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Record W4388703196 · doi:10.26434/chemrxiv-2023-jbz23

Supported metal catalysts with single-atom promoters via reductive atom trapping

2023· preprint· en· W4388703196 on OpenAlexfundno aff
Dong Jiang, Hien N. Pham, Yixiao Li, Yubing Lu, Wenda Hu, Gang Wan, Chaochao Dun, Junrui Li, Carlos Garcia Vargas, Yipeng Sun, Anthony W. Savoy, Weixin Huang, Rui Zhang, Andrew DeLaRiva, R. Soyoung Kim, Xiang Li, Jeffrey J. Urban, Junko Yano, K. M. Shelly, Cheng‐Jun Sun, Konstantin Khivantsev, Christopher J. Tassone, Jian Zhi Hu, János Szanyi, Abhaya K. Datye, Yong Wang

Bibliographic record

VenueChemRxiv · 2023
Typepreprint
Languageen
FieldMaterials Science
TopicCatalytic Processes in Materials Science
Canadian institutionsnot available
FundersSLAC National Accelerator LaboratoryArgonne National LaboratoryBasic Energy SciencesU.S. Department of EnergyOffice of Energy Efficiency and Renewable EnergyOffice of ScienceCanadian Light Source
KeywordsCatalysisCeriumMaterials scienceCerium oxideOxygen storageAtom (system on chip)NanoparticleRhodiumMetalNanotechnologyChemical engineeringChemistryOrganic chemistryMetallurgy

Abstract

fetched live from OpenAlex

Nanosized cerium oxide (CeO2) has been extensively used as an oxygen storage component in automotive emission control systems. However, the possible involvement of atomically dispersed cerium (Ce) has not been explored. Here, we demonstrate the controllable transformation of CeO2 nanoparticles into isolated Ce1 cations on the surface of gamma-type alumina (γ-Al2O3) via reductive atom trapping, achieving over half-monolayer coverage. Supported single-atom rhodium (Rh1) surrounded by dispersed Ce1 shows superior performance to Rh1 on bare Al2O3 or crystalline CeO2 in catalyzing NO reduction, exhibiting a striking one-order-of-magnitude increase in turnover frequency. Dispersed Ce1 also exhibits greatly enhanced oxygen transfer capability and introduces a modified reaction mechanism that involves adjacent Rh1-Ce1 dual-sites, resulting in a greatly decreased activation barrier (96 vs. 192 kJ/mol). The understanding of reductive atom trapping of Ce1 as well as its structure-property relationships obtained in this work could be implemented in the rational design of Ce1-promoted catalysts for many other applications. Benefiting from the greatly enhanced OSC, activity enhancements are also seen with Ce1-promoted platinum nanoparticles for the oxidation of CO and hydrocarbons. Additionally, dispersing Ce1 on Al2O3 results in modified surface properties, which could be further utilized to explore the field of acid-base 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.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation 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 score0.001
Threshold uncertainty score0.003

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0010.001

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 head0.040
GPT teacher head0.270
Teacher spread0.230 · 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 source (direct Gemma or distilled Codex), 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

Citations1
Published2023
Admission routes1
Has abstractyes

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