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Record W4223498063 · doi:10.1021/acscatal.2c00684

Disordered, Sub-Nanometer Ru Structures on CeO<sub>2</sub> are Highly Efficient and Selective Catalysts in Polymer Upcycling by Hydrogenolysis

2022· article· en· W4223498063 on OpenAlex
Linxiao Chen, Laura C. Meyer, Libor Kovařík, Debora Meira, Xavier Isidro Pereira Hernández, Honghong Shi, Konstantin Khivantsev, Oliver Y. Gutiérrez, János Szanyi

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.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueACS Catalysis · 2022
Typearticle
Languageen
FieldEnvironmental Science
TopicMicroplastics and Plastic Pollution
Canadian institutionsCanadian Light Source (Canada)
FundersBasic Energy Sciences
KeywordsHydrogenolysisPolyolefinCatalysisMaterials scienceCationic polymerizationCrystallinityChemical engineeringIsomerizationNanotechnologyChemistryOrganic chemistryPolymer chemistryComposite material

Abstract

fetched live from OpenAlex

Nondegradable polyolefin plastics pose severe environmental threats and thus demand efficient upcycling technologies. In this work, we discovered that low-loading (≤0.25 wt %) Ru/CeO2 exhibits remarkable catalytic performance in the hydrogenolysis of polypropylene (PP), polyethylene (PE), and n-C16H34 that is superior to high-loading (≥0.5 wt %) Ru/CeO2. They possess high PP conversion efficiency (sevenfold increase over current literature reports), low selectivity toward undesired CH4, and good isomerization ability. In the low-loading range, the intrinsic activity of Ru in PP hydrogenolysis increases as the particle size decreases, opposite of the trend in the high-loading range. Detailed characterization revealed that the abrupt changes in catalytic behaviors coincide with Ru species transitioning from well-defined to highly disordered structures in the low-loading domain. The disordered Ru species were shown to be sub-nanometer in size and cationic. Mechanistically, the regioselectivity and the rate dependence on hydrogen pressure of C–C bond cleavage are different on low- and high-loading Ru/CeO2, both explained by the higher coverage of adsorbed hydrogen (*H) on low-loading Ru/CeO2. This work reveals the remarkable catalytic performance of highly disordered, sub-nanometer, cationic Ru species in polyolefin hydrogenolysis, opening immense opportunities to develop effective, selective, and versatile catalysts for plastic upcycling.

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)0.000
metaresearch head score (Gemma)0.000
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 score0.017
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
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 head0.003
GPT teacher head0.172
Teacher spread0.169 · 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