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Record W3009486424 · doi:10.1021/jacs.9b13347

Enhanced Nitrate-to-Ammonia Activity on Copper–Nickel Alloys via Tuning of Intermediate Adsorption

2020· article· en· W3009486424 on OpenAlexafffund
Yuhang Wang, Aoni Xu, Ziyun Wang, Linsong Huang, Jun Li, Fengwang Li, Joshua Wicks, Mingchuan Luo, Dae‐Hyun Nam, Chih‐Shan Tan, Yu Ding, Jiawen Wu, Yanwei Lum, Cao‐Thang Dinh, David Sinton, Gengfeng Zheng, Edward H. Sargent

Bibliographic record

VenueJournal of the American Chemical Society · 2020
Typearticle
Languageen
FieldChemical Engineering
TopicAmmonia Synthesis and Nitrogen Reduction
Canadian institutionsUniversity of Toronto
FundersNatural Sciences and Engineering Research Council of CanadaMitacsUniversity of TorontoGovernment of CanadaOffice of ScienceGovernment of OntarioCanadian Light SourceCanadian Institute for Advanced ResearchArgonne National LaboratoryOntario Centres of ExcellenceU.S. Department of Energy
KeywordsChemistryCatalysisAdsorptionElectrochemistryNickelAmmoniaAlloyCopperNitrateInorganic chemistryHydrogenAmmonia productionDensity functional theoryElectrodePhysical chemistryComputational chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Electrochemical conversion of nitrate (NO 3 – ) into ammonia (NH 3 ) recycles nitrogen and offers a route to the production of NH 3, which is more valuable than dinitrogen gas. However, today’s development of NO 3 – electroreduction remains hindered by the lack of a mechanistic picture of how catalyst structure may be tuned to enhance catalytic activity. Here we demonstrate enhanced NO 3 – reduction reaction (NO 3 – RR) performance on Cu 50 Ni 50 alloy catalysts, including a 0.12 V upshift in the half-wave potential and a 6-fold increase in activity compared to those obtained with pure Cu at 0 V vs reversible hydrogen electrode (RHE). Ni alloying enables tuning of the Cu d- band center and modulates the adsorption energies of intermediates such as *NO 3 –, *NO 2, and *NH 2 . Using density functional theory calculations, we identify a NO 3 – RR-to-NH 3 pathway and offer an adsorption energy–activity relationship for the CuNi alloy system. This correlation between catalyst electronic structure and NO 3 – RR activity offers a design platform for further development of NO 3 – RR catalysts.

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 score0.003
Threshold uncertainty score0.006

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 head0.014
GPT teacher head0.241
Teacher spread0.228 · 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

Citations1,336
Published2020
Admission routes2
Has abstractyes

Explore more

Same venueJournal of the American Chemical SocietySame topicAmmonia Synthesis and Nitrogen ReductionFrench-language works237,207