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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 OpenAlexafffund
Madhusudan Chaudhary, Elisabeth Springl, Daniel Fabian Weindl, Diganta Sarkar, Amy Yu, Dmitry Vrublevskiy, Tom Nilges, Arthur Mar, Vladimir K. Michaelis

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.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
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 score0.001
Threshold uncertainty score0.002

Distilled classifier scores by category (both heads)

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

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

Classification

machine, unvalidated

Machine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

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Citations3
Published2025
Admission routes2
Has abstractyes

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