Threefold reactivity of a COF-embedded rhenium catalyst: reductive etherification, oxidative esterification or transfer hydrogenation

Goralski, Sean T.; Cid-Seara, Krystal M.; Jarju, Jenni J.; Rodríguez‐Lorenzo, Laura; LaGrow, Alec P.; Rose, Michael J.; Salonen, Laura M.

doi:10.1039/d2cc03173f

Cited by 3 publications

(1 citation statement)

References 45 publications

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“…Covalent organic frameworks (COFs) are polymeric crystalline porous network materials with high specific surface area, diverse structure, and adjustable composition. − Therefore, COFs have been widely studied in catalysis, adsorption, and energy storage. Due to the clear composition and ordered pore structure of the intrinsic COFs precursor, the carbon-based materials obtained by pyrolysis can retain the original properties of the COFs template, so they can provide more information on the structure of the carbon materials in the catalysts. , In addition, COFs usually contain N, S, P, and other heteroatoms, which are usually retained in the pyrolysis process. , Due to the differences in size, bond length, coordination, and charge between carbon and heteroatoms, heteroatoms can regulate the electronic structure of the carbon substrate and even produce the defect sites with local charge . Moreover, heteroatoms are usually Lewis base sites, which are easy to form strong interactions with metal oxide nanoparticles, thus promoting electron transfer .…”

Section: Introductionmentioning

confidence: 99%

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H₂ Evolution from NaBH₄

et al. 2023

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Developing nonprecious metal catalysts with fast charge transfer ability, abundant active sites, and easy recovery is of great significance toward sodium borohydride (NaBH 4 ) hydrolysis for hydrogen (H 2 ) production in alkaline solutions. Herein, magnetically separated nitrogen-doped carbonsupported cobalt oxide (Co x O y @NC) nanoparticles were prepared successfully by converting pyrazine-based covalent organic frameworks (COFs). Due to the porous structure and nitrogen-rich characteristics of the precursor, the prepared catalyst Co x O y @NC exhibited good conductivity and charge transfer ability. Cobalt oxide nanoparticles and nitrogen-doped carbon matrix are bonded by the Co−N bond, which makes full use of the conductivity of the substrate and the high activity of the cobalt oxide catalyst. Therefore, Co x O y @NC exhibits an excellent synergistic effect between Co x O y and NC. The H 2 generation rate reaches a maximum of 2082.13 mL/min/g from NaBH 4 in alkaline solutions. In addition, Co x O y @NC also exhibits good magnetic separation capability, which greatly simplifies the catalyst separation process. Density functional theory (DFT) calculation results indicate that Co 2+ is the dominant active component in the heterogeneous catalyst Co x O y @NC. This work broadens new horizons for the development of COFs derivative catalysts for hydrogen production from sodium borohydride hydrolysis.

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Section: Introductionmentioning

confidence: 99%

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H₂ Evolution from NaBH₄

et al. 2023

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Immobilized di(hydroperoxy)propane adducts of phosphine oxides as traceless and recyclable oxidizing agents

Hoefler

Perez

et al. 2023

Applied Surface Science

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Metallocavitins as Advanced Enzyme Mimics and Promising Chemical Catalysts

Shteinman

2023

Catalysts

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The supramolecular approach is becoming increasingly dominant in biomimetics and chemical catalysis due to the expansion of the enzyme active center idea, which now includes binding cavities (hydrophobic pockets), channels and canals for transporting substrates and products. For a long time, the mimetic strategy was mainly focused on the first coordination sphere of the metal ion. Understanding that a highly organized cavity-like enzymatic pocket plays a key role in the sophisticated functionality of enzymes and that the activity and selectivity of natural metalloenzymes are due to the effects of the second coordination sphere, created by the protein framework, opens up new perspectives in biomimetic chemistry and catalysis. There are two main goals of mimicking enzymatic catalysis: (1) scientific curiosity to gain insight into the mysterious nature of enzymes, and (2) practical tasks of mankind: to learn from nature and adopt from its many years of evolutionary experience. Understanding the chemistry within the enzyme nanocavity (confinement effect) requires the use of relatively simple model systems. The performance of the transition metal catalyst increases due to its retention in molecular nanocontainers (cavitins). Given the greater potential of chemical synthesis, it is hoped that these promising bioinspired catalysts will achieve catalytic efficiency and selectivity comparable to and even superior to the creations of nature. Now it is obvious that the cavity structure of molecular nanocontainers and the real possibility of modifying their cavities provide unlimited possibilities for simulating the active centers of metalloenzymes. This review will focus on how chemical reactivity is controlled in a well-defined cavitin nanospace. The author also intends to discuss advanced metal–cavitin catalysts related to the study of the main stages of artificial photosynthesis, including energy transfer and storage, water oxidation and proton reduction, as well as highlight the current challenges of activating small molecules, such as H2O, CO2, N2, O2, H2, and CH4.

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Threefold reactivity of a COF-embedded rhenium catalyst: reductive etherification, oxidative esterification or transfer hydrogenation

Abstract: The reactivity of the novel Re(i) catalyst [Re(C12Anth-py2)(CO)3Br] is modulated by its interactions with the covalent organic framework (COF) TFB-BD.

Cited by 3 publications

References 45 publications

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H₂ Evolution from NaBH₄

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H₂ Evolution from NaBH₄

Immobilized di(hydroperoxy)propane adducts of phosphine oxides as traceless and recyclable oxidizing agents

Metallocavitins as Advanced Enzyme Mimics and Promising Chemical Catalysts

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Threefold reactivity of a COF-embedded rhenium catalyst: reductive etherification, oxidative esterification or transfer hydrogenation

Abstract: The reactivity of the novel Re(i) catalyst [Re(C12Anth-py2)(CO)3Br] is modulated by its interactions with the covalent organic framework (COF) TFB-BD.

Cited by 3 publications

References 45 publications

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H2 Evolution from NaBH4

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H2 Evolution from NaBH4

Immobilized di(hydroperoxy)propane adducts of phosphine oxides as traceless and recyclable oxidizing agents

Metallocavitins as Advanced Enzyme Mimics and Promising Chemical Catalysts

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Product

Resources

About

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H₂ Evolution from NaBH₄

Covalent Organic Framework-Derived Nitrogen-Doped Carbon-Supported Cobalt Oxide Nanoparticles for Synergistic Boosting H₂ Evolution from NaBH₄