The synthesis of important organic chemicals through sustainable and green methods is always demanding for the scientific community. Fixation of carbon dioxide for this purpose is very attractive as CO2 is non‐toxic, easily available, naturally abundant, recyclable, non‐flammable and an inexpensive C1 resource, and also the concentration of CO2 (most responsible greenhouse gas) is reduced. This article demonstrates the synthesis of silver nanoparticles (AgNPs) by an eco‐friendly method and incorporation of the particles into a covalent organic framework in order to obtain a sustainable heterogeneous catalyst, AgN@COF. The catalyst has been characterized in detail by FT‐IR,UV‐Vis. spectroscopy, FE‐SEM, TEM, EDAX, XPS, PXRD, ICP‐AES, TG‐DTA and N2 absorption‐desorption studies. The synthesized catalyst is able to fix CO2 to terminal propargylic amine and propargylic alcohol for the production of 2‐oxazolidinones and α‐alkylidene cyclic carbonates, respectively, through two different catalytic pathways. In both catalytic protocols, one atmospheric carbon dioxide was used. Production of α‐alkylidene cyclic carbonates occurred at room temperature and solvent‐free condition, and 2‐oxazolidinones were obtained under mild reaction conditions. Moreover, the catalyst is recyclable and reusable. Its catalytic efficacy was preserved even after the use of six consecutive catalytic cycles.

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Mesoporous zirconium oxophosphate (MZrP‐1) composed of porous interconnected network and high specific surface area has been synthesized by using Pluronic P123 as template under evaporation‐induced self‐assembly (EISA) method. The prepared mesoporous material has been characterized by small‐angle powder X‐ray diffraction, UHR‐TEM (Ultra‐high Resolution‐Transmission Electron Microscopy) image analysis, and N2 adsorption‐desorption, FTIR (Fourier‐transform Infrared Spectroscopy) and FE‐SEM (Field Emission‐Scanning Electron Microscopy) analysis. Mesoporous MZrP‐1 catalyst exhibited excellent catalytic activity for the synthesis of cyclic acetals from glycerol and cyclic carbonates from epoxide as starting under solvent‐free green conditions. High surface area and abundant acid sites present at the surface of the mesoporous zirconium oxophosphate is responsible for high catalytic activity. The catalyst can be reusable for several reaction cycles without any significant loss in its catalytic activity.

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