Spin engineering of single-site metal catalysts
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.
Full frame distilled prediction
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.
- Candidate categories
- none
- Consensus categories
- none
- Domain
- Candidate signal: noneConsensus signal: none
- Study design
- Candidate signal: Bench or experimentalConsensus signal: Bench or experimental
- Genre
- Candidate signal: EmpiricalConsensus signal: Empirical
- Teacher disagreement score
- 0.086
- Threshold uncertainty score
- 0.284
- Validation status
machine_predicted_unvalidated·codex-gemma-dda1882f352a
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.002 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
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.
- Teacher spread
- 0.199 · 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
•Single-site FeN4 species are designed to dangle over axial carbon micropores (d-FeN4)•d-FeN4 shows much superior oxygen reduction reactivity to traditional FeN4•d-FeN4 facilitates the formation of singlet-state oxygen-containing species with optimized spin states by micropore•This work provides in-depth understanding of spin tuning for advanced catalyst design Single-site metal atoms (SMAs) on supports are attracting extensive interest as new catalytic systems because of maximized atom utilization and superior performance. However, rational design of configuration-optimized SMAs with high activity from the perspectives of fundamental electron spin is highly challenging. Herein, N-coordinated Fe single atoms are successfully distributed over axial carbon micropores to form dangling-FeN4 centers (d-FeN4). This unique d-FeN4 demonstrates much higher intrinsic activity toward oxygen reduction reaction (ORR) in HClO4 than FeN4 without micropore underneath and commercial Pt/C. Both theoretical calculation and electronic structure characterization imply that d-FeN4 endows central Fe with medium spin (t2g4 eg1), which provides a spin channel for electron transition compared with FeN4 with low spin. This leads to the facile formation of the singlet state of oxygen-containing species from triplet oxygen during the ORR, thus showing faster kinetics than FeN4. This work provides an in-depth understanding of spin tuning on SMAs for advanced energy catalysis. Single-site metal atoms (SMAs) on supports are attracting extensive interest as new catalytic systems because of maximized atom utilization and superior performance. However, rational design of configuration-optimized SMAs with high activity from the perspectives of fundamental electron spin is highly challenging. Herein, N-coordinated Fe single atoms are successfully distributed over axial carbon micropores to form dangling-FeN4 centers (d-FeN4). This unique d-FeN4 demonstrates much higher intrinsic activity toward oxygen reduction reaction (ORR) in HClO4 than FeN4 without micropore underneath and commercial Pt/C. Both theoretical calculation and electronic structure characterization imply that d-FeN4 endows central Fe with medium spin (t2g4 eg1), which provides a spin channel for electron transition compared with FeN4 with low spin. This leads to the facile formation of the singlet state of oxygen-containing species from triplet oxygen during the ORR, thus showing faster kinetics than FeN4. This work provides an in-depth understanding of spin tuning on SMAs for advanced energy 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.
The record
- Venue
- The Innovation
- Topic
- Electrocatalysts for Energy Conversion
- Field
- Energy
- Canadian institutions
- Western University
- Funders
- Basic Energy SciencesProgram of Shanghai Academic Research LeaderOffice of ScienceNatural Sciences and Engineering Research Council of CanadaU.S. Department of EnergyState Key Laboratory of ASIC and System, Fudan UniversityNational Natural Science Foundation of China
- Keywords
- Spin (aerodynamics)CatalysisMicroporous materialSinglet stateSpin statesSpin crossoverTransition metalChemistryNanotechnologyChemical physicsMaterials scienceAtomic physicsCrystallographyPhysicsInorganic chemistryThermodynamicsExcited state
- Has abstract in OpenAlex
- yes