Highlights from our research utilizing heterogeneous catalysis for conversion of parahydrogen singlet nuclear spin order into hyperpolarized magnetization are presented. Heterogeneous catalysis offers important advantages over other hyperpolarization techniques for applications such as biomedical imaging and drug discovery. One of the main challenges to achieve efficient conversion is suppression of the fast diffusion of H ad-atoms that occurs on the surface of catalytically active metals such as platinum. Through rational catalyst design, significant improvements in the efficiency of the singlet-to-magnetization transformation have been realized. Three different examples are presented. In the first, atomic layer deposition was used to prepare ultra-low loadings of Pt on shaped cerium oxide nanocrystal supports, where surface interactions on the (111) facets of the CeO2 nano-octahedra stabilize atomically dispersed Pt. The Pt/CeO2(111) catalyst exhibits significantly higher selectivity toward pairwise hydrogenation compared to CeO2-supported Pt nanoparticles. Secondly, PtSn intermetallic nanoparticles are shown to catalyze addition of parahydrogen to gaseous alkenes and alkynes with unprecedented pairwise selectivity and NMR signal enhancement factors. Lastly, the surfaces of Pt3Sn intermetallic nanoparticles are shown to mediate singlet-to-magnetization conversion yielding hyperpolarized liquid HDO. In all three examples, the surface structure and composition were tailored to favor high singlet-to-magnetization conversion efficiency. In some cases, NMR signal enhancements exceeding three orders of magnitude were observed.

Rational design of heterogeneous catalysts for efficient nuclear spin singlet-to-magnetization conversion

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.