Materials World Network (MWN) for Particle-mediated Control Over Crystallization: From the Pre-nucleation Stage to the Final Crystal

用于粒子介导的结晶控制的材料世界网络 (MWN)：从预成核阶段到最终晶体

• 批准号: 238873356
• 负责人: Professor Dr. Helmut Cölfen (†)
• 金额: --
• 依托单位: Arbeitsgruppe Physikalische Chemie (AG Cölfen)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2013
• 资助国家: 德国
• 起止时间: 2012-12-31 至 2016-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/238873356?language=en
• 关键词: Materials; World; Network; MWN; Particle

A Materials World Network (MWN) will be formed to investigate mechanisms of particle-mediated crystallization through which mesocrystals — crystals structured on the mesoscale — are created. In biomineral systems, mes-ocrystal formation is a widespread phenomenon mediated by biomolecules and leading to the hierarchical organization commonly associated with these materials. Our ultimate goal is a mechanistic understanding of this process and a set of principles to guide biomimetic strat-egies to create hierarchically organized materials (e.g. bioceramics, photonic solids, energy harvesting materials). The value added by the international collaboration is that it facilitates this goal by combining expertise in chemistry and growth of mesocrystals with capabilities in high-resolution in situ imaging, measurement of interactions, determination of structure, and modeling and simulation from the atomic to mesoscale. Using the calcium carbonate, iron oxide and calcium-silicate hydrate (C-S-H) systems combined with polymers, the project will pursue three thrusts, structured around the key scientific questions: Thrust 1: The pre-nucleation stage, nucleation of primary nanoparticles and intermediate phases - The nature of pre-nucleation clusters will be determined using ion potential measurements, titration and ultracentrifugation. Their solution interaction dynamics will be probed through liquid cell TEM. Thrust 2: Interactions forces between nanocrystals and organic mediators of mesocrystal formation – The interactions responsible for particle co-orientation and reorientation will be determined through a combination of dynamic force spectroscopy (DFS) and modeling. DFS will provide a direct measure of the free energy of the orientation dependent crystal-crystal and -polymer interactions. Experimental measurements are supported by molecular model-ing, which allows us to determine molecular details of the effective interactions and provides parameters for the phase field calculations in Thrust 3. Thrust 3: Post-nucleation particle ag-gregation and co-orientation – The kinetics of particle aggregation, crystallographic orienta-tions of the aggregating particles as a function of time, and structural evolution of mesocrys-talline aggregates will be investigated by liquid cell TEM and ex situ HRTEM. Emphasis will be placed on distinguishing between oriented attachment and orientation following random aggregation either through whole-particle rotation or atomic-scale ripening. These data will be compared to phase-field models of mesocrystal assembly that utilize the interaction energies determined in Thrust 2.

将形成一个材料世界网络（MWN）来研究粒子介导的结晶机制，通过该机制产生介晶（介观结构的晶体）。在生物矿物系统中，介晶形成是一种由生物分子介导的普遍现象，并导致了介晶的形成。我们的最终目标是对这一过程的机械理解以及指导仿生策略创建分层组织材料的一套原则。 （例如生物陶瓷、光子固体、能量收集材料）国际合作的附加价值在于，它通过将化学和介晶生长方面的专业知识与高分辨率原位成像、相互作用测量、确定等能力相结合，促进了这一目标的实现。该项目将利用碳酸钙、氧化铁和水合硅酸钙 (C-S-H) 系统与聚合物相结合，进行从原子到介观尺度的结构、建模和模拟。围绕关键科学问题构建的主旨：主旨 1：预成核阶段、初级纳米颗粒和中间相的成核 - 预成核簇的性质将通过离子电势测量、滴定和超速离心来确定，它们的溶液相互作用动力学将被确定。通过液体细胞 TEM 进行探测：纳米晶体和介晶形成的有机介体之间的相互作用力——导致粒子的相互作用。共取向和重新取向将通过动态力谱（DFS）和建模的结合来确定，DFS将提供取向依赖的晶体-晶体和聚合物相互作用的自由能的直接测量。实验测量由分子模型支持。 -ing，它使我们能够确定有效相互作用的分子细节，并为推力 3 中的相场计算提供参数。推力 3：成核后粒子聚集和共取向——颗粒聚集的动力学、聚集颗粒的晶体取向随时间的变化以及中晶聚集体的结构演化将通过液体单元 TEM 和异位 HRTEM 进行研究，重点将放在区分上。通过全粒子旋转或原子尺度成熟来确定定向附着和随机聚集后的定向之间的关系。这些数据将与相场模型进行比较。利用推力 2 中确定的相互作用能量的介晶组装。

项目成果

Analytical band centrifugation revisited

• DOI: 10.1007/s00249-018-1315-1
• 发表时间: 2018-10-01
• 期刊: EUROPEAN BIOPHYSICS JOURNAL WITH BIOPHYSICS LETTERS
• 影响因子: 2
• 作者: Schneider, Cornelia M.;Coelfen, Helmut
• 通讯作者: Coelfen, Helmut

Polyaspartic acid facilitates oxolation within iron(iii) oxide pre-nucleation clusters and drives the formation of organic-inorganic composites.

聚天冬氨酸促进氧化铁(iii)预成核簇内的氧化反应并驱动有机-无机复合材料的形成

• DOI: 10.1063/1.4963738
• 发表时间: 2016
• 期刊: The Journal of chemical physics
• 作者: Scheck;Drechsler;Stöckl;Konsek;Schwaderer;Stadler;De Yoreo;Gebauer
• 通讯作者: Gebauer

The Molecular Mechanism of Iron(III) Oxide Nucleation.

• DOI: 10.1021/acs.jpclett.6b01237
• 发表时间: 2016-08
• 期刊: The journal of physical chemistry letters
• 作者: Johanna Scheck;Baohu Wu;M. Drechsler;R. Rosenberg;A. V. Van Driessche;T. Stawski;D. Gebauer