Passivation by Ultimate Ligand-Surface Activation Rationalized by NMR

通过 NMR 合理化最终配体表面活化的钝化

• 批准号: EP/Y023781/1
• 负责人: Ran Abutbul
• 金额: $ 25.55万
• 依托单位: University of Manchester
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2023
• 资助国家: 英国
• 起止时间: 2023 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FY023781%2F1
• 关键词: Passivation; Ultimate; Ligand; Surface; Activation

Dynamic nuclear polarization (DNP)-enhanced solid-state NMR spectroscopy has proven in recent years to be a powerful technique for the characterization of challenging solid materials and their interfaces. Substantially increased sensitivity of NMR experiments becomes possible through DNP, where the large polarization of unpaired electron spins is transferred to the desired nuclei. For inorganic nanoparticles (NPs) surrounded with sources of unpaired electrons, known as polarizing agents, polarization transfers are mainly to their surfaces. Therefore, surface selectivity, in addition to increased sensitivity, is achieved and this can be used to study the surface chemistry of NPs. The capping of NPs with inorganic ligands (ILs), rather than conventional organic ligands, has been proposed to improve charge carrier lifetime in solids composed of assemblies of NPs, usually termed colloidal quantum dot solids (CQDSs). Substantial increases in transport properties and method versatility have led researchers to explore many types of IL to improve the mobility of charge carriers. However, gaining a detailed understanding of the surface chemistry of IL-capped NPs remains a challenging task and is thus still lacking. This project aims to correlate the surface chemistry and interfaces of ligand-capped CQDSs with their performance. Surface characterization of IL-capped NPs will be carried out by advanced DNP-enhanced solid-state NMR spectroscopy. Photoluminescence and conductivity measurements will indicate the effect on charge carrier lifetimes in assembled CQDSs. Therefore, the proposed research will result in a breakthrough atomic-level understanding of how IL choice and surface chemistry influences charge transport and will lead to a generalized method for achieving single-crystal-grade mobility values in CQDSs.

近年来，动态核极化 (DNP) 增强固态核磁共振波谱已被证明是一种用于表征具有挑战性的固体材料及其界面的强大技术。通过 DNP 可以显着提高 NMR 实验的灵敏度，其中不成对电子自旋的大极化被转移到所需的原子核。对于被不成对电子源（称为极化剂）包围的无机纳米颗粒（NP）来说，极化转移主要发生在其表面。因此，除了提高灵敏度之外，还实现了表面选择性，这可用于研究纳米颗粒的表面化学。已提出用无机配体（IL）而不是传统的有机配体对纳米粒子进行封端，以提高由纳米粒子组装体组成的固体（通常称为胶体量子点固体（CQDS））中的载流子寿命。传输特性和方法多功能性的大幅提高促使研究人员探索多种类型的离子液体以提高电荷载流子的迁移率。然而，详细了解 IL 封端的纳米粒子的表面化学仍然是一项具有挑战性的任务，因此仍然缺乏。该项目旨在将配体封端的 CQDS 的表面化学和界面与其性能相关联。 IL 封端的纳米粒子的表面表征将通过先进的 DNP 增强固态核磁共振波谱进行。光致发光和电导率测量将表明对组装的 CQDS 中载流子寿命的影响。因此，拟议的研究将在原子水平上对 IL 选择和表面化学如何影响电荷传输产生突破性的理解，并将导致在 CQDS 中实现单晶级迁移率值的通用方法。