Paving the road towards automated homogeneous catalyst design

ChemPlusChem, Journal Year: 2024, Volume and Issue: 89(7)

Published: Jan. 26, 2024

In the past decade, computational tools have become integral to catalyst design. They continue offer significant support experimental organic synthesis and catalysis researchers aiming for optimal reaction outcomes. More recently, data-driven approaches utilizing machine learning garnered considerable attention their expansive capabilities. This Perspective provides an overview of diverse initiatives in realm design introduces our automated tailored high-throughput silico exploration chemical space. While valuable insights are gained through methods analysis space, degree automation modularity key. We argue that integration data-driven, modular workflows is key enhancing homogeneous on unprecedented scale, contributing advancement research.

Language: Английский

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Base- and Additive-Free Carbon Dioxide Hydroboration to Methoxyboranes Catalyzed by Non-Pincer-Type Mn(I) Complexes

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(8), P. 5236 - 5244

Published: March 31, 2023

Well-defined, bench stable Mn(I) non-pincer-type complexes were tested as earth-abundant transition metal catalysts for the selective reduction of CO2 to boryl-protected MeOH in presence pinacolborane (HBpin). Essentially, quantitative yields obtained under mild reaction conditions (1 bar CO2, 60 °C), without need any base or additives, alkylcarbonyl bis(phosphine) fac-[Mn(CH2CH2CH3)(dippe)(CO)3] [Mn1, dippe = 1,2-bis(diisopropylphosphino)ethane] and [Mn(dippe)(CO)2{(μ-H)2(Bpin)}] (Mn4), that is by bench-stable precatalyst Mn1 with HBpin via elimination butanal. Preliminary mechanistic details a combination NMR experiments monitoring catalytic reactions.

Language: Английский

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Automated de Novo Design of Olefin Metathesis Catalysts: Computational and Experimental Analysis of a Simple Thermodynamic Design Criterion

Journal of Chemical Information and Modeling, Journal Year: 2024, Volume and Issue: 64(2), P. 412 - 424

Published: Jan. 10, 2024

Methods for computational de novo design of inorganic molecules have paved the way automated homogeneous catalysts. Such studies so far relied on correlation-based prediction models as fitness functions (figures merit), but soundness these approaches has yet to be tested by experimental verification novo-designed Here, a previously developed criterion optimization dative ligands L in ruthenium-based olefin metathesis catalysts RuCl2(L)(L′)(═CHAr), where Ar is an aryl group and L′ phosphine ligand dissociating activate catalyst, was used experiments. These experiments predicted bearing N-heterocyclic carbene (L = 9) substituted two N-bound mesityls tert-butyl groups at imidazolidin-2-ylidene backbone promising. Whereas phosphine-stabilized precursor assumed model could not made, pyridine-stabilized ruthenium alkylidene complex (17) 9 less active than known leading Grubbs-type catalyst (18, H2IMes). A density functional theory-based analysis showed that unsubstituted metallacyclobutane (MCB) intermediate generated presence ethylene likely resting state both 17 18. via its correlation between stability MCB rate-determining barrier indeed seeks stabilize MCB, it relies RuCl2(L)(L′)(═CH2) adducts states. The change explains discrepancy actual performance 17. To avoid such discrepancies better address multifaceted challenges predicting catalytic performance, future should explore test criteria incorporating information from more single relative energy or intermediate.

Language: Английский

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Thermodynamically Leveraged Solventless Aerobic Deconstruction of Polyethylene-Terephthalate Plastics Over a Single-Site Molybdenum-Dioxo Catalyst

Green Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This study reports the ambient catalytic depolymerization of PET under solvent-free conditions, using a carbon-supported single-site molybdenum-dioxo catalyst.

Language: Английский

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Application of Nickel Copper Ferrite Nanoparticles Immobilized on Mesoporous Carbon as a Novel Reusable Catalyst for the Synthesis of 14‐Aryl‐14‐H‐Dibenzo [a,j]Xanthene Derivatives

Applied Organometallic Chemistry, Journal Year: 2025, Volume and Issue: 39(3)

Published: Feb. 25, 2025

ABSTRACT Xanthenes are widely used in pharmacology, and other essential fields, making them a global derivative. An endeavor strategy for one‐pot synthesis of 14‐aryl‐14‐H‐dibenzo[a,j]xanthene derivatives has been contributed through reaction between various aldehydes 2‐naphthol the presence NiCuFe 2 O 4 immobilized on carbon mesoporous (Ni/Cu/Fe 3 @MPCS) as recoverable reactive catalyst. This nanocomposite was catalyst this to provide quicker easier process with energy readily available, biodegradable non‐toxic ethanol solvent. provides promising pathway synthesize 14‐aryl‐14‐H‐dibenzo[a,j]xanthene, allowing its recyclability without any noticeable decline catalytic performance. Characterization prepared conducted utilizing different methods, counting FT‐IR, XRD, FE‐SEM, EDS, BET, TGA, VSM, Elemental mapping techniques. The results recommend that novel possesses potential be profitable tool improvement modern engineered approaches broad range applications.

Language: Английский

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One-pot facile synthesis of ruthenium nanoparticles with Co3O4 support at room temperature to enhance the catalytic efficiency in 4-nitrophenol reduction

Journal of Water Process Engineering, Journal Year: 2025, Volume and Issue: 75, P. 107866 - 107866

Published: May 9, 2025

Language: Английский

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Antioxidant-driven activity and stability enhancement in multiphase bicarbonate hydrogenation catalysis with a Ru-PNP pincer complex

Journal of CO2 Utilization, Journal Year: 2024, Volume and Issue: 81, P. 102718 - 102718

Published: Feb. 24, 2024

Herein, we present a practical strategy to enhance the performance of multiphase system for bicarbonate hydrogenation based on molecular Ru-PNP pincer catalyst. This study demonstrates that use organic antioxidants not only mitigates catalyst degradation but also significantly boosts its intrinsic activity. enables efficient recycling at ultra-low concentrations. Systematic screening and optimization range has identified TDTBP (tris(2,4-di-tert-butylphenyl) phosphite) as being exceptionally in stabilizing enhancing With optimized an unprecedented integral turnover frequency (TOF) 115,000 h−1 total number (TTON) 9.43×106 across four tests were demonstrated, conducted reaction temperature 90 ºC H2 pressure 50 bar. These findings represent substantial advancement sustainable formate/formic acid production, offering scalable highly method suitable industrial-scale application.

Language: Английский

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Topological graphs: a review of some of our achievements and perspectives in physical chemistry and homogeneous catalysis

Comptes Rendus Chimie, Journal Year: 2024, Volume and Issue: 27(S5), P. 1 - 23

Published: Nov. 27, 2024

This paper reviews some of our developments in algorithmic graph theory, with applications physical chemistry and catalysis. Two levels granularity the topological graphs have been developed: atomistic 2D-MolGraphs coarse-grained polygraphs H-bonded cycles. These implemented key algorithms isomorphism polymorphism, order to analyze molecular dynamics simulations complex systems. are transferable without modification from "simple" gas molecules, liquids, more inhomogeneous interfaces between solid liquid for instance. We show hereby that use theory provides a direct fast approach identify actual conformations sampled over time trajectory. Graphs transitions can also be extracted, showing at first glance all interconversions these conformations. H-bond networks condensed matter systems such as aqueous shown easily captured through graphs. how included automated high-throughput silico reactivity workflows, essential they decisive steps taken workflows. The cycles flexible molecules hexapeptide phase. Cet article passe en revue certains de nos développements dans le domaine la théorie algorithmique des graphes, avec quelques physico-chimie et catalyse. Deux niveaux granularité les graphes topologiques ont été développés : atomistiques polygraphes à gros grain liaisons hydrogènes. Ces mis œuvre algorithmes clés l'isomorphisme du polymorphisme, pour l'analyse l'interprétation trajectoires dynamique moléculaire systèmes moléculaires complexes. peuvent être transférés sans molécules présentes phase gazeuse aux liquides, passant par inhomogènes plus complexes entre un solide liquide, exemple. Nous montrons ici que l'utilisation fournit une approche directe rapide identifier réelles qui sont échantillonnées au fil temps trajectoire. Des également extraits, montrant d'un seul coup d'œil toutes ces Les réseaux hydrogènes matière condensée, tels aqueuses, facilement capturés topologiques. comment inclus flux travail automatisés réactivité haut débit, quel point ils essentiels certaines étapes décisives franchir travail. se révèlent flexibles telles qu'un gazeuse.

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Model-based evaluation and data requirements for parallel kinetic experimentation and data-driven reaction identification and optimization

Digital Discovery, Journal Year: 2023, Volume and Issue: 2(4), P. 994 - 1005

Published: Jan. 1, 2023

Chemfit uses kinetic data to facilitate the discovery of rates within chemical models, quantification model accuracy, and exploration quality quantity requirements needed for reliable parameter discovery.

Language: Английский

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Micropores in Hollow Organic Cage Nanocapsule as a Size Exclusion Gate: Cage Entrapped Pd(II)-Catalyst for Efficient Cross-Coupling Reaction

Langmuir, Journal Year: 2024, Volume and Issue: 40(17), P. 8820 - 8826

Published: April 15, 2024

Hollow porous organic capsules (HPOCs) with an entrapped active catalyst have nanosized cavities, providing the benefits of a nanoreactor, as well separation catalysts from reaction medium via pores acting size-exclusion gate. Such purpose-built HPOCs desired molecular weight cutoffs offer advantages semipermeable membrane and sustainable chemical process that excludes energy-extensive separation. Here, we report newly synthesized HPOC Pd(PPh3)2Cl2 for demonstrating Suzuki–Miyaura coupling proof concept.

Language: Английский

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