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Record W2530402207 · doi:10.1021/acscatal.6b01449

Understanding Catalytic Reactions over Zeolites: A Density Functional Theory Study of Selective Catalytic Reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub> over Cu-SAPO-34

2016· article· en· W2530402207 on OpenAlex

Why this work is in the frame

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

fundA Canadian funder is recorded on the work.
no affNo Canadian affiliation: this work is invisible to an affiliation-only frame.
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.

Bibliographic record

VenueACS Catalysis · 2016
Typearticle
Languageen
FieldMaterials Science
TopicCatalytic Processes in Materials Science
Canadian institutionsnot available
FundersFundamental Research Funds for the Central UniversitiesScience and Technology Commission of Shanghai MunicipalityQueen's UniversityShanghai Rising-Star ProgramNational Natural Science Foundation of China-Guangdong Joint FundMinistry of Science and Technology of the People's Republic of ChinaQueen's University BelfastMinistry of Education of the People's Republic of ChinaShanghai Municipal Education CommissionNational Natural Science Foundation of ChinaChina Scholarship CouncilShanghai Education Development Foundation
KeywordsCatalysisDensity functional theorySelective catalytic reductionNOxChemistrySelective reductionReduction (mathematics)Inorganic chemistryComputational chemistryPhysical chemistryOrganic chemistryCombustion

Abstract

fetched live from OpenAlex

Metal-exchanged CHA-type (SAPO-34 and SSZ-13) zeolites are promising catalysts for selective catalytic reduction (SCR) of NO x by NH 3 . However, an understanding of the process at the molecular level is still limited, which hinders the identification of its mechanism and the design of more efficient zeolite catalysts. In this work, modeling the reaction over Cu-SAPO-34, a periodic density functional theory (DFT) study of NH 3 -SCR was performed using the hybrid functional (HSE06) with the consideration of van der Waals (vdW) interactions. A mechanism with a low N–N coupling barrier is proposed to account for the activation of NO. The redox cycle of Cu 2+ and Cu +, which is crucial for the SCR process, is identified with detailed analyses. In addition, the decomposition of NH 2 NO is shown to readily occur on the Brønsted acid site by a hydrogen push–pull mechanism, confirming the collective efforts of Brønsted acid and Lewis acid (Cu 2+ ) sites. The special electronic and structural properties of Cu-SAPO-34 are demonstrated to play an essential role in the reaction, which may have general implications on the understanding of zeolite catalysis.

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.

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)0.002
metaresearch head score (Gemma)0.002
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
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 score0.008
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0020.002
Meta-epidemiology (narrow)0.0010.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0010.002
Science and technology studies0.0000.001
Scholarly communication0.0000.002
Open science0.0010.001
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 head0.025
GPT teacher head0.244
Teacher spread0.219 · 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