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Entropy-Driven Disorder and Aliovalent Substitution Induce Defects in Na<sub>3</sub><i>Pn</i>S<sub>4</sub> (<i>Pn</i> = P, As, Sb) Solid-State Electrolytes: A Sluice Gate for Sodium Ions

2025· article· en· W4414112736 on OpenAlex
Madhusudan Chaudhary, Elisabeth Springl, Daniel Fabian Weindl, Diganta Sarkar, Amy Yu, Dmitry Vrublevskiy, Tom Nilges, Arthur Mar, Vladimir K. Michaelis

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenueACS Materials Letters · 2025
Typearticle
Languageen
FieldMaterials Science
TopicSolid-state spectroscopy and crystallography
Canadian institutionsUniversity of Alberta
FundersAlberta InnovatesCanada Research ChairsCanada Foundation for InnovationUniversity of AlbertaNatural Sciences and Engineering Research Council of CanadaGovernment of Alberta
KeywordsIonic conductivityTernary operationVacancy defectIonic bondingTetragonal crystal systemIonConductivitySolid solution

Abstract

fetched live from OpenAlex

Sodium-containing chalcogenides are attractive candidates for use as solid-state electrolytes; however, their ionic conductivities remain a challenge. Simultaneously applying isovalent and aliovalent substitution can enhance ionic conductivity by generating substantial site disorder and high vacancy concentrations. To elucidate the mechanism that facilitates sodium ion conduction, a series of mixed-pnicogen solid solutions were prepared from the parent ternary sulfides Na 3 Pn S 4 ( Pn = P, As, Sb) by high-temperature reactions, including an entropy-driven W-substituted phase, Na 3−δ P 0.32 As 0.32 Sb 0.32 W 0.04 S 4 (N-PASS-W). N-PASS-W exhibits a very high ionic conductivity of 10 mS cm –1 and a low activation energy of 0.15 eV. Using PXRD and NMR spectroscopy, an atomic-level model for N-PASS-W was proposed, in which ion hopping occurs over two Na sites within a tetragonal structure ( P 4̅2 1 c ). Relationships were also established between the structure and ionic conductivities of the other members to evaluate the influence of crystalline phase, cation size, and site disorder.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.006
Threshold uncertainty score0.999

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0010.001
Science and technology studies0.0010.001
Scholarly communication0.0010.001
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.006
GPT teacher head0.238
Teacher spread0.233 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it