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Screening Strategies for Diatom Metal-Doped β-Borophene Nanosheet Catalysts for Electrochemical Synthesis of Ammonia Using Density Functional Theory

2023· article· en· W4379618567 on OpenAlexaff
Li Liu, Lei Yang, Haiyang Zhang, Wumaier Tuerdi, Zhiyong Shang, Jinli Zhang

Bibliographic record

VenueEnergy & Fuels · 2023
Typearticle
Languageen
FieldChemical Engineering
TopicAmmonia Synthesis and Nitrogen Reduction
Canadian institutionsUniversity of Waterloo
FundersScience Fund for Distinguished Young Scholars of Xinjiang Autonomous RegionXinjiang Uygur Autonomous Region Department of Education
KeywordsOverpotentialCatalysisElectrocatalystDensity functional theoryChemistryAdsorptionFaraday efficiencyElectrochemistryNanosheetBoropheneSelectivityInorganic chemistryPhysical chemistryComputational chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Electrocatalysis is a promising approach for ammonia production under ambient conditions. However, practically, owing to the competing hydrogen evolution reaction (HER), the Faradaic efficiency is low, and it is difficult to activate the inert N≡N. The theoretical screening method based on density functional theory calculations is a novel technique for developing and designing nitrogen reduction reaction (NRR) diatom catalysts (DACs). We proposed an NRR new type of DAC doped on β-borophene (B-β) nanosheets exhibiting enhanced catalytic activities for the NRR through the pull–pull effect of dual-metal sites and donor–acceptor coupling. By systematically evaluating the stabilities, selectivities, and activities of 24 diatom-doped β-borophene (M 2 @B-β) candidates, Mo 2 @B-β was found to be a promising NRR electrocatalyst with a low limiting potential of −0.23 V for the NRR and a high overpotential of −0.16 V for the HER. The limiting potentials for Cr 2 @B-β, Mn 2 @B-β, and Re 2 @B-β were −0.52, −0.51, and −0.35 V, respectively, making them suitable electrocatalysts for the NRR. Based on the Sabatier principle, we proposed two descriptors, Δ G (*N) and d-band center, as the criteria for screening and designing catalysts with high catalytic activities to reveal the intrinsic correlation between adsorption properties and structural properties. Based on the Δ G (*N) function, a volcano plot was built to predict trends in the activities. The difference, Δ G (*N 2 ) – Δ G (*H), was used as the selectivity descriptor, where the negative values of Δ G mean that the adsorption of N 2 dominates over the adsorption of H on the surface of M 2 @B-β. This study thus provides a feasible strategy for designing NRR electrocatalysts and is helpful for the fast screening of efficient DACs for other electroreduction reactions.

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)0.000
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 score0.242
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

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)0.0000.000

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 head0.024
GPT teacher head0.243
Teacher spread0.219 · 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.

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

Citations17
Published2023
Admission routes1
Has abstractyes

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