Atomic and Macro-scale Studies of Surface Processes: Towards a Mechanistic Understanding of Surface Reactivity and Radionuclide Binding Mechanisms

在这个项目中，我们寻求在地质处置设施(GDF)中可能存在的条件下，发展对放射性核素(RN)与矿物表面相互作用的机械理解。本建议描述了对选定的关键表面进行的综合实验和多尺度模拟研究，旨在解决以下基本问题：(I)工程屏障系统(EBS)中候选材料的表面在典型处置环境中的行为；以及(Ii)任何改变过程对RN/表面相互作用的影响。至关重要的是，我们的方法代表了基础性的科学研究，将提供对关键RN延迟过程的机械理解，模拟候选EBS和自然表面上的一系列关闭后RN延迟场景。这种方法寻求开发一种可转移到其他材料和系统的方法。这种可转让的方法支持目前英国处置方案的通用阶段，以便随着英国地质概念的进展，所开发的方法可以用于使用其他感兴趣的RN对其他材料进行实验。它允许我们进行关键的实验，并用机械的预测方法来支持这些实验。通过量化反应的能量和动力学，我们将创建一个预测工具，用于开发和修订更准确的现场规模计算模型。该提案汇集了一个新的跨学科协作团队，具有一系列互补的专业知识，能够采取整体方法来解决这个复杂和具有挑战性的问题。将应用先进的原位表面敏感实验技术，并开发适用于超碱性和放射性的实验技术。一个关键的组成部分是在真实的RN材料上工作，为模型开发提供准确和明确的数据。这项工作将为监管机构提供信息，对新的GDF安全案例的发展产生深远影响，并在更广泛的科学背景下产生影响。

In this programme we seek to develop a mechanistic understanding of radionuclide (RN) interactions with mineral surfaces, under conditions likely to exist in a geological disposal facility (GDF). This proposal describes integrated experimental and multi-scale modelling studies on selected key surfaces which are designed to address fundamental questions on: (i) how the surfaces of candidate materials in an engineered barrier system (EBS) behave in a typical disposal environment; and (ii) the effect of any alteration processes on RN/surface interactions. Crucially, our approach represents fundamental, underpinning scientific research that will provide mechanistic understanding of key RN retardation processes, simulating a range of post-closure RN retardation scenarios on to candidate EBS and natural surfaces. This approach seeks to develop a methodology that is transferrable to other materials and systems. Such a transferrable, approach supports the current generic stage of the UK disposal programme so that methods developed can be used to perform experiments on other materials using other RNs of interest as the UK geological concept progresses. It allows us to perform key experiments and underpin these with mechanistic prediction approaches. By quantifying the energetic and kinetics of reactions we will create a predictive tool for use in developing and revising more accurate field-scale computational models.The proposal brings together a new, interdisciplinary collaborative team with a range of complementary expertise capable of taking a holistic approach to this complex and challenging issue. Advanced, in-situ surface sensitive experimental techniques will be applied, and developed for hyper-alkaline and radioactive applicability. A key component is to work on real RN materials to provide accurate and unambiguous data for model development. This work will inform regulatory bodies, have a profound impact on the development of the new GDF safety case, and has implications in a wider scientific context.