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Record W4404638613 · doi:10.26434/chemrxiv-2024-ln5f6

Migrative Reductive Amination of Ketones Enabled by Multitasking Reagents

2024· preprint· en· W4404638613 on OpenAlexafffund
Artem Khegay, Dennis G. Hall

Bibliographic record

VenueChemRxiv · 2024
Typepreprint
Languageen
FieldBiochemistry, Genetics and Molecular Biology
TopicChemical Synthesis and Analysis
Canadian institutionsUniversity of Alberta
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsReductive aminationReagentChemistryCombinatorial chemistryDrug discoveryPiperidineAminationChemical spaceHuman multitaskingOrganic synthesisMoleculeOrganic chemistryCatalysis

Abstract

fetched live from OpenAlex

Skeletal editing and “single-atom logic” are emerging strategies that accelerate compound synthesis and open new chemical space by modifying organic molecules using unconventional bond forming processes. These new strategies are particularly attractive to access important biologically active classes of compounds, such as secondary amines, which are key synthetic intermediates and components found in numerous pharmaceutical agents. Herein, a practical modification of the classical reductive amination of ketones and aldehydes, a staple reaction in drug discovery research, was developed to provide isomeric amines by way of a migratory reductive amination (MRA). This one-pot method combines three distinct chemical reactions in a single flask, without solvent changes, via the orchestrated addition of two inexpensive and non-toxic multitasking reagents: Zn(II) salts and a hydrosilane. Both reagents display exceptional orthogonality with a synergetic role in all three stages of the process, lending a procedure that embodies many of the ideals of green chemistry. This MRA method demonstrates a wide scope of acyclic and cyclic ketones and aldehydes with aliphatic or aromatic groups, including complex molecules such as drug intermediates and natural products with an exceptionally low E-factor compared to established methods. Remarkably, MRA enables the expeditious preparation of cyclic secondary amines of varying ring size, including a cyclopentanone-to-piperidine ring-edit that provides a direct access to the most common saturated heterocycle in drug discovery.

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)0.0010.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
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 head0.010
GPT teacher head0.260
Teacher spread0.250 · 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

Citations0
Published2024
Admission routes2
Has abstractyes

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