2021, Vol. 37
引用本文
陈涛亮, 任志, 李凯旋, 刘飞, 段丰浩, 冷成彪. 2021. 斑岩铜-钼成矿体系中铼含量分布特征及其制约因素探讨. 岩石学报, 37(9): 2677-2690, doi: 10.18654/1000-0569/2021.09.05
Chen TL, Ren Z, Li KX, Liu F, Duan FH and Leng CB. 2021. Distribution characteristics and influencing factors of rhenium concentrations in molybdenite from the porphyry Cu-systems: A review. Acta Petrologica Sinica, 37(9): 2677-2690(in Chinese with English abstract)
斑岩铜-钼成矿体系中铼含量分布特征及其制约因素探讨
1. 东华理工大学核资源与环境国家重点实验室, 南昌 330013;
2. 东华理工大学地球科学学院, 南昌 330013
2. 东华理工大学地球科学学院, 南昌 330013
摘要: 金属铼(Re)是支撑航空航天等高科技产业高质量发展的重要原材料，具不可替代性。研究表明，世界上绝大部分的Re都赋存在斑岩型矿床的辉钼矿之中，且Re含量在矿床、矿石、矿物颗粒等不同尺度上均存在较大差异，但目前学术界对导致这些差异的影响因素尚不清楚。本文通过对全球斑岩型Cu(Mo)、Mo(Cu)矿床中Mo品位、辉钼矿的微量元素组成和Re-Os年龄、成矿岩体的化学组成、Sr-Nd同位素等数据的汇总，深入探讨了影响该类矿床辉钼矿中Re含量变化的主要因素。结果显示，Re含量与矿床中钼的平均品位呈负相关，地幔物质的加入可能是形成高Re辉钼矿的基础。本研究证实，辉钼矿Re含量与其成矿时代不具耦合关系，并且Re的含量与辉钼矿沉淀的位置、以及辉钼矿多型之间亦无明显相关性，而可能与成矿岩体的成分、岩浆分异程度、成矿流体的性质、热液蚀变及表生作用过程有关。
关键词:
斑岩型矿床 辉钼矿 铼含量 分布特征 影响因素
Distribution characteristics and influencing factors of rhenium concentrations in molybdenite from the porphyry Cu-systems: A review
1. State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang 330013, China;
2. College of Earth Sciences, East China University of Technology, Nanchang 330013, China
2. College of Earth Sciences, East China University of Technology, Nanchang 330013, China
Abstract: As one of key metals, rhenium (Re) is extensively used in high-tech fields such as aerospace due to its refractory geochemical properties, which is irreplaceable. Previous studies have shown that most of Re in the world is concentrated in molybdenite of porphyry Cu-Mo deposits, but Re concentrations vary significantly on the scale of ore deposits, samples and even individual molybdenite particles. At present, understanding of such difference is still unclear. Based on the data of molybdenum grades, trace elements contents of molybdenite, molybdenite Re-Os ages, lithogeochemical and Sr-Nd isotopic compositions of porphyry Cu(Mo) and Mo(Cu) deposits in the world, key factors of affecting Re concentrations in molybdenite from porphyry deposits are discussed. The results show that Re concentrations are negatively correlated with the average molybdenum grades, and mantle-derived component input may be in favor of high Re molybdenite formation. This study confirmed that there were no direct relationships between Re concentrations of molybdenite and metallogenic ages of porphyry deposits, molybdenite precipitation locations, and molybdenite polytypes. In contrast, rhenium concentrations in molybdenite may be related to the compositions of ore-forming rocks, magmatic differentiation degree, nature of ore-forming fluids, hydrothermal alteration and supergenesis.
Key words:
Porphyry deposit Molybdenite Re concentrations Distribution characteristics Influencing factors
斑岩型矿床又称“细脉浸染型”矿床，通常与中酸性侵入体有关，具有规模大、品位低、矿化均匀、埋藏浅、适于露天开采等特点(Melfos et al., 2002; Seedorff et al., 2005)，它们主要分布在环太平洋成矿域、特提斯-喜马拉雅成矿域和中亚成矿域(申志超, 2015)。斑岩型矿床作为全球最重要的Cu、Mo、Au矿床类型之一，为世界提供了75% Cu、90% Mo和20% Au(Sillitoe, 2010)。同时，工业所需的铼亦主要来自该类矿床(图 1)(Sillitoe, 2010; John et al., 2017)。
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图 1 全球含Re斑岩型Cu(Mo)和Mo(Cu)矿床分布简图 Fig. 1 Global distribution map of rhenium-bearing porphyry Cu (Mo) and Mo (Cu) deposits |
金属铼(Re)具有难熔、耐腐蚀的特点以及较高的机械强度、稳定性和良好的塑性等物理性能(刘红召等, 2014; 廖仁强等, 2020)，在国防、航空航天和医疗器械等尖端技术领域应用十分广泛。据统计，全球超过80%的Re被用于制造喷射引擎的高温合金部件(如喷气式飞机燃烧室、涡轮叶片等)，10%被应用于生产石油重整催化剂(如铂铼合金)(John, 2015)。优良的物理化学特性及其不可替代性，使Re成为支撑我国战略性新兴产业高质量发展的重要原材料。
针对辉钼矿中Re的研究，前人工作主要集中在Re-Os同位素年代学方面(赵一鸣等, 1997; Stein et al., 2001; 杨泽强, 2007)，也有部分学者对辉钼矿的Re等微量元素组成开展了研究(Ciobanu et al., 2013; Voudouris et al., 2013; Pašava et al., 2016; Ren et al., 2018)，但对于Re含量影响因素的研究相对较少(Newberry, 1979a, b; Mao et al., 1999; 杨宗锋等, 2011; 廖仁强等, 2020; Golden et al., 2013)，且关于Mo品位、成矿时代、物质来源、辉钼矿多型等因素对Re含量变化的影响尚未达成一致。为深入探究Re的富集机制，本文系统收集了前人已发表的国内外斑岩型Cu(Mo)、Mo(Cu)矿床的辉钼矿Re含量、同位素年龄、辉钼矿多型(电子版附表 1-附表 4)，以及成矿岩体的Sr-Nd同位素等数据(表 1)，系统探讨了Re含量变化的控制因素，以期深化对Re成矿理论的认识，并为Re的找矿勘探提供理论支撑。
1 铼的地球化学性质及分布特征Re的原子序数为75，原子量为186.207，位于元素周期表第六周期第ⅦB族。Re作为稀散元素之一，主要富集在地核中，在地幔和地壳的丰度较低，分别为0.28×10-9(McDonough and Sun, 1995)和2×10-9(廖仁强等, 2020; Sun et al., 2003c)。自然界中的Re通常难以形成独立矿物，但含Re矿物较多，如磁黄铁矿、辉钼矿等(温汉捷等, 2019; 廖仁强等, 2020)，其中辉钼矿是Re的主要载体矿物。Re的价态具有较宽的变化范围(-1~+7价)，其中以+2、+4、+6和+7价最为常见(Liao et al., 2019)，Re的变价性导致其对氧化还原过程比较敏感(Znamensky et al., 2005; 温汉捷等, 2019; 廖仁强等, 2020)。Re为中度不相容性的亲铁、亲铜元素，与大多数造岩矿物(如，橄榄石、辉石、斜长石等)都不相容(Righter and Hauri, 1998; Watson et al., 1987)。此外，在岩浆演化过程中，相比于硅酸盐熔体，Re优先富集在流体中(Li, 2014)。同时，Re还具有很强的挥发性，通常富集在火山喷出物中或者辉钼矿精矿焙烧冶炼产生的烟尘中(Fleischer, 1959; Korzhinsky et al., 1994; Znamensky et al., 2005; Liao et al., 2019)。
Re主要分布在斑岩型矿床、层控砂岩型铜矿床及砂岩型铀矿床中(温汉捷等, 2019; John et al., 2017)。斑岩型矿床中Re的平均品位较低，但其规模大，贡献了全球90%的Re(Sinclair, 2007)。同时，Re在不同矿床中的分布不均(Fleischer, 1959; Sinclair et al., 2009)，如Fleischer (1959)统计全球82个矿床中辉钼矿的Re含量，发现其具有很大的变化范围(0~3250×10-6)。
不仅如此，Re在同一矿床不同样品或同一样品不同颗粒中的含量分布也极不均匀(Plotinskaya et al., 2018; Voudouris et al., 2009; Rathkopf et al., 2017; Ren et al., 2018)。例如，Bagdad矿床辉钼矿的Re含量从 < 15×10-6到4450×10-6不等(Rathkopf et al., 2017)；同一辉钼矿晶体中Re含量变化幅度甚至可达3个数量级(Košler et al., 2003; Selby and Creaser, 2004)，这种不均匀分布可能与Re在辉钼矿中以固溶体形式赋存有关(Voudouris et al., 2013)。
2 铼富集的控制因素尽管Re主要赋存在斑岩型矿床的辉钼矿中，但以Mo为主的斑岩矿床中的Re含量似乎普遍低于以Cu为主的斑岩矿床(Newberry, 1979b; Berzina et al., 2005)，这通常被认为与矿床中Mo的品位有关(Stein et al., 2001)。除此之外，影响辉钼矿中Re含量的控制因素可能还包括成矿时代(Golden et al., 2013; 黄凡等, 2014, 2019)、物质来源(Mao et al., 1999; Stein et al., 2001)、岩浆过程(Shirey and Walker, 1998; Sun et al., 2003a)、成矿流体物理化学性质(Xiong and Wood, 2001, 2002; Xiong et al., 2006; Berzina et al., 2005)、辉钼矿多型(Newberry, 1979a, b)以及成矿后热液蚀变(Newberry, 1979b; Aminzadeh et al., 2011)和表生作用过程(Liao et al., 2019; McCandless et al., 1993)。
2.1 铼的富集与矿床类型不同类型矿床中Re含量存在较大差异。据统计，辉钼矿中Re的含量在火山沉积型矿床、斑岩型矿床、矽卡岩型矿床、石英脉型矿床依次降低(Terada et al., 1971)。而在斑岩型矿床中，Cu(Mo)矿床辉钼矿的Re含量普遍高于Mo(Cu)矿床，且Re的含量似乎与矿床中Mo的品位呈负相关(Newberry, 1979b; Stein et al., 2001; Berzina et al., 2005)。Stein et al. (2001)将这一现象归因于质量平衡，他们指出由于斑岩体系中的Re均赋存在辉钼矿之中，以Cu为主的矿床辉钼矿的体量较小，因此Re含量相对较高；而以Mo为主的矿床辉钼矿的体量较大，因此Re含量相对较低。但这一观点值得商榷，如McFall et al. (2019)发现Muratdere矿床晚期辉钼矿较早期辉钼矿更富Re，因而与质量平衡的解释相背。此外，Voudouris et al.(2010, 2013)指出Melitena斑岩型矿床中Mo品位很高，但辉钼矿的Re含量仍然高达7900×10-6，并据此认为Re含量与Mo品位无明显相关性。
本文统计了全球主要斑岩型Cu(Mo)、Mo(Cu)矿床的Mo品位及其平均Re含量(图 2；附表 1)。据此可知，斑岩型Cu(Mo)矿床中Re含量的确高于斑岩型Mo(Cu)矿床，且当Mo品位升高时，Re的含量降低，似乎暗示Mo品位是影响Re富集的因素之一。但是，同为低Mo品位的矿床，如斑岩型W矿，其Re含量通常也较低(Mao et al., 1999; 杨宗锋等, 2011)，这表明Mo品位并不是控制Re富集的关键因素。该结果与Barton et al. (2020)的认识类似，他们依据Re和Mo含量的对数线性回归得到了m=-0.4(R2=0.29)的最佳拟合直线，指出这种质量平衡仅仅可以解释40%的Re的富集，其余部分则与Mo品位无关。
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图 2 辉钼矿中Re的含量与矿床Mo品位数据协变图 Fig. 2 Correlation between Re concentrations in molybdenite and Mo grades of porphyry deposits |
前人研究认为辉钼矿中Re的含量与成矿时代有一定相关性(黄凡等, 2019; Golden et al., 2013)，总体上表现为成矿时代越新，辉钼矿中Re含量越高。黄凡等(2014)将这种变化归因于Re的放射性衰变，但研究表明，Re在3.0Ga内因衰变而损失的量并不会超过其本身的5%(Barton et al., 2020)。Golden et al. (2013)则指出辉钼矿中Re的含量随着时间推移而逐渐增加的现象可能与地壳的逐渐氧化有关。
本文将主要斑岩型Cu(Mo)、Mo(Cu)矿床的辉钼矿Re-Os年龄与Re含量绘制成图 3(附表 2)。结果可知，斑岩型矿床主要形成于中生代-新生代，且也显示出与图 2类似的规律，Cu(Mo)矿床中Re含量普遍高于Mo(Cu)矿床，但不同时代之间并未显示出成矿时代越新，辉钼矿中Re含量越高的变化规律。
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图 3 斑岩型矿床辉钼矿Re含量与成矿时代的关系 Fig. 3 Relationship between Re concentrations in molybdenite and ages of porphyry deposits |
有学者提出，在800~542Ma存在全球性大氧化事件，使得全球大气氧含量大幅上升(Holland, 2006; Planavsky et al., 2014; Reinhard et al., 2017)，由于Re对氧化还原过程敏感，大气氧含量上升能够使其活化迁移加强(Znamensky et al., 2005; 温汉捷等, 2019; 廖仁强等, 2020)，因此也有观点认为Re含量的变化或许与此次大氧化事件有关(廖仁强等, 2020)。然而，由于本文所统计的斑岩型矿床均形成于550Ma之后，因此，仅依据本文数据无法判断Re的富集是否与大氧化事件有关。
2.3 铼的富集与成矿物质来源毛景文等(1999)统计了磁铁矿系列花岗岩有关的Mo-Cu矿床以及与钛铁矿系列花岗岩有关的W-Sn矿床中辉钼矿的Re含量，提出自幔源、壳幔混源到壳源，Re含量依次降低一个数量级。孟祥金等(2007)也得到了相似结论。Stein et al. (2001)同样认为地幔底侵或交代作用伴生的辉钼矿中Re含量高于地壳来源的辉钼矿；但目前这些观点仍存在较大争议(杨宗锋等, 2011; Berzina et al., 2005)，例如，Berzina et al. (2005)的研究显示Sora矿床的物质来源虽然为地幔，但是其Re含量仅为6×10-6~18×10-6，甚至低于地壳来源的Zhireken矿床(Re=12×10-6~57×10-6)；杨宗锋等(2011)统计了全国744个辉钼矿的Re含量，指出Re的富集受多种因素控制，不能简单的运用Re含量判断成矿物质来源。
图 4中自亏损地幔沿主地幔趋势线向下，地壳混入组分逐渐增多，物质来源由幔源逐渐向壳源过渡，其Re含量却并未显示出较为一致的变化趋势(表 1)，如物质来源为华北上地壳的千鹅冲矿床其铼含量为15.5×10-6~18.6×10-6，反而高于壳幔混源的石家湾矿床(Re=10.2×10-6)；而成矿物质以幔源为主的纳日贡玛斑岩Cu(Mo)矿床其Re含量为35.5×10-6~75.0×10-6，甚至低于成矿物质来源于地壳的八里坡矿床(Re=38.4×10-6~155×10-6)，这一结果与Berzina et al. (2005)类似，可能反映了地幔的不均一性，因此不能仅仅依据Re含量判别成矿物质来源。同时，图 4及表 1也显示所有Re含量在200×10-6以上的矿床，均有地幔物质的加入，这一结果可能指示地幔物质加入是形成高Re辉钼矿的必要条件。成矿物质单纯来源于地壳的矿床似乎很难形成高Re辉钼矿，希腊东北部所有低Re辉钼矿的成矿金属主要来自地壳(Voudouris et al., 2013)。尽管也有研究表明，在黑色页岩中检测到较高的Re含量，指示Re似乎在表生环境下也能富集形成较高Re含量的辉钼矿(Liao et al., 2019; 廖仁强等, 2020)，如，华南黑色页岩Re含量为0.10×10-6~0.69×10-6(Jiang et al., 2007)，但经过相同表生富集过程且后期存在地幔物质加入的Kurile-Kamchatka的火山沉积矿床(Liao et al., 2019)，其Re含量可达74.5%(Znamensky et al., 2005)，远远大于仅接受表生富集的华南黑色页岩，这也暗示地幔物质的加入对高Re辉钼矿的形成具有重要作用。
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图 4 斑岩型Cu(Mo)和Mo(Cu)矿床成矿岩体(87Sr/86Sr)i-εNd(t)图解(底图据Jahn et al., 1999) ①~ ⑳为表 1中矿床编号 Fig. 4 (87Sr/86Sr)i vs. εNd(t) diagram for the ore-forming porphyries from some porphyry systems in China (base map modified after Jahn et al., 1999) ①~ ⑳ is the deposit number in Table 1 |
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表 1 斑岩型Cu(Mo)和Mo(Cu)矿床Re含量与成矿岩体的(87Sr/86Sr)i和εNd(t)值 Table 1 Re concentrations in molybdenite, (87Sr/86Sr)i and εNd(t) values for ore-forming porphyries from some porphyry systems in China |
岩浆去气过程、岩浆分异过程均能对Re的富集产生影响。如前所述，Re是中度不相容元素(Sun et al., 2003a)，在壳幔分异过程中，如果地幔源区部分熔融时没有石榴子石和硫化物的残留，Re倾向富集在熔体中(Shirey and Walker, 1998)；否则，Re将残留在源区(Feng and Li, 2019)。火成岩的化学成分通常在岩浆去气过程会发生显著变化(Rollinson, 1993)，Re具有较强的挥发性，在岩浆去气过程中，Re容易以铼酸(H2ReO4)的形式进入气相(Candela and Holland, 1986)。据报道，Kudeyavy火山喷气冷凝物中发现Re矿石晶体以及大量富Re的辉钼矿颗粒(Korzhinsky et al., 1994)，而Sun et al.(2003a, b)指出夏威夷火山海底喷出的洋岛玄武岩Re含量高于近地表喷出的玄武岩，表明Re在岩浆去气过程中会发生损失。
火成岩的成分对Re的富集也有影响(Ishihara, 1988; Sun et al., 2004; Berzina et al., 2005; Barton et al., 2020)，与中性岩共生的辉钼矿往往比与长英质岩共生的辉钼矿更富Re(Ishihara, 1988; Barton et al., 2020)，而与高分异花岗岩有关的矿床Re含量通常较低(Berzina et al., 2005)。
与斑岩型Mo(Cu)矿床相比，斑岩型Cu(Mo)矿床Re含量普遍较高，且成矿岩体具有更低的SiO2含量，Re含量与成矿岩体的SiO2呈负相关(图 5a，附表 3)，这一统计结果与前人的结论一致。斑岩型Mo(Cu)矿床相比于斑岩型Cu(Mo)矿床，其岩浆分异程度更高，Re含量随着岩浆分异程度的增加，呈现出降低的趋势，Re含量与岩浆分异程度呈负相关(图 5a, b)。Re作为中度不相容元素，在岩浆分异过程中，倾向于残留在熔体相，随着分异程度增加，Re含量理应更高，似乎与本文统计结果相矛盾。据图 5c-d，Fe、Ti含量随着岩浆分异程度增加而降低，这与Re的变化是完全耦合的，表明这一结果或许与钛磁铁矿的结晶有关(孙卫东等, 2007)。钛磁铁矿的结晶能够使得流体氧逸度降低，致使正六价的Re被还原为正四价的Re，增大Re在矿物/岩浆之间的分配系数(孙卫东等, 2007)，因此，随着结晶分异程度增加，辉钼矿中Re含量降低。
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图 5 辉钼矿Re含量与成矿岩体平均SiO2含量(a)和分异指数(b)协变关系图及TiO2 (c)和FeOT (d)与成矿岩体SiO2协变关系图 Fig. 5 Covariant diagrams of Re concentrations in molybdenite vs. SiO2 contents (a), vs. DI index (b) for ore-forming porphyries, and SiO2 vs. TiO2 (c), vs. FeOT (d) contents for ore-forming porphyries |
研究表明，早期形成的辉钼矿在遭受后期热液蚀变作用时，可能发生Re的丢失(Newberry, 1979b; McCandless et al., 1993)。美国Arizona州的Eagle矿床中发生硅化作用的辉钼矿中Re含量降低，而硅化带中与之共生的方解石中Re含量却高达5.45%；同样，Arizona州的Bagdad矿床中，发生蚀变的辉钼矿边缘相比核部具有较低的Re含量(0.4%~0.5%)，而矿脉边缘以钾、铝和硅为主要成分，疑似伊利石的蚀变矿物却含有高达0.14%的Re(McCandless et al., 1993)。这些现象表明热液蚀变作用会引起Re进入到对应蚀变矿物中，并造成辉钼矿Re的含量降低。
也有研究指出辉钼矿中Re的含量似乎与蚀变类型、蚀变程度之间存在联系(Newberry, 1979b; Berzina et al., 2005)。钾化蚀变环境中，辉钼矿Re含量通常较低，如Climax矿床钾化阶段辉钼矿的Re含量很低(Newberry, 1979b)，这可能是由于碱性热液形成的钾长石蚀变环境具有运移Re的能力(Berzina et al., 2005)。在Sar Cheshmeh斑岩型Cu(Mo)矿床中，辉钼矿中Re含量随硅化程度的减弱和绢云母化程度的增强而升高(Aminzadeh et al., 2011)。
2.5.2 与流体物理化学性质的关系流体的物理化学性质对Re的迁移和富集同样具有重要影响，主要体现在流体温度、氧逸度、pH值和卤素组成等方面，以下分别给予阐述。
(1) 温度
Terada et al. (1971)最早提出温度相对较低的矿床中辉钼矿相对更富Re，如低温浸染辉钼矿(Sanaeda、Sodagawa和Atsuho矿床)Re/Mo的平均原子比为73×10-6，而高温浸染型(Shiro、Sekigane、Kamioka和Climax矿床)是3.4×10-6。此后，大量研究证实了这一认识(Plotinskaya et al., 2018; Ren et al., 2018)，如，Plotinskaya et al. (2018)利用与辉钼矿紧密共生的绿泥石成分计算其形成温度，发现Re含量较高的样品其形成温度低于Re含量低的样品，温度与Re含量之间呈显著负相关。
实验研究发现ReS2在400~500℃，升高温度，溶解度略微升高，意味着在较高温度时会有更多的ReS2溶解(Xiong and Wood, 2002)，这可以解释为什么较低温度下形成的辉钼矿具有较高的Re含量。
温度与Re含量间的关系在空间上往往表现为：由矿体中心向外围，辉钼矿的Re含量可能逐渐升高(Austen and Ballantyne, 2010)，因此部分矿床Re的含量与其辉钼矿沉淀高度会呈正相关(图 6)。
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图 6 Sar Cheshmeh矿床辉钼矿沉淀高度与辉钼矿中Re含量关系图(据Aminzadeh et al., 2011) Fig. 6 Plot of elevation vs. Re concentrations in molybdenite from the Sar Cheshmeh (modified after Aminzadeh et al., 2011) |
但也有观点指出，Cu、Au为主和W、Sn为主的斑岩型、矽卡岩型或石英脉型矿床的成矿温度范围没有明显差异，温度或许对辉钼矿中Re含量有相关影响，但在不同矿床类型之间却并未像Re一样有着巨大变化，故温度不是控制Re含量的主要因素(Barton et al., 2020)。Re富集是由多种因素控制的，不同类型的矿床成矿条件存在较大差异，Barton et al. (2020)所列举的事例仅能表明不同矿床类型对铼富集也能产生较大影响，并不能否定温度对Re富集所起到的作用。
(2) 氧逸度
不同类型斑岩矿床中Re含量变化呈现出一定的规律性，Cu-Au矿床(n×10-4)>Cu-Mo矿床(n×10-5)>Mo-W矿床(n×10-6)(Mao et al., 1999; 李诺等, 2007; 杨宗锋等, 2011)，这一现象与Thompson et al. (1999)提出的与岩浆热液有关的Cu-Au、Cu-Mo、Mo-W矿床氧逸度依次降低的结论高度重合，这表明Cu(Mo)矿床与Mo(Cu)矿床中的Re含量除了与Mo品位存在相关性，还可能与氧逸度有关。
Berzina et al. (2005)测定了多个矿床的(CO2/CH4)/CO2的比值，指出氧化性流体有利于Re的迁移富集。在不考虑pH的情况下，只有高氧逸度流体才可以运移大量的Re(Xiong et al., 2006)；而还原性流体，携带Re的能力较弱(Xiong and Wood, 2001)，很难形成较为富Re的矿床，如在希腊北部偏还原性的成矿系统中，辉钼矿Re含量通常较低(Voudouris et al., 2010)。在相似条件下，使用ReS2得到的Re浓度比使用Re-ReO2缓冲剂组合的实验得到的Re浓度大约低两个数量级，Re的氧化性流体和含还原硫的流体发生混合可能是Re的有效沉积机制之一(Xiong and Wood, 2002)。
氧逸度对Re含量的影响在不同成矿阶段也有体现，如Ren et al. (2018)通过对沙坪沟斑岩型Mo矿床中的辉钼矿开展LA-ICP-MS分析，发现成矿晚期相比于成矿早期，成矿流体的氧逸度升高，同时辉钼矿中Re含量从0.3×10-6~7×10-6增至3×10-6~120×10-6，类似的例子还有Muratdere矿床(McFall et al., 2019)及EI Teniente矿床(Spencer et al., 2015)等。
(3) 卤素组成
流体中卤素的组成似乎也能对Re的运移起到促进作用。实验表明，Re在400~500℃的弱酸性至中性流体中，主要以氯配合物ReCl40和ReCl3+的形式迁移，其稳定性与氯离子浓度有很强的依赖关系(Xiong and Wood, 2002)。如，在高Re辉钼矿的矿床中，流体的f(HCl)/f(HF)比值通常较高(Berzina et al., 2005)，岩浆流体中较高的Cl和F含量降低了流体中的羟基含量，这可能减少了以羟基络合物形式输送的Mo含量，从而使得流体中的Re/Mo比值升高，有利于高Re辉钼矿的形成(Selby and Creaser, 2001)。
(4) pH值
pH值在热液过程中的影响主要体现在对Re溶解度的控制方面。在富氯流体中，随着pH值的升高，ReO2或ReS2的溶解度明显降低(Xiong and Wood, 2002)；在无氯化物的流体中，Re的羟基络合物则更为重要(Xiong and Wood, 2001)，在这种情况下，pH值的升高可能会导致Re的溶解度增加(Xiong and Wood, 2002)。
2.6 铼的富集与表生作用过程Re在表生环境通常会富集在黑色、深灰色沉积物中，这一富集过程通常与表生的氧化还原过程关系密切。表生条件下，随着辉钼矿等含Re矿物的化学分解，其中的Re4+经氧化作用将转化成水溶性的ReO4-，并随表生流体运移，在缺氧环境下，ReO4-将被有机质或硫化物等还原(Liao et al., 2019; 廖仁强等, 2020)，从而导致Re富集于某些含碳沉积物中。这与王正其等(2006, 2007)提出的层间氧化带型Re富集机制类似：表生含氧水的不断补给会在合适的砂岩中形成层间承压水，层间承压水在砂岩中渗透、径流会使围岩的Re活化并将其运移至还原性的深灰色砂岩中沉淀。
表生过程除能够将Re富集至深色沉积物中，似乎也能将早期矿床中的Re重新分配。Newberry (1979b)研究证实表生环境下低pH流体能够将辉钼矿中Re浸出；McCandless et al. (1993)的实验结果也表明表生作用能够在不改变红外透射率的情况下，将辉钼矿中Re重新分配，造成Re的丢失。
前文提及，由于较低温度下形成的辉钼矿通常具有较高的Re含量，空间上远离矿化点处通常会具有较高Re含量，因此有时沉淀高度与Re含量之间会呈现出正相关。然而，更多的研究结果显示辉钼矿沉淀高度与Re含量之间并无这种相关性，如Voudouris et al. (2013)统计了希腊东北部多种矿床的数据，认为没有迹象表明辉钼矿的Re值在这些矿点中随深度或横向变化；Rathkopf et al. (2017)也指出Bagdad矿床和矿体周围辉钼矿Re浓度的分布是不稳定的，与矿床海拔、距矿石的距离以及其他空间特征无关。表生作用可能是导致这一现象的原因之一，越靠近地表(离矿化点越远)，表生作用的影响越强。此外，不同矿床的地质特征、当地气候、蚀变等可以影响表生作用强度的因素，均可以对其造成很大影响，从而导致辉钼矿Re含量与其沉淀高度之间缺乏应有的相关性。
2.7 铼的富集与辉钼矿多型的关系辉钼矿在自然界中主要有2H和3R两种多型，其中2H多型较为常见，3R型较为少见(王翠芝和刘文元, 2013; 杨宜坪等, 2018)。3R多型通常含有较多的杂质，2H多型则较为纯净(Chukhrov et al., 1970)。研究指出杂质含量的增多，有利于3R多型晶体结构的形成(韩吟文, 1988; 黄凡等, 2012; 王翠芝和刘文元, 2013; Newberry, 1979a)。Newberry (1979a)认为3R多型的出现与晶体结构的螺旋位错机制有关。螺旋位错理论认为由于杂质元素(内应力)和热应力分布的不均匀，晶体内会产生特殊的定向内应力，在其达到极限时，元素离子间存在的内应力作用将产生“螺旋状力”，进而导致3R多型的形成(王翠芝和刘文元, 2013)，并且Newberry (1979a)还指出，在无外力作用下，杂质含量大于500×10-6，一定会有3R多型的存在。
Frondel and Wickman (1970)首先提出辉钼矿中Re富集可能与辉钼矿的多型有关，随后引起了大量学者的关注(Newberry, 1979a, b; Ayres, 1974; 韩吟文, 1988; Aminzadeh et al., 2011; Voudouris et al., 2009)，但辉钼矿多型是否与Re含量之间存在联系，目前尚未达成共识。
Re是辉钼矿中最主要的杂质元素(Newberry, 1979a)，有学者指出Re含量与辉钼矿多型具有一定的规律性，即2H多型通常含Re量低，而3R多型含Re量高，因而Re的含量和辉钼矿中3R多型含量呈正相关(Newberry, 1979a, b; Ayres, 1974; Melfos et al., 1991; McCandles et al., 1993)，如，Melfos et al. (1991)得出Maronia矿床中富Re辉钼矿和贫Re辉钼矿分别为3R多型和2H多型的结论；McCandles et al. (1993)对Copper Creek角砾岩筒中的原生结晶辉钼矿的研究也显示辉钼矿中3R多型含量越高，其Re含量越高。
然而，更多的证据表明多型和Re含量之间或许并无相关性(黄典豪, 1992; Pašava et al., 2016)。黄典豪(1992)通过对东秦岭地区不同类型钼矿床中辉钼矿多型及Re含量的研究认为辉钼矿多型的发育与其Re含量之间并无相关性；Pašava et al. (2016)统计了4种不同矿化类型的矿床，发现这些矿床中的辉钼矿均为2H多型，且部分样品超过500×10-6；Aminzadeh et al. (2011)发现伊朗Sar Cheshmeh矿床存在早世代贫Re辉钼矿和晚世代富Re辉钼矿，但二者均为2H多型；Voudouris et al. (2009)对4个自然界Re含量最高的辉钼矿晶体的结构分析，证实它们的结晶类型均为2H多型，而不是先前假设的3R多型。同时朱砂红及小狐狸山等矿床中的具较低Re含量的3R多型(曲焕春等, 2015; 位鸥祥, 2019)，似乎也显示Re的含量与特定多型之间并无相关性。
图 7的统计结果显示Re含量与某一多型之间不存在特定的相关性(附表 4)。不过，仅据这一结果无法排除辉钼矿两种多型相互间转变的影响(Newberry, 1979b)。表生环境下低pH的流体以及蚀变作用能够将已形成辉钼矿中的Re重新运移分配，这一过程或许是低铼3R多型形成的原因之一(Newberry, 1979b; McCandless et al., 1993)，而高铼2H多型则被认为是高铼3R多型在遭受后期较高温热液蚀变重结晶形成的(Newberry, 1979a)，但这一转变需要较多的能量供应，因此低温的表生作用下难以发生这种重结晶过程，而在能量充足的情况下，转变后的高铼2H多型在高杂质含量的作用下，又会重新形成高铼3R多型，故此过程必须损失一部分Re含量才能进行(Newberry, 1979a)。而McCandless et al. (1993)指出高温流体发生Re损失的过程几乎没有或者不存在多型的转变，同时前人所测的自然界4个Re含量最高的辉钼矿均为2H多型，但却缺乏含相同层次Re含量的3R多型的报道，这或许表明部分高铼2H多型的形成未受到后期的多型转变的影响，仅与辉钼矿的生长机制有关。
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图 7 Re含量与辉钼矿多型直方图 Fig. 7 Histogram of Re concentrations and molybdenite polytypes |
前已述及，2H多型在流体存在较高Re含量时或许会转变成3R多型，但Drábek et al. (2010)由钼粉(纯度99.99%)、Re粉(纯度99.95%)和硫在400~1200℃的温度范围内进行了120次实验，在产物中并未检测到辉钼矿的3R多型，仅有2H多型，这表明高Re含量并不一定能引起多型的转变，辉钼矿的多型更有可能受其他因素的制约。因此，未受转变机制影响的高铼2H多型完全是有可能存在的，结合图 7的统计结果，本文认为辉钼矿中Re的富集与辉钼矿特定多型之间无相关性，或者说多型并不是控制Re富集的关键因素。
此外，大量研究表明Re含量、辉钼矿的多型与Mo同位素的分馏之间存在联系。Mathur et al. (2010)提出辉钼矿中Re含量与Mo同位素组成具有微弱相关关系，即Mo同位素值随Re含量降低而升高。Segato (2018)在统计分析了不同类型矿床的Mo同位素组成后，也得出相似的结论，即辉钼矿的Mo同位素组成与Re含量存在负相关关系。Shafiei et al. (2015)利用分子振动理论解释了辉钼矿多型与Mo同位素组成的关系，即较重的Mo同位素优先分配进入较致密的原生2H型辉钼矿晶格中。因此，开展Mo同位素相关工作或许能进一步论证辉钼矿的Re含量与多型之间关系。
3 结论Re的富集与矿床Mo的平均品位、成矿物质来源、岩浆去气过程、岩浆分异过程、流体的物理化学性质(如：温度、氧逸度、卤素组成、pH值等)以及表生过程密切相关，而与辉钼矿成矿时代、沉淀的位置以及辉钼矿多型之间无明显相关性。
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附表 1 辉钼矿中Re的含量与矿床Mo品位数据 Appendix Table 1 Re concentrations in molybdenite and Mo grades of porphyry deposits |
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附表 2 斑岩型矿床辉钼矿Re含量与成矿时代数据 Appendix Table 2 Re concentrations in molybdenite and ages of porphyry deposits |
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附表 3 辉钼矿Re含量与成矿岩体平均SiO2含量、分异指数及TiO2和FeOT含量 Appendix Table 3 Re concentrations in molybdenite and SiO2 content, DI, TiO2 and FeOT contents for ore-forming porphyries |
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附表 4 Re含量与辉钼矿多型关系 Appendix Table 4 Re concentrations and molybdenite polytypes |
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