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Record W4392166721 · doi:10.1021/acs.jpcc.3c07776

MXenes as Effective Sulfur Hosts and Electrocatalysts to Suppress Lithium Polysulfide Shuttling: A Computational Study

2024· article· en· W4392166721 on OpenAlexafffund
Thilini Boteju, Sathish Ponnurangam, Venkataraman Thangadurai

Bibliographic record

VenueThe Journal of Physical Chemistry C · 2024
Typearticle
Languageen
FieldMaterials Science
TopicMXene and MAX Phase Materials
Canadian institutionsUniversity of Calgary
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsPolysulfideMXenesSulfurLithium–sulfur batteryLithium (medication)ChemistryNanotechnologyMaterials scienceBiologyElectrochemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Exploring electrocatalysts for the sulfur reduction reaction (SRR) has emerged as a promising strategy to suppress the shuttle effect and enhance the kinetics in lithium–sulfur (Li–S) batteries. A comprehensive understanding of the electrocatalytic mechanism within Li–S batteries remains elusive, which hinders the rational design of advanced electrocatalysts for these systems. In this study, two-dimensional (2D) transition metal carbides and nitrides (MXenes) have been investigated for the catalytic conversion of lithium polysulfides (LiPSs) using density functional theory (DFT). Our findings reveal that MXenes show a moderate binding affinity for LiPSs, suggesting favorable thermodynamics for their role as electrocatalysts for the SRR. This thermodynamic favorability promotes the suppression of the LiPSs’ shuttle effect and the enhancement of the SRR kinetics. The SRR process in Li–S batteries consists of multiple steps with varying activation energies. Our analysis by constructing the energy diagram for the multistep SRR indicates that the initial reduction of S 8 to Li 2 S 8 is facile with a lower activation energy, while the last step where Li 2 S 2 converts to Li 2 S appears to be a rate-limiting step. To predict the catalytic abilities of MXene structures, we built a volcano-shaped relationship between the adsorption of LiPSs and catalytic activity. We show three MXenes─Ta 2 CO 2, Zr 2 NO 2, and Mo 2 NO 2 as potential electrocatalysts that exhibit lower thermodynamic overpotentials for the SRR. These findings represent a significant step toward developing advanced electrocatalysts that may unlock the full potential of Li–S batteries, paving the way for improved energy storage systems with enhanced efficiency and performance.

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 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 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 score0.002
Threshold uncertainty score0.408

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
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)0.0000.000

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 head0.285
Teacher spread0.279 · 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 teacher head, 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".

Quick stats

Citations19
Published2024
Admission routes2
Has abstractyes

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