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Record W4386836254 · doi:10.1007/s12274-023-6068-1

High-throughput screening of single-atom catalysts confined in monolayer black phosphorus for efficient nitrogen reduction reaction

2023· article· en· W4386836254 on OpenAlexaff
Xiaoyan Li, Man-Yi Duan, Pengfei Ou

Bibliographic record

VenueNano Research · 2023
Typearticle
Languageen
FieldChemical Engineering
TopicAmmonia Synthesis and Nitrogen Reduction
Canadian institutionsUniversity of Toronto
Fundersnot available
KeywordsCatalysisChemistryMonolayerSelectivityElectrochemistryDensity functional theoryTransition metalNitrogenSubstrate (aquarium)Inorganic chemistryElectrocatalystRational designCombinatorial chemistryNanotechnologyMaterials scienceComputational chemistryPhysical chemistryElectrodeOrganic chemistry

Abstract

fetched live from OpenAlex

The discovery of metal-nitrogen centers as the active sites for electrolysis has aroused significant interest in utilizing single-atom catalysts for nitrogen reduction reaction (NRR). Properly designed nanostructured catalysts that strongly interact with nitrogen molecules (N 2 ) can promote adsorption and activation, thereby resulting in efficient catalysts with high stability, activity, and selectivity. In this study, using density functional theory calculations, we selected monolayer black phosphorus (BP) as the substrate and screened a series of single-atom transition metals confined in tri-coordinated and tetra-coordinated active centers (without and with N dopants) to electro-catalyze NRR. As a result, we have identified two promising candidates (Hf 1 -N 1 P 2 -1 and Tc 1 -N 4 ), which exhibit not only low overpotentials of 0.56 and 0.49 V but also high thermodynamic and electrochemical stability, as well as good selectivity towards NRR over the competing hydrogen evolution reaction. We also demonstrate the ability of Hf 1 -N 1 P 2 -1 and Tc 1 -N 4 to activate and hydrogenate N 2 by donating electrons and regulating charge transfer. This study not only predicts new BP-based promising catalysts but also provides guidance for the rational design of high-performance NRR electrocatalysts under ambient conditions.

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: Simulation or modeling · Consensus signal: none
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 head0.074
GPT teacher head0.327
Teacher spread0.253 · 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 designSimulation or modeling
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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