ItemArticle

Free COOH-tethered layered Co(ii) framework and flexible composite as a size-reliant, tandem and robust catalyst for mild and scalable synthesis of bioactive molecules

Title
Free COOH-tethered layered Co(ii) framework and flexible composite as a size-reliant, tandem and robust catalyst for mild and scalable synthesis of bioactive molecules
Creator
Chand, Rudra; Mondal, Partha P.; Muthukumar, Devaraj; Pillai, Renjith S.; Neogi, Subhadip
Description
Pore-functionalization in metalorganic frameworks (MOFs) through the immobilization of free carboxylic sites offers a promising strategy for designing high-performance materials with potential applications, including selective and benign chemical transformations. However, this feat is tricky because of their extreme tendency to coordinate with the concerned metal ions. Herein, we developed a layer-stacked and thermo-chemically stable two-dimensional MOF, encompassing flanked carboxylic acid and [Co2(COO)4] unit-decked porous channel, using a mixed-ligand approach. The guest-free structure serves as a one-of-a-kind superior heterogeneous catalyst for tricomponent KnoevenagelMichael condensation, yielding a multitude of 2-amino-3-cyano-4H-pyrans with low catalyst loading, short duration and mild temperature compared to the majority of reported materials. The role of Lewis and Brsted acidic sites in the MOF catalyst is comprehensively supported by control experiments, analyte-induced emission articulation, inferior activity of a task-specific site-truncated iso-skeletal framework, and density-functional theory results. Importantly, the MOF demonstrated the first-ever deacetalization multi-component reaction (MCR) with admirable and recyclable conversion under relatively green conditions. Besides covering twenty-two electronically diverse substrates, the MOF can synthesize nine bioactive pyrans with excellent yield and gram scale. Notably, fifteen 4H-pyrans are first-time characterized in their purest forms via X-ray crystallography besides other spectro-analytical studies. Larger-sized substrates failed to diffuse inside MOF's micropores and illustrate unprecedented molecular-dimension-mediated MCR. The in situ-grafted MOF inside melamine-foam (MF) yielded a reconfigurable composite that promotes this one-pot reaction with similar activity and reusability to that of the sole MOF and demarcates a paradigm shift toward cutting-edge sustainable catalysis over a practical platform. This journal is The Royal Society of Chemistry, 2025
Source
Journal of Materials Chemistry A;Volume;13;Issue;47;pp.40741-40756
Date
01-01-2025
Publisher
Royal Society of Chemistry
Coverage
Chand R., Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India, Inorganic Materials & Catalysis Division, CSIR-Central Salt & Marine Chemicals Research Institute, Gujarat, Bhavnagar, 364002, India; Mondal P.P., Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India, Inorganic Materials & Catalysis Division, CSIR-Central Salt & Marine Chemicals Research Institute, Gujarat, Bhavnagar, 364002, India; Muthukumar D., Department of Chemistry, Christ University, Karnataka, Bangalore, 560029, India; Pillai R.S., Department of Chemistry, Christ University, Karnataka, Bangalore, 560029, India, Analytical and Spectroscopy Division, ASCG/PCM, Indian Space Research Organization, Vikram Sarabhai Space Centre, Thiruvananthapuram, Kerala, 695022, India; Neogi S., Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, 201002, India, Inorganic Materials & Catalysis Division, CSIR-Central Salt & Marine Chemicals Research Institute, Gujarat, Bhavnagar, 364002, India
Rights
Restricted Access; Hardcopy may be available in the library
Relation
ISSN: 20507488; CODEN: JMCAE
Format
online
Language
English
Type
Article

Citation

Chand, Rudra; Mondal, Partha P.; Muthukumar, Devaraj; Pillai, Renjith S.; Neogi, Subhadip, “Free COOH-tethered layered Co(ii) framework and flexible composite as a size-reliant, tandem and robust catalyst for mild and scalable synthesis of bioactive molecules,” CHRIST (Deemed To Be University) Institutional Repository, accessed June 19, 2026, https://archives.christuniversity.in/items/show/22596.

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