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辐照后矿物反应性变化差异的直接实验证据:方解石和石英的案例

Direct Experimental Evidence for Differing Reactivity Alterations of Minerals following Irradiation: The Case of Calcite and Quartz.

作者信息

Pignatelli Isabella, Kumar Aditya, Field Kevin G, Wang Bu, Yu Yingtian, Le Pape Yann, Bauchy Mathieu, Sant Gaurav

机构信息

Laboratory for the Chemistry of Construction Materials (LC2), Department of Civil and Environmental Engineering, University of California, Los Angeles, CA 90095.

Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37861.

出版信息

Sci Rep. 2016 Jan 29;6:20155. doi: 10.1038/srep20155.

Abstract

Concrete, used in the construction of nuclear power plants (NPPs), may be exposed to radiation emanating from the reactor core. Until recently, concrete has been assumed immune to radiation exposure. Direct evidence acquired on Ar(+)-ion irradiated calcite and quartz indicates, on the contrary, that, such minerals, which constitute aggregates in concrete, may be significantly altered by irradiation. More specifically, while quartz undergoes disordering of its atomic structure resulting in a near complete lack of periodicity, calcite only experiences random rotations, and distortions of its carbonate groups. As a result, irradiated quartz shows a reduction in density of around 15%, and an increase in chemical reactivity, described by its dissolution rate, similar to a glassy silica. Calcite however, shows little change in dissolution rate - although its density noted to reduce by ≈9%. These differences are correlated with the nature of bonds in these minerals, i.e., being dominantly ionic or covalent, and the rigidity of the mineral's atomic network that is characterized by the number of topological constraints (nc) that are imposed on the atoms in the network. The outcomes have major implications on the durability of concrete structural elements formed with calcite or quartz bearing aggregates in nuclear power plants.

摘要

用于核电站建设的混凝土可能会受到反应堆堆芯发出的辐射。直到最近,人们还认为混凝土对辐射具有免疫能力。然而,对氩离子辐照方解石和石英获得的直接证据表明,构成混凝土骨料的此类矿物可能会因辐照而发生显著变化。更具体地说,石英的原子结构会发生无序化,导致几乎完全缺乏周期性,而方解石仅会经历随机旋转以及其碳酸根基团的扭曲。结果,辐照后的石英密度降低约15%,其化学反应活性(以溶解速率来描述)增加,类似于玻璃态二氧化硅。然而,方解石的溶解速率变化很小——尽管其密度据观察降低了约9%。这些差异与这些矿物中的键的性质有关,即主要是离子键还是共价键,以及矿物原子网络的刚性,这由施加在网络中原子上的拓扑约束数量(nc)来表征。这些结果对核电站中由含方解石或石英骨料形成的混凝土结构元件的耐久性具有重大影响。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/59f1/4731743/e263a212b464/srep20155-f1.jpg

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