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The impact of cyclical, multi-decadal to centennial climate variability on arsenic sequestration in lacustrine sediments
Palaeogeography, Palaeoclimatology, Palaeoecology ( IF 2.6 ) Pub Date : 2020-12-24 , DOI: 10.1016/j.palaeo.2020.110189
B.R.B. Gregory , R.T. Patterson , J.M. Galloway , E.G. Reinhardt

Examining paleoclimate-driven changes of elemental contaminants, such as Arsenic (As), increases the understanding of the mobility and fate of elements under a warming climate scenario. To characterize the variability in As sequestration in the sediments of a freshwater system in response to decadal- to centennial-scale climate oscillations, a freeze-core (CON01) was recovered from Control Lake, Northwest Territories. Radiocarbon dating of 13 bulk-organic samples provided temporal reference to core depth. Sediment geochemistry was determined using Itrax X-ray fluorescence core-scanning (Itrax-XRF). Elemental concentrations were measured on a sub-set of samples using ICP-MS after multi-acid (MA) digestion to assess the accuracy of Itrax-XRF results through a multivariate log-ratio (MLC) calibration. Comparison of Itrax-XRF to ICP-MS using the MLC in ItraXelerate software show Pearson's R2 values >0.75, with the exception of As (R2 = 0.44). MLC-calibrated Itrax-XRF elemental data were centered log-ratio (CLR) transformed to eliminate issues related to data closure. During the ca. 3300-yr sedimentary record, moderate-strength negative correlations between AsCLR and KCLR (Spearman's ρ = −0.38, p-value < 0.001, n = 785), and AsCLR and TiCLR, (Spearman's ρ = −0.52, p-value < 0.001, n = 785) suggest that As is primarily sequestered in sediments during intervals of warmer temperatures and higher productivity. Proxies for sediment particle size (TiCLR, KCLR) and As concentration (AsCLR) were examined for response to quasi-periodic climate oscillations using spectral analysis. Significant periodicities were observed with approximately 4–13, 30–60, 90–120, and 160–280 yr periods in TiCLR, KCLR, and AsCLR records. These frequencies are interpreted as corresponding to the North Atlantic Oscillation and/or 8–14-yr Schwabe sunspot cycles, 30–60-yr Pacific Decadal Oscillation, and centennial-scale solar cycles (e.g., 90-yr Gleissberg cycle; 205-yr Suess cycle). Coeval occurrence of these periodicities revealed through wavelet analysis of Control Lake geochemistry data suggests that these climate cycles only impact Control Lake when they occur concurrently.



中文翻译:

周期性,十年到百年的气候变化对湖相沉积物中砷螯合的影响

研究古气候驱动的元素污染物(例如砷)的变化,可以增加对气候变暖情况下元素的迁移率和命运的了解。为了表征淡水系统沉积物中As的固存变化,以响应年代际到百年尺度的气候振荡,从西北地区的Control Lake中回收了一个冰冻核心(CON01)。13个大有机样品的放射性碳测年为岩心深度提供了时间参考。使用Itrax X射线荧光岩心扫描(Itrax-XRF)确定了沉积物地球化学。多酸(MA)消化后,使用ICP-MS对子集中的样品进行元素浓度测量,以通过多元对数比(MLC)校准评估Itrax-XRF结果的准确性。2个值> 0.75,但As(R 2  = 0.44)除外。对MLC校准的Itrax-XRF元素数据进行中心对数比(CLR)转换,以消除与数据关闭相关的问题。在ca。3300年沉积记录,As CLR和K CLR(Spearmanρ= −0.38,p值<  0.001,n =  785)和As CLR和Ti CLR之间(Spearmanρ= −0.52,p)中强度负相关-值<  0.001,n =  785)表明,在温度升高和生产率较高的时间间隔内,砷主要被隔离在沉积物中。沉积物粒度的代理(Ti CLR,K使用光谱分析检查了CLR和As浓度(As CLR)对准周期性气候振荡的响应。在Ti CLR,K CLR和As CLR记录中,观察到明显的周期,周期约为4-13、30-60、90-120和160-280年。这些频率被解释为对应于北大西洋涛动和/或8-14年的Schwabe太阳黑子周期,30-60年的太平洋年代际涛动和百年尺度的太阳周期(例如90年的Gleissberg周期; 205年的Suess周期)。通过对Control Lake地球化学数据进行小波分析揭示的这些周期的同时发生表明,这些气候周期仅在同时发生时才影响Control Lake。

更新日期:2021-01-11
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