Nickel‐Based Single‐Molecule Catalysts with Synergistic Geometric Transition and Magnetic Field‐Assisted Spin Selection Outperform RuO 2 for Oxygen Evolution

Saini, Kavish; Nair, Aruna N.; Yadav, Anju; Enriquez, Lissette Garcia; Pollock, Christopher J.; House, Stephen D.; Yang, Shize; Guo, Xin; Sreenivasan, Sreeprasad T.

doi:10.1002/aenm.202302170

Title: Nickel‐Based Single‐Molecule Catalysts with Synergistic Geometric Transition and Magnetic Field‐Assisted Spin Selection Outperform RuO ₂ for Oxygen Evolution

Journal Article · 25 September 2023 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.202302170 · OSTI ID:2006547

^[1]; Nair, Aruna N. ^[1]; Yadav, Anju ^[1]; Enriquez, Lissette Garcia ^[1]; Pollock, Christopher J. ^[2]; House, Stephen D. ^[3]; Yang, Shize ^[4]; Guo, Xin ^[4];

^[1]

Department of Chemistry and Biochemistry The University of Texas at El Paso El Paso TX 79968 USA
Cornell High Energy Synchrotron Source Wilson Laboratory Cornell University Ithaca NY 14853 USA
Center for Integrated Nanotechnologies Sandia National Laboratories Albuquerque NM 87111 USA
Eyring Materials Center Arizona State University Tempe AZ 85287 USA

Abstract Overcoming slow kinetics and high overpotential in electrocatalytic oxygen evolution reaction (OER) requires innovative catalysts and approaches that transcend the scaling relationship between binding energies for intermediates and catalyst surfaces. Inorganic complexes provide unique, customizable geometries, which can help enhance their efficiencies. However, they are unstable and susceptible to chemical reaction under extreme pH conditions. Immobilizing complexes on substrates creates single‐molecule catalysts (SMCs) with functional similarities to single‐atom catalysts (SACs). Here, an efficient SMC, composed of dichloro(1,3‐bis(diphenylphosphino)propane) nickel [NiCl ₂ dppp] anchored to a graphene acid (GA), is presented. This SMC surpasses ruthenium‐based OER benchmarks, exhibiting an ultra‐low onset and overpotential at 10 mAcm ⁻² when exposed to a static magnetic field. Comprehensive experimental and theoretical analyses imply that an interfacial charge transfer from the Ni center in NiCl ₂ dppp to GA enhances the OER activity. Spectroscopic investigations reveal an in situ geometrical transformation of the complex and the formation of a paramagnetic Ni center, which under a magnetic field, enables spin‐selective electron transfer, resulting in enhanced OER performance. The results highlight the significance of in situ geometric transformations in SMCs and underline the potential of an external magnetic field to enhance OER performance at a single‐molecule level.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; EE0010431; FE0031908

OSTI ID:: 2006547

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 42 Vol. 13; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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