Arctic Neodymium Isotope Traces for the Atlantic Water Layer at the Chukchi Continental Margin
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摘要: 温暖的“大西洋水层”为北冰洋提供了重要的热量来源，是决定其海冰状况、冰架分布及周边冰盖稳定性的关键因素. 通过分析M04孔沉积物中稀土元素（REE）的含量及其配分模式和Fe-Mn氧化物组分的钕同位素组成，探讨了晚更新世以来楚克奇陆架边缘REE的富集机制、εNd示踪水团性质的有效性以及“大西洋水层”的强弱变化. 结果表明，间冰期Fe-Mn氧化物是溶解态REE沉淀的主要载体，但冰期缺少Fe-Mn氧化物的灰色层中也富集了大量的溶解态REE. 同时，Fe-Mn氧化物萃取液中εNd介于-5.50~-8.74之间，呈现出冰期高，间冰期低的特点，有效指示了“大西洋水层”在楚克奇陆架边缘的活动. 在间冰期，“大西洋水层”增强，为陆架输入的Fe2+和Mn2+创造了再氧化的条件；而在冰期，“大西洋水层”几乎退出了楚克奇陆架边缘. 参照现代冰川溶水的化学组成，导致冰期M04孔Fe-Mn氧化物萃取液中REE富集和εNd显著正偏的环境要素，很可能是东西伯利亚冰盖的扩张及其冰下排水，而不是海冰排盐形成的“卤水”. 这些发现进一步揭示了北冰洋REE的富集机制，论证了εNd示踪“大西洋水层”的有效性，并深化了对“大西洋水层”演变规律的认知.Abstract: In the Arctic Ocean, the Atlantic water layer is an essential source of heat that regulates sea ice, ice shelves, and surrounding ice sheets. By analyzing the content and pattern of rare earth elements (REE) and Nd isotopic composition (εNd) in the sediments of Hole M04 and its distribution pattern and Nd isotopic composition of Fe-Mn oxide fraction, this study explores the enrichment mechanism of REE on the edge of Chukchi shelf since Late Pleistocene, the effectiveness of εNd tracer water mass properties, and the strength and weakness of the "Atlantic water layer".The records indicate that Fe-Mn oxides were the primary carriers for dissolved REE during the interglacial period, but a large quantity of dissolved REE was also enriched in the gray layer lacking Fe-Mn oxides. In addition, there is a significant spike of εNd in Fe-Mn oxide leachate during the glacial period and a drop during the interglacial period corresponding to values between -5.50 and -8.74. Therefore, we conclude that the Atlantic water layer strengthened during the interglacial period, which allowed re-oxidation of Fe2+ and Mn2+ input from the shelf, but withdrew almost entirely from the Chukchi continental margin during the glacial period. Similar to the chemical composition of modern glacial meltwater, the development of the East Siberian ice sheet and its subglacial drainage are more likely to lead to the REE enrichment and εNd positive bias in Core M04 Fe-Mn oxide extraction solution than sea ice production brine. These findings further illustrate the process of enrichment of REEs in the Arctic Ocean, demonstrate the effectiveness of εNd as a marker of the Atlantic water layer, and contribute to an understanding of the Atlantic water layer evolution.
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图 1 研究站位及区域概况
红色五角星指示M04孔位置；TPD、BG和ACC及虚线箭头分别代表穿极流、波弗特环流和北冰洋沿岸流；橙色、紫色和黄色实线箭头分别指示大西洋输入流、河流和白令海峡穿越流（Talley，2011）；红色和黄色实线分别指示MIS4和MIS2期东西伯利亚冰盖及其冰架的北部界线（Ye et al., 2019）；椭圆中的数字为不同水体中的εNd（Dahlqvist et al., 2007；Andersson et al., 2008；Porcelli et al., 2009；Zimmermann et al., 2009）；CB、MR、LR和GR分别代表楚克奇盆地、门捷列夫洋脊、罗蒙洛索夫洋脊和盖克尔洋中脊
Fig. 1. Core sites and geographic setting of the study areas
图 2 M04孔沉积地层及元素含量
B1和B2指示富锰褐色层；W3指示富钙白色层；IRD表示冰阀碎屑（Stein et al., 2010）带数字的黑色箭头指示AMS14C年龄，引自Ye et al.（2019），深海氧同位素阶段（MIS）用白色框（间冰期）和黑色框（冰期）表示，灰色条带指示间冰期
Fig. 2. Sedimentary stratigraphy and element contents in Core M04
图 3 Fe-Mn氧化物萃取液中元素含量及钕同位素组成
Fig. 3. Element contents and neodymium isotopic compositions in Fe-Mn oxide leachate
图 4 不同类型载体中稀土元素配分模式
a. M04孔沉积物PAAS标准化REE模式；b. M04孔Fe-Mn氧化物萃取液PAAS标准化REE模式；c. 研究区周围河流、海洋沉积物、M04孔PAAS标准化REE模式（Fagel et al., 2014）；d. 研究区周围铁锰结核、M04孔Fe-Mn氧化物萃取液PAAS标准化REE模式（Winter et al., 1997；Baturin and Dubinchuk, 2011；Kolesnik and Kolesnik, 2015）
Fig. 4. REE distribution patterns in different carriers
图 5 不同类型载体稀土元素斜率和中稀土异常
红色圆点代表M04孔Fe-Mn氧化物萃取液；橙色菱形代表M04孔全样沉积物；其他稀土元素来源引自Parker et al.（2022）和其中的文献
Fig. 5. REE slopes and MREE anomalies in different carriers
图 6 北冰洋表层沉积物中锰含量和εNd分布
锰含量来自全样沉积物，引自Ye et al.（2019）及其中文献；εNd来自Fe-Mn氧化物萃取液，引自Haley et al.（2008）、Haley and Polyak（2013）、Jang et al.（2013）和Meinhardt et al.（2016）
Fig. 6. Distributions of Mn and εNd in the Arctic Ocean surface sediments
图 7 晚更新世以来基于εNd的“大西洋水层”强度变化
门捷列夫洋脊PS72/410-1孔记录引自Jang et al.（2013）；罗蒙诺索夫洋脊PS2185孔记录引自Haley et al.（2007）；231Pa/230Th表示AMOC强度，引自Böhm et al.（2014）；蓝色表示间冰期，黑白条带表示深海氧同位素阶段
Fig. 7. Variations in the Atlantic water layer based on εNd since the Late Pleistocene
表 1 北冰洋周围主要河流流量及钕同位素组成
Table 1. Major river´s discharge and εNd around the Arctic Ocean
主要大洋及河流 流量（Sv） εNd CNd (pM) Nd通量（10-3 mol/s） 弗莱姆海峡输入流 9.5 -9.8 26.4 250.8 巴伦支海输入流 2.3 -10.8 15.5 35.7 白令海峡穿越流 0.8 -5.0 30 24 勒拿河 0.017 -14.2 477~826 8.1~14 麦肯齐河 0.011 -12.9 111 1.2 科雷马河 0.004 -6.0 129 0.5 注：弗莱姆海峡和巴伦支海输入流量引自 Schauer et al.(2002) ，εNd值和CNd引自Andersson et al.(2008) ；太平洋入流水流量引自Roach et al.(1995) ，εNd值和CNd引自Dahlqvist et al.(2007) ；勒拿河、科雷马河、麦肯齐河流量引自Holmes et al.(2002) ; Gordeev(2006)，εNd值和CNd引自Porcelli et al.(2009) ;Zimmermann et al.(2009) 
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表 2 钕同位素测试结果
Table 2. Results of neodymium isotope analysis
深度（cm） 年龄（ka） 143Nd/144Nd 2SE εNd 1 2.32 0.512 261 0.000 007 -7.354 117 9 4.85 0.512 203 0.000 005 -8.489 421 35 13.05 0.512 268 0.000 005 -7.223 421 65 17.32 0.512 357 0.000 004 -5.479 500 105 22.24 0.512 359 0.000 005 -5.450 240 145 27.16 0.512 326 0.000 004 -6.078 363 167 30.38 0.512 190 0.000 006 -8.746 913 185 33.92 0.512 229 0.000 004 -7.974 438 205 37.85 0.512 312 0.000 009 -6.365 115 221 41.00 0.512 346 0.000 004 -5.694 077 241 52.03 0.512 348 0.000 006 -5.664 816 281 58.40 0.512 346 0.000 004 -5.703 830 321 60.21 0.512 359 0.000 005 -5.444 388 401 63.82 0.512 353 0.000 004 -5.551 676 注：单位：南京聚谱检测科技有限公司；测试者：郭燕；测试手段：Nu Plasma Ⅱ MC-ICP-MS；测试精度：0.000 001;误差：2SE（SE表示标准误差）.
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