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基于孤子的动态核极化:高场和室温下环状聚乙炔中的奥弗豪泽效应

Soliton Based Dynamic Nuclear Polarization: An Overhauser Effect in Cyclic Polyacetylene at High Field and Room Temperature.

作者信息

Miao Z, Scott F J, van Tol J, Bowers C R, Veige A S, Mentink-Vigier F

机构信息

Center for Catalysis, Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States.

National High Magnetic Field Laboratory, Florida State University, 1800 E. Paul Dirac Drive, Tallahassee, Florida 32310, United States.

出版信息

J Phys Chem Lett. 2024 Mar 28;15(12):3369-3375. doi: 10.1021/acs.jpclett.3c03591. Epub 2024 Mar 18.

Abstract

Polyacetylene, a versatile material with an electrical conductivity that can span 7 orders of magnitude, is the prototypical conductive polymer. In this letter, we report the observation of a significant Overhauser effect at the high magnetic field of 14.1 T that operates at 100 K and room temperature in both linear and cyclic polyacetylene. Significant NMR signal enhancements ranging from 24 to 45 are obtained. The increased sensitivity enabled the characterization of the polymer chain defects at natural abundance. The absence of end methyl group carbon-13 signals provides proof of the closed-loop molecular structure of cyclic polyacetylene. The remarkable efficiency of the soliton based Overhauser effect DNP mechanism at high temperature and high field holds promise for applications and extension to other conductive polymer systems.

摘要

聚乙炔是一种具有广泛用途的材料,其电导率可跨越7个数量级,是典型的导电聚合物。在本信函中,我们报告了在14.1 T的高磁场下观察到的显著的奥弗豪泽效应,该效应在100 K和室温下在线性和环状聚乙炔中均起作用。获得了24至45范围内的显著核磁共振信号增强。灵敏度的提高使得能够在自然丰度下对聚合物链缺陷进行表征。端甲基碳-13信号的缺失证明了环状聚乙炔的闭环分子结构。基于孤子的奥弗豪泽效应动态核极化机制在高温和高场下的显著效率为应用以及扩展到其他导电聚合物系统带来了希望。

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