A NEW APPROACH TO EXPERIMENTAL DETERMINATION OF COUPLED SILICATE DISSOLUTION - PRECIPITATION REACTION RATES AT AMBIENT CONDITIONS WITH SI ISOTOPE SPIKES

实验测定耦合硅酸盐溶解的新方法 - 环境条件下使用 SI 同位素尖峰的沉淀反应速率

• 批准号: 1225733
• 负责人: Chen Zhu
• 金额: $ 30万
• 依托单位: Indiana University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-10-01 至 2016-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1225733&HistoricalAwards=false
• 关键词: NEW; APPROACH; EXPERIMENTAL; DETERMINATION; COUPLED

Many of society's urgent environmental concerns and problems, such as global warming and strategies that mitigate it, and the stresses on the Earth's Critical Zone - the thin veneer on the Earth's Crust from vegetation canopy to the soil and groundwater which sustains human life and is where most terrestrial life thrives on Earth - have something to do with the rates of feldspar dissolution. Feldspars are the most abundant minerals in the Earth's crust, comprising of more than 50% of the Crust volume. For the former, one global warming mitigation strategy is geological carbon sequestration, for which CO2 is stored in deep underground geological formations. However, the injected CO2 will acidify the native brine and dissolve feldspars in the reservoirs, which could affect the reservoir quality and the long-term safety of storage. For the latter, the weathering of feldspars as an abundant mineral in the Critical Zone is critical to rates of soil development and the buffer capacity of the Critical Zone to stresses. However, to assess how fast feldspar dissolution or weathering takes place (chemical kinetics), we need to wrestle with one of the fundamental challenges in geochemistry. It has been known for a long time that the laboratory measured dissolution rates of feldspars are two to five orders of magnitude faster than rates estimated from field studies. Without resolving this seemingly intractable obstacle, we cannot quantitatively evaluate a number of environmental and geological processes, such as those mentioned above. This study is designed to test the promising hypothesis that would partly resolve the apparent discrepancy: A large part of the discrepancy between in situ field and laboratory rates results from the coupling of the dissolution and precipitation reaction in the field systems which is absent in most laboratory experiments. Historically, the determination of very slow feldspar dissolution rates in laboratory at ambient temperatures has been problematic. Slow reaction rates mean that solutes may be below analytical detection limits, thus affecting the accuracy of the experiments. Here, the investigator proposes an innovative utilization of newly developed technology - High-Resolution Multi-Collector Inductively-Coupled Plasma Mass Spectrometry - and uses a novel design of stable silicon isotope 'spikes' to overcome these obstacles in order to determine feldspar reaction rates at ambient and near equilibrium conditions, not previously possible. The work will involve cooperation among the investigator at Indiana University and his colleagues at Ben-Gurion University of the Negev in Israel, and at Trent University in Canada. Funding is requested only for the US organization. This study will enhance international and multi-disciplinary collaboration and contribute to the training of a post-doctoral associate and an exchange student from Israel. Te investigator is currently conducting research on the industrial scale CO2 storage project in Norway (the Sleipner project) and will communicate the results from this study to the CO2 storage community and the Critical Zone research community.

社会上许多紧急的环境问题和问题，例如减轻它的全球变暖和策略，以及地球临界区的压力 - 从植被冠层到持续人类生命的土壤和地下水的地壳上的薄贴面，这是大多数地球上的生命 - 在地球上繁荣发展 - 与Feldsparparparparparparparparparpar的释放相处。长石是地壳中最丰富的矿物质，其中超过50％的地壳体积。对于前者而言，一种全球变暖策略是地质碳固存，二氧化碳被存储在深地下地质地层中。但是，注射的二氧化碳将使天然盐水酸酸并溶解在储层中，这可能会影响储层质量和储存的长期安全性。对于后者而言，在临界区域中，长石作为大量矿物的风化对于土壤发育速率和关键区域对压力的缓冲能力至关重要。但是，要评估长石的溶解或风化的速度（化学动力学），我们需要应对地球化学的基本挑战之一。很长一段时间以来，实验室测量的长石的溶解速率比野外研究估计的速率快两到五个数量级。如果不解决这个看似棘手的障碍，我们将无法定量评估许多环境和地质过程，例如上述的环境和地质过程。这项研究旨在检验一个有希望的假设，该假设将部分解决明显的差异：原位场和实验室速率之间的很大一部分是由于大多数实验室实验中不存在的田间系统中溶解和降水反应的耦合而导致的。从历史上看，确定在环境温度下实验室中非常缓慢的长石溶解率是有问题的。缓慢的反应速率意味着溶质可能低于分析检测极限，从而影响实验的准确性。在这里，研究人员提出了新开发的技术的创新利用 - 高分辨率的多组耦合等离子体质谱 - 并使用稳定的硅同位素“尖峰”的新设计来克服这些障碍，以确定在环境和近乎平衡条件下的野性反应速率，而不是以前可能。这项工作将涉及印第安纳大学的调查员与他在以色列内盖夫本·古里安大学以及加拿大特伦特大学的研究人员之间的合作。仅向美国组织要求资金。这项研究将增强国际和多学科的合作，并有助于对以色列的博士后同学和交换学生的培训。 TE研究人员目前正在对挪威工业规模的CO2存储项目（Sleipner Project）进行研究，并将将本研究的结果传达给CO2存储社区和关键区域研究社区。

项目成果

Measuring silicate mineral dissolution rates using Si isotope doping

使用硅同位素掺杂测量硅酸盐矿物溶解速率

• DOI: 10.1016/j.chemgeo.2016.02.027
• 发表时间: 2016
• 期刊: Chemical Geology
• 影响因子: 3.9
• 作者: Zhu, Chen;Liu, Zhaoyun;Zhang, Yilun;Wang, Chao;Scheafer, Augustus;Lu, Peng;Zhang, Guanru;Georg, R. Bastian;Yuan, Hong-lin;Rimstidt, J. Donald
• 通讯作者: Rimstidt, J. Donald

A new approach for measuring dissolution rates of silicate minerals by using silicon isotopes

利用硅同位素测量硅酸盐矿物溶解速率的新方法

• DOI: 10.1016/j.gca.2012.11.022
• 发表时间: 2013
• 期刊: Geochimica et Cosmochimica Acta
• 影响因子: 5
• 作者: Gruber, Chen;Harpaz, Liat;Zhu, Chen;Bullen, Tom D.;Ganor, Jiwchar
• 通讯作者: Ganor, Jiwchar

SUPCRTBL: A revised and extended thermodynamic dataset and software package of SUPCRT92

SUPCRTBL：SUPCRT92 的修订和扩展热力学数据集和软件包

• DOI: 10.1016/j.cageo.2016.02.013
• 发表时间: 2016
• 期刊: Computers & Geosciences
• 影响因子: 4.4
• 作者: Zimmer, Kurt;Zhang, Yilun;Lu, Peng;Chen, Yanyan;Zhang, Guanru;Dalkilic, Mehmet;Zhu, Chen
• 通讯作者: Zhu, Chen

A stable isotope doping method to test the range of applicability of detailed balance

一种稳定同位素掺杂方法测试详细天平的适用范围

• DOI: 10.7185/geochemlet.1608
• 发表时间: 2016
• 期刊: Geochemical Perspectives Letters
• 影响因子: 4.9
• 作者: Liu, Z.;Rimstidt, J.D.;Zhang, Y.;Yuan, H.;Zhu, C.
• 通讯作者: Zhu, C.

Rate equations for sodium catalyzed amorphous silica dissolution

钠催化无定形二氧化硅溶解的速率方程

• DOI: 10.1016/j.gca.2016.09.020
• 发表时间: 2016
• 期刊: Geochimica et Cosmochimica Acta
• 影响因子: 5
• 作者: Rimstidt, J. Donald;Zhang, Yilun;Zhu, Chen
• 通讯作者: Zhu, Chen