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Record W4396906948 · doi:10.1016/j.xcrp.2024.101977

Sequential electrocatalytic reactions along a membrane electrode assembly drive efficient nitrate-to-ammonia conversion

2024· article· en· W4396906948 on OpenAlexafffund
Tiange Yuan, Min Li, Siddhartha Subramanian, Jesse Kok, Mengran Li, Atsushi Urakawa, Oleksandr Voznyy, Thomas Burdyny

Bibliographic record

VenueCell Reports Physical Science · 2024
Typearticle
Languageen
FieldChemical Engineering
TopicAmmonia Synthesis and Nitrogen Reduction
Canadian institutionsUniversity of Toronto
FundersAustralian Research CouncilUniversity of Toronto ScarboroughNatural Sciences and Engineering Research Council of CanadaMitacsCanada Foundation for Innovation
KeywordsAmmoniaElectrodeNitrateMembraneInorganic chemistryMembrane electrode assemblyChemistryChemical engineeringMaterials scienceOrganic chemistryEngineeringAnodeBiochemistry

Abstract

fetched live from OpenAlex

Electrochemical ammonia (NH3) synthesis from nitrate (NO3-) (NO3RR) offers a promising green alternative to the fossil fuel-based Haber-Bosch approach to support the increasing global demand for nitrogen fertilizers, while removing environmental waste. Previous efforts have centered on designing catalysts to promote the direct conversion from NO3- àNH3 while suppressing the two-step reaction pathway: NO3- àNO2-àNH3. We took the view that efficient NO3RR is possible on simple catalysts by instead promoting the two-step reaction process, and using chemical reactor principles in a membrane electrode assembly (MEA) to drive high ammonia current densities and Faradaic efficiency, despite nitrite intermediates. Here we use an unmodified copper catalyst in an MEA and control reactivity through current density, flow rate, and electrolyte recycling. We show that balancing the electrolyte flow rates with current density results in ideal residence times of NO2- by-products, allowing for 91% FENH3 in a 5 cm2 electrolyzer with a NO3- to NH3 partial current 1.8 A. Full NO3- conversion was also achieved via recycling with FENH3 maintained > 60% with H2 as a by-product. Importantly this work shows how traditional engineering principles can substantially boost ammonia production, even for simple 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 score0.001
Threshold uncertainty score0.003

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 science0.0010.000
Research integrity0.0010.000
Insufficient payload (model declined to judge)0.0010.001

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 head0.008
GPT teacher head0.241
Teacher spread0.233 · 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

Citations10
Published2024
Admission routes2
Has abstractyes

Explore more

Same venueCell Reports Physical Science→Same topicAmmonia Synthesis and Nitrogen Reduction→French-language works237,207→