably extend under the thick graben fill. The agreement of the geochemical indicators suggests that these bituminous rocks are a potential source of the asphalts and oils in the Dead Sea area. Differences between the various types of hydrocarbon occurrences are due to a combination of several effects such as variations in source material, the thermal history of the different downwarped blocks, water washing, and biodegradation. The distribution characteristics of hydrocarbons (Q to C]s and Q to C,) is sensitive to biodegradation and/or water washing. The aromatic fractions (except very soluble compounds like benzene, toluene, etc) are less affected by these processes and record the variability due to source and possibly thermal history. The interpretation of the triterpane and sterane distribution corroborates that of other hydrocarbons with respect to maturation and type of source rock. Differences in maturation are pronounced: the bituminous rocks and asphalts are immature, and the oils are derived from source rocks in an initial stage of petroleum generation.

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Asphalts, heavy oils, ozocerite and gases in the Dead Sea Basin
Arie Nissenbaum

Organic Geochemistry, 1980

Solid, liquid and gaseous hydrocarbons occur throughout the Dead Sea Basin (Israel and Jordan) both in surface exposures and in drillings. The unaltered asphalts and heavy oils are characterized by very high sulfur content (ca. 1 I%) with ~34S = +5%0 and c$~3C =-28%o to-29%o, low content of n-paraffins, pristane to phytane ratio of 0.5 and by containing almost exclusively VO-porphyrins. The distribution of n-paraffins in samples from deep sources shows a smooth envelope maximizing at Ct 5-20. Surface and shallow samples show clear evidence of biodegradation. The ozokerite, known only from the east side of the basin, is composed primarily of long chain n-paraffins with a maximum at C39. The gases known from the southern margin of the basin are composed mostly of methane. The source for the bitumens is unknown. Two hypotheses are discussed. The first is that the asphalts and heavy oils represent an alteration products of crude oil which migrated into the basin or which might have been generated in the basin itself. The second hypothesis favors an origin from low temperature alteration of organic matter from a thermally immature source.

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Classification of the asphalts and their source rock from the Dead Sea Basin (Israel): the asphaltene/kerogen vanadyl porphyrins
Liliana López

Fuel, 1998

The asphaltenes of the asphalts from the Dead Sea Basin were examined for the occurrence of vanadyl porphyrins. These examinations demonstrate that the asphalts fall into two broad class types: one which exhibits a relatively high vanadyl porphyrins content (Ͼ 300 ppm), and the other characterized with no vanadyl porphyrins ð Ͻ 10 ppm). It is concluded that these asphalts belong to two distinct types and have separate origins. The kerogens isolated from the petroleum-source rock of the Dead Sea Basin were also analyzed. Two genetic types of kerogen appeared to exist: a marine one highly enriched with these pigments and a terrestrial one with no vanadyl porphyrins. For comparison, the asphaltenes of typical asphaltic crude oils from Western Venezuela and kerogen from their La Luna source rock were also examined. Previous detailed geochemical studies 1 indicated that the La Luna kerogen is derived from marine organic matter source. These materials have higher concentrations of vanadyl porphyrins than the Dead Sea asphaltenes and kerogens are enriched with these compounds. Our results strengthen the potential of vanadyl porphyrins of both petroleum asphaltenes and source-rock kerogen for use in genetic and correlation studies.

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    Dead Sea Asphalt in Ancient Egyptian Mummies-Why?
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    ABSTRACT The asphalt from the Dead Sea was an important item of trade in antiquity. Among its many uses, the most widespread was its export to Egypt for use in the mummification process, albeit at a relatively late date; that is, post 1000 BC. Its use became particularly important in the Ptolemaic–Roman period, as demonstrated by a war in the fourth century BC specifically to gain commercial control of this product. Although the reasons why the Egyptians wanted Dead Sea asphalt at this specific time are nowhere specified, the answer may lie in its increasing availability as a (partial) replacement for the plant resins used previously. A review of the historical literature shows that Dead Sea asphalt was used for at least two millennia as a biocidal agent in agricultural practices. It is proposed that the reasons for using Dead Sea asphalt in the mummification process are due to its dual role; first, as an external mechanical shield, when smeared on the exterior of mummy wrapping, to prevent ingress by insects, fungi, bacteria and moisture; and, second, as a biocidal agent (perhaps due to its high sulphur content), which prevented the flesh from decaying, the prime concern for the ancient Egyptians.

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    Bitumen has been identified for the first time in Egyptian occupied Nubia, from within the town of Amara West, occupied from around 1300 to 1050 BC. The bitumen can be sourced to the Dead Sea using biomarkers, evidencing a trade in this material from the eastern Mediterranean to Nubia in the New Kingdom or its immediate aftermath. Two different end uses for bitumen were determined at the site. Ground bitumen was identified in several paint palettes, and in one case can be shown to have been mixed with plant gum, which indicates the use of bitumen as a ground pigment. Bitumen was also identified as a component of a friable black solid excavated from a tomb, and a black substance applied to the surface of a painted and plastered coffin fragment. Both contained plant resin, indicating that this substance was probably applied as a ritual funerary liquid, a practice identified from this time period in Egypt. The use of this ritual, at a far remove from the royal Egyptian burial sites at ...

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