Next-generation hyperpolarising agents for NMR Spectroscopy

EPSRC项目相关研究领域：分析科学;碳捕获和储存;催化;功能陶瓷和无机物;石墨烯和碳纳米技术;表面科学。高场动态核极化（DNP）是革命性的固体核磁共振（NMR）光谱，由于核自旋的相关超极化导致信号增强的数量级。然而，DNP并不广泛适用，特别是对于较高温度（>100 K）和环境敏感的分析物，例如沸石催化剂和用于气体捕获和转化的高级多孔吸附剂。该项目将独特地结合联合收割机在材料科学，EPR和DNP-NMR在曼彻斯特的专业知识。目前，用于DNP的超极化剂是昂贵的有机自由基，其被外源地添加到分析物中。这需要分散在（冷冻）溶液中以确保均匀分布。然而，该项目提出了一种范式转变，即分析物将沉积在优化的2D材料上，该材料包含具有受控特性的电子自旋。沿着样品制备的简便性，缺少添加的溶剂将有助于在“自然”状态下表征样品，并使实验能够在更高的温度下进行-这是DNP-NMR的当前圣杯。此外，这项工作可以扩展到各种其他领域，如生物分子研究以及增强MRI。因此，这个项目将导致专利，以及出版物，并使原子尺度的理解反应机制在非均相催化。

EPSRC Research Areas relevant to the project:Analytical science; Carbon capture and storage; Catalysis; Functional ceramics and inorganics; Graphene and carbon nanotechnology; Surface science.High-field dynamic nuclear polarisation (DNP) is revolutionising nuclear magnetic resonance (NMR) spectroscopy of solids owing to the associated hyperpolarisation of nuclear spins leading to orders of magnitude of signal enhancements. However, DNP is not widely applicable, particularly for higher temperatures (>100 K) and for environment-sensitive analytes such as zeolite catalysts and advanced porous adsorbents for gas capture and conversion. This project would uniquely combine expertise at Manchester in materials science, EPR, and DNP-NMR. Currently, hyperpolarising agents for DNP are expensive organic radicals that are added exogenously to an analyte. This requires dispersion in a (frozen) solution to ensure a homogeneous distribution. However, this project proposes a paradigm shift in that the analyte would be deposited on an optimised 2D material that contains electron spins with controlled properties. Along with the ease of sample preparation, the lack of added solvent would facilitate sample characterisation in a "natural" state and enable experiments at higher temperatures - a current Holy Grail for DNP-NMR. Moreover, this work could be extended to various other fields such as for biomolecular studies as well as for enhanced MRI. This project would thus lead to patents, as well as publications, and enable an atomic-scale understanding of reaction mechanisms in heterogenous catalysis.