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Record W3049239298 · doi:10.1021/acscatal.0c02680

Electrosynthesis of Ammonia Using Porous Bimetallic Pd–Ag Nanocatalysts in Liquid- and Gas-Phase Systems

2020· article· en· W3049239298 on OpenAlexaff
Mohammadreza Nazemi, Pengfei Ou, Abdulaziz Alabbady, Luke Soule, Alan Liu, Jun Song, Todd Sulchek, Meilin Liu, Mostafa A. El‐Sayed

Bibliographic record

VenueACS Catalysis · 2020
Typearticle
Languageen
FieldChemical Engineering
TopicAmmonia Synthesis and Nitrogen Reduction
Canadian institutionsMcGill University
FundersNational Science Foundation
KeywordsFaraday efficiencyElectrosynthesisElectrochemistryElectrolyteNanomaterial-based catalystChemical engineeringElectrolysisChemistryInorganic chemistryFaradaic currentReversible hydrogen electrodeMaterials scienceCatalysisElectrodeElectrode potentialWorking electrodeOrganic chemistryPhysical chemistry

Abstract

fetched live from OpenAlex

Cost-effective production of ammonia via electrochemical nitrogen reduction reaction (NRR) hinges on N2 electrolysis at high current densities with suitable selectivity and activity. Here, we report our findings in electrochemical NRR for ammonia synthesis using porous bimetallic Pd–Ag nanocatalysts in both gas-phase and liquid-phase electrochemical cells at current densities above 1 mA cm–2 under ambient conditions. While the gas-phase cell has lower Ohmic losses and higher energy efficiency, the liquid-phase cell achieved higher selectivity and Faradaic efficiency, attributed to the presence of concentrated N2 molecules dissolved in an aqueous electrolyte and the hydration effects. The liquid cell demonstrated notable performance for electrocatalytic NRR, achieving an NH3 production rate of 45.6 ± 3.7 μg cm–2 h–1 at a cell voltage of −0.6 V (vs RHE) and current density of 1.1 mA cm–2, corresponding to a Faradaic efficiency of ∼19.6% and an energy efficiency of ∼9.9%. Similarly, the gas-phase cell achieved a NH3 yield rate of 19.4 ± 2.1 μg cm–2 h–1 at −0.07 V (vs RHE) and 1.15 mA cm–2 with a Faradaic efficiency of 7.9% and an energy efficiency of 27.1%. Further, operando surface-enhanced Raman spectroscopy and density functional theory (DFT) are used to identify intermediate species relevant to the NRR at the electrode–electrolyte interfaces to provide insights into the NRR mechanism on Pd–Ag nanoparticles. This work highlights the importance of design and optimization of cell configuration in addition to the modification of the catalyst to achieve high-performance N2 electrolysis for ammonia synthesis.

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 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 score0.027
Threshold uncertainty score0.988

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.001
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 head0.020
GPT teacher head0.245
Teacher spread0.224 · 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.

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

Citations47
Published2020
Admission routes1
Has abstractyes

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