Composition and provenance analysis of rare-earth elements in the manganese-rich brown layers of the Mendeleev Ridge, Arctic Ocean
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摘要: 北冰洋深海广泛分布的富锰棕色沉积层(棕色层)是海冰、洋流、物源供给等多种因素共同作用的结果，本文基于西北冰洋门捷列夫海岭ARC07-E25岩芯沉积物稀土元素与微量元素含量、颜色反射率参数、粗颗粒组分和无机碳含量的变化特征，对该类沉积层中稀土元素的组成特征、形成机制和物质来源进行了综合分析。结果显示，沉积物稀土元素总含量(∑REE)在122.37×10−6～231.94×10−6之间变化，北美页岩标准化配分模式显示出轻微的中稀土(MREE)富集以及由La、Ce、Nd主导的较强的轻稀土(LREE)优势。沉积物中∑REE随着粗组分颗粒(如冰筏碎屑)的增多而呈现降低趋势，表明门捷列夫海脊沉积物中的稀土元素主要富集在细粒沉积物中。根据∑REE在沉积物中的变化特征将E25岩芯沉积物划分为4种地层，反映出了冰期/间冰期的气候转变过程中温暖条件下形成的棕色层与寒冷条件下形成的浅灰绿色沉积层(灰色层)的岩性旋回中稀土元素组成的差异，由于两种沉积层在形成时受到不同的底层水氧化还原环境的控制，导致了铈(Ce)元素在氧化水体中会由Ce3+氧化为Ce4+并发生沉降，而在还原水体中则由Ce4+还原为Ce3+发生溶解，这一特性使LREE含量产生较大波动，进而影响到∑REE，使之趋于在代表氧化条件的棕色层中升高而在代表还原条件的灰色层中降低。R型因子分析和物质来源判别结果显示，E25岩芯沉积物中稀土元素与亲碎屑元素(Nb、U、Th)有较好的相关性，主要来源于东西伯利亚海和新西伯利亚群岛的近岸侵蚀物质以及勒拿河物质的输入。Abstract: The Mn (manganese)-rich brown layers (brown layers) distribute widely in the Arctic Ocean seafloor which controlled by sea ice, surface currents, material supply and so on. In this study, we investigate the provenance and composition feature of brown layers based on changes of contents on rare earth and trace elements, coarse fraction, inorganic carbon and colour reflectance of core ARC07-E25 retrieved from the Mendeleev Ridge, western Arctic Ocean. Total rare earth elements (∑REE) changes between 122.37×10−6 to 231.94×10−6, the north American Shale normalized records of the sediments generally show enrichment in medium rare earth element (MREE) and light rare earth element (LREE) which dominated by lanthanum (La), cerium (Ce) and neodymium (Nd), respectively. With the increase of coarse fraction, such as ice rafted detritus (IRD), the decrease trend of ∑REE indicates REE mainly enrich in fine grain fraction in the Mendeleev Ridge sediments. The differences of REE contents between brown and gray layers, which are classified in the core based on various characteristics of ∑REE, demonstrate distinct Ce anomalies in the brown layer and grey layer associated with different redox conditions: it will be oxidized from Ce3+ to Ce4+ in oxic brown layers and be reduced from Ce4+ to Ce3+ in gray layers. This behavior favors the large variation of ∑LREE content and affects the ∑REE content in the sediments. Consequently, the ∑REE contents are increasing in the brown layers representing oxidation condition and decreasing in the gray layer representing reduction condition. The results of R-type factor analysis show that the REE in sediments have a good correlation with the detritus elements (Nb, U and Th), and mainly derived from inshore erosion of the East Siberian continental shelf, New Siberian Islands and input of the Lena River.
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图 1 北冰洋海底及周边大陆地形地貌
图中红色六角星代表本文研究站位；浅色半透明区域为北冰洋周边晚更新世主要冰盖的推测位范围[9-10]；红色箭头为洋流移动方向；图中涉及到的洋流如下，TPD：穿极流；BG：波弗特环流。底图根据IBCAO Data团队水深模型进行重绘（https://ngdc.noaa.gov/mgg/bathymetry/arctic/arctic.html）
Fig. 1 Topographical and geomorphic of the Arctic Ocean seafloor and surrounding continents
The red hexagonal star represents the research station of this paper. Light-colored semi-transparent area is the potential range of the main ice sheets around the Arctic Ocean in the late Pleistocene[9-10]. The red arrow shows the direction of surface current movement. The ocean currents involved in the figure are as follows: TPD: Trans Polar Drift; BG: Beaufort Gyre. According to IBCAO reproduction Data team depth model redraw (https://ngdc.noaa.gov/mgg/bathymetry/arctic/arctic.html)
图 2 E25岩芯岩性描述、颜色反射率参数以及Mn含量的分布
Fig. 2 Lithology description, color reflectance and distribution of Mn content in Core E25
图 3 ∑REE与IRD含量（a）和∑REE与Ce含量（b）相关关系
Fig. 3 Scatter diagram of correlation of ∑REE and IRD content (a), and ∑REE and Ce content (b)
图 4 稀土元素相关要素、部分氧化还原敏感元素以及IRD含量对比
深色区域为识别出的棕色层，白色区域为灰色层，NASC为北美页岩标准化
Fig. 4 Comparison of rare-earth elements, some redox sensitive elements and IRD content
The dark areas are the identified brown layers, light areas indicate gray layers, and the NASC is normalization by North American Shale Composite
图 5 E25岩芯中粉白层的划分
深色区域为识别出的棕色层，白色区域为灰色层，黑色加粗线条为识别出的粉白层并逐层以PWL1−PWL5标识
Fig. 5 Classification of pink-white layers in Core E25
The dark area is the identified brown layer, light areas indicate gray layers, and the black thick lines recognize as pink-white layers marked by PWL1−PWL5
图 6 经北美页岩标准化后的勒拿河、雅拿河、麦肯锡河河口悬浮体[46-47]和拉普捷夫海、东西伯利亚海表层沉积物[29]稀土元素配分模式图（a）；E25站位代表性棕色层与灰色层的北美页岩标准化稀土元素配分模式图（b）
带深度橙色线为棕色层各层位稀土元素配分模式曲线；带深度浅蓝色线为灰色层各层位稀土元素配分模式曲线
Fig. 6 Rare-earth distribution pattern of suspension matters in the estuaries of the Lena, Yana and Mackenzie rivers[46-47] and surface sediments in the Laptev Sea and East Siberian Sea[29] (a), and pattern of rare earth elements in representative brown and gray layers of Core E25, each data has normalized by NASC (b)
Orange lines with depth indicate curves of rare earth elements in brown layesr; blue lines with depth indicate curves of rare earth elements in gray layer
图 7 对E25岩芯沉积物中主要化学元素组成的R型因子分析
I.与氧化还原环境相关的元素；II.与陆源碎屑输入相关的元素；III.与细组分及再搬运有关的元素；IV.与粗组分及重矿物相关的元素；粗组分大于63 μm，细组分小于63 μm
Fig. 7 R-type factor analysis of major elements in Core E25 sediments
I. Elements related to the redox environment; II. elements related to terrigenous detritus input; III. elements related to fine size composition and resuspension; IV. elements related to coarse grains and heavy minerals; coarse component >63 μm, fine component <63 μm
表 1 北冰洋部分海域和主要河流沉积物中平均稀土元素含量（10−6）
Tab. 1 Average rare earth element content (10−6) in sediments of some sea areas and major rivers in the Arctic Ocean
元素 勒拿河（SPM）[45] 拉普捷夫海（SS）[29] 东西伯利亚海（SS）[30] 麦肯锡河（SPM）[32, 46] E25（ACC） 西部 东部 La 43.20 45.50 37.30 24.40 32.10 37.74 Ce 94.80 90.10 76.60 52.20 62.08 81.09 Pr 10.08 9.95 8.18 6.05 7.46 8.95 Nd 36.90 36.60 30.20 23.30 28.47 33.83 Sm 6.58 6.29 5.94 4.80 5.51 6.39 Eu 1.49 1.42 1.19 1.00 1.14 1.48 Gd 6.21 5.64 4.94 4.25 4.86 5.70 Tb 0.81 0.83 0.76 0.61 0.75 0.94 Dy 4.50 4.39 4.08 3.35 4.62 5.57 Ho 0.85 0.83 0.79 0.67 0.95 1.06 Er 2.54 2.48 2.13 1.86 2.71 3.10 Tm 0.32 0.34 0.33 0.27 N.D. 0.49 Yb 2.47 2.35 2.23 1.75 2.60 3.09 Lu 0.32 0.34 0.32 0.25 0.41 0.49 ∑REE 211.07 207.06 174.99 124.76 153.65 189.92 注：SS表示表层沉积物；ACC表示平均含量；SPM表示悬浮体；N.D.表示无数据。 
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表 2 旋转后的变量载荷矩阵及各因子方差
Tab. 2 Rotated factor matrix and variance contribution of each factor
变量 因子1 因子2 因子3 因子4 方差/% 28.79 22.33 18.97 16.71 Mg/Al 0.959 0.143 –0.089 0.153 Mn/Al 0.958 0.145 –0.091 0.155 Mo/Al 0.941 0.094 –0.131 0.193 Ni/Al 0.870 0.397 0.102 0.046 Co/Al 0.798 0.486 0.119 0.094 Cd/Al 0.796 0.293 0.001 0.387 Sr/Al 0.658 0.177 –0.294 0.547 Nb/Al 0.194 0.872 –0.279 –0.068 Ce/Al 0.364 0.846 0.097 0.112 REE/Al 0.432 0.817 0.031 0.268 Th/Al 0.091 0.812 0.408 0.222 U/Al 0.341 0.685 –0.016 0.514 Ti/Al 0.190 0.621 –0.581 –0.161 Sc/Al 0.099 0.015 0.860 –0.178 Rb/Al –0.359 0.054 0.840 –0.008 Li/Al 0.081 0.229 0.776 –0.162 Zr/Al 0.012 0.383 –0.694 0.489 Hf/Al 0.010 0.475 –0.594 0.520 Ca/Al 0.303 0.204 0.153 0.818 粗组分(粒径>63 μm) 0.230 0.020 –0.413 0.806 细组分(<63 μm) –0.230 –0.020 0.413 –0.806 注：较为显著载荷用（大于0.3）加粗数值进行标识。
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