The Magmatic Activity in Paleoproterozoic Global Magmatic Quiescence: Take the ~2.3 Ga Henglingguan Granites from Zhongtiao Mountains in the Southern North China Craton as an Example
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摘要: 在全球岩浆活动静寂期，人们在华北克拉通内相继识别出大量~2.3 Ga的地质体，对探讨华北克拉通古元古代地质演化过程具有十分重要的意义.选择中条山地区横岭关二长花岗岩进行了地球化学、锆石U-Pb年代学和Hf同位素研究.横岭关二长花岗岩LA-ICPMS锆石U-Pb年龄结果为2 308±12 Ma，代表岩体的形成时代.横岭关二长花岗岩高硅、高钾、高铝、富碱，贫钙、低钠和低钛，A/CNK主要集中在1.0~1.1之间，为高钾钙碱性偏铝－过铝质花岗岩系列.岩石的稀土元素含量相对高，轻重稀土元素分异强烈，并具有明显的Eu负异常.高场强元素Nb、Ta、Zr、Hf、U和大离子亲石元素Rb等相对富集，亏损V、Cr、Co、Ni等相容元素，具有I型花岗岩的特征.横岭关二长花岗岩锆石εHf（t）为0.52~6.24，平均值为2.06，单阶段和两阶段模式年龄分别为2 419~2 642 Ma和2 438~2 738 Ma.横岭关二长花岗岩具有同碰撞花岗岩的特征，推测来源于~2.5 Ga古老地壳岩石在挤压碰撞环境下的部分熔融，揭示了华北克拉通在古元古代全球岩浆静寂期并不静寂.Abstract: A large number of ~2.3 Ga geologic bodies have been identified in the North China Craton (NCC) in global magmatic quiescence, which is vital for unveiling the Paleoproterozoic geological evolution on the NCC. This paper presents the whole rock geochemical data, zircon U-Pb ages and Hf isotopes of the Henglingguan monzogranite in Zhongtiao mountains area. LA-ICPMS dating of zircon from the Henglingguan monzogranite yields an age of 2 308±12 Ma. The Henglingguan monzogranite is high in SiO2, K2O, Al2O3 and alkali, and low in CaO, NaO and TiO2, with A/CNK concentrated between 1.0 and 1.1, which belongs to high-K calc-alkaline and metaluminous-peraluminous series. The monzogranite is high in total REE contents, showing strong fractionation of LREE and HREE and obvious negative Eu anomaly. As to the trace elements, the monzogranite shows enrichment in Nb, Ta, Zr, Hf, U and Rb, and depletion in V, Cr, Co and Ni, which is consistent with characteristics of I-type granite. Zircons in the Henglingguan monzogranite have εHf(t) values ranging from 0.52 to 6.24, with an average of 2.06, and Hf model TDM1 age of 2 419-2 642 Ma and TDM2 age of 2 438-2 738 Ma. The Henglingguan monzogranite shows the features of syn-collision granites originated from partial melting of the ~2.5 Ga ancient crust in collision environment, which shows the NCC was not quiet during the Paleoproterozoic global magmatic quiescence.
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挥发性氯代有机化合物是重要的化工原料和有机溶剂, 广泛的应用于化工、医药、制革、电子等行业.加上挥发性氯代烃还是饮用水氯气消毒的副产物, 使其成为地下水和饮用水中最常见的有机污染之一[1, 2].许多氯代有机化合物具有“三致效应” (致癌、致畸、致突变) 或可疑“三致效应”, 是各国优先控制的污染物.因此对此类污染物污染的环境水体进行恢复处理已迫在眉睫.氯代有机化合物的种类很多, 其中最常见的是三氯乙烯(TCE) 和四氯乙烯(PCE), 它们是美国和日本等国的地下水中检出率最高的有机污染物[3, 4].随着工业化进程的加速, TCE和PCE对地下水污染有着进一步扩大的趋势.由于TCE和PCE都为非混溶相液体, 污染范围大, 容易扩散, 而且很难被生物降解, 因而以TCE和PCE为目标污染物研究地下水中的氯代有机物污染有着明显的实际意义[5].本文主要在实验室条件下, 用零价铁作为反应介质的批实验方法, 对脱氯效果和影响因素进行初步的研究.
1. 实验方法
(1) 实验材料.机械加工厂的生铁废料, 粒径为20~40目和60~80目, 自来水, 分析纯的四氯乙烯和四氯化碳. (2) 实验仪器.恒温水浴振荡器; 带HP-7694自动顶空进样器的HP-6890气相色谱.仪器条件: 进样口温度, 160 ℃; 色谱柱柱流量, 1.0 mL/min; 炉温, 70 ℃; 保留时间, 10 min; 检测器ECD温度, 300 ℃[6].顶空部分: 瓶区, 50 ℃; Loop: 60 ℃; 传输线, 70 ℃; 瓶平衡时间, 10 min; 注射时间, 1.00 min; 振摇时间, 5 min; 载气流量, 约30 mL/min[7].实验装置: 用120 mL玻璃钳口瓶, 带有聚四氟乙烯膜的瓶盖. (3) 批实验程序.称10.00 g生铁放于钳口瓶中, 将配好的氯代烃溶液缓缓注入瓶中[8], 封口.配置储备液用地质大学的自来水, 其成分如表 1.将瓶放于往复式恒温水浴中振荡, 每隔一定时间间隔取水样进行分析, 每个取样时间点有3个瓶, 一个不放铁只放原溶液作为控制样, 另外两个瓶作为反应液做平行样.取样时, 用注射器抽取瓶中液体0.5 mL, 用纯净水稀释到1.0 mL, 用自动顶空进样器进样于气相色谱上测定, 方法的检出限为0.05 μg/L.
表 1 储备液用水的化学成分Table Supplementary Table Composition of water prepared solution
2. 实验结果与讨论
(1) 零价铁(20~40目) 降解四氯化碳.图 1a是以四氯化碳为研究对象的批实验结果, 四氯化碳初始质量浓度为1 844 μg/L, 从图中可以看到, 随着实验的进行原溶液的质量浓度基本保持不变.当t=71 h时, 测定低于检出限0.05 μg/L, 该点不作为线性回归点.相对质量浓度的对数值对时间作图[9], 进行回归, 其r2为0.993 2表明反应是准一级反应.回归方程: y=-0.025 6x+0.020 8, 反应速率常数为: k=2.303×k′=0.058 96 h-1, t1/2=ln 2/k=11.76 h.通过对三氯甲烷的检测发现, 三氯甲烷质量浓度逐渐上升, 而通过对摩尔数的比较, 与四氯化碳的减少又不是1∶1的关系, 说明除三氯甲烷外还有其他类型的降解产物如二氯甲烷等生成. (2) 零价铁(60~80目) 降解四氯乙烯.图 1b是初始质量浓度为3 225 μg/L的四氯乙烯, 通过在反应过程当中四氯乙烯和三氯乙烯的测定, 四氯乙烯逐渐减少, 120 h时还有662 μg/L的四氯乙烯.原溶液中有14.5~15.1 μg/L的三氯乙烯, 属于溶液配置时四氯乙烯不纯带入的, 但在反应过程中质量浓度基本不变, 说明四氯乙烯的还原性脱氯过程可能不是逐级进行的, 而是与反应介质一接触就在表面直接脱氯成二氯乙烯或一氯乙烯或乙烯、乙炔等, 或者可能是三氯乙烯一经形成马上降解, 这有待于以后完善测试方法进行中间产物的研究.回归方程为y=-0.004 9 x-0.123 5, k=0.011 h-1, r2=0.910 3, t1/2=36.23 h. (3) 零价铁(20~40目) 降解四氯乙烯.图 1c初始质量浓度为3 225 μg/L的四氯乙烯, 初始质量浓度与图 1b相近但反应介质粒度不同, 本实验中回归方程为: y=-0.002 8 x-0.070 2, k=0.006 4, t1/2=82.44 h, r2=0.953 5.可以看出60~80目的零价铁比20~40目的零价铁反应速率大一倍, 即半衰期短一倍.这是由于随着粒度减小, 比表面积增大, 增加了反应介质与溶液的接触的机会, 反应加快的结果[10]. (4) 零价铁(20~40目) 降解不同起始质量浓度的四氯乙烯(表 2).同一粒度的铁屑(20~40目) 对四氯乙烯的降解作用.当原溶液质量浓度ρ0为292 μg/L时, 速率常数为0.018 4 h-1; 当原溶液质量浓度为2 802 μg/L时, 速率常数为0.006 4 h-1.前者是后者的2.875倍, 但没有线性相关关系.据分析应是由在相对浓的溶液中, 反应介质上反应点位很快被占据而影响反应动力学[11].
图 1 Fe0降解CT, PCE曲线a.CT, 20~40目; b.PCE, 60~80目; c.PCE, 20~40目Fig. 1. Degradation of CT, PCE using Fe0表 2 Fe0 (20~40目) 对不同起始质量浓度四氯乙烯的降解原溶液PCETable Supplementary Table Degradation of different initial concentrations using Fe0 (20~40目)
3. 结论
(1) 零价铁对氯代烃有明显的脱氯作用; (2) 相同氯代程度的烷烃和烯烃, 烷烃的脱氯速度快; (3) 反应符合一级反应动力学方程, 反应是准一级反应; 反应速率受到传质速率即零价铁颗粒比表面积的影响; (4) 零价铁对氯代烃的还原性脱氯是否完全, 中间产物的存在和降解情况还有待于进一步研究.
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图 1 华北克拉通~2.3 Ga地质体分布
底图据Zhao et al.（2005）、Zhai and Santosh（2011）；~2.3 Ga年龄数据见附表1文献.图中简写含义：AL.阿拉善; CD.承德; DF.登封; EH.冀东; ES.胶东; FP.阜平; GY.固阳; HA.怀安; HL.贺兰山; HS.恒山; JN.集宁; LL.吕梁; MY.密云; NH.冀北; QL.千里山; NL.辽北; SJ.吉南; SL.辽南; TH.太华; WD.乌拉山-大青山; WH.五河; WL.辽西; WS.鲁西; WT.五台; XH.宣化; ZT.中条
Fig. 1. The distribution map of ~2.3 Ga geologic bodies in the North China Craton
图 2 华北克拉通中条山地区地质简图(据白瑾等，1997；刘树文等, 2007)
Fig. 2. Geological sketch map of Zhongtiao mountains in the North China Craton (after Bai et al., 1997; Liu et al., 2007)
图 3 横岭关二长花岗岩的野外及显微镜下照片（矿物缩写据沈其韩，2009）
a.二长花岗质片麻岩的野外特征；b.二长花岗质片麻岩的显微镜下特征，单偏光；c.绢云石英片岩的野外特征；d.绢云石英片岩的显微镜下特征，单偏光
Fig. 3. Field and microscopic photographs of the Henglingguan monzogranite (abbreviation of minerals after Shen, 2009)
图 4 横岭关二长花岗岩锆石U⁃Pb年龄谐和图（a）和锆石年龄与εHf(t)关系图（b）
球粒陨石（CHUR）根据Blichert⁃Toft and Albereade（1997）; 亏损地幔（DM）根据Griffin et al.（2000）; 长英质上地壳的计算根据Vervoort et al.（2000）
Fig. 4. U⁃Pb Concordia diagram of zircons from the Henglingguan adamellite (a) and zircon ages vs. εHf(t) (b)
图 5 横岭关二长花岗岩SiO2-K2O（a）和A/CNK-A/NK（b）关系图解
图a据Peccerillo and Taylor（1976）、Middlemost（1985）；图b中A/CNK=Al2O3/(CaO+Na2O+K2O), A/NK=Al2O3/(Na2O+K2O)
Fig. 5. Geochemical diagram of SiO2 vs. K2O (a) and A/CNK vs. A/NK (b) for the Henglingguan monzogranit
图 6 横岭关二长花岗岩球粒陨石标准化稀土元素配分图（a）和原始地幔标准化微量元素蛛网图解（b）（标准化值根据Sun McDonough, 1989）
Fig. 6. Chondrite-normalized REEs (a) and PM-normalized trace elements (b) patterns for the Henglingguan monzogranite (normalization values after Sun McDonough, 1989)
图 7 横岭关二长花岗岩10 000 Ga/Al-TFeO/MgO（a）和SiO2-P2O5（b）判别图
Fig. 7. 10 000 Ga/Al vs. TFeO/MgO (a) and SiO2 vs P2O5 (b) diagram of the Henglingguan monzogranite
图 8 横岭关二长花岗岩Nb-Y（a）和Rb-（Y+Yb）（b）图解（底图据Pearce et al., 1984）
Syn⁃COLG.同碰撞花岗岩; VAG.火山弧花岗岩; WPG.板内花岗岩; ORG.洋脊花岗岩
Fig. 8. Nb vs. Y (a) and Rb vs. (Y+Yb) (b) diagrams of the Henglingguan monzogranite (after Pearce et al., 1984)
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