{"doi":"10.1021/jacs.5c07442","title":"Mg-Ion Conduction in Antiperovskite Solid Electrolytes Revealed by <sup><b>25</b></sup>Mg Ultrahigh Field NMR and First-Principles Calculations","abstract":"Magnesium-ion batteries hold the potential to outperform the energy density of lithium-ion batteries, given the divalent charge carried by each Mg 2+ cation, but remain in an early stage of development. Here, 25 Mg solid-state nuclear magnetic resonance (ssNMR) is used to gain insight into the local structure and Mg-ion dynamics of candidate Mg-ion solid electrolytes, the antiperovskites Mg 3 SbN and Mg 3 AsN. Using the highest available magnetic field (35.2 T) for high-resolution solid-state NMR, the largest 25 Mg quadrupole coupling constants ( C Q ) yet measured of up to 22 MHz are reported and corroborated by first-principles calculations. Predicted C Q values are shown to correlate with the antiperovskite’s tolerance factor; thus, 25 Mg NMR linewidths can report on lattice distortions and phase stability of these antiperovskites. Variable-temperature 25 Mg NMR spectra demonstrate changes at elevated temperatures, ascribed to Mg-ion motional effects. 25 Mg T 1 relaxometry measurements at ultrahigh field reveal a lower activation energy for the more distorted Mg 3 AsN phase, matching computational predictions of a lower energy barrier for Mg 2+ ion migration and suggesting that additional scrutiny of antiperovskites as Mg-ion conductors is warranted. Given the inherent challenges of 25 Mg NMR, this work demonstrates the benefits of combining ultrahigh field NMR spectroscopy, advanced pulse sequences, modern signal processing, and first-principles calculations to facilitate NMR of quadrupolar nuclei as a tool to probe the local structure and ion dynamics in beyond-Li battery materials.","journal":"Journal of the American Chemical Society","year":2025,"id":534259,"datarank":0.0,"base_score":0.0,"endowment":0.0,"self_citation_contribution":0.0,"citation_network_contribution":0.0,"self_endowment_contribution":0.0,"citer_contribution":0.0,"corpus_percentile":null,"corpus_rank":null,"citation_count":2,"citer_count":0,"citers_with_citation_signal":0,"citers_with_endowment":0,"datacite_reuse_total":0,"is_dataset":false,"is_dataset_confidence":0.944,"is_data_producer":false,"deposit_databanks":null,"is_oa":false,"file_count":0,"downloads":0,"has_version_chain":false,"published_date":"2025-01-01","fair_score":null,"fair_percentile":null,"algorithm_id":"datarank_citation_only_1hop_v6","ranking_scope":"data_only","authors":[{"id":1416856,"name":"Haoyu Liu","orcid":"0000-0002-6741-7295","position":1,"is_corresponding":false},{"id":1416857,"name":"Kwangnam Kim","orcid":"0000-0003-1149-1733","position":2,"is_corresponding":false},{"id":1416858,"name":"Grant C. B. Alexander","orcid":"0000-0002-6041-4737","position":3,"is_corresponding":false},{"id":291986,"name":"Xiao-Ling Wang","orcid":"0000-0002-8718-0408","position":4,"is_corresponding":false},{"id":1174136,"name":"Amrit Venkatesh","orcid":"0000-0001-5319-9269","position":5,"is_corresponding":false},{"id":1416859,"name":"Adam R. Altenhof","orcid":"0000-0002-8095-6373","position":6,"is_corresponding":false},{"id":1416860,"name":"Harris E. Mason","orcid":"0000-0002-1840-0550","position":7,"is_corresponding":false},{"id":1416861,"name":"Saul H. Lapidus","orcid":"0000-0002-7486-4325","position":8,"is_corresponding":false},{"id":1416862,"name":"Jeong Seop Yoon","orcid":"0000-0002-9002-094X","position":9,"is_corresponding":false},{"id":240798,"name":"Ivan Hung","orcid":"0000-0001-8916-739X","position":10,"is_corresponding":false},{"id":240800,"name":"Zhehong Gan","orcid":"0000-0002-9855-5113","position":11,"is_corresponding":false},{"id":1416863,"name":"Jordi Cabana","orcid":"0000-0002-2353-5986","position":12,"is_corresponding":false},{"id":1416864,"name":"Donald J. Siegel","orcid":"0000-0001-7913-2513","position":13,"is_corresponding":false},{"id":228307,"name":"Jeffrey A. Reimer","orcid":"0000-0002-4191-3725","position":14,"is_corresponding":false},{"id":1416865,"name":"Baris Key","orcid":"0000-0002-1987-1629","position":15,"is_corresponding":false},{"id":322376,"name":"David M. Halat","orcid":"0000-0002-0919-1689","position":0,"is_corresponding":true}],"reference_count":116,"raw_metadata":null,"created_at":"2026-07-19T02:51:47.434742Z","pmid":"40705608","pmcid":null,"fwci":null,"citation_percentile":null,"influential_citations":0,"oa_status":null,"license":null,"views":0,"total_file_size_bytes":0,"version_count":0,"fair_f":null,"fair_a":null,"fair_i":null,"fair_r":null,"fair_zscore":null,"fair_rationale":null,"fair_model":null,"fair_agent_version":null,"fair_fulltext_source":null,"fair_has_llm":null,"fair_computed_at":null,"clinical_trials":[],"software_tools":[],"db_accessions":[],"linked_datasets":[],"topics":[]}