Collaborative Research: Exploiting Spin Networks and Efficient Catalyst/Substrate Separations for NMR "SABRE" Enhancement of Complex Systems

合作研究：利用自旋网络和高效的催化剂/底物分离来增强复杂系统的 NMR“SABRE”

• 批准号: 1905341
• 负责人: Boyd Goodson
• 金额: $ 25.8万
• 依托单位: Southern Illinois University at Carbondale
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-08-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1905341&HistoricalAwards=false
• 关键词: Collaborative; Research; Exploiting; Spin; Networks

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professors Boyd Goodson at Southern Illinois University (SIU) and Eduard Chekmenev at Wayne State University (WSU) are working to improve the sensitivity of nuclear magnetic resonance (NMR), an important method of chemical analysis which underlies the well-known clinical imaging modality, magnetic resonance imaging (MRI). The Goodson/Chekmenev team is developing new, inexpensive, and easy-to-make means of enhancing nuclear magnetization - a sensitivity-limiting factor in many NMR and MRI applications, including diagnostic tests for a host of diseases. Anticipated cost savings can also make these methods more available for other lab settings, particularly those that have more limited research infrastructure and/or that feature undergraduate research. Several students are involved, gaining exposure to highly interdisciplinary training. The team is also engaged in efforts to recruit undergraduate students and match them with a variety of mentored research opportunities on both campuses, with a goal of increasing the numbers and diversity of undergraduate students seeking STEM careers. The NMR/MRI approaches being used are based on Signal Amplification by Reversible Exchange, or SABRE. In SABRE, an organometallic catalyst is used to co-locate parahydrogen and a target molecule (substrate) within a transient complex; with properly matched external magnetic fields, nuclear spin order can transfer spontaneously and efficiently from parahydrogen to the substrate, giving rise to NMR and MRI signals that are increased by several orders of magnitude. Work by the Goodson/Chekmenev team seeks to: (1) improve the understanding and utility of long-range SABRE polarization transfer via spin-relay networks in model systems, for both homonuclear and heteronuclear cases; (2) develop and characterize new heterogeneous catalysts for SABRE ("HET-SABRE"), as well as approaches for catalyst recovery; and (3) broaden the range of substances amenable to SABRE through improved understanding of the fundamental quantum mechanics of complex spin behavior in model extended networks.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.

在化学系化学测量和成像项目的支持下，南伊利诺伊大学（SIU）的Boyd Goodson教授和韦恩州立大学（WSU）的Eduard Chekmenev教授正在努力提高核磁共振（NMR）的灵敏度，这是一种重要的化学分析方法，是众所周知的临床成像模式磁共振成像（MRI）的基础。 Goodson/Chekmenev团队正在开发新的，廉价的，易于制造的增强核磁共振的方法-这是许多NMR和MRI应用中的灵敏度限制因素，包括许多疾病的诊断测试。 预期的成本节约也可以使这些方法更适用于其他实验室环境，特别是那些研究基础设施有限和/或具有本科研究的实验室环境。 几个学生参与，获得接触到高度跨学科的培训。 该团队还致力于招募本科生，并在两个校区为他们提供各种指导研究机会，目标是增加寻求STEM职业的本科生的数量和多样性。 使用的NMR/MRI方法基于可逆交换信号放大或SABRE。 在SABRE中，有机金属催化剂用于将仲氢和靶分子（底物）共同定位在瞬态复合物中;在适当匹配的外部磁场下，核自旋顺序可以自发地有效地从仲氢转移到底物，从而产生增加几个数量级的NMR和MRI信号。 Goodson/Chekmenev团队的工作旨在：（1）提高对通过模型系统中的自旋中继网络进行远程SABRE极化转移的理解和实用性，无论是homonucleus还是heteronucleus情况;（2）开发和表征SABRE的新型非均相催化剂（“HET-SABRE”），以及催化剂回收方法;以及（3）通过提高对模型扩展网络中复杂自旋行为的基本量子力学的理解，拓宽了适用于SABRE的物质范围。该奖项反映了NSF的法定使命，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，认为值得支持。

项目成果

High-Pressure Clinical-Scale 87% Parahydrogen Generator

• DOI: 10.1021/acs.analchem.0c03358
• 发表时间: 2020-12-01
• 期刊: ANALYTICAL CHEMISTRY
• 影响因子: 7.4
• 作者: Birchall, Jonathan R.;Coffey, Aaron M.;Chekmenev, Eduard Y.
• 通讯作者: Chekmenev, Eduard Y.

Spin dynamics of [1,2- 13 C 2 ]pyruvate hyperpolarization by parahydrogen in reversible exchange at micro Tesla fields

微特斯拉场可逆交换中仲氢引起的[1,2- 13 C 2 ]丙酮酸超极化的自旋动力学

• DOI: 10.1039/d3cp00843f
• 发表时间: 2023
• 期刊: Physical Chemistry Chemical Physics
• 影响因子: 3.3
• 作者: Browning, Austin;Macculloch, Keilian;TomHon, Patrick;Mandzhieva, Iuliia;Chekmenev, Eduard Y.;Goodson, Boyd M.;Lehmkuhl, Sören;Theis, Thomas
• 通讯作者: Theis, Thomas

Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K.

• DOI: 10.1021/acs.analchem.1c00716
• 发表时间: 2021-06-22
• 期刊: Analytical chemistry
• 影响因子: 7.4
• 作者: Chapman B;Joalland B;Meersman C;Ettedgui J;Swenson RE;Krishna MC;Nikolaou P;Kovtunov KV;Salnikov OG;Koptyug IV;Gemeinhardt ME;Goodson BM;Shchepin RV;Chekmenev EY
• 通讯作者: Chekmenev EY

A modular apparatus for use in high-precision measurements of parity violation in polarized eV neutron transmission

一种用于高精度测量偏振 eV 中子传输中奇偶校验破坏的模块化装置

• DOI: 10.1016/j.nima.2020.163961
• 发表时间: 2020
• 期刊: Detectors and Associated Equipment
• 作者: Schaper, D.C.;Auton, C.;Barrón-Palos, L.;Borrego, M.;Chavez, A.;Cole, L.;Crawford, C.B.;Curole, J.;Dhahri, H.;Dickerson, K.A.
• 通讯作者: Dickerson, K.A.

Cobalt-Catalyzed Hyperpolarization of Structurally Intact Olefins

• DOI: 10.1021/acscatal.0c03727
• 发表时间: 2021-02-01
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Muhammad, Safiyah R.;Greer, Rianna B.;Fout, Alison R.
• 通讯作者: Fout, Alison R.