International Collaboration in Chemistry: Collaborative Research: Development of Novel Catalysts and Approaches for Parahydrogen-Induced Enhancement of Magnetic Resonance

通过这一奖项，化学测量和成像计划支持一个由俄罗斯(由ITC新西伯利亚分校的Igor Koptyug领导)和美国(由Carbondale南伊利诺伊大学的Boyd Goodson和Vanderbilt大学的Eduard Chekmenev领导)组成的合作团队，进行研究以提高核磁共振或核磁共振的能力，核磁共振是磁共振成像(MRI)背后的关键技术，磁共振成像是现代医学中广泛使用的诊断工具。研究人员正在探索一种可能的修改，可以将这项技术的灵敏度提高许多个数量级，从而改进MRI，同时也有助于改进其他类型系统的可视化技术。这项研究正在探索一种特殊形式的氢的使用，这种氢被称为仲氢，已被证明可以增强核磁共振信号。为了开发更准确和更灵敏的成像方法，这项工作正在利用各种技术来理解这种特殊形式的氢是如何工作的。这项工作正在对新的科学仪器的发展产生广泛的影响，这些仪器将在从医学到化学制造的广泛领域得到应用。它正在产生更广泛的影响，将科学家们聚集在一起，共同研究共同关心的全球问题。该项目为下一代科学家的培训做出了贡献，为各级学生提供了参与高度跨学科、多地点培训环境的机会。具体地说，美国网站的学生能够参观国际合作者在亚洲最重要的研究中心之一新西伯利亚的网站并开展研究项目。总体目标是开发新的催化材料和方法，可以显著提高仲氢激发极化(PhIP)技术的适用性。低检测灵敏度仍然是许多传统方法的致命弱点，如核磁共振和核磁共振。然而，对氢的纯反相自旋有序(PH2)可以被用来在某些类型的分子中实现高度非平衡的核自旋布居分布(极化)，从而使核磁共振/核磁共振检测灵敏度提高数量级。更具体地说，这些工作涉及以下方面的合成、评估和核磁共振演示：1)用于传统PhIP的新型多相催化剂(涉及不饱和部分与PH2的氢化)；以及2)用于SABRE的新型均相和非均相催化剂(通过可逆交换进行信号放大-一种无需不可逆化学变化即可将自旋有序从PH2转移到分子的技术)。开发就地高场军刀的新方法也在研究中。此外，这些实验还得到了自动便携式HET-PhIP/SABRE偏振器的支持，该偏振器具有原位MR检测和自动PH2生成功能。这些研究努力为关键PhIP方法的当前限制提供更多的洞察力，同时努力显著提高它们的实用性。

With this award, the Chemical Measurement and Imaging Program is supporting a collaborative team comprised of research groups in Russia (led by Igor Koptyug of ITC Novosibirsk) and the US (led by Boyd Goodson of Southern Illinois University at Carbondale and Eduard Chekmenev of Vanderbilt University) for research to improve the capabilities of nuclear magnetic resonance, or NMR, the key technology behind magnetic resonance imaging (MRI), a widely used diagnostic tool in modern medicine. The investigators are exploring a possible modification that could enhance the sensitivity of this technique by many orders of magnitude, thus improving MRI while also contributing to the improvement of technologies for visualizing other types of systems. The research is exploring the use of a special form of hydrogen known as parahydrogen that has been shown to enhance an NMR signal. The work is bringing a variety of techniques to bear on the task of understanding how this special form of hydrogen works in order to develop more accurate and sensitive imaging methods. The work is having a broad impact on the development of new scientific instruments that will find applications in a wide variety of fields from medicine to chemical manufacturing. It is having a further broad impact by bringing scientists together across borders to work on problems of mutual global interest. This project is contributing to the training of the next generation of scientists by providing opportunities for students at all levels to participate in a highly interdisciplinary, multi-site training environment. Specifically, students at the US sites are able to visit and carry out research projects at the international collaborator's site in Novosibirsk, one of Asia's most important research hubs.The overall objective is to develop new catalytic materials and approaches that can dramatically improve the applicability of parahydrogen induced polarization (PHIP) techniques. Low detection sensitivity remains an Achilles Heel of many conventional methods such as NMR and MRI. However, the pure anti-phase spin order of parahydrogen (pH2) can be exploited to achieve highly non-equilibrium nuclear spin population distributions ("polarizations") in certain types of molecules, thereby enabling the enhancement of NMR/MRI detection sensitivity by orders of magnitude. More specifically, these efforts concern the synthesis, evaluation, and NMR demonstration of: 1) new heterogeneous catalysts for traditional PHIP (which involves the hydrogenation of unsaturated moieties with pH2); and 2) new homogeneous and heterogeneous catalysts for SABRE (signal amplification by reversible exchange - a technique where spin order is transferred from pH2 to molecules without requiring irreversible chemical change). New approaches exploiting in situ high-field SABRE are also under study. Additionally, these experiments are supported by the construction of an automated portable HET-PHIP/SABRE polarizer with in situ MR detection and automated pH2 generation. These research efforts endeavor to provide greater insight into current limitations for key PHIP approaches, while working to dramatically improve their utility.