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Record W2990354746 · doi:10.1021/acscatal.9b01925

MXene Materials for the Electrochemical Nitrogen Reduction—Functionalized or Not?

2019· article· en· W2990354746 on OpenAlexfundno aff
Luke R. Johnson, Sudiksha Sridhar, Liang Zhang, Kurt Fredrickson, Abhinav S. Raman, Joonbaek Jang, Connor T. Leach, Ashwin Padmanabhan, Christopher C. Price, Nathan C. Frey, Abhishek Raizada, Vishwanathan Rajaraman, Sai Aparna Saiprasad, Tang Xiaoxin, Aleksandra Vojvodić

Bibliographic record

VenueACS Catalysis · 2019
Typearticle
Languageen
FieldMaterials Science
TopicMXene and MAX Phase Materials
Canadian institutionsnot available
FundersCanadian Institute for Advanced Research
KeywordsMXenesOverpotentialChemistryNonmetalRedoxElectrochemistryInorganic chemistryMaterials scienceMetalPhysical chemistryOrganic chemistryElectrode

Abstract

fetched live from OpenAlex

We use density functional theory calculations to study a group of 2D materials known as MXenes toward the electrochemical nitrogen reduction reaction (NRR) to ammonia. So far, all computational studies have only considered the NRR chemistry on unfunctionalized (bare) MXenes. In this study, we investigate a total of 65 bare and functionalized MXenes. We establish free energy diagrams for the NRR on the basal planes of 55 different M 2 XT x MXenes (M = Ti, V, Zr, Nb, Mo, Ta, W; X = C, N) to span a large variety of possible chemistries. Energy trends with respect to the metal as well as nonmetal constituent of the MXenes are established for both bare and functionalized MXenes. We determine the limiting potentials and find that either the formation of NH 3 from *NH 2 or the formation of *N 2 H is the potential limiting reaction step for bare and functionalized MXenes, respectively. We find several Mo-, W-, and V-based MXenes (Mo 2 C, Mo 2 N, W 2 N, W 2 NH 2, and V 2 N) to have suitable theoretical overpotentials for the NRR. Importantly, calculated Pourbaix stability diagrams combined with selectivity analysis, however, reveal that all bare MXenes are not stable under relevant NRR operating conditions. The only functionalized MXene with the three minimum required properties (i) having a low theoretical overpotential, (ii) being stable under NRR conditions, and (iii) having selectivity toward NRR rather than the parasitic HER is W 2 CH 2, which is a H-terminated MXene. Finally, on the basis of our findings, we explore other routes for improving the NRR chemistry by studying 10 additional MXenes with the chemical formula M 3 X 2 T x and MXenes with other functional groups (T x = S, F, Cl). This opens up a larger variety and tunability of MXenes to be considered for the NRR.

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 score0.002
Threshold uncertainty score0.007

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)0.0020.000

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 head0.018
GPT teacher head0.265
Teacher spread0.246 · 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".

Quick stats

Citations189
Published2019
Admission routes1
Has abstractyes

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