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Electric Field Effects in Electrochemical CO<sub>2</sub> Reduction

2016· article· en· 673 citations· W2522135447 on OpenAlex· 10.1021/acscatal.6b02299

Why is this work in the frame?

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

Canadian funderA Canadian agency funded it. The work may carry no Canadian affiliation at all.

No Canadian affiliation. An affiliation-only frame — the usual design — would never have seen this work. It is one of the works that make the case for inverting the frame.

Machine scores (provisional)

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

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.

Opus teacher head0.004
GPT teacher head0.222
Teacher spread
0.217 · how far apart the two teachers sit on this one work
Validation status
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Abstract

Electrochemical reduction of CO 2 has the potential to reduce greenhouse gas emissions while providing energy storage and producing chemical feedstocks. A mechanistic understanding of the process is crucial to the discovery of efficient catalysts, and an atomistic description of the electrochemical interface is a major challenge due to its complexity. Here, we examine the CO 2 → CO electrocatalytic pathway on Ag(111) using density functional theory (DFT) calculations and an explicit model of the electrochemical interface. We show that the electric field from solvated cations in the double layer and their corresponding image charges on the metal surface significantly stabilizes key intermediates—*CO 2 and *COOH. At the field-stabilized sites, the formation of *CO is rate-determining. We present a microkinetic model that incorporates field effects and electrochemical barriers from ab initio calculations. The computed polarization curves show reasonable agreement with experiment without fitting any parameters.

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.

The record

Venue
ACS Catalysis
Topic
CO2 Reduction Techniques and Catalysts
Field
Energy
Canadian institutions
Funders
Basic Energy SciencesNatural Sciences and Engineering Research Council of CanadaOffice of ScienceU.S. Department of Energy
Keywords
Density functional theoryElectrochemistryAb initioChemistryPolarization (electrochemistry)CatalysisElectric fieldChemical physicsAb initio quantum chemistry methodsComputational chemistryMoleculeElectrodePhysical chemistryOrganic chemistry
Has abstract in OpenAlex
yes