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Article

Origin of the Kunduleng Granite and Its Associated Uranium Anomaly in the Southern Great Xing’an Range, NE China

by
Jiaxing Sun
1,
Deyou Sun
1,2,
Jun Gou
1,*,
Dongguang Yang
3,
Changdong Wang
4,
Li Tian
1 and
Duo Zhang
1
1
College of Earth Sciences, Jilin University, Changchun 130061, China
2
State Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China
3
Radioactive Geology and Exploration Technology Laboratory, East China University of Technology, Nanchang 330013, China
4
Nuclear Industry Team 243, Chifeng 024000, China
*
Author to whom correspondence should be addressed.
Minerals 2024, 14(7), 666; https://doi.org/10.3390/min14070666
Submission received: 30 April 2024 / Revised: 23 June 2024 / Accepted: 26 June 2024 / Published: 27 June 2024
(This article belongs to the Special Issue Mineralization in Subduction Zone)
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Versions Notes

Abstract

:
The Kunduleng granite hosts one of several significant uranium anomalies within the southern Great Xing’an Range, NE China. Whole-rock geochemistry and mineral chemistry data, along with the zircon U-Pb-Hf isotope have been used to constrain the petrogenesis of this granitic intrusion and the origin of the uranium anomaly. Microscopically, quartz, alkali-feldspar, and plagioclase are the essential mineral constituents of the granite, with minor biotite, while monazite, apatite, xenotime, and zircon are accessory minerals. Geochemically, the silica- and alkali-rich granites show a highly fractionated character with “seagull-shaped” REE patterns and significant negative anomalies of Ba and Sr, along with low Zr/Hf and Nb/Ta ratios. The granite has positive zircon εHf(t) values ranging from +12.7 to +14.5 and crustal model ages (TDM2) of 259–376 Ma, indicating a Paleozoic juvenile crustal source. Uraninite and brannerite are the main radioactive minerals responsible for the uranium anomaly within the Kunduleng granite. Uraninite presents well-developed cubic crystals and occurs as tiny inclusions in quartz and K-feldspar with magmatic characteristics (e.g., elevated ThO2, Y2O3, and REE2O3 contents and low CaO, FeO, and SiO2 concentrations). The calculated U-Th-Pb chemical ages (135.4 Ma) are contemporaneous with the U-Pb zircon age (135.4–135.6 Ma) of the granite, indicating a magmatic genesis for uraninite. The granites are highly differentiated, and extreme magmatic fractionation might be the main mechanism for the initial uranium enrichment. Brannerite is relatively less abundant and typically forms crusts on ilmenite and rutile or it cements them, representing the local redistribution and accumulation of uranium.

1. Introduction

China Nuclear Geology has conducted over half a century of uranium prospecting and exploration, leading to the discovery of many granite-related uranium deposits in South China. Most scholars believe that the uranium source of granite-type uranium deposits in South China is mainly provided by uranium-producing granite [1,2,3,4,5,6,7], as the host granites have lost 12% to 23.9% of their uranium [8]. A few scholars argue that some uranium also came from the enriched mantle [9,10], because uranium mineralization is accompanied by the enrichment of deep mantle-derived trace elements such as Cr, V, and Ni [11]. Uranium mineralization in this area is spatially associated with the Indosinian granite. Large-scale early Yanshanian magmatic activities caused biotite chloritization and alteration of U-bearing accessory minerals such as monazite and xenotime, which promoted the mobilization of uranium in the Indosinian granite. During the late Yanshanian tectonic-magmatic thermal event, fault structures and heat sources were generated, facilitating mineralization and creating conditions conducive to fluid circulation. The metallogenic ages are predominantly concentrated in the Cretaceous period, particularly during the Late Cretaceous epoch. Moreover, not all Indosinian granite may have served as the uranium source. The uranium-producing granites are S-type, while the uranium-deposit barren granites belong to the I-type [12,13,14].
Generally, granites and rhyolites are the primary sources of uranium for the formation of uranium deposits [15,16,17]. Among the broad range of granite varieties, only four types have the capacity to be sufficiently enriched in U to serve as a significant source for the uranium: metaluminous high-K calc-alkaline, peraluminous, and peralkaline granites, as well as alaskite or anatectic pegmatoid [18,19,20,21,22,23]. The first two types of granite-hosted uranium deposits are formed dominantly by hydrothermal processes, while the latter two types are generally associated with magmatic processes, such as extreme fractional crystallization or a very low degree of partial melting. The fourth type of granite example is the Rössing deposit in Namibia, where mineralization is hosted by small pegmatite-alaskite bodies [23].
Geological exploration and research have recently been conducted in the Great Xing’an Range (NE China) to enhance China’s uranium resources (Figure 1). These programs have resulted in the identification of multiple uranium mineralizations and abundant uranium anomalies. Despite intensive prospecting, no mineralogy and geochemistry study has been conducted in this region. The Kunduleng radiometric anomaly is one of several significant uranium anomalies in NE China. Different from uranium deposits in South China, which are mainly hosted in Indosinian uraniferous granites and characterized by an apparent age gap between magmatism and uranium mineralization [12], this radioactive anomaly is possibly associated with an evolved (fractionated) Yanshanian granite similar to the pegmatitic-alaskite type granite present in the Rössing deposit in Namibia. Investigating the petrogenesis of this granite and the origin of its associated uranium anomaly plays an important role in understanding the uranium enrichment process in NE China. The purpose of this study was to enhance our understanding of the Kunduleng uranium-anomalous granite geochemically and mineralogically, to determine the chemical compositions of uranium minerals, the mechanisms responsible for the formation of the granite, and the occurrence of uranium anomalies.

2. Geology and Petrography

The Xing’an-Mongolian Orogenic Belt, situated between the Siberian and North China Cratons, is divided into four main tectonic units: the Erguna, Xing’an, Songnen, and Jiamusi blocks (Figure 1). These blocks experienced complex geological evolution involving the Palaeo-Asian, Palaeo-Pacific, and Mongol–Okhotsk domains. Following the closure of the Palaeo-Asian Ocean and its subsidiary branches, the amalgamation of the Erguna, Xing’an, and Songnen blocks led to the formation of a composite continental block. During the Late Paleozoic era, this composite block collided with the North China Craton along the Xar Moron–Changchun–Yanji Suture Zone. The amalgamation of the Siberian Craton with the composite block occurred along the Mongol–Okhotsk Suture Zone in the Mesozoic era. During the Late Jurassic to Early Cretaceous period, the closure of the Mongol–Okhotsk Ocean, along with the subduction of the Paleo-Pacific oceanic plate resulted in extensive magmatism and metallogenesis in NE China. Early Cretaceous extension-related magmatism and associated ore deposits were extensively developed in the southern Great Xing’an Range [25,26,27,28].
The Kunduleng granite, which contains uranium anomalies, is situated in the southern Great Xing’an Range, positioned in tectonically the western Songnen Block. Precambrian basement rocks occur as small inliers in the western Songnen Block at two specific locations (Figure 1). In the Xilinhot area, Precambrian rocks consist of Mesoproterozoic supercrustal rocks of the Xilinhot Group (1286 Ma) [29] and gneissic granite (1373–1399 Ma) [30] as well as Neoproterozoic metagabbro (739.6 Ma) [31]. The Precambrian rocks in the Longjiang area are predominantly composed of Neoarchean granite (2579–2699 Ma) [32,33] and Paleoproterozoic high greenschist facies to low amphibolite facies metamorphic rocks (1864 Ma) [34] and associated granitoids (1808–1879 Ma) [35]. The majority of the crust in the western Songnen Block is juvenile and was primarily accreted during the Phanerozoic period [36].
The NE-trending Duribuleji-Wulanhada fault identified along the Kunduleng River [37] and the NW-EW trending fault observed along the Huolinhe River controlled the volcanic eruptions, the emplacement of granite plutons, and the occurrence of uranium anomalies in the region. The uranium anomalous granite under investigation is located approximately 6 km southeast of the Kunduleng town in Inner Mongolia, China. The Kunduleng pluton is relatively diminutive in comparison to numerous other plutons, with dimensions of approximately 14 km along its longest axis (NE-SW), 3 km along its shortest axis (NW-SE) and covering an area of about 42 km2. The granite intruded into the intermediate to acid volcanic rocks of the Early Permian Dashizhai Formation and the rhyolitic pyroclastic rocks of the Late Jurassic Manketouebo Formation. Subsequently, it was overlain by the rhyolitic lava flows and welded tuffs of the Early Cretaceous Baiyingaolao Formation (Figure 2).
The predominant lithology of the pluton consists of massive, porphyritic, medium- to coarse-grained granite with a pale red color (Figure 3a–c). The sample comprises subhedral to euhedral quartz phenocrysts (20–25 vol. %) in a fine-grained matrix (75–80 vol. %) composed of alkali-feldspar, quartz, plagioclase, and minor amounts of biotite. The principal accessory minerals include zircon, monazite, apatite, xenotime, and uraninite. Alkali-feldspar presents as granular grains (0.3–2.5 mm) and consists mainly of microcline and perthite. Plagioclase occurs as subhedral laths (0.2–2 mm) with polysynthetic twinning. Quartz is present in the form of euhedral to subhedral phenocrysts (up to 7 mm) and is also found in a fine-grained groundmass (Figure 3d). Slightly altered biotite (0.5–1 mm) can also be identified. The mineral compositions of the fine-grained granite are similar to those of the porphyritic granite (Figure 3e,f).
No faults have been observed within the Kunduleng pluton, with jointing being the predominant structural feature. Three intersecting joint sets are present: a northwest trend, a northeast trend, and a horizontal trend (Figure 3a). There are four locations of high radioactive anomalies within the Kunduleng pluton. The anomalous area is about 3 km2 in total, accounting for 7% of the surface exposure of the granite pluton. Detailed examination of the identified uranium anomalies found they were confined to the area characterized by well-developed joints. In the vicinity of joints, these granites frequently undergo varying degrees of hydrothermal alteration (Figure 3b), leading to the formation of reddish altered rocks containing elevated concentrations of radiogenic elements. Sericitization of plagioclase is extensively developed in the radiometrically anomalous granites (Figure 4a). The K-feldspar appears to be relatively fresh, yet it also shows signs of clayization. Secondary muscovite replacing K-feldspar also occurred locally (Figure 4b). Biotite is partially converted to muscovite (Figure 4c) and there is rare fluorite observed in the altered biotite (Figure 4d).
Uraninite present as small cubic euhedral crystals (2–20 μm) within the major rock-forming minerals such as K-feldspar and quartz (Figure 5a–d). Brannerite is closely associated with ilmenite and rutile, forming crusts on ilmenite or sometimes penetrating into them (Figure 5e,f).

3. Analytical Methods

3.1. Zircon U–Pb Dating and Lu–Hf Isotope Analysis

Zircon U–Pb isotopic analysis was conducted at the Key Laboratory of Mineral Resources Evaluation in Northeast Asia, Jilin University, using an Agilent 7900 ICP–MS coupled with a GeoLas 200M 193 nm ArF excimer laser ablation system. In this study, the diameter, energy density, and repetition rate of the laser beam were 30 μm, 10 J/cm2 and 8 Hz. Each sample analysis consists of a 20-s gas blank followed by a 40-s ablation data acquisition. Harvard zircon 91500 was used for age calculation, while silicate glass NIST SRM 610 was used for concentration calculations. The Plesovice zircon was utilized as a secondary standard for assessing precision and accuracy. During our analyses, the weighted mean 206Pb/238U age of Plešovice is 337.7 ± 4.0 Ma, consistent with the recommended age of 337.13 ± 0.37 Ma [38].
Lu–Hf isotope analysis was performed utilizing a laser ablation–multi-collector–inductively coupled plasma–mass spectrometer at the Key Laboratory of Deep-Earth Dynamics of the Ministry of Natural Resources, China. The analysis was conducted using a Nu Plasma II MC-ICP-MS equipped with a 193 nm ArF excimer laser-ablation system. A total of eight zircon grains were analyzed for Lu-Hf isotopes using a 60 μm laser beam spot diameter to target specific dated domains. The methodology utilized in this analysis closely corresponds to the approach delineated by Tian et al. [39].

3.2. Whole-Rock Element Analyses

Following petrographic examination, eleven samples were selected for bulk rock geochemical analysis. Initially, the fresh rock samples were fragmented into smaller pieces before being finely ground into a powder using an agate swing mill to achieve a particle size of approximately 200 mesh. The powdered samples were sent to the laboratory located at Jilin University for analysis. The major components were analyzed using an X-ray fluorescence spectrometer on glass disks. The disks were formed through the process of melting a mixture of rock dust and lithium metaborate. Trace elements were analyzed in samples subjected to acid digestion (HF, HNO3) using an Agilent 7500a ICP-MS instrument. The precision of the analysis is greater than 5% for major components and 10% for trace elements.

3.3. Electron Probe Microanalysis of Minerals

The mineral compositions were analyzed using an electron microprobe (JEOL JXA 8100) that was equipped with wavelength dispersive spectroscopy at the State Key Laboratory of Nuclear Resources and Environment at East China University of Technology. The operational parameters comprised an accelerating voltage of 15 kV, a beam current of 20 nanoamps, and a beam diameter of 2 μm. For uraninite and other associated minerals, the major standards were uraninite (U, Th, and Pb), monazite (La, Ce, Pr, Nd, and P), rutile (Ti), REE-phosphate (Sm-Yb and Y), zircon (Si, Zr), olivine (Mg), plagioclase (Al), magnetite (Fe), pyrophanite (Mn), apatite (F, Cl, and Ca), sanidine (K), celestite (Sr), niobate (Nb), and tantalite (Ta). Detailed descriptions of the analytical method can be found in the work of Wu et al. [40]. U-Th-Pb chemical age estimates for each uranium mineral were computed based on the concentrations of U, Th, and Pb determined by EPMA. The calculations were performed using age determination software developed by Guo et al. [41], which was modified from multiple iterations in Bowles [42] and Pommier et al. [43].

4. Results

4.1. Zircon U–Pb Age

Twenty zircon grains from sample 20S59-1 (porphyritic granite) were analyzed. All analyses form a tight cluster with a weighted mean 206Pb/238U age of 135.6 ± 1.3 Ma (Figure 6a), which is interpreted as the crystallization age of the porphyritic granite. Fifteen analyses were performed on 15 individual zircon grains extracted from sample 23S02 (fine-grained granite). The results yielded 206Pb/238U ages ranging from 131 ± 3 to 139 ± 4 Ma (Table 1). The weighted mean 206Pb/238U age was determined to be 135.4 ± 1.7 Ma (Figure 6b), interpreted as the time of emplacement and crystallization of the fine-grained granite.

4.2. Whole-Rock Major and Trace Element Composition

The Kunduleng granites are high-silica (SiO2 = 74.52–76.98 wt%) and alkali-rich (K2O + Na2O = 7.90–9.75 wt%) rocks. They contain high concentrations (in ppm) of Rb (313–470) and relatively low contents of MgO (0.04–0.09 wt%), CaO (0.21–0.44 wt%), and TiO2 (0.06–0.16 wt%) (Table 2). These characteristics, coupled with their high differentiation indexes (DI = 92.7–97.6), suggest that the granites have experienced strong magmatic differentiation. Rb is incompatible in feldspars and accumulates significantly in the residual melt during fractionation. The notably elevated Rb content is a distinctive feature of highly fractionated granite. The highly evolved nature of the granites was further evidenced by the SiO2 versus K/Rb diagram (Figure 7a). The notably low Nb/Ta and Zr/Hf ratios further indicate strong fractionation within the Kunduleng granites (Figure 7b). In the Ba-Rb-Sr diagram of Figure 7c, samples mostly plot in the field of strongly differentiated granites.
The absence of aluminum-rich minerals, such as cordierite and garnet, coupled with a relatively high Na2O content, a molecular A/CNK ratio around or less than 1.1 (excluding uranium-anomalous samples), precludes the possibility of S-type affinity. A higher degree of differentiation poses challenges in distinguishing between fractionated I-type and A-type granites [44]. Wu et al. [45] point out that in the 10000Ga/Al versus Zr diagram, the fractional crystallization of high-temperature A-type granitic magma will exhibit a trend from A-type to highly fractionated granites. In contrast, the fractional crystallization of I/S-type granitic magmas lead to a gradual increase in 10000Ga/Al ratios. The Kunduleng granites are highly fractionated I-type rather than A-type granites (Figure 7d). In the A-B diagram proposed by Debon and Le Fort (1983) [46], modified by Cuney (2014) [23] and Villaseca et al. (1998) [47], the Kunduleng granites plot in the felsic peraluminous field (Figure 7e), mostly fall in the field of pegmatites and alaskites (Rössing), which are characteristic of melts generated by low-degree partial melting of crustal rocks.
The whole-rock Th/U ratio serves as a valuable indicator for assessing the fractionation and enrichment resulting from magmatic and metasomatic processes [23,48]. In the Th versus U diagram (Figure 7f), there is a significant enrichment of U and Th in the Kunduleng granite in comparison to the average crust. Meanwhile, the samples that have undergone alteration exhibit significantly higher U concentrations of 20.71–68.52 ppm and lower Th/U ratios of 0.83–2.29 than the relatively fresh samples (Figure 7). Therefore, a decrease in the Th/U ratio and its deviation from the unaltered samples typically signify the accumulation and redistribution of uranium in the Kunduleng granite.
Minerals 14 00666 g007
Figure 7. (a) K/Rb vs. SiO2 plot (after [49]); (b) Nb/Ta vs. Zr/Hf diagram (after [50]); (c) the Ba-Rb-Sr ternary diagram (after [51]); (d) 10000Ga/Al vs. Zr diagram (after [45,52]); (e) A-B diagram (after [23,46,47]); and (f) U vs. Th diagram (after [23,48]).
Figure 7. (a) K/Rb vs. SiO2 plot (after [49]); (b) Nb/Ta vs. Zr/Hf diagram (after [50]); (c) the Ba-Rb-Sr ternary diagram (after [51]); (d) 10000Ga/Al vs. Zr diagram (after [45,52]); (e) A-B diagram (after [23,46,47]); and (f) U vs. Th diagram (after [23,48]).
Minerals 14 00666 g007
The total REE (∑REE) ranges from 101.47 to 211.82 ppm and the REE distribution in the Kunduleng granite exhibits a V-shaped (seagull-shaped) pattern (Figure 8a), characterized by a prominent europium anomaly (δEu = 0.06–0.24). Slight MREE depletion relative to LREE ((La/Sm)N = 2.27–5.38) and HREE ((Gd/Yb)N = 0.23–0.77) could be linked to fractionation of hornblende or its presence as a residual phase during the melting process. This is because hornblende, the primary mineral hosting the MREE, is deficient in HREE. The depletion of MREE and the presence of a negative Ti anomaly may also be attributed to the fractional crystallization of sphene. The trace element patterns of the Kunduleng rocks are enriched in K, Rb, and depleted in Ba, Sr, P, and Ti (Figure 8b). The concentrations of Sr (9.4 to 87.3 ppm) and Ba (26 to 169 ppm) are relatively low, which is likely attributed to significant feldspar fractionation. Plagioclase and K-feldspar preferentially retain these elements and gradually deplete them from the evolved residual melt. The REE patterns and multi-element spider diagrams are similar overall to those of the uraniferous leucogranites in the Rössing area, Namibia (Figure 8).

4.3. Zircon Hf isotopic Composition

Eight zircons extracted from the porphyritic granite sample 20S59-1 exhibited εHf(t) values spanning from 12.7 to 14.5. Additionally, the two-stage model ages (TDM2) ranged from 259 to 376 Ma (Figure 9; Table 3).

4.4. Chemical Compositions of Uraninite and Brannerite

A total of 12 uraninite grains were analyzed, as shown in Table 4. Lowering of the analytical totals (sums < 100 wt%) and its deviation from the theoretical substitution line may suggest potential oxidation of uraninite or could be caused by the presence of elements not included in the analysis, such as Tm2O3 and Lu2O3. The uraninite exhibits variable concentrations of UO2 (71.16–84.07 wt%) and PbO (1.17–1.59 wt%), with relatively high concentrations in ThO2 (3.50–5.08 wt%), REE (5.14 < ∑REE2O3 < 9.86 wt%), and Y2O3 (4.04–6.17 wt%). The uraninite exhibits U/Th ratios ranging from 11 to 45 (with an average of 17) and low total CaO + FeO + SiO2 contents ranging from 0.05 to 1.09 wt% (with an average of 0.40 wt%). Low concentrations of SiO2 suggest a reduced level of post-crystallization alteration.
Brannerite is also detected; however, its occurrence is significantly less prevalent compared to uraninite. Brannerite contained 34.17–38.55 wt% TiO2, 38.38–43.18 wt% UO2, 2.32–3.41 wt% ThO2, 2.19–3.76 wt% FeO, 1.26–2.52 wt% CaO, 1.17–2.41 wt% Nb2O5, 0.0–1.01 wt% SiO2, 0.49–0.97 wt% PbO, 0–0.84 wt% Y2O3, 0–0.05 wt% ZrO2, and 5.82–7.22 wt% REE2O3.

5. Discussion

5.1. Magma Source of the Granite

The Kunduleng granites are high in silica and low in iron and magnesium. The samples exhibit enrichment in large ion lithophile elements and strong depletion in high field strength elements, which are typical characteristics of melts derived from enriched mantle or crustal sources. The Kunduleng granite has highly positive zircon εHf(t) values, isotopically more depleted than the coeval mantle-derived mafic-intermediate rocks, which have less positive and negative εHf(t) values (Figure 9). Thus, it is unlikely to have originated from contemporaneous mantle-derived mafic magma. On the contrary, the granite has zircon Hf isotope composition overlapping those of the felsic rocks in the southern Great Xing’an Range, most of which were derived from partial melting of the juvenile mafic crust. A large number of studies have shown that significant Neoproterozoic–Phanerozoic crustal growth occurred in the Great Xing’an Range and the juvenile lower crust was formed directly by underplating of mantle-derived mafic magma [36]. The Kunduleng granite has εHf(t) values ranging from 12.7 to 14.5 and TDM2 ages between 260 and 377 Ma. Late Paleozoic gabbroic rocks were present in the Great Xing’an Range, which were derived from the partial melting of the metasomatized lithospheric mantle [56,57], and display compositions similar to those observed in the juvenile lower crust. Therefore, these units may be considered representative of the Late Paleozoic juvenile crust. The Hf isotopic composition of the Kunduleng granite is similar to the zircon Hf isotopic data previously documented in these rocks (Figure 5d), suggesting their formation from juvenile Late Paleozoic crust. Therefore, it is probable that the Kunduleng highly fractionated granites originated from the partial melting of newly underplated material, subsequently undergoing significant fractionation.
The process of magmatic differentiation can be evaluated by modeling trace elements. Sample 23S01 with the highest Fe content was chosen to represent the parent melt. The estimated proportions of fractionating minerals are approximately 35% K-feldspar, 25% plagioclase, and 10% biotite. The trace element modeling of Rb, Ba, and Sr (Figure 10) shows that the evolutionary trajectory match very well with the bulk compositions of the Kundeleng granites. The progressive depletion of Sr and Ba, coupled with the enrichment of Rb, is related to fractional crystallization involving plagioclase, K-feldspar, and biotite.

5.2. Magmatic Origin of Uraninite

The variation of major elements in uraninite is controlled by specific processes, including the initial incorporation of Th, Y, and REE substituting for U, as well as the replacement of Pb by Ca, Si, and Fe during alteration. The incorporation of Th, Y, and REEs into the uraninite lattice is generally controlled by its crystallization temperature [69,70,71]. The higher the temperature, the greater the substitution [72]. The uraninite of the Kunduleng granites exhibits elevated levels of REE2O3 (averaging 5.98 wt%), Y2O3 (0.66 wt%), and ThO2, along with a Th/U ratio ranging from 0.02 to 0.09, as illustrated in Figure 11a,b. These characteristics are typical of magmatic uraninite. The correlation between the REE patterns of uraninite and deposit type is also feasible. The Kunduleng uraninite have large amounts of REEs and displays flat REE-patterns, resembling high-temperature intrusive-related uraninite rather than the low-temperature hydrothermal uraninite in volcanic-related and vein-type deposits (Figure 11c). The uraninite at the Kunduleng granite exhibits minimal concentrations of silicon, calcium, and iron, with an average total SiO2 + FeO + CaO content of 0.40 wt%. This suggests that post-crystallization alteration is relatively insignificant, and there is also minimal lead loss after initial crystallization. Thus, the lead in uraninite primarily originates from the radioactive decay of uranium, and the time since the mineral’s formation can be calculated. The U-Th-Pb chemical age of uraninite is 135.4 ± 5.2 Ma (Figure 11d), which is consistent with the zircon age (135.4–135.6 Ma) of the Kunduleng granite, compatible with a predominantly magmatic origin. The uraninite crystals are preserved from alteration which is likely due to their smaller size, inclusion in quartz as well as their high Th and REE contents, which collectively reduce and immobilize the oxidation of uraninite.

5.3. Hydrothermal Formation of Brannerite

The formation of brannerite is usually associated with the fluid-assisted (U-bearing hydrothermal fluids) alteration of Ti minerals, such as ilmenite and rutile [77,78]. In the Kunduleng granites, brannerite is restricted to red-stained granite (somewhat altered) adjacent to joint structures where uranium has been mobilized and precipitated. Backscattered electron images of the altered and reddened granite show that brannerite is intimately intergrown with ilmenite, forming crusts on ilmenite or occasionally extending into them (Figure 5e). The presence of a U-concentration gradient can also be observed in the brannerite-rutile aggregates (Figure 5f), with a uraniferous rutile core intergrown with or cemented by U-rich brannerite. The existence of a rimmed replacement texture suggests the formation of brannerite through in-situ replacement, where uranium migrates to Ti-rich phases. The alteration initiates at the surface of ilmenite and rutile and advances inward through fractures, indicating a hydrothermal genesis of brannerite. Alteration of the granite appears to be associated with the heating attendant with volcanic eruptions and dike intrusions. The Kunduleng granite was later intruded by granite porphyry and overlain by rhyolitic volcanics, which were dated to 118.4 Ma and 117.3 Ma (Figure 2), respectively. Minor uranium occurrences have also been identified in these volcanic rocks [79]. Although variational, the U-Th-Pb chemical ages of the brannerite (on average 118.4 Ma) determined by electron probe microanalysis are generally consistent with the later erupted and intruded rocks. Thus, this episode of silicic magmatism might have resulted in another stage of uranium enrichment within the Kunduleng granite.

6. Conclusions

The Early Cretaceous Kunduleng granites in NE China are felsic peraluminous and produced by partial melting of a Paleozoic juvenile protolith. Uraninite is the main radioactive mineral responsible for the uranium anomaly in the Kunduleng area, characterized by elevated levels of Th, Y, and rare earth elements (REE). It occurs as tiny cubic euhedral crystals (2–20 μm) within the major rock-forming minerals and has the same age as the host granite, suggesting its crystallization from the highly evolved granitic melts. Locally, secondary brannerite is observed rimming and replacing ilmenite and rutile within the sericitized and muscovitized granite and in that vicinity, well-developed joints are conspicuous, indicating post-magmatic uranium redistribution. The Kunduleng uranium-anomalous granites share some similarities with the uraniferous leucogranites in the Rössing area, Namibia.

Author Contributions

Investigation, D.S., J.G., L.T. and C.W.; formal analysis, J.G., D.Y. and D.Z.; software, J.S. and J.G.; writing—original draft, J.S., D.S. and J.G.; writing—review and editing, D.S., J.G. and C.W.; visualization, J.S.; funding acquisition, D.S. and J.G. All authors have read and agreed to the published version of the manuscript.

Funding

This work was supported by the China National Uranium Co., Ltd. and the Nuclear Industry Team 243 (Grant No. 202003 and 202210-3), the State Key Laboratory of Ore Deposit Geochemistry open project foundation (Grant No. 201903) and Fundamental Science on Radioactive Geology and Exploration Technology Laboratory, East China University of Technology (Grant No. 2020RGET02).

Data Availability Statement

The data presented in this study are available on request from the corresponding author.

Acknowledgments

We sincerely appreciate the reviewers for dedicating their valuable time to thoroughly review our manuscript. Their insightful comments and detailed suggestions have significantly contributed to enhancing the quality of our paper. We appreciate Wenqing Li and Yujin Li for their assistance with major and trace element analyses. We are grateful to Yujie Hao for his help with the zircon U–Pb analysis.

Conflicts of Interest

The authors declare no conflicts of interest.

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Figure 1. The tectonic position of the studied granite (after reference [24]).
Figure 1. The tectonic position of the studied granite (after reference [24]).
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Figure 2. Distribution of the granite in the Kunduleng area [25,26,27,28].
Figure 2. Distribution of the granite in the Kunduleng area [25,26,27,28].
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Figure 3. Field and petrographic characteristics of the Kunduleng granites. (a) Well-developed joints are present in the granite. (b) A vein composed of fine-grained granite within a host rock of porphyritic granite. Hand specimen (c) and thin section (d) images of the porphyritic granite. Hand specimen (e) and thin section (f) images illustrate the characteristics of the fine-grained granite. Abbreviations: Qtz = quartz; Pl = plagioclase; Mic = microcline; and Pth = perthite.
Figure 3. Field and petrographic characteristics of the Kunduleng granites. (a) Well-developed joints are present in the granite. (b) A vein composed of fine-grained granite within a host rock of porphyritic granite. Hand specimen (c) and thin section (d) images of the porphyritic granite. Hand specimen (e) and thin section (f) images illustrate the characteristics of the fine-grained granite. Abbreviations: Qtz = quartz; Pl = plagioclase; Mic = microcline; and Pth = perthite.
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Figure 4. Photomicrographs illustrating typical petrographic characteristics of altered granites. (a) Sericitization of plagioclase. (b) Locally, K-feldspar is muscovitized. (c) Muscovitization of biotite. (d) Fluorite in altered biotite. Abbreviations: Qtz = quartz; Pl = plagioclase; Kfs = K-feldspar; Bt = biotite; Ms = muscovite; and Fl = fluorite.
Figure 4. Photomicrographs illustrating typical petrographic characteristics of altered granites. (a) Sericitization of plagioclase. (b) Locally, K-feldspar is muscovitized. (c) Muscovitization of biotite. (d) Fluorite in altered biotite. Abbreviations: Qtz = quartz; Pl = plagioclase; Kfs = K-feldspar; Bt = biotite; Ms = muscovite; and Fl = fluorite.
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Figure 5. BSE images of uraninite and brannerite. Minute uraninite is present in quartz (a–c) and K-feldspar (d). Brannerite is closely associated with ilmenite and rutile (e,f). Abbreviations: Urn = uraninite; Brn = brannerite; Rt = rutile; Ilm = ilmenite; Qtz = quartz; and Kfs = K-feldspar.
Figure 5. BSE images of uraninite and brannerite. Minute uraninite is present in quartz (a–c) and K-feldspar (d). Brannerite is closely associated with ilmenite and rutile (e,f). Abbreviations: Urn = uraninite; Brn = brannerite; Rt = rutile; Ilm = ilmenite; Qtz = quartz; and Kfs = K-feldspar.
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Figure 6. 206Pb/238U versus 207Pb/235U concordia diagram for U–Pb data obtained on zircons from porphyritic granite (a) and fine-grained granite (b).
Figure 6. 206Pb/238U versus 207Pb/235U concordia diagram for U–Pb data obtained on zircons from porphyritic granite (a) and fine-grained granite (b).
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Figure 8. REE patterns (a) and trace element spider diagrams (b) for the Kunduleng granites. Values for normalization are sourced from references [53,54]. The uraniferous leucogranites are sourced from reference [55].
Figure 8. REE patterns (a) and trace element spider diagrams (b) for the Kunduleng granites. Values for normalization are sourced from references [53,54]. The uraniferous leucogranites are sourced from reference [55].
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Figure 9. Zircon εHf(t) versus age diagram for the Kunduleng granite. The U–Pb ages and Hf isotopic composition of zircon in magmatic rocks from the Great Xing’an Range are sourced from references [56,57,58,59,60,61,62,63,64,65,66,67].
Figure 9. Zircon εHf(t) versus age diagram for the Kunduleng granite. The U–Pb ages and Hf isotopic composition of zircon in magmatic rocks from the Great Xing’an Range are sourced from references [56,57,58,59,60,61,62,63,64,65,66,67].
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Figure 10. (a) Ba vs. Sr and (b) K/Rb vs. Sr diagrams of the Kunduleng granites. For modeling Rayleigh fractionation, the FC–AFC–FCA and mixing modeler developed by Ersoy and Helvacı (2010) [68] is employed.
Figure 10. (a) Ba vs. Sr and (b) K/Rb vs. Sr diagrams of the Kunduleng granites. For modeling Rayleigh fractionation, the FC–AFC–FCA and mixing modeler developed by Ersoy and Helvacı (2010) [68] is employed.
Minerals 14 00666 g010
Minerals 14 00666 g011
Figure 11. (a) Total REE content (wt%) versus U/Th diagram of uraninite (after [73,74]); (b) ThO2 + Y2O3 versus UO2 (wt%) diagram of uraninite (after [70]); (c) chondrite-normalized rare earth element patterns for uraninite from the Kunduleng granite. The data for uraninite in intrusive, vein-type, and volcanic-related deposits are from reference [75]. The values utilized for normalization come from the reference [76]. (d) Weighted mean U–Th–Pb EPMA chemical ages of uraninite.
Figure 11. (a) Total REE content (wt%) versus U/Th diagram of uraninite (after [73,74]); (b) ThO2 + Y2O3 versus UO2 (wt%) diagram of uraninite (after [70]); (c) chondrite-normalized rare earth element patterns for uraninite from the Kunduleng granite. The data for uraninite in intrusive, vein-type, and volcanic-related deposits are from reference [75]. The values utilized for normalization come from the reference [76]. (d) Weighted mean U–Th–Pb EPMA chemical ages of uraninite.
Minerals 14 00666 g011
Table 1. Zircon U–Pb isotopic data of the granite in the Kunduleng area, NE China.
Table 1. Zircon U–Pb isotopic data of the granite in the Kunduleng area, NE China.
Sample No.ThUIsotopic RatiosAge (Ma)
207Pb/206Pb207Pb/235U206Pb/238U208Pb/232Th207Pb/206Pb207Pb/235U206Pb/238U208Pb/232Th
Ratio1σRatio1σRatio1σRatio1σAge1σAge1σAge1σAge1σ
20S59-1-0188216500.059110.001700.173260.005160.021260.000480.004780.00011571.361.4162.24.5135.63.096.42.2
20S59-1-0271918450.051200.001590.150500.004800.021320.000480.006300.00015249.969.7142.44.2136.03.0127.03.1
20S59-1-03117922990.061460.001920.180440.005780.021290.000480.006330.00015655.365.5168.45.0135.83.1127.53.0
20S59-1-04111320600.056970.001840.166960.005530.021250.000480.006800.00016489.970.3156.84.8135.63.1136.93.2
20S59-1-0589023980.061640.001610.181370.004970.021340.000480.008680.00019661.654.9169.24.3136.13.0174.73.8
20S59-1-06150128420.052220.001390.154130.004390.021410.000490.005720.00012294.959.6145.63.9136.53.1115.32.4
20S59-1-07105622970.053200.003370.152790.008960.020830.000500.006530.00014337.0148.0144.08.0133.03.0131.03.0
20S59-1-08100834010.050520.001430.146250.004370.021000.000480.006180.00014218.864.0138.63.9133.93.1124.42.7
20S59-1-09143629090.051270.001440.149400.004450.021130.000490.006590.00014252.963.5141.43.9134.83.1132.82.8
20S59-1-1091322860.050220.001360.149520.004310.021590.000500.006220.00013205.161.6141.53.8137.73.1125.42.7
20S59-1-11122433180.053780.001340.158050.004240.021320.000490.006440.00013361.655.3149.03.7136.03.1129.82.7
20S59-1-12102655380.050210.001260.147170.003960.021260.000480.007100.00016204.757.1139.43.5135.63.1142.93.2
20S59-1-1393242910.050880.002240.148150.005600.021120.000480.006650.00014235.0104.0140.05.0135.03.0134.03.0
20S59-1-14124528360.052070.001420.153730.004430.021410.000490.006740.00015288.361.1145.23.9136.63.1135.72.9
20S59-1-15153725400.059650.001690.174390.005200.021200.000490.006610.00014590.960.4163.24.5135.33.1133.12.9
20S59-1-16113323300.050590.001710.147230.005120.021110.000490.006510.00016222.076.4139.54.5134.73.1131.23.1
20S59-1-17138126220.059440.001620.176580.005060.021550.000490.006270.00014583.158.0165.14.4137.43.1126.22.8
20S59-1-1892122320.059480.001520.175240.004770.021370.000480.006470.00014584.954.6164.04.1136.33.1130.42.8
20S59-1-19188627430.052530.001670.150580.004940.020790.000480.006180.00014308.670.6142.44.4132.63.0124.62.8
20S59-1-2074520370.053450.001640.158460.005040.021500.000490.004800.00013347.868.0149.44.4137.13.196.72.5
23S02-01167417820.142110.021440.418000.060570.021330.000890.006010.0002022532763554313661214
23S02-02303126430.085930.009450.249780.026430.021080.000630.006260.0001613372222262113441263
23S02-0339411990.110330.004470.324030.012960.021330.000540.028620.0008618053828510136357017
23S02-04188023300.144310.004740.425620.013960.021410.000520.006420.000152280273601013731293
23S02-0559220760.050550.002090.147370.006140.021160.000500.006110.0002322054140513531235
23S02-06159520350.125790.002920.368630.009090.021260.000480.006250.00012204041319713631262
23S02-07312623980.127180.014680.376630.041590.021480.000720.006120.0001920592123253113751234
23S02-08389924750.046050.002860.130600.007560.020570.000470.009320.00036 136125713131887
23S02-0935216860.049620.002990.143880.008000.021030.000490.006640.00015177138136713431343
23S02-10207619150.143160.011900.429970.033370.021780.000650.006140.0001722661483632413941243
23S02-11213120980.152010.009710.456780.026340.021790.000600.006100.0001623691123821813941233
23S02-12369926080.135940.011630.400210.032100.021350.000630.006040.0001621761543422313641223
23S02-13123721480.085530.006050.256620.016950.021760.000550.006460.0001513281412321413931303
23S02-14120821640.091600.006790.269250.018700.021320.000550.006280.0001714591452421513631273
23S02-15244227650.046050.003530.130670.009540.020580.000480.007370.00045 170125913131489
Table 2. Major (wt%) and trace element (ppm) compositions of the granite in the Kunduleng area, NE China.
Table 2. Major (wt%) and trace element (ppm) compositions of the granite in the Kunduleng area, NE China.
Sample20S59-123S0517S31-123S0620S59-423S0123S0217S32-323S0723S0417S32-2
LithologyPorphyritic GraniteFine-Grained GraniteUranium-Anomalous Granite
SiO275.5574.6974.5276.9474.8474.6475.7976.9876.1976.0574.64
TiO20.060.070.060.070.060.130.160.090.080.070.08
Al2O313.7914.1614.0612.6913.8513.6813.2112.4012.9013.1714.08
TFe2O30.481.080.471.310.682.141.521.001.401.270.74
MnO0.030.060.010.060.010.070.080.010.070.070.01
MgO0.060.060.040.070.070.090.070.080.060.050.06
CaO0.290.360.210.250.270.440.260.280.330.410.35
Na2O4.233.814.563.394.153.803.483.373.423.654.26
K2O4.785.105.194.515.114.424.935.025.214.774.90
P2O50.010.010.010.010.020.020.010.010.010.010.02
LOI0.580.280.430.270.560.350.130.520.240.280.62
Total99.8699.6799.5599.5899.6099.7899.6499.7599.9199.8199.72
A/CNK1.091.141.041.161.081.161.151.081.091.101.09
A/NK1.141.201.071.211.121.241.191.131.151.181.14
DI96.5694.7697.6494.9096.5692.7394.6396.1395.1494.7395.97
La9.8813.7512.3415.2417.6325.7943.1621.6928.2323.9320.80
Ce72.6836.9159.3770.2958.1950.2797.6348.9372.5959.5282.85
Pr2.662.853.164.364.566.689.724.777.827.195.53
Nd8.369.039.6813.6714.2122.7028.8114.8626.2524.4816.78
Sm2.112.712.063.472.904.784.882.696.116.413.06
Eu0.050.150.080.130.060.450.230.200.250.200.06
Gd2.313.531.993.842.424.644.192.136.066.612.64
Tb0.591.050.461.110.481.020.900.371.391.570.57
Dy4.608.293.559.033.426.766.032.349.9711.564.31
Ho1.142.090.872.340.831.661.490.522.332.831.03
Er4.127.453.168.732.955.605.091.778.089.953.68
Tm0.771.460.591.790.551.111.050.321.571.970.70
Yb5.4810.534.2913.213.847.577.442.2011.2514.385.04
Lu0.821.660.652.070.581.221.210.341.712.250.76
∑REE115.56101.47102.26149.27112.62140.24211.82103.14183.62172.84147.81
δEu0.060.150.120.110.070.290.150.240.120.090.06
(La/Yb)N1.190.861.890.763.022.243.826.491.651.102.72
Rb416.1346.6470.3437.5405.9313.2454.4364.7432.8374.0454.3
Ba26.4763.9437.8846.5936.56308.046.71169.0109.077.7430.33
Th41.8147.3439.0844.6339.8147.9163.7332.7447.5148.8756.80
U4.495.847.512.608.008.006.103.3220.7138.9868.52
Nb40.5931.4031.9633.1435.3113.2059.559.6839.5737.0248.05
Ta7.718.346.028.027.424.0918.381.9612.4811.3710.73
Sr16.3826.999.4021.5712.5487.2521.7044.5423.2126.9511.94
Zr143.0153.5124.1144.8144.395.9487.2960.45162.3148.3168.2
Hf8.508.077.157.597.893.294.382.628.147.059.23
Y28.4847.7224.5154.5720.5136.9232.4312.4362.8685.4924.69
Ga20.1536.3618.2435.1718.0027.0231.4716.2431.3833.9520.61
104Ga/Al2.764.852.455.232.463.734.502.484.604.872.77
Th/U9.318.105.2017.154.985.9910.459.852.291.250.83
Rb/Sr25.4012.8450.0420.2832.373.5920.948.1918.6513.8838.05
K/Rb95.36122.091.5585.55104.4117.289.97114.399.79105.889.46
Nb/Ta5.263.765.314.134.763.233.244.943.173.264.48
Zr/Hf16.8219.0317.3519.0918.2929.2019.9423.0719.9421.0418.23
Note. TFe2O3 is the total iron as Fe2O3. LOI is loss on ignition. DI is the differentiation index. A/CNK = molar ratio Al2O3/(CaO + Na2O + K2O); A/NK = molar ratio Al2O3/(Na2O + K2O); δEu = 2EuN/(SmN + GdN), subscript N represents chondrite normalization.
Table 3. Zircon Lu–Hf isotopic data of the granite in the Kunduleng area, NE China.
Table 3. Zircon Lu–Hf isotopic data of the granite in the Kunduleng area, NE China.
Sample No.t(Ma)176Yb/177Hf2σ176Lu/177Hf2σ176Hf/177Hf2σεHf(0)εHf(t)2σTDM1TDM2fLu/Hf
20S59-1-01135.60.1744590.0011450.0060680.0000340.2830740.00001110.713.10.39291351−0.82
20S59-1-020.0722710.0003310.0027100.0000090.2830820.00001011.013.70.37252312−0.92
20S59-1-030.0878580.0001930.0033510.0000060.2830800.00001010.913.60.35260321−0.90
20S59-1-040.1111460.0002800.0043110.0000070.2830590.00001010.212.80.36299374−0.87
20S59-1-050.0823400.0001740.0032430.0000090.2830970.00001111.514.20.37234283−0.90
20S59-1-060.0924420.0002030.0037120.0000050.2830930.00000911.414.00.32242293−0.89
20S59-1-070.1056500.0008380.0041020.0000260.2831090.00001411.914.50.48220259−0.88
20S59-1-080.0733960.0001250.0030280.0000040.2830550.00001110.012.70.40295376−0.91
Table 4. Oxide concentrations (wt%) and Th-U-Pb chemical ages of uraninite and brannerite from the Kunduleng granite.
Table 4. Oxide concentrations (wt%) and Th-U-Pb chemical ages of uraninite and brannerite from the Kunduleng granite.
UO2ThO2PbOLa2O3Ce2O3Pr2O3Nd2O3Sm2O3Gd2O3Dy2O3Ho2O3Er2O3Yb2O3Y2O3SiO2FeOCaOTiO2MgOMnOP2O5Al2O3Nb2O5Ta2O5ZrO2TotalAgeU/Th
uraninite73.973.801.39-0.54-0.590.681.172.740.700.861.524.040.49-0.09--0.000.04-0.03--92.65137.615.1
75.953.501.490.120.44-0.880.851.182.470.761.051.434.960.170.010.05-0.05---0.01-0.0495.42143.916.8
75.113.901.260.020.380.170.810.870.922.620.781.151.404.210.560.020.050.030.030.02----0.0494.33123.114.9
74.043.731.410.000.970.281.350.771.112.220.750.841.576.150.15-0.01--0.060.00---0.0895.47139.415.4
71.163.651.350.111.000.131.130.570.922.010.610.951.345.790.39-0.09-0.01---0.02-0.0191.62139.015.1
74.033.711.35-0.85-0.780.600.951.950.440.951.295.540.21----0.020.03----92.70134.215.4
75.673.721.480.010.820.130.910.681.152.480.721.121.685.75-0.040.01-0.020.01----0.0196.40143.515.7
74.884.641.430.031.290.030.920.410.891.670.620.961.455.010.18-0.06--0.020.02----94.51139.412.5
74.475.081.260.091.29-1.080.760.882.020.760.771.255.810.96-0.130.00-0.01----0.0296.61123.111.4
76.184.351.41-1.150.271.300.590.792.240.730.911.306.17-0.090.07--0.02--0.02-0.1197.69135.813.6
79.973.901.59-0.24-0.410.450.592.010.300.971.594.910.210.060.05---0.01-0.03-0.1197.38146.015.9
84.071.451.580.100.720.150.760.070.631.440.140.160.974.360.63-0.04-0.030.020.02-0.01-0.0197.36139.244.9
brannerite38.683.110.97-0.960.311.050.540.801.690.510.630.733.020.612.261.7737.380.010.140.110.052.410.110.0597.88180.8
39.863.410.66-1.150.131.280.610.621.350.410.450.843.250.022.891.6038.55-0.12-0.021.170.120.0398.52119.7
62.190.430.72-0.25-0.13-0.070.16---0.110.720.782.3816.820.13-2.481.911.85-0.0691.7086.5
57.011.221.09-0.26-0.080.150.040.22-0.04-0.191.131.642.4419.790.080.042.371.642.350.220.0692.18141.0
61.040.730.53-0.390.11-0.040.040.100.060.05-0.030.980.982.7915.550.190.032.581.980.75-0.0389.5064.4
38.382.320.49-0.950.061.050.510.701.390.250.370.553.56-3.762.5237.390.030.090.04-1.450.00-95.8592.8
43.182.890.85-1.110.081.070.640.791.340.390.450.632.501.012.191.2634.17-0.14-0.081.51-0.0196.29143.3
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Sun, J.; Sun, D.; Gou, J.; Yang, D.; Wang, C.; Tian, L.; Zhang, D. Origin of the Kunduleng Granite and Its Associated Uranium Anomaly in the Southern Great Xing’an Range, NE China. Minerals 2024, 14, 666. https://doi.org/10.3390/min14070666

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Sun J, Sun D, Gou J, Yang D, Wang C, Tian L, Zhang D. Origin of the Kunduleng Granite and Its Associated Uranium Anomaly in the Southern Great Xing’an Range, NE China. Minerals. 2024; 14(7):666. https://doi.org/10.3390/min14070666

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Sun, Jiaxing, Deyou Sun, Jun Gou, Dongguang Yang, Changdong Wang, Li Tian, and Duo Zhang. 2024. "Origin of the Kunduleng Granite and Its Associated Uranium Anomaly in the Southern Great Xing’an Range, NE China" Minerals 14, no. 7: 666. https://doi.org/10.3390/min14070666

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