Strong, Yet Split Hydrogen Bonding with Ice Rules in Delafossite (H/D)RhO <sub>2</sub>

M Matthew A. Wright (Materials Department) A Anya S. Mulligan (Materials Department University of California Santa Barbara CA USA) D Dibyata Rout (Materials Department University of California Santa Barbara CA USA) J Jerry G. Hu (Materials Research Laboratory University of California Santa Barbara CA USA) J Jue Liu R Rachel L. Behrens (Materials Research Laboratory University of California Santa Barbara CA USA) J Juan R. Chamorro (Materials Science and Engineering Carnegie Mellon University Pittsburgh PA USA) S Stephen D. Wilson A Anthony K. Cheetham (Department of Materials, Materials Research Laboratory) R Ram Seshadri (Materials Department and Materials Research Laboratory)

Abstract

Abstract Despite remaining enigmatic, strong hydrogen bonding provides an advanced design handle for tailoring the properties of functional materials. Here, 3 R –(H/D)RhO 2 delafossites (prepared by ion exchange of Na + from NaRhO 2 ) contain H/D in linear coordination with O, linking Rh III O 2 layers. Bragg and real‐space X‐ray and neutron scattering analysis, vibrational and solid‐state NMR spectroscopy, and density functional theory (DFT)–based electronic structure calculations have been employed to understand the nature of the hydrogen bonding. Despite short distances between H/D and the two O to which they are bonded, a clear double‐minimum corresponding to a shorter and longer (H/D)–O distance is established. The triangular lattices formed by H/D appear to display ice‐like disorder, corroborated by low‐temperature heat capacity measurements.

Article Details

Volume / Issue Vol. 64, Issue 52
Published December 22, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (10)

M

Matthew A. Wright

Materials Department

A

Anya S. Mulligan

Materials Department University of California Santa Barbara CA USA

D

Dibyata Rout

Materials Department University of California Santa Barbara CA USA

J

Jerry G. Hu

Materials Research Laboratory University of California Santa Barbara CA USA

J

Jue Liu

R

Rachel L. Behrens

Materials Research Laboratory University of California Santa Barbara CA USA

J

Juan R. Chamorro

Materials Science and Engineering Carnegie Mellon University Pittsburgh PA USA

S

Stephen D. Wilson

A

Anthony K. Cheetham

Department of Materials, Materials Research Laboratory

R

Ram Seshadri

Materials Department and Materials Research Laboratory