Multiscale Chemistry of U, Np, and Pu Under Acidic and Basic Conditions

该奖项是根据2009年美国复苏和再投资法案（公法111-5）资助的。无机，生物无机和有机化学计划支持博士的努力。克拉克的华盛顿州立大学的合理设计的分离和废物储存战略的铀，镎，钚复合物使用多尺度计算化学方法。 核裂变产物的储存和分离是一个首要问题，对环境修复、美国国防和国内能源技术产生影响。 裂变产物的安全和有效处理要求详细了解它们在各种环境条件（例如pH值）下的化学行为。 特别是，在III-VII氧化态的锕系元素的行为在多个长度和时间尺度的理解是必要的。 这种多尺度行为的表征需要在实验能力方面取得重大进展，因此，严格的理论描述，其预测能力可以指导未来的研究和系统设计，具有重要价值。 目前，关于锕系元素溶液的分级凝聚相顺序的信息很少，这阻碍了核燃料循环中可以利用其在各种pH制度下的反应性的新技术。 该项目利用最先进的密度泛函理论，经典模拟和从头算分子动力学相结合，在极端pH条件下研究锕系元素（铀，镎和钚）。 这些数据提供了深入了解酸/碱连接，抗衡离子的影响，溶剂化特性，这些锕系元素的反应性。 为了简化锕系元素化学的计算工作并加强大学的基础设施，克拉克教授建立了WSU计算锕系元素和核科学数据库，这是一个数据库和她所在小组开发的新计算工具。 这项工作的影响将通过对研究生、本科生和高中生进行核科学方面的培训得到进一步加强，因为这些领域对美国的专业知识有很大的需求。 克拉克教授还与爱达荷州的莫斯科高中的合作者合作，将核科学教育和计算化学实验扩展到高中生。

This award is funded under the American Recovery and Reinvestment Act of 2009 (Public Law 111-5). The Inorganic, Bioinorganic, and Organometallic Chemistry Program supports the efforts of Dr. Aurora E. Clark of Washington State University for the rational design of separation and waste storage strategies of uranium, neptunium, and plutonium complexes using multi-scale computational chemistry methodologies. The storage and separations of nuclear fission products is an overarching problem with implications for environmental remediation, US defense, and domestic energy technologies. The safe and effective treatment of fission products mandates a detailed understanding of their chemical behavior under a variety of environmental conditions (e.g. pH). In particular, an understanding of the behavior of actinides in the III-VII oxidation states across multiple length and time scales is needed. Characterization of this multiscale behavior requires major advancements in experimental capabilities thus, rigorous theoretical descriptions, whose predictive capability can guide future studies and system design, are of great value. Currently, there is little information regarding the hierarchical condensed phase order of actinide solutions and this hinders new technologies within the nuclear fuel cycle that can capitalize upon their reactivity under various pH regimes. This project utilizes a combination of state-of-the-art density functional theory, classical simulations, and ab-initio molecular dynamics to examine actinides (uranium, neptunium and plutonium ) under extreme pH conditions. This data provides insights into acid/base ligation, counter ions effects, solvation properties, and reactivities of these actinides. To streamline computational efforts in actinide chemistry and to enhance the University's infrastructure, Professor Clark has established the WSU Computational Actinide and Nuclear Science database, a repository for the data and new computational tools developed within her group. The impact of this work will be further enhanced through the training of post-graduate, undergraduate and high school students in nuclear science where there is large demand and need for US expertise. Professor Clark also works with collaborators at Moscow High School in Idaho to extend nuclear science education and computational chemistry experiments to high school students.