Research Progress on the Geological Application of a Flow-Through Time-Resolved Analysis System
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摘要:
流通式-时间分辨分析系统(简称FT-TRA)是二十一世纪初新发展起来的一种快速反应(溶解)-在线分析系统，由淋洗液混合单元、反应单元与分析单元组成，核心功能是通过特定流动相淋洗样品池中的微量样品，分离或去除样品中的特定组分，并监测样品不同元素和矿物组分的出溶特征，实现高分辨的在线过程分析。本文综述了FT-TRA系统的技术原理与软硬件组成、实验方法与操作要点及地质应用发展过程，重点对该系统在地质应用过程中出现的争议点进行阐释与分析，并基于其发展现状展望其未来发展方向与潜力。FT-TRA系统目前主要的地质应用包括古海洋学与古环境学研究代用指标的验证(如有孔虫、介形虫淋洗)、矿物溶解过程与反应动力学研究、环境样品的元素相态分析等。FT-TRA系统以溶解并提取有孔虫/介形虫壳体的元素组成信号作为还原古海洋指标的重要手段，与传统批处理法相比，该方法被认为具有实时监测清洁程度、降低损失率并实现差异溶解的优势，能够获取更精细的壳体化学组成信息；测试矿物溶解态与溶解参数也是FT-TRA系统的重要功能之一，该系统的实验室模拟能够与模型结合探究不同类型矿物在稳态下的溶解动力学，为研究矿物在自然状态下的溶解过程提供启示；近些年来该系统还逐渐被用于矿物反应性测试，其中将气相CO2作为淋滤液与矿物反应的研究可能在全球变暖及CO2的人工捕捉课题上具有潜在应用价值。FT-TRA系统运行中涉及的不同组分的溶解机制是其应用过程中亟待解决的重要问题，进一步完善其溶解动力学原理必然将为该系统的未来发展提供更多如多类型地质样品溶解、矿物的模拟合成等新思路。
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关键词:
- 流通式-时间分辨分析系统(FT-TRA) /
- 在线地球化学分析 /
- 地质应用 /
- 环境研究
Abstract:FT-TRA is a rapid reaction (dissolution)-on-line analysis system newly developed in the early 21st century. It consists of an eluent mixing unit, a reaction unit and an analysis unit. Its core function is to wash trace samples in the sample reactor with a specific mobile phase, separate or remove specific components in the sample, and monitor the exsolution characteristics of different elements and mineral components of the sample to achieve high resolution online process analysis. In this article, the technical principle, hardware and software composition, experimental method, operation key points and geological application development process of the FT-TRA system are reviewed. The controversial points in the geological application of the system are explained and analyzed, and its future development direction and potential are forecasted based on its development status. At present, the main geological applications of this system include the verification of proxy indicators for paleoceanography and paleo-environment research (such as foraminifera and ostracod leaching), the study of the mineral dissolution process and reaction kinetics, and the analysis of the elemental phase of environmental samples. The dissolution mechanism of different components involved in the operation of the FT-TRA system is an important problem to be solved in its application process. Further improvement of its dissolution dynamics principle will inevitably provide more new ideas for the future development of the system, such as multi-type geological sample dissolution and mineral simulation synthesis. The BRIEF REPORT is available for this paper at
http://www.ykcs.ac.cn/en/article/doi/10.15898/j.ykcs.202304130048 . -
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表 1 FT-TRA系统应用实例总结
Table 1. Summary of FT-TRA system application examples
FT-TRA
应用领域文献来源 研究方法 研究指标 研究亮点 对于FT-TRA系统的意义 以有孔虫壳体成分为指标的古海洋学研究 Haley等
(2002)FT-TRA 浮游有孔虫壳体REEs、Mg、Sr、Cd、Ba、Mn、Mg/Ca、Sr/Ca 提出FT-TRA系统作为一种新的清洗溶解有孔虫壳体的技术手段 FT-TRA系统的设计与最初应用 Benway等
(2003)FT-TRA 浮游有孔虫壳体Mg/Ca 首次评估该系统提取有孔虫壳体Mg/Ca作为还原古海水表层温度指标的可行性 首次提出FT-TRA系统可根据溶解度差异提取不同成因方解石的化学信号 Klinkhammer等 (2005) FT-TRA 浮游有孔虫壳体Mg/Ca 进一步提出采用在FT-TRA系统中溶解最敏感的方解石部分作为反映表层海水温度的准确值 实现了系统自动化运行；肯定了前处理/清洗过程对于FT-TRA系统提取有孔虫Mg/Ca的非必要性 Haley等
(2005)FT-TRA 底栖及浮游有孔虫壳体REEs 运用FT-TRA系统分析底栖及浮游有孔虫壳体中的REEs作为古环境指标的潜力 / Hoogakker等 (2009) FT-TRA、
电子探针、
传统批次
溶解法浮游有孔虫壳体Mg/Ca 对比高盐度与正常盐度环境中的浮游有孔虫壳体Mg/Ca，证明盐度高低不会影响有孔虫壳体Mg/Ca，变化是由次生生长导致 首次质疑FT-TRA系统可根据溶解度差异提取生物方解石的观点，但提出可通过Mg/Ca斜率变化进行判断 Klinkhammer等 (2009) FT-TRA 有孔虫壳体Mn/Ca 测定钻孔中不同种属有孔虫壳体Mn/Ca在过去3万年间的变化趋势，得出陆源输入改变、表层生产力改变等结论 / Sadekov等
(2010)FT-TRA、
LA-ICP-MS有孔虫壳体Mg/Ca 针对部分溶解对有孔虫壳体Mg/Ca的影响作了针对性研究 提出有孔虫壳体在FT-TRA系统内部的溶解仅是由外至内进行，并不能提取特定组分方解石 Torres等
(2010)FT-TRA 有孔虫壳体Mg/Ca、Ba/Ca、
Sr/Ca、Mn/Ca测定受次生矿化影响的有孔虫的El/Ca，并结合C/O同位素识别其是否生长在甲烷泄露区 / Boussetta等
(2011)FT-ICP-AES、SEM、XRD 浮游有孔虫壳体Mg/Ca 对地中海钻孔浮游有孔虫Mg/Ca进行研究，证明地中海有孔虫Mg/Ca高于开阔海洋不是由于盐度效应，而是与成岩作用有关 提出FT-TRA系统并没有分离出次生方解石的效果 Haarmann等 (2011) 离线FT-TRA 清洗有孔虫壳体 使用FT-TRA系统清洗样品以防止壳体损失，用于测试单个有孔虫壳体的Mg/Ca变化探究季节温度变化 / Kraft等
(2013)FT-TRA、
传统批次
溶解法有孔虫壳体Al/Ca、Mn/Ca和Nd 同位素组成 详细比较了手动批次清洗和 FT-TRA 清洗有孔虫壳体的效果，证明两者清洗效率相同且批次清洗法对于Nd的重吸附效应更小 认为FT-TRA系统清洗有孔虫并不具备优势 Mckay等
(2015)SIMS、FT-ICP-OES 底栖有孔虫壳体Mn/Ca 评估底栖有孔虫壳体Mn/Ca作为记录东北大西洋低纬度上升流系统底层水氧化还原条件变化的替代物的潜力 / 矿物溶解动力学研究 de Baere等
(2015)FT-TRA 镁橄榄石溶解
参数以镁橄榄石为例，探索FT-TRA在恒定和瞬态洗脱条件下测量矿物溶解速率、确定溶解参数和溶解化学计量学的适用性 首次将FT-TRA系统应用于矿物溶解动力学领域 de Baere等
(2016)FT-TRA、孔隙尺度建模 镁橄榄石、
方解石溶解态对镁橄榄石和方解石的溶解态进行了经验测定表明FT-TRA系统能够判断矿物溶解态 提出方解石在系统内部溶解是受转运控制，首次从理论上反驳FT-TRA系统进行差异溶解的能力 矿物反应性研究 Power等
(2020)FT-TRA 尾矿与CO2的反应性 使用与CO2气体达到平衡的NaCl溶液作为洗脱液，在FT-TRA系统中测试尾矿与CO2的反应性 FT-TRA系统首次运用于矿物反应性研究；首次将气相作为系统洗脱液组分 以介形虫壳体成分为指标的古海洋学研究 Börner等
(2017)FT-TRA、
LA-ICP-MS介形虫壳体El/Ca 与LA-ICP-MS的测试结果对照，探究FT-TRA提取介形虫壳体环境信号的潜力 首次根据FT-TRA系统由外至内的溶解特性进行介形虫壳体研究 Rodríguez等 (2021) FT-TRA、
电子探针介形虫壳体微量元素 探究微量元素在介形虫壳体内的分布，评价其作为古海洋学指标的潜在价值 / 
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