CAREER: Unveiling the structure and stability of prenucleation clusters and their roles in crystallization pathway and final crystal structure

职业：揭示成核前团簇的结构和稳定性及其在结晶途径和最终晶体结构中的作用

• 批准号: 2338173
• 负责人: John Lee
• 金额: $ 66.02万
• 依托单位: Iowa State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-03-01 至 2029-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2338173&HistoricalAwards=false
• 关键词: CAREER; Unveiling; structure; stability; prenucleation

NON-TECHNICAL SUMMARYFor over a century, scientists have been studying nucleation because it greatly affects various aspects of our lives, such as public health through drug production and dealing with urinary stones, as well as impacting industries like fertilizers and foods. Despite the long history of research, understanding the mechanism and influence of nucleation on crystal structures is still challenging due to the difficulty in characterizing tiny and random phenomena at the sub-nanoscale level. This CAREER award, jointly funded by the Solid State and Materials Chemistry program in NSF’s Division of Materials Research and the Established Program to Stimulate Competitive Research (EPSCoR), aims to figure out how the structure of salt solutions changes as their concentration increases and how this structure affects the final crystal formation. To overcome the challenges, a levitation technique and powerful X-ray and neutron scattering will be combined, collaborating with Argonne National Laboratory and Oak Ridge National Laboratory. The outcomes of this study will significantly enhance our understanding of the complex process of crystallization and its impact on the final crystal structure. This knowledge could benefit industries like pharmaceuticals, fertilizers, and batteries. Throughout the project, a consortium will be formed as an educational platform to promote diversity in the STEM field, educate young scientists and engineers, and share our findings with K-12 students, teachers, and parents in Iowa through existing outreach programs led by Iowa State University.TECHNICAL SUMMARYNucleation dominates the subsequent crystallization, crystal growth, and the structure and properties of final crystals. Recently, nucleation has been reported to occur in multiple steps, forming pre-nucleation clusters (PNCs). It is apparent that PNCs play a critically important role in multi-step nucleation and the final crystal structure, yet their nature is poorly understood. The rationale for the proposed research is that a mechanistic understanding of complex crystallization will likely provide new opportunities to develop a method to control the nucleation and growth of desired crystal phases. For this reason, this CAREER award, jointly funded by the Solid State and Materials Chemistry program in NSF’s Division of Materials Research and the Established Program to Stimulate Competitive Research (EPSCoR), aims to identify the concentration-dependent structural evolution of PNCs in aqueous salt solutions and the influence of solution structure on the crystallization pathways and the final crystal structure. The current experimental obstacles will be overcome by integrating the solution electrostatic levitator (SEL) with synchrotron X-ray scattering at Argonne National Laboratory and neutron scattering at Oak Ridge National Laboratory. The long-term goal of the project is to develop a predictive framework to anticipate and control the multi-pathway and multi-step crystallization in various aqueous solutions to obtain desired microstructures in the final crystal products. The proposed research will lead to a vertical-step advancement toward elucidating the mechanism of complex crystallization in electrolyte solutions and its influence on the final crystal structure.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

非技术总结世纪以来，科学家们一直在研究成核，因为它极大地影响了我们生活的各个方面，例如通过药物生产和处理尿结石的公共卫生，以及影响化肥和食品等行业。 尽管研究历史悠久，但由于难以在亚纳米级表征微小和随机现象，因此了解成核对晶体结构的机制和影响仍然具有挑战性。 该CAREER奖由NSF材料研究部门的固态和材料化学计划以及刺激竞争研究的既定计划（EPSCoR）共同资助，旨在弄清楚盐溶液的结构如何随着其浓度的增加而变化，以及这种结构如何影响最终的晶体形成。 为了克服这些挑战，将与阿贡国家实验室和橡树岭国家实验室合作，将悬浮技术与强大的X射线和中子散射相结合。 这项研究的结果将大大提高我们对结晶过程及其对最终晶体结构的影响的理解。 这些知识可以使制药，化肥和电池等行业受益。 在整个项目过程中，将成立一个联盟作为教育平台，以促进STEM领域的多样性，教育年轻的科学家和工程师，并通过爱荷华州立大学领导的现有推广计划与爱荷华州的K-12学生，教师和家长分享我们的发现。技术总结成核主导了随后的结晶，晶体生长以及最终晶体的结构和性质。 最近，据报道，成核发生在多个步骤中，形成预成核团簇（PNC）。 很明显，PNC在多步成核和最终晶体结构中起着至关重要的作用，但对其性质了解甚少。 提出的研究的基本原理是，复杂结晶的机械理解将可能提供新的机会，开发一种方法来控制所需的晶相的成核和生长。 出于这个原因，这个CAREER奖由NSF材料研究部门的固态和材料化学计划以及刺激竞争研究的既定计划（EPSCoR）共同资助，旨在确定PNC在盐水溶液中的浓度依赖性结构演变以及溶液结构对结晶途径和最终晶体结构的影响。 目前的实验障碍将克服集成的解决方案静电悬浮器（SEL）与同步加速器X射线散射在阿贡国家实验室和中子散射在橡树岭国家实验室。 该项目的长期目标是开发一个预测框架，以预测和控制各种水溶液中的多途径和多步骤结晶，从而在最终晶体产品中获得所需的微观结构。 该研究将有助于阐明电解质溶液中复杂结晶的机理及其对最终晶体结构的影响。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。