Atomic-Scale Mapping of Atomically Dispersed Light-Element Species in Oxide Nanomaterials by Solid-State NMR

Light-element isolated species represent an emerging class of atomically dispersed nanomaterials, yet their precise local and higher-shell coordination environments remain largely inaccessible due to the intrinsic limitations of conventional nanoscale probes. Here, we establish a solid-state NMR method, combining 23Na and 17O spectroscopy with first-principles calculations, to directly resolve the atomic-scale structure of light-element isolated species beyond the first coordination shell. Using Na-modified CeO2 as a representative system, isolated and aggregated sodium species are distinguished by characteristic 23Na NMR signatures, while 17O NMR further reveals how light element dopants perturb oxygen coordination across the first to third atomic shells. This approach enables clear differentiation of Na–O–Ce linkages from more remote Na–O–Ce–O environments that are inaccessible to electron microscopy and X-ray-based techniques. As a demonstration of atomic-scale structure-adsorption correlation, CO2 is shown to preferentially adsorb at Na–O–Ce sites rather than at Na–O–H groups.