造山带铜镍硫化物矿床的岩浆起源:以东天山黄山南铜镍矿床为例

位于中亚造山带南缘的新疆东天山地区因其出露大量的二叠纪镁铁质-超镁铁质岩体并产出一系列铜镍硫化物矿床而成为近年来地质学界关注的焦点.选择新疆东天山地区黄山南含铜镍矿镁铁质-超镁铁质岩体为研究对象,对其开展了系统的岩石学、矿物学和地球化学研究,以探讨造山带铜镍硫化物矿床的岩浆起源与性质.黄山南岩体主要由方辉橄榄岩、二辉橄榄岩、橄榄二辉岩、（橄榄）辉长苏长岩和闪长岩组成.各岩相显示富集大离子亲石元素和轻稀土元素、强烈亏损Nb-Ta、Ti,类似于典型岛弧火山岩特征.黄山南镁铁质-超镁铁质岩具有较大变化范围的ε_Nd（t=282.5 Ma）值（-1.31~4.22）和（87Sr/86Sr）_i比值（0.703 2~0.706 9）以及高的（206Pb/204Pb）_i比值（17.67~18.90）,暗示其来源于一个适度富集的亏损地幔并经历了5%~20%新生地壳物质混染和~5%上地壳物质混染.根据橄榄石最高Fo牌号（摩尔含量为86.6%）计算的黄山南母岩浆为苦橄质岩浆（MgO=12.11%、FeO_Total=11.14%、Ni=306×10-6）,指示其岩浆源区应为软流圈和交代地幔楔共同熔融的源区.黄山南橄榄石低的Ca（< 725×10-6）和100×Mn/Fe（1.18~1.38）、高的Ni（1 451×10-6~2 813×10-6）和Mn/Zn（11.09~23.53）,暗示黄山南母岩浆来源于含有辉石岩的不均一橄榄岩地幔源区.因此,我们推测黄山南岩体的原始岩浆来源于早期经历过俯冲流体改造的含有辉石岩的交代岩石圈地幔源区.      

新疆黄山铜镍硫化物矿床成矿岩浆作用过程

黄山铜镍硫化物矿床镁铁．超镁铁质岩体岩相发育良好,主要包括橄榄岩、辉石岩、辉长岩和闪长岩,橄榄岩中部分橄榄石包含有硫化物珠滴。对该岩体不同岩相进行了主元素、微量元素、铂族元素和单矿物的分析,结果表明,不同类型岩石的化学组成受橄榄石、辉石和斜长石结晶分异作用的控制。微量元素和稀土元素具有相似的分布模式,（La／Yb）N介于1．14—3．65之间,明显亏损Nb和Ta,富集Sr。含矿岩石Cu／Pd和Ti／Pd比值大于原生地幔岩浆。上述结果揭示黄山镁铁-超镁铁质岩体不同岩性的岩石具有不同的主元素和微量元素特征,但母岩浆来自同一源区。根据橄榄石的F0值和全岩的主要氧化物组成估算出母岩浆为高镁（MgO约为15％）玄武岩岩浆,在岩浆作用过程中地壳富硅组分的混染是导致硫化物熔离的主要机制。     

新疆东天山铜镍成矿带西段镁铁—超镁铁质岩体成因及成矿潜力研究

新疆东天山铜镍成矿带铜镍总储量达百万吨,是我国重要的铜镍矿集区。以往的研究多集中在成矿带的东段和中段,而本文选择成矿带西段的典型岩体进行详细的地质年代学、矿物学和岩石地球化学研究。东天山铜镍成矿带西段镁铁—超镁铁质岩体以大草滩和白鑫滩岩体为代表,可分为四种岩相:闪长岩相、辉长岩相、橄榄辉长岩相和橄榄岩相,其中橄榄岩相为主要含矿岩相。白鑫滩岩体橄榄辉长岩锆石U-Pb年龄为286.4±1.6Ma,与岩体含长辉石橄榄岩(~278 Ma)相差~7 Ma。大草滩和白鑫滩岩体样品主量元素投影点都处于主要造岩矿物化学成分之间,表明岩体的主量元素主要受堆晶矿物控制。大草滩和白鑫滩岩体的微量元素标准化图解与东天山典型成矿岩体相似,均具有明显的Nb,Ta亏损,且具有较高的ε_(Nd)(t)值(+6.01~+8.9,t=286 Ma)和ε_(Hf)(t)值(+11.62~+16,t=286 Ma)。大草滩和白鑫滩岩体岩浆源区是软流圈上涌导致被俯冲事件改造的交代地幔发生部分熔融的产物。岩体橄榄石Fo值与Ni的关系表明岩浆在橄榄石结晶过程中存在硫化物熔离。模拟计算表明上述岩体母岩浆在上侵过程中在深部与新生的岛弧地壳发生5%~15%的混染后达到了硫饱和,造成了硅酸盐岩浆PGE的亏损。分离结晶和地壳硫的加入是导致岩浆在地壳层位发生二次熔离的主要因素。不同岩相的年龄数据表明大草滩和白鑫滩岩体形成于多期次岩浆作用,有助于形成具有经济价值的铜镍矿体。对比可得新疆东天山铜镍成矿带西段的镁铁—超镁铁质岩体的年龄和硫化物饱和过程与东段和中段的成矿岩体相似,故成矿带西段有寻找大中型铜镍硫化物矿床的潜力。     

新疆东天山天宇、白石泉杂岩体岩石学、矿物学特征对比研究

天宇和白石泉铜镍矿区含矿镁铁-超镁铁质杂岩体是东疆铜镍成矿带的重要组成部分。天宇矿区杂岩体以角闪辉长岩、角闪单辉橄榄岩、橄榄辉石岩、二辉辉石岩为主;白石泉矿区杂岩体则以辉石闪长岩、角闪辉长岩、橄榄辉石岩、辉石辉长岩、辉石橄榄岩、橄长岩为主;天宇矿区含矿超基性岩中SiO2,Al2O3,CaO,K2O,Na2O的质量分数比白石泉岩体低,Fe2O3,MgO相对较高;两个杂岩体的主要造岩矿物均以橄榄石、辉石、斜长石为主;铜镍矿石的矿物组成都较简单,金属矿物种类基本一致;两个杂岩体基性-超基性岩的成分接近原始岩浆,均来自于地幔,均属含铜镍中等的镁铁质岩石。     

岩浆铜镍矿与钒钛磁铁矿的过渡类型--新疆哈密香山西矿床

铜镍硫化物矿床与钒钛磁铁矿矿床虽然同属与镁铁-超镁铁质岩有关的岩浆型矿床范畴,但在一般情况下,二者是不共生的.新疆东天山地区的香山西矿床则是一个铜镍矿与钛铁矿共生的实例.香山地区为一复式含矿杂岩体,最早期形成辉长岩(如角闪辉长岩、灰白色细粒辉长岩等)为主体的侵入;第二期侵入的是以辉橄岩、单辉橄榄岩、二辉橄榄岩等为主的超镁铁质岩,含铜镍硫化物矿化;第三期则为岩浆期后残余岩浆形成的含钛铁矿化的辉长岩(脉).香山西铜镍-钛铁矿床含矿岩石的碱度、镁铁指数、岩浆酸度、钙碱富集指数等地球化学参数,氧逸度和硫逸度等物理化学参数均介于独立的典型铜镍硫化物和典型钒钛磁铁矿矿床之间.矿床中磁铁矿较其他钒钛磁铁矿矿床(尾亚)具较高的V和Ti含量,同时黄铁矿和黄铜矿具较高的Co、Ni和Cu含量,反映出成矿过程中,Cu-Ni-Co系列与V-Ti-Fe系列的分离不够彻底.形成本区CuNi-VTi复合型矿床的原因,可能在于矿床所处独特的构造环境--产于造山带,而不是克拉通(边缘).     

吉林磐石三道岗含铜镍硫化物矿床岩体群年代学意义

吉林省中南部产出系列铜镍硫化物矿床,形成于中生代早期的含矿镁铁-超镁铁质岩体在含矿岩体空间上受断裂构造控制,并且在一定范围内集中出现,构成具有成因联系的含矿岩体群。三道岗含矿岩体主要岩石类型为闪长岩、辉长岩、角闪辉石岩-辉石岩、含长角闪橄榄岩等组合,侵位于下二叠统范家屯组浅变质岩系中。辉长岩中LA-ICP-MS锆石原位定年得到(232.75±0.95)Ma(MSWD=0.87)的岩体结晶年龄,同时,角闪石单矿物40Ar-39Ar法测年得到(121.45±2.52)Ma的蚀变年龄,暗示三道岗含矿岩体群与红旗岭一样形成于印支中亚造山晚期,燕山期岩浆活动产生的热液叠加蚀变对矿床形成产生重要影响。     

东天山四顶黑山层状岩体地质特征及成矿潜力分析

东天山黄山岩带因发育众多镁铁质-超镁铁质岩体和岩浆铜镍硫化物矿床而备受地质学者关注。四顶黑山岩体位于该岩带最东端,具有层状岩体特征;岩石类型有单辉橄榄岩、橄榄辉石岩、橄榄苏长辉长岩、橄榄辉长岩、辉石角闪岩、辉长岩、角闪辉长岩、闪长岩,主要造岩矿物为贵橄榄石、古铜辉石、透辉石、普通角闪石和斜长石,岩体分异较好,蚀变较发育。通过矿物显微结构特征观察以及计算得出:四顶黑山岩体中橄榄石最先结晶,其开始结晶温度大约在1419℃左右;古铜辉石和透辉石在橄榄石之后开始结晶,结晶温度分别在1100℃左右和900～1100℃之间,两矿物相在岩石中可以共存。岩体中橄榄岩相、苏长岩相发育,以及贵橄榄石+古铜辉石的矿物组合特征,表明岩体具有形成铜镍(铂)矿床的有利条件。     

新疆东天山黄山岩体岩石地球化学特征与岩石成因

黄山岩体位于东天山北部的土墩-黄山-图拉尔根镁铁-超镁铁质岩带中段,受康古尔塔格-黄山韧性剪切带控制,主要由橄榄岩、橄榄二辉岩、辉石岩、辉长苏长岩、辉长岩以及辉长闪长岩组成.岩石化学组成属拉斑玄武岩系列,普遍富集大离子亲石元素(Rb,Ba,Sr),亏损高场强元素(Nb,Ta,Ti).岩体εNd(t)=+4.1～+9.2,除3件样品εSr(t)为+2.2,+12.5和+15.4,大部分εSr(t)=(-22.5～-4.5),Nd,Sr同位素组成基本属亏损型地幔特征;Pb同住素初始值(206Pb/204Pb)i=18.081～18.413,(207Pb/204Pb)i=15.441～15.513,(208Pb/204Pb)i=37.461 6～37.899,具有MORB亲和性.岩相学及岩石地球化学特征显示岩浆演化过程中主要发生了橄榄石、斜方辉石、单斜辉石和斜长石的分离结晶作用.岩浆演化晚期阶段发生了一定程度的同化混染作用,元素地球化学和Nd,Sr,Pb同位素体系证明,岩浆源区主体由软流圈地幔物质组成,同时也有一定量富集型岩石圈地幔组份加入.黄山岩体是岩石圈根部拆沉加热熔融和软流圈地幔上涌减压熔融的产物,这种地幔动力学机制应该对应于后碰撞伸展环境.     

甘肃北山二叠纪镁铁- 超镁铁质岩体地质、地球化学特征及铜镍成矿潜力

北山造山带是中亚造山带南缘镁铁- 超镁铁质岩体的集中分布区之一，因其赋含二叠纪铜镍硫化物矿床而受到广泛关注。以往的研究多集中在北山造山带西部的新疆坡北地区，近年来随着对甘肃北山地区二叠纪镁铁- 超镁铁岩体认识逐渐深入，新发现的矿化岩体有逐渐向东延伸的趋势。本文选择北山造山带中东部柳园地区骆驼山和西南山两个典型含铜镍硫化物岩体进行地质年代学、岩相学和岩石地球化学及同位素地球化学研究。岩体主要岩相包括橄榄岩相、辉石岩相、橄榄辉长岩相、橄长岩相和辉长岩相，其中硫化物主要出现在橄榄岩相和辉石岩相中。骆驼山岩体辉长岩锆石的U- Pb年龄为282. 6 Ma，与坡北地区矿化岩体的形成时代一致。骆驼山和西南山岩体母岩浆稀土元素配分模式为轻微右倾型，富集大离子亲石元素，强烈亏损高场强元素Nb- Ta，中等亏损Zr- Hf，与坡北和东天山地区同时代矿化岩体母岩浆特征相似。岩体具有较高的全岩εNd(t)值(+0. 42~+6. 10)和锆石εHf(t)值(+7. 9~+14. 1)的特征，与坡北地区矿化岩体类似，表明具有相似的亏损地幔源区。橄榄石Fo值与Ni含量的关系和母岩浆微量元素Cu/Zr比值特征表明岩浆在橄榄石结晶过程中发生了硫化物熔离。同位素模拟计算表明母岩浆在上升侵位过程中发生了约5%~15%的地壳物质混染，可能是岩浆硫饱和的主要原因。相同的成岩成矿时代、相似的岩石地球化学特征、母岩浆特征及硫化物饱和机制，表明甘肃北山地区二叠纪镁铁- 超镁铁质岩体具有与坡北地区类似的成矿潜力，为在北山地区中东部进一步寻找铜镍硫化物矿床提供了重要信息。     

新疆东天山二红洼岩体岩浆演化特征与成矿潜力分析

二红洼岩体位于康古尔-黄山韧性剪切带东段,主要由含长二辉橄榄岩、橄榄辉长岩、辉长苏长岩和淡色辉长岩组成。岩石相对富集LREE,亏损高场强元素(Nb、Ta、Ti)。岩体原生岩浆为普通拉斑玄武岩(MgO=7.3%)。通过对元素地球化学和Nd、Sr、Pb同位素体系研究证明,岩浆源区以软流圈物质为主,混入了少量富集岩石圈地幔组分,岩浆遭受了约5%上地壳物质的混染。与同岩带典型含矿岩体对比研究表明,岩体在岩石组合、原生岩浆性质、同化混染程度等方面存在显著差异,这些因素可能制约了成矿潜力。     

Partition of Ni between olivine and sulfide and its application to Ni-Cu sulfide deposits

Equilibration of natural olivine with (Fe, Ni)S in sealed silica glass tubes yields a value for the distribution constant for Ni/Fe exchange (K_D3) of 27.7±3.5, for 1,200° C, product olivine and sulfide compositions in the ranges 96 to 97 mol% Fo and 15 to 70 mol% NiS, respectively, and run durations of 28 days. Electron microprobe analysis of product olivine was made on ～50 μm diameter grains separated from the sulfide matrix to eliminate the severe matrix interference experienced with in situ determination of trace and minor amounts of Ni. The present K_D3 value is in general agreement with previous experimental results indicating K_D 3～30 in the temperature range applicable to hypothesized magmatic models for Ni-Cu sulfide ore formation and with inferred K_D3 values for the temperature range 400 to 600° C. The olivine and sulfide compositions of a selection of Ni-Cu sulfide deposits yield K_D3 values appreciably lower than the corresponding equilibrium values, which argues against concentration of the sulfides to ore grade in their present locations as early magmatic sulfides. However, K_D3 is significantly higher for Ni-Cu sulfide deposits metamorphosed to medium and high grade conditions. The good correlation of increasing approach to chemical equilibrium with increasing grade and pervasiveness of metamorphism is related to the marked temperature dependence of the mobility of Ni in olivine.     

Partition of nickel between olivine and sulfide: A test for immiscible sulfide liquids

The partition of Ni between olivine, crystallised from basalt liquids, and iron-nickel monosulfide has been determined experimentally at 1160 and 1050 °C using alumina crucibles in sealed silica glass tubes. The compositional ranges investigated are 83 to 88 mol. % Fo and 5 to 50 mol. % NiS. The average distribution coefficient for the exchange reaction FeS +NiSi_0.5O₂NiS+FeSi_0.5O₂ is remarkably similar to the literature value of 33.2 for 900 °C. It is concluded that within the temperature and pressure range of magmatic olivine crystallisation the exchange reaction is effectively independent of temperature, pressure, olivine composition and composition and physical state of the sulfide.The NiO contents of early magmatic olivine are appreciably greater than the calculated NiO contents for equilibration with any hypothetical iron-rich immiscible sulfide liquid, suggesting that an immiscible sulfide liquid may not be a normal product of upper mantle magmatic processes. Similarly, it appears unlikely that sulfide liquid immiscibility had any role in the genesis of nickel sulfide ores.Olivine from upper mantle and crustal rock associations has characteristic NiO/MgO distributions. Both distributions appear to be the products of extensive fractionation by crystal-liquid processes although the crustal olivine distribution may be complicated by the added factor of heterogeneity of mantle magma source.     

Convergence of sulfide deposits

Sulfide deposits are believed to be convergent, that is, similar in composition, structure, and geologic location, but different in genesis. The three chief genetic classifications of sulfide deposits are: 1) sedimentary - exhalational, 2) subvolcanic exhalational - hydrothermal, and 3) plutonic hydrothermal. The first two groups are very closely related,frequently forming almost simultaneously with the same stage of volcanic activity in spilite-keratophyre rocks of eugeosynclines. They are associated with the derivatives of basaltic magmas. The plutonic hydrothermal sulfide deposits are associated with porphyry series of rocks in the marginal zones of geosynclines, generated by a granitoid magma.—E. K. Russell.     

Geochemical and mineralogical aspects of sulfide mine tailings

Tailings generated during processing of sulfide ores represent a substantial risk to water resources. The oxidation of sulfide minerals within tailings deposits can generate low-quality water containing elevated concentrations of SO₄, Fe, and associated metal(loid)s. Acid generated during the oxidation of pyrite [FeS₂], pyrrhotite [Fe_(1−x)S] and other sulfide minerals is neutralized to varying degrees by the dissolution of carbonate, (oxy)hydroxide, and silicate minerals. The extent of acid neutralization and, therefore, pore-water pH is a principal control on the mobility of sulfide-oxidation products within tailings deposits. Metals including Fe(III), Cu, Zn, and Ni often occur at high concentrations and exhibit greater mobility at low pH characteristic of acid mine drainage (AMD). In contrast, (hydr)oxyanion-forming elements including As, Sb, Se, and Mo commonly exhibit greater mobility at circumneutral pH associated with neutral mine drainage (NMD). These differences in mobility largely result from the pH-dependence of mineral precipitation–dissolution and sorption–desorption reactions. Cemented layers of secondary (oxy)hydroxide and (hydroxy)sulfate minerals, referred to as hardpans, may promote attenuation of sulfide-mineral oxidation products within and below the oxidation zone. Hardpans may also limit oxygen ingress and pore-water migration within sulfide tailings deposits. Reduction–oxidation (redox) processes are another important control on metal(loid) mobility within sulfide tailings deposits. Reductive dissolution or transformation of secondary (oxy)hydroxide phases can enhance Fe, Mn, and As mobility within sulfide tailings. Production of H₂S via microbial sulfate reduction may promote attenuation of sulfide-oxidation products, including Fe, Zn, Ni, and Tl, via metal-sulfide precipitation. Understanding the dynamics of these interrelated geochemical and mineralogical processes is critical for anticipating and managing water quality associated with sulfide mine tailings.     

Evidence of sulfide melting and melt fractionation during amphibolite facies metamorphism of the Rajpura–Dariba polymetallic sulfide ores

Partial melting of sulfide ores during prograde metamorphism could have been more prevalent than generally accepted. However, identification of such melting is difficult as sulfide melts do not form glasses and the textures generated on quenching are obliterated due to the tendency of sulfides for ready recrystallization. The polymetallic base metal sulfide deposit at Rajpura–Dariba, Rajasthan, India is a typical stratiform ore metamorphosed to the middle amphibolite facies. The peak metamorphic temperature of 600 °C should have been sufficient to initiate sulfide melting as evident from experimental studies in the ZnS–PbS–Cu₂S–FeS₂–S system. Further, syn-metamorphic melting of the original SEDEX ore was abetted by the high f_S2 condition that prevailed as a consequence of barite dissolution. A Zn–Fe–S melt containing minor Pb, Sb and Cu but no Ag fractionated from an initial melt in the above system resulting in a residual immiscible sulfosalt-bearing PbS melt. The final metallic melts, represented by formation of dyscrasite (Ag₃Sb) from the sulfosalt-bearing melt and breithauptite (NiSb) or ullmannite (NiSbS) from the sulfosalt-absent melt, were a product of independent fractional crystallization of the immiscible sulfide and PbS–sulfosalt melts.     

Empirical equations to predict the sulfur content of mafic magmas at sulfide saturation and applications to magmatic sulfide deposits

Empirical equations to predict the sulfur content of a mafic magma at the time of sulfide saturation have been developed based on several sets of published experimental data. The S content at sulfide saturation (SCSS) can be expressed as:

High temperature calorimetry of sulfide systems

Enthalpies of solution of synthetic pentlandite Fe_4.5Ni_4.5S₈, natural violarite (Fe_0.2941Ni_0.7059)₃S₄ from Vermillion mine, Sudbury, Ontario, synthetic pyrrhotite, FeS, synthetic high temperature NiS, synthetic vaesite, NiS₂, synthetic pyrite, FeS₂, Ni and Fe have been measured in a Ni_0.6S_0.4 melt at 1,100 K. Using these data and the standard enthalpies of formation of binary sulfides, given in literature, standard enthalpies of formation of pentlandite and violarite were calculated. The following values are reported: ΔH _f ^{o, Pent} =?837.37±14.59 kJ mol^?1 and ΔH _f ^{o, Viol} =?378.02±11.81 kJ mol^?1. While there are no thermo-chemical data for pentlandite with which our new value can be compared, an equilibrium investigation of stoichiometric violarite by Craig (1971) gives a significantly less negative enthalpy of formation. It is suggested that the difference may be due to the higher degree of order in the natural sample.     

High temperature calorimetry of sulfide systems

The standard enthalpies of formation of FeS (troilite), FeS₂ (pyrite), Co_0.9342S, Co₃S₄ (linnaeite), Co₉S₈ (cobalt pentlandite), CoS₂ (cattierite), CuS (covellite), and Cu₂S (chalcocite) have been determined by high temperature direct reaction calorimetry at temperatures between 700 K and 1021 K. The following results are reported: $$\Delta {\rm H}_{f,FeS}^{tr} = - 102.59 \pm 0.20kJ mol^{ - 1} ,$$ $$\Delta {\rm H}_{f,FeS}^{py} = - 171.64 \pm 0.93kJ mol^{ - 1} ,$$ $$\Delta {\rm H}_{f,Co_{0.934} S} = - 99.42 \pm 1.52kJ mol^{ - 1} ,$$ $$\Delta {\rm H}_{f,Co_9 S_8 }^{ptl} = - 885.66 \pm 16.83kJ mol^{ - 1} ,$$ $$\Delta {\rm H}_{f,Co_3 S_4 }^{In} = - 347.47 \pm 7.27kJ mol^{ - 1} ,$$ $$\Delta {\rm H}_{f,CoS_2 }^{ct} = - 150.94 \pm 4.85kJ mol^{ - 1} ,$$ $$\Delta {\rm H}_{f,Cu_2 S}^{cc} = - 80.21 \pm 1.51kJ mol^{ - 1} ,$$ and $$\Delta {\rm H}_{f,CuS}^{cv} = - 53.14 \pm 2.28kJ mol^{ - 1} ,$$ The enthalpy of formation of CuFeS₂ (chalcopyrite) from (CuS+FeS) and from (Cu+FeS₂) was determined by solution calorimetry in a liquid Ni_0.60S_0.40 melt at 1100 K. The results of these measurements were combined with the standard enthalpies of formation of CuS, FeS, and FeS₂, to calculate the standard enthalpy of formation of CuFeS₂. We found \(\Delta {\rm H}_{f,CuFeS_2 }^{ccp} = - 194.93 \pm 4.84kJ mol^{ - 1}\) . Our results are compared with earlier data given in the literature; generally the agreement is good and our values agree with previous estimates within the uncertainties present in both.     

Iron sulfide oxidation and the chemistry of acid generation

Acid mine drainage, produced from the oxidation of iron sulfides, often contains elevated levels of dissolved aluminum (AI), iron (Fe), and sulfate (SO₄) and low pH. Understanding the interactions of these elements associated with acid mine drainage is necessary for proper solid waste management planning. Two eastern oil shales were leached using humidity cell methods. This study used a New Albany Shale (4.6 percent pyrite) and a Chattanooga Shale (1.5 percent pyrite). The leachates from the humidity cells were filtered, and the filtrates were analyzed for total concentrations of cations and anions. After correcting for significant solution species and complexes, ion activities were calculated from total concentrations. The results show that the activities of Fe³⁺, Fe²⁺, Al³⁺, and SO₄ ²⁻ increased due to the oxidation of pyrite. Furthermore, the oxidation of pyrite resulted in a decreased pH and an increased pe+pH (redox-potential). The Fe³⁺ and Fe²⁺ activities appeared to be controlled by amorphous Fe(OH)₃ solid phase above a pH of 6.0 and below pe+pH 11.0. The Fe³⁺, Fe²⁺, and SO₄ ²⁻ activities reached saturation with respect to FeOHSO₄ solid phase between pH 3.0 and 6.0 and below pe+pH 11.0 Below a pH of 3.0 and above a pe+pH of 11.0, Fe²⁺, Fe³⁺, and SO₄ ²⁻ activities are supported by FeSO₄·7H₂O solid phase. Above a pH of 6.0, the Al³⁺ activity showed an equilibrium with amorphous Al(OH)₃ solid phase. Below pH 6.0, Al³⁺ and SO₄ ²⁻ activities are regulated by the AlOHSO₄ solid phase, irrespective of pe+pH. The results of this study suggest that under oxidizing conditions with low to high leaching potential, activities of Al and Fe can be predicted on the basis of secondary mineral formation over a wide range of pH and redox. As a result, the long-term chemistry associated with disposal environments can be largely predicted (including trace elements).