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Rare earth elements and yttrium in ferromanganese deposits from the South China Sea: distribution, composition and resource considerations
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Yi ZHONG1, 2, 3, Zhong CHEN1, *, Francisco Javier GONZALEZ4, Xufeng ZHENG1, Gang LI1, Yun LUO1, 3, Aibin MO1, 3, Antao XU1, 3, Shuhong WANG1
Acta Oceanologica Sinica | 2018, 37(7) : 41 - 54
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Acta Oceanologica Sinica | 2018, 37(7): 41-54
• Marine Geology •
Rare earth elements and yttrium in ferromanganese deposits from the South China Sea: distribution, composition and resource considerations
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Yi ZHONG1, 2, 3, Zhong CHEN1, *, Francisco Javier GONZALEZ4, Xufeng ZHENG1, Gang LI1, Yun LUO1, 3, Aibin MO1, 3, Antao XU1, 3, Shuhong WANG1
Affiliations
  • 1 Key Laboratory of Ocean and Marginal Sea Geology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China
  • 2 Department of Marine Science and Engineering, Southern University of Science and Technology of China, Shenzhen 518055, China
  • 3 University of Chinese Academy of Sciences, Beijing 100049, China
  • 4 Geological Survey of Spain (IGME), Madrid 28003, Spain
Published: 2018-07-25 doi: 10.1007/s13131-018-1205-5
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Ferromanganese nodules and crusts contain relatively high concentration of rare earth elements (REE) and yttrium (REY), with a growing interest in exploitation as an alternative to land-based REY resources. On the basis of comprehensive geochemical approach, the abundance and distribution of REY in the ferromanganese nodules from the South China Sea are analyzed. The results indicate that the REY contents in ferromanganese deposits show a clear geographic regularity. Total REY contents range from 69.1×10–6 to 2 919.4×10–6, with an average value of 1 459.5×10–6. Especially, the enrichment rate of Ce content is high, accounting for almost 60% of the total REY. This REE enrichment is controlled mainly by the sorption of ferromanganese oxides and clay minerals in the nodules and crusts. Moreover, the total REY are higher in ferromanganese deposits of hydrogenous origin than of diagenetic origin. Finally, Light REE (LREE) and heavy REE (HREE) oxides of the ferromanganese deposits in the study area can be classified into four grades: non-enriched type, weakly enriched type, enriched type, and extremely enriched type. According to the classification criteria of rare earth resources, the Xisha and Zhongsha platform-central deep basin areas show a great potential for these rare earth metals.

ferromanganese deposits  /  rare earth elements and yttrium  /  abundance characteristics  /  controlling factors  /  potential source  /  South China Sea
Yi ZHONG, Zhong CHEN, Francisco Javier GONZALEZ, Xufeng ZHENG, Gang LI, Yun LUO, Aibin MO, Antao XU, Shuhong WANG. Rare earth elements and yttrium in ferromanganese deposits from the South China Sea: distribution, composition and resource considerations[J]. Acta Oceanologica Sinica, 2018 , 37 (7) : 41 -54 . DOI: 10.1007/s13131-018-1205-5
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1 Introduction
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The rare earth elements (REE) are a group of 15 “lanthanide” elements from lanthanum to lutetium on the periodic table, as well as yttrium, which is usually comprised because of similar chemical properties (Long et al., 2012). Over recent decades, rare earth elements and yttrium (REY) play essential roles in a variety of highly advanced devices and green technologies such as defence metallurgy, consumer electronics, medical applications, etc (Kynicky et al., 2012; Van Gosen et al., 2014). The world’s most commercially important REE deposits are found in alkaline igneous rocks and carbonatites (Orris and Grauch, 2002). The estimated total world reserve of rare earth oxides on land is about 114 Mt, 48% of which is in China (Kynicky et al., 2012), such as Bayan Obo Mining District in northern China (Chi et al., 2012; Su, 2009). As a result, global rare metals consumption has been steadily increased, but supplies have not always been reliable due to the limited number of leading manufacturers. Increased competition for metal resources from rapidly expanding economies, such as China, India, Brazil and Indonesia, may lead to a shortage in the future (Hein et al., 2013). Demand for the REE is expected to grow by at least 6% per year over the next 25 a, particularly for permanent magnets and medical technologies (Alonso et al., 2012), and this, coupled with China’s increased internal demand (Weng et al., 2015), has led to concern about the risk of supply shortage. Therefore, to maintain a stable supply of REEs to industry, it is important to ensure there are a variety of REE resources.
Recently, Kato et al. (2011) have discovered a new type of mineral resource, named REY-rich mud, distributed in vast quantities throughout a large part of the Pacific Ocean. There is no doubt that the index of progress in the exploration, exploitation, beneficiation technologies as well as mining technology concerning deep sea mineral resources, proved that in addition to the REY-rich deep sea mud, there is also a distinct REE type of mineralization associated with deep sea ferromanganese crusts and polymetallic nodules (Papavasileiou, 2014). New REY mines such as nodule/crust or deep see mud in deep sea have been paid a lot of attention for their high content of REY and enrichment of HREE recently. Ferromanganese crusts, also referred to as Co-rich crusts, are formed principally by hydrogenetic precipitation from the cold sea water of colloidal particles of Fe and Mn oxyhydroxides onto rock substrates (Dymond et al., 1984; Bau et al., 1996; Hein et al., 2000; Schulz, 2006). Hydrogenetic crusts concentrate REY at many orders of the magnitude above their concentration in sea water (Bau et al., 1996; Hein et al., 2013), which is promoted by the high reaction surface area of Fe-Mn oxyhydroxides (Hein et al., 2013; Pourret and Davranche, 2013), slow oxidation reaction kinetics, and slow growth rates (Bau and Dulski, 1996). Polymetallic nodules constitute mixed-source deposits formed by hydrogenetic and diagenetic precipitation of Fe-Mn colloids around a nucleus on the surface of soft sediments (Halbach et al., 1988). Interactions of both hydrogenetic and diagenetic processes lead to a range of bulk Mn/Fe ratios from 1.0 to 2.5 for oxic diagenesis and up to 50.0 when the sedimentary column is suboxic near the seabed (Calvert and Piper, 1984; Schulz, 2006). Metals (Ni, Cu and Co), REY in nodules are mainly derived from sea water through hydrogenetic precipitation and further enrichment in metallic elements (Mn, Cu, Ni and Zn) occurs via diagenetic precipitation (Ohta et al., 1999). This makes ferromanganese deposits a potential resource for many of the metals used in emerging high-technology and green-technology applications (Hein et al., 2013), thus, mapping the global distribution of REY-rich ferromanganese deposits has become an important issue.
Recent studies on REE geochemical characteristics of ferromanganese nodules and crusts have focused more on open-oceans from areas such as the prime crust zone in the equatorial Pacific, the central East Indian Basin, the Peru Basin and Penrhyn-Samoa Basins in the southeastern Pacific Ocean (Rona, 2008; Kuhn et al., 2012; Hein et al., 2013). Only a few studies have focused on continental margin ferromanganese nodules and crusts from Galicia Bank (NW Atlantic Iberia margin) (González et al., 2016), the Gulf of Cadiz (González et al., 2012), California continental-margin (Hein et al., 2005; Conrad et al., 2017), Canary Island Seamount Province (Marino et al., 2017) and the Philippine Sea (Xu et al., 2006).
As is one of the largest marginal seas in the western Pacific Ocean, the South China Sea (SCS) is subjected to relatively large terrigenous inputs, metal fluxes from continental shelf and slope hypoxic sediment, seasonal upwelling, high primary productivity, and a well-developed oxygen minimum zone (Liu and Colin, 2010; Milliman and Farnsworth, 2011). A large number of ferromanganese nodules have been found to be densely distributed on the Jiaolong Seamount in the deep-sea basin, where their source potential is more promising than ocean nodules (Zhang et al., 2015). Many researchers have pointed out that REY as a powerful tool for defining modern and past geological environments and helps to understand its source and distribution because of their unique behavior during various geochemical process (Wang et al., 1984; Bao and Li, 1993; Zhang et al., 2012). However, the systematic study of the potential REY mineral sources for the nodule/crust in the SCS, and the knowledge of their distribution and enrichment mechanism are uncertain.
This paper presents geochemical and mineralogical descriptions of ferromanganese nodule and crust samples recovered from the SCS from 2005 to 2013. Then, by combining the new data with previously constructed data set, we determine the spatial distribution and variations of REE in the ferromanganese nodules and crusts throughout the SCS. In addition, we also discuss the key controlling factors that lead to REE enrichment and its global significances.
2 Sampling and experiments
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2.1 Sampling
As part of the integrated investigation cruises organized by the South China Sea Institute of Oceanology (SCSIO, Chinese Academy of Sciences), 16 ferromanganese nodule and crust samples have been collected from eight stations in the SCS since 2005 (Fig. 1 and Table 1). Five stations (05E105, 05E202, 05E204, 10E204B and ZX31) are located in the northeastern SCS, while two stations (05E107 and 09KJ22) are in the northwestern SCS. The Station J-158 is located in the central basin of the SCS and with the water depth of 3 573 m on the Jiaolong Seamount.
2.2 Mineralogical and geochemical analysis
The X-ray powder diffraction (XRD) was conducted using a PANalytical X’Pert PRO diffractometer equipped with Cu-Kα radiation, carbon monochromator and automatic slit (PTRX-004). The analytical conditions for the XRD were: Cu-Kα radiation at 40 kV and 30 mA, a curved graphite secondary monochromator, scans from 2–70 (2θ), step size of 0.017 0 (2θ) and step time 0.5°/min. As the intensity of a mineral diffraction pattern in a mixture is proportional to its concentration, measuring a mineral peak areas provide an estimate for the relative mineral abundance in a sample.
For major, trace and REE analysis, 40 mg of dried and ground sample powders were weighed into a teflon beaker. After 0.5 mL HF, 0.5 mL HNO3 and 1.5 mL HCl were added, the sealed bombs were then placed in an electric oven and heated to 180°C for about 12 h. After cooling, the bombs were heated on a hot plate to evaporate to dryness, then 1 mL HNO3 and 1 mL H2O were added. The bomb was again sealed and placed in an electric oven at 150°C for about 12 h to dissolve the residue. Major elements were determined using a Thermo-Fisher IRIS II Intrepid XSP ICP-OES. Trace elements and REEs were determined using a Perkin-Elmer ELAN 9000 ICP-MS. All the samples were analyzed at the Institute of Oceanology, Chinese Academy of Sciences (IOCAS).
The sensitivity of the instrument was adjusted to about 30 000 s–1 for 1 ng/mL medium-155. The analysis of the reference materials (GBW07315, GBW07316, BCR-2, BHVO-2, GBW0725, GBW07296, NOD-P-1 and NOD-A-1) which are either sediment, basalt or manganese nodules, agree well with the certified value. The accuracies of the analyses are estimated to be better than ±5%–10% (relative) for most elements.
3 Results and discussion
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3.1 REE distribution characteristics in ferromanganese deposits
3.1.1 REE content, mineralogical composition and geographical distribution
The REEs are conventionally subdivided into light REEs (LREE: La to Sm) and heavy REEs (HREE: Eu to Lu and Y) (Kato et al., 2011). The ferromanganese deposits mainly formed of Mn-oxides intergrown with Fe oxyhydroxides, are a potential source of REE (Hein et al., 2013). High concentrations of the REY, up to 3 000×10–6 total REY, comparable with the level in ore deposits in southern China, are reported for ferromanganese crust-nodule deposits from the Shatsky Rise, Northwest Pacific (Hein et al., 2012).
The SCS developed from continental margin rift to ocean basin with an area of 3.5×106 km2 and a maximal depth of 5 500 m (Fig. 1). Ferromanganese oxide deposits from the SCS are found in a wide variety of oceanographic and tectonic settings such as the northeastern slope, northwestern and central basin (Fig. 1) (Lin et al., 2003; Zhang et al., 2012; Zhong et al., 2017a). On the basis of their morphology and size, ferromanganese oxide deposits can be divided into ferromanganese crusts, polymetallic nodules, and micronodules (<1 mm in diameter). Ferromanganese micronodules are an important reservoir for Mn and associated transition elements in oxic deep-sea sediments (Stoffers et al., 1984). The abundance of micronodules seems to be correlated reciprocally with the sedimentation rate and highest abundance occurring in dark brown clay where the sedimentation rate is very low (Banerjee and Iyer, 1991; Chauhan, 2003; Dekov et al., 2003; Duliu et al., 2009). They tend to predominate in the coarse fraction of the surface sediment and spread unevenly, especially in the eastern deep basin (Fig. 2). According to percentage composition of micronodules concentrated in the coarse silt sediment, it can be divided into a high content area, a middle content area and a low content area. The distribution of ferromanganese nodules and crusts controlled by the distribution trend of micronodules, are roughly parallel to the NE-striking faults.
Combined with mineral composition (Fig. 3 and Table 1), most of ferromanganese crusts, essentially composed of todorokite, are widely distributed on the volcanic seamounts which formed after the cessation of the sea floor spreading in the basin (Fig. 1), such as the Daimao Seamount (Sta. 8), the Xianbei Seamount (Sta. Xianbei), and the Zhenbei Seamount (Sta. 9). On the other hand, they also spread on the lower continental slope, such as the Jianfeng Seamount, the Shuangfeng Seamount (Sta. KD17), the Zhongsha and Xisha platforms (Stas KD21 and KD29). The content of LREE in the polymetallic nodules/crusts is obviously higher than that of HREE, with the total LREE ranging from 50.5×10–6 to 2 584.3×10–6. There are four stations (such as Stas KD20, KD18, Xianbei and NS57) found on the slope and southern subbasin area, whose REE content is more than 2 000×10–6. Most of nodules with the total LREE content are larger than 1 000×10–6, appearing mainly in the Zhongsha and Xisha platforms and spreading sparsely on the southwest subbasin. The high contents of REEs normally are in relation with hydrogenesis and the abundance of vernadite. The nodules with the total LREE content is less than 1 000×10–6, are mainly distributed in the northeastern SCS. And the minimum value appears in Sta. 05E202 of the northeastern SCS (Fig. 4c). These nodules have a pristine mineralogy formed by pyrite and barite which cannot accumulate REEs (Fig. 3 and Table 1). The total HREE content ranges from 18.6×10–6 to 442×10–6, which is much smaller than that of the total LREE, indicating that the polymetallic nodules in the SCS are dominated by the total LREE (Fig. 4d). REY range from 69.1×10–6 to 2 919×10–6, and the maximum appears at the Sta. KD18 in the deep sea basin, and the minimum also appears at the Sta. 05E202 in the northeastern SCS (Fig. 4a). The high and low value distributions of the total HREE and REY are basically consistent with the distribution of the total LREE: the high-value area is located on the slope of the Zhongsha and Xisha Islands, the low-value area is located on the northeastern slope.
3.1.2 Ce enrichment
Ce has been widely applied for catalytic converters in cars, petroleum refining, steel production, corrossion protection, carbon arc lamps, and cigarette lighter flints (Dutta et al., 2016). As is also the most abundant natural element in lanthanide elements, the Ce content of the polymetallic nodules/crusts in the SCS ranges from 22.43×10–6 to 2 040×10–6, accounting for almost 60% of the total REE content. The maximum value appears at the Sta. KD18 at the deep sea basin and the minimum value appears at Sta. 05E202 in the northeastern SCS. These high value areas are mainly distributed on the island slope of Zhongsha and Xisha platforms (c(Ce)=642×10–6–2 040×10–6) (Fig. 4b). Most of Ce contents are within the scope of 900×10–6–2 000×10–6, which is basically consistent with the distribution of the total HREE, REY, and LREE. The distribution relatively to water depth is similar to that of the ratio of LREE content to HREE one and Ce anomaly ratios in the deposits (Fig. 5). However, the correlation coefficient between Ce and water depth is only 0.01 and the strong positive Ce anomalies in nodules and crusts from the SCS imply that Ce in deposits come from seawater (Fig. 5). The correlation coefficients between Ce and Fe, Mn are –0.60 and 0.68, respectively (Table 2). Ce enrichment in nodules and crusts depends on a preferential fractionation to the Fe and Mn phases, with a slight relative preference for Fe oxyhydroxides (Table 2) (Hein et al., 1988; Bau and Koschinsky, 2009). The results provided by these authors indicate that the transfer of Ce from seawater does not occur via a discrete solid Ce (IV) oxide phase from dissolved Ce (III), but rather Ce dissolved in waters remains trivalent and its oxidation to the tetravalent form occurs at the surface of Fe-Mn oxyhydroxides after its sorption into their structure (Fig. 6). Therefore, the Ce element may be the first REE separated and extracted from sedimentary mineral resources in the ocean in the future.
3.2 Comparison with other marine REY-rich deposits
The deep-sea REY-rich deposits of polymetallic nodules, Co-rich crusts and soft mud are reported from many parts of the world (Rona, 2008) (Fig. 7). The SCS is an important tectonic unit of the western Pacific Ocean active continental margins. Because of the enormous amount of terrigenous sediment input into marginal seas, Fe- and Mn-oxide precipitates are easily diluted making it difficult to enrich metals of potential economic interest, and deposits can be buried quickly by sediments (Zhang et al., 2013). However, the enrichment of REE and Ce in polymetallic nodules and crusts in the SCS provides a good premise for the comprehensive development of seabed mineral resources.
The SCS deposits are characterized by Fe-oxyhydroxides predominating over Mn-oxides, which in samples from the Pacific Ocean the Mn oxide vernadite is predominant (Hein et al., 2012). This predominance of goethite-family minerals in the SCS deposits is similar to other locations from the Philippine area (Xu et al., 2006). Quartz grains and other clay minerals, abundant in the deposits can be probably related to the terrigenous input, as has been found for crusts from the California continental-margin (Conrad et al., 2017). A comparison between REY contents in the SCS samples and other ferromanganese deposits and deep-sea mud from other oceans is provided in Fig. 8. The maximum total REY content of the polymetallic nodule/crust in the SCS is lower than that of the Northwest Pacific (Hein et al., 2012) and California marginal sea (Conrad et al., 2017), but similar to the total REY of the Northeast Atlantic (Muinos et al., 2013) and southern Pacific nodules (Hein et al., 2015). Especially, the total REY of the SCS (c(REY)=69×10–6–2 919×10–6) were significantly higher than that in the central Pacific Basin (Cui et al., 2009) and the Philippine Sea (Xu et al., 2006). At the same time, the maximum total REY content value of polymetallic nodule/crust in the SCS is also significantly higher than that in the eastern Pacific Ocean CCFZ, southeastern Pacific and western Pacific mud. In regard to Ce content, the maximum content in the SCS is the same as that in the southern Pacific, which is lower than that in the Northwest Pacific (Hein et al., 2012) and the California marginal sea (Conrad et al., 2017), but higher than that in the Central Indian Basin (Cui et al., 2009), the northeastern Atlantic (Muinos et al., 2013), the Philippine Sea (Xu et al., 2006) and the central Pacific Basin.
Therefore, the rare earth resources in seabed polymetallic nodules and Co-rich crusts have attracted the attention of the international seabed authority and governments. Since the development of submarine technology, a research into ferromanganese nodules and crusts has become more sophisticated. Especially, the production cost and difficulty of rare earth resource in polymetallic nodules and crusts in the SCS are less than that in the deep-sea basin because they mainly occur at comparatively shallow depth, forming along the continental margin (Conrad et al., 2017; González et al., 2016; Marino et al., 2017). Moreover, the resource potential and economic value of the REEs, especially Ce, are much larger than those central Pacific Basin, the CCFZ in the eastern Pacific (Wegorzewski and Kuhn, 2014) and the Indian Ocean Basin (Pattan and Parthiban, 2011) where China participates in the exploration or attention.
3.3 Main factors affecting the Ferromanganese deposits and REY distribution
Many ferromanganese deposits from different parts of the world oceans have been studied extensively (Calvert, 1978; Aplin and Cronan, 1985; Bau et al., 1996; Hein et al., 1997; Mills et al., 2001; Koschinsky and Hein, 2003; Rajani et al., 2005). Traditionally, hydrogenous precipitate from sea water, whereas diagenetic nodules form from metal ions in sub-oxic pore waters, and hydrothermal nodules form from metals supplied by hydrothermal vent fluids (Bau et al., 2014). Ferromanganese deposits of different genetic origins are characterized by distinctive composition of REEs (Byrne and Kim, 1990; German and Elderfield, 1990). In addition, several factors such as the rate of precipitation, nature of geochemical components in oxides, speciation of elements from sea water and hydrothermal fluid are major cause of such compositional variations (Koschinsky and Halbach, 1995; Bau and Dulski, 1996; Koschinsky et al., 1996; Takahashi et al., 2007).
To better quantify and understand the processes that control the REY composition of the ferromanganese deposit samples, the elemental data were subjected to a statistical factor analysis. The results of this analysis are shown in Tables 2 and 3. Differences in the chemical composition of the ferromanganese deposit samples can be accounted for statistically by changes in the relative proportions of three principal factors [with eigenvalues, or sums of squared (SS) loadings, of being greater than 1] which together account for 82% of the sample variance. The total REY concentrations are positively correlated with Ti which is enriched in detrital minerals; titanium mainly forms a hydrogenetic phase, probably consisting of TiO2*H2O intergrowth with the amorphous FeOOH phase (Koschinsky and Hein, 2003). The factor analysis reveals that the REY are also located in association with Mn, Fe, Cu, Co and Ni that are generally considered have a significant hydrogenous source in the ferromanganese deposits (Koschinsky and Halbach, 1995). Uptake of REY from seawater is widely considered to occur via scavenging by Fe-Mn oxide phases (Piper, 1974; German et al., 1991; Bau and Koschinsky, 2009). Sequential leaching of some samples reveals that REEs and yttrium are mainly associated with Fe-Mn oxyhydroxide phase, both Mn-oxide and Fe-oxyhydroxide phases contain the major fraction of these elements (Zhong et al., 2017b), which is consistent with comparative study of hydrogenous and hydrothermal deposits collected from two seamounts in the Andaman Sea (Prakash et al., 2012).
On the other hand, the degree of enrichment of REY is related to a genetic model and nodules and crusts growth rates (Bau and Koschinsky, 2009). Different types of ferromanganese deposits can be distinguished by the field on which they plot on a Mn-Fe-(Cu+Co+Ni) ternary diagram, which delimitates the diagenetic, hydrogenous and hydrothermal fields according to the relative proportions of these groups of elements. Compared with the geochemical values of typical oceanic diagenetic nodules from the CCFZ (Wegorzewski and Kuhn, 2014) and hydrogenetic-diagenetic nodules from the Indian Ocean (Pattan and Parthiban, 2011), most of the nodules and crusts from the SCS fall within the hydrogenetic field on this ternary diagram (Fig. 9) in an area superimposed by other samples from the Philippine Sea (He, 1991; Xu et al., 2006) and more enriched in Fe than the crusts from the northwestern Pacific Ocean (Hein et al., 2012). It is consistent with previous reported results of ferromanganese nodules and crusts found in the SCS (Bao and Li, 1993; Chen and Gui, 1998; Chen et al., 2006a). Hydrogenesis via very slow growth rates (1–2 mm/Ma) allows REY to accumulate in ferromanganese oxyhydroxide structures on nodules and crusts surfaces. According to Sholkovitz et al. (1994) and Moffett (1990), this enrichment is strongly dependent on time in which ferromanganese minerals are in contact with sea water, therefore supporting the control of growth rates.
However, the study nodules and previous data present the ratio of Mn/Fe < 0.25 and low contents of Co, Ni, Cu and REE in the Dongsha Islands. The diagram discriminate these nodules as diagenetic in origin, but overlaps slightly with the hydrothermal field (Fig. 8). Abundant references report on nodules from shallow waters and continental margins where Fe, Mn and trace metals contents are rather similar to these Fe-rich nodules from the Dongsha Islands (Calvert, 1978; Glasby et al., 1997; Baturin et al., 2002). They all display very low Mn/Fe ratios as a result of their fast growth rates by combined diagenetic-hydrogenous processes. In this sense, fast growth rates emphasize the importance of sediment diagenetic processes (Reyss et al., 1982). This relatively rapid accumulation is one of the main causes for the overall low content of rare earth metals in these nodules.
3.4 Resource potential of SCS ferromanganese deposits
3.4.1 Classification standard of REY sources of ferromanganese deposits
The deep-sea mud, polymetallic nodules and Co-rich crusts are enriched in rare earth elements, but no exact resource grade standard system has been established. Huang et al. (2014) proposed classification criteria for rare earth resources in deep-sea sediments. However, the REY value of the ferromanganese nodules and crusts has not been yet proposed exact quantitative criteria. Usually, the industrial evaluation of land rare-earth minerals takes the form of measuring an oxide content. In this paper, according to “land-based REE mines exploration norms” (Industrial standard, DZ/T 0204–2002), referring to the industrial grade of land-based weathering crust ion-adsorption rare earth mining: the border grade of LREE is 700×10–6 rare earth oxides (REO) and its industrial grade reaches 1 000×10–6 REO; border grade of HREE is 300×10–6 REO and its industrial grade reaches 500×10–6 REO.
According to the above classification standard, the measured REE content is converted into the REO content, LREE and HREE of the ferromanganese deposits in the study area could be divided into four levels, as shown in Table 4.
Ⅰ. Non-enriched type: REO content is less than or equal to the border grade;
Ⅱ. weakly enriched type: REO content is greater than the border grade, less than or equal to industrial grade;
Ⅲ. enriched type: REO content is greater than the industrial grade, less than or equal to two times of industrial grade;
Ⅳ. extremely enriched type: REO content is more than two times of the industrial grade.
3.4.2 Quality characteristics of REO deposits and its resource perspective
In this study, the REEs should be converted to oxidation level and likely to be close to the industrial grade because the current measurement only examines single element. On the basis of the classification standard in Table 4, if there are more than one datum at one station, each datum is classified by the grade level, the level of most data is taken as this station’s level. In addition to REE, ferromanganese deposits have long been considered a potential resource for metals, such as Ni, Co, Co and Li, that are important in contemporary technology (Hein et al., 2013). If the account of level of different data is consistent, comprehensively taking into account of other metals, the maximum level is taken as this station’s grade. As shown in Table 5 and Fig. 2, the LREE in the ferromanganese deposits from the SCS is relatively enriched. There are nine enriched type stations and seven extremely enriched type stations, respectively. The most abundant station is KD18, with the REO content is 3 145×10–6, more than three times of the industrial grade, which appears on the island slope of the Xisha and Zhongsha platforms. The non-enriched station is 05E202 (the REO content is 60.5×10–6), distributed on the northeastern slope. Compared with the LREE, HREE of ferromanganese nodules and crusts is not enriched. Non-enriched and enriched stations account for 54% and 38% of the total stations, respectively. The most abundant station is KD17, with the REO content is 532.4×10–6, which is slightly higher than the industrial grade value. And the lowest w(REO) value is 27.2×10–6, far below the border grade, also located on the northeastern slope. Combined with topography and formation environment, according to the LREE and HREE grade level of the SCS sample stations, the rare earth resources of ferromanganese nodules and crusts from the South China Sea are divided into three prospective areas (Fig. 2).
(1) Zhongsha and Xisha platform-deep central basin prospective area. The prospective fields are distributed on the northern slope of the SCS where the Pacific Ocean deep water (PDW) influence is stronger. The basin-scale oxygen distribution suggests that the PDW intrudes into the SCS through the Luzon Strait, and is transported north and westward, and then southward along its western margin (Qu et al., 2006). These currents, which are strongest along the SCS slope, promote nodules and crusts formation, enhance turbulent mixing, and produce upwelling, leading to increased primary productivity and the maintenance of an oxygen minimum zone (Hein et al., 2010). In hydrogenetic ferromanganese nodules and crusts, the trace elements appear to be selectively distributed between Mn oxide and Fe oxide phases. It is characterized by extremely enriched LREE resource. And the majority stations are enriched with HREE, higher than the border grade value. Although their distribution is not consistent with the high content area of micro-nodules and micro-crusts and is distributed in low-content areas. According to the comparative study of nodules and micro-nodules, the high content of micro-nodules and crusts appears in the northeastern deep-sea basin, which is consistent with the high value area of REE of fine-grained fraction of the surface sediment (Fig. 2) (Liu et al., 2010a). They can not reach the border grade. Therefore, the Xisha and Zhongsha platform-central deep basin area shows a significant resource potential for these rare earth metals due to their high nodule abundance, and high enrichment.
(2) Southern slope of the southwest sub-basin prospective area. There are only two stations (NS52 and NS57) in this area. Unlike the low concentration (143×10–6–200×10–6) of HREE, the content of LREE oxides ranges between 2 279×10–6 and 2 411×10–6, which falls into extremely enriched type. The prospective area is located on the western island of the southwestern subbasin, where crusts are found to be growing together with phosphate rocks (Chen et al., 2006b). It is generally known that apatite is one of the most critical mineral species, which can acquire REY from a wide variety of sea water occurring on the sea floor of continental shelves and slopes along the western continental margins of the Pacific and Atlantic Oceans (Hucrrns et al., 1991; Hughes and Rakovan, 2015). Marine phosphorites deposits are known to concentrate REY during early diagenetic formation (Hein et al., 2016). In general, the discovery and delineation of the prospective area break through the limitations of understanding on previous knowledge of distribution, but the formation mechanism of these crusts needs to further study.
(3) Northeast slope prospective area. Fe-rich nodules in the SCS were first collected on the northeastern slope, however, detailed geochemical studies about the total REY contents are still limited, and the systematization and the regularity are not evident in this area, so the results could not reflect its potential distribution of rare earth. The ferromanganese nodules shaped by rod, rodlike, spherical and block type, covered under the shallow mud in this area. The minimum values of light and heavy rare earth oxides in ferromanganese nodules are found in this area, and the heavy and light rare earths are characterized by non-enriched and weakly enriched type. The economic value of rare earth resources is not great, but its Fe content is very high. Within the study area, the widespread faults systems of the Dongsha Islands are the main migration system of fractured conduits or channels for gas and methane bearing fluids migrate from the deep parts of the basin into shallow sediments (Hui et al., 2016). It needs to further study whether the Fe-rich nodules on the northeastern slope of the SCS with high Fe content, low Mn content (c(Mn)/c(Fe) = 0.02) and low trace metals content and rare earth elements are closely related to leakage of cold spring fluid.
4 Conclusions
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The REY enrichment in ferromanganese deposits from the SCS has high potential for economic interests. Overall, the contents and distribution of REY in the ferromanganese nodules and crusts from the SCS show a geographic variation. REY is essentially enriched in LREE. High REY content peak in the Xisha Islands, but has lower values in the Dongsha Islands. Our results indicate that the contents of REY depend strictly on the crust mineralogy and especially on the abundance of Fe-oxyhydroxides. On the basis of the criteria of the land-based REE mines, we calculated grades for LREE and HREE in ferromanganese deposits from the SCS. A comprehensive analysis shows that ferromanganese deposits from the Zhongsha and Xisha platform may contain abundant rare metal minerals, with a good prospect as rare metal placer resource, and the hydrocarbon seep may also have good metallogenic prospects in the local area of the Dongsha Islands.
Acknowledgements
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The authors are grateful to Usui Akira and Liu Qingsong for their guidance and constructive discussions. This study is benefited from the scientific cooperation between the South China Sea Institute of Oceanology, Chinese Academy Sciences and the Geological Survey of Spain (IGME).
Funding
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  • The National Natural Science Foundation of China under contract Nos 41376057, 41306047, 41676056; the Spanish project SUBVENT under contract No. CGL2012-39524-C02.
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doi: 10.1007/s13131-018-1205-5
  • Receive Date：2017-06-14
  • Online Date：2026-04-14
  • Published：2018-07-25
Article Data
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  • Received：2017-06-14
  • Accepted：2017-10-10
Funding
The National Natural Science Foundation of China under contract Nos 41376057, 41306047, 41676056; the Spanish project SUBVENT under contract No. CGL2012-39524-C02.
Affiliations
    1 Key Laboratory of Ocean and Marginal Sea Geology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China
    2 Department of Marine Science and Engineering, Southern University of Science and Technology of China, Shenzhen 518055, China
    3 University of Chinese Academy of Sciences, Beijing 100049, China
    4 Geological Survey of Spain (IGME), Madrid 28003, Spain

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表12种不同金属材料的力学参数
科
Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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