An lcy-topology amino acid MOF as eco-friendly catalyst for cyclic carbonate synthesis from CO<sub>2</sub>: Structure-DFT corroborated study

Kathalikkattil, Amal Cherian; Babu, Robin; Roshan, Roshith; Lee, Hankyul; Kim, Hyungjun; Tharun, Jose; Suresh, Eringathodi; Park, Dae‐Won

doi:10.1039/c5ta05688h

Cited by 117 publications

(64 citation statements)

References 71 publications

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“…As summarized in Table 1 , MOFs have been reported to catalyze CO 2 with the epoxides shown in Figure , under different reaction conditions. These MOFs are further categorized into four subcategories based on different catalytic sites . The subcategories promoting catalysis include: structural defects in the MOF, open metal sites from metal clusters, tandem Lewis acid sites from the metal cluster and organometallic linker, and co‐catalyst functionalized MOFs.…”

Section: Chemical Fixation Of Co2 With Epoxides Into Cyclic Organic Cmentioning

confidence: 99%

“…Representative studies for the chemical transformation of CO 2 with epoxides into cyclic organic carbonates using MOFs with unsaturated metal cations are reviewed . The accessible and unsaturated metal cations function as Lewis acid sites to activate the epoxide substrates, but these reactions require a co‐catalyst such as a Lewis base to open the epoxide ring.…”

Section: Chemical Fixation Of Co2 With Epoxides Into Cyclic Organic Cmentioning

confidence: 99%

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Metal‐Organic Frameworks for CO₂ Chemical Transformations

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Zhu

et al. 2016

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Carbon dioxide (CO ), as the primary greenhouse gas in the atmosphere, triggers a series of environmental and energy related problems in the world. Therefore, there is an urgent need to develop multiple methods to capture and convert CO into useful chemical products, which can significantly improve the environment and promote sustainable development. Over the past several decades, metal-organic frameworks (MOFs) have shown outstanding heterogeneous catalytic activity due in part to their high internal surface area and chemical functionalities. These properties and the ability to synthesize MOF platforms allow experiments to test structure-function relationships for transforming CO into useful chemicals. Herein, recent developments are highlighted for MOFs participating as catalysts for the chemical fixation and photochemical reduction of CO . Finally, opportunities and challenges facing MOF catalysts are discussed in this ongoing research area.

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Section: Chemical Fixation Of Co2 With Epoxides Into Cyclic Organic Cmentioning

confidence: 99%

Section: Chemical Fixation Of Co2 With Epoxides Into Cyclic Organic Cmentioning

confidence: 99%

Metal‐Organic Frameworks for CO₂ Chemical Transformations

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Zhu

et al. 2016

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“…The proposed mechanism is in agreement with recent studies based on experimental and DFT studies . Interestingly, ZnMOF‐1 showed a better catalytic efficiency in CO 2 epoxide cycloaddition than ZnMOF‐2 under the ambient reaction conditions tested.…”

Section: Resultsmentioning

confidence: 99%

Efficient Solvent‐Free Carbon Dioxide Fixation Reactions with Epoxides Under Mild Conditions by Mixed‐Ligand Zinc(II) Metal–Organic Frameworks

et al. 2018

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Mixed‐ligand 3 D/2 D Zn metal–organic frameworks (MOFs) {[Zn(bdc)(L1)]⋅x G}n (ZnMOF‐1) and {[Zn(ipa)(L2)]}n (ZnMOF‐2; in which H2BDC=benzene‐1,4‐dicarboxylic acid, L1=4‐pyridyl carboxaldehyde isonicotinoylhydrazone, H2IPA=isophthalic acid, L2=3‐pyridyl carboxaldehyde nicotinoyl hydrazone, and G=lattice guests) were synthesized using versatile synthetic routes that include a green mechanochemical (grinding) reaction. Chemical and thermal stability, phase purity, and characterization of the ZnMOFs synthesized by different approaches were established by using various analytical methods. Both ZnMOFs can be used as a highly active, solvent‐free, binary catalyst for CO2 cycloaddition with epoxides under ambient reaction conditions of 1 atm pressure and room temperature/40 °C, in the presence of the cocatalyst nBu4NBr. The yield, recyclability, and stability of ZnMOF‐1 as a potential catalyst towards epoxide to cyclic carbonate conversion are excellent under ambient conditions. From literature and experimental inferences, a rationalized mechanism mediated by the Zn center of ZnMOFs for the CO2‐epoxide cycloaddition reaction has been proposed. To the best of our knowledge, very few MOF‐based catalysts have been reported to realize the conversion of CO2 to useful products under similar mild conditions. In the present investigation, that is, catalyst preparation by green mechanochemical synthesis and catalysis under ambient, solvent‐free conditions were performed with minimum energy utilization.

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“…Some natural amino acids that contain dicarboxylate groups can be regarded as functional ligands to obtain various MOFs . For instance, cobalt‐aspartate MOF has been used as the precursor in the synthesis of porous tubular Co 3 O 4 .…”

Section: Various Precursors To Hierarchically Porous Micro‐/nanostrucmentioning

confidence: 99%

Morphology‐Conserved Transformations of Metal‐Based Precursors to Hierarchically Porous Micro‐/Nanostructures for Electrochemical Energy Conversion and Storage

et al. 2017

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To meet future market demand, developing new structured materials for electrochemical energy conversion and storage systems is essential. Hierarchically porous micro-/nanostructures are favorable for designing such high-performance materials because of their unique features, including: i) the prevention of nanosized particle agglomeration and minimization of interfacial contact resistance, ii) more active sites and shorter ionic diffusion lengths because of their size compared with their large-size counterparts, iii) convenient electrolyte ingress and accommodation of large volume changes, and iv) enhanced light-scattering capability. Here, hierarchically porous micro-/nanostructures produced by morphology-conserved transformations of metal-based precursors are summarized, and their applications as electrodes and/or catalysts in rechargeable batteries, supercapacitors, and solar cells are discussed. Finally, research and development challenges relating to hierarchically porous micro-/nanostructures that must be overcome to increase their utilization in renewable energy applications are outlined.

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An lcy-topology amino acid MOF as eco-friendly catalyst for cyclic carbonate synthesis from CO₂: Structure-DFT corroborated study

Abstract: A Zn(ii)-amino acid MOF catalyst and its use for CO2fixation are reported, in addition to corresponding structure-topology-DFT studies.

Cited by 117 publications

References 71 publications

Metal‐Organic Frameworks for CO₂ Chemical Transformations

Metal‐Organic Frameworks for CO₂ Chemical Transformations

Efficient Solvent‐Free Carbon Dioxide Fixation Reactions with Epoxides Under Mild Conditions by Mixed‐Ligand Zinc(II) Metal–Organic Frameworks

Morphology‐Conserved Transformations of Metal‐Based Precursors to Hierarchically Porous Micro‐/Nanostructures for Electrochemical Energy Conversion and Storage

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An lcy-topology amino acid MOF as eco-friendly catalyst for cyclic carbonate synthesis from CO2: Structure-DFT corroborated study

Abstract: A Zn(ii)-amino acid MOF catalyst and its use for CO2fixation are reported, in addition to corresponding structure-topology-DFT studies.

Cited by 117 publications

References 71 publications

Metal‐Organic Frameworks for CO2 Chemical Transformations

Metal‐Organic Frameworks for CO2 Chemical Transformations

Efficient Solvent‐Free Carbon Dioxide Fixation Reactions with Epoxides Under Mild Conditions by Mixed‐Ligand Zinc(II) Metal–Organic Frameworks

Morphology‐Conserved Transformations of Metal‐Based Precursors to Hierarchically Porous Micro‐/Nanostructures for Electrochemical Energy Conversion and Storage

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An lcy-topology amino acid MOF as eco-friendly catalyst for cyclic carbonate synthesis from CO₂: Structure-DFT corroborated study

Metal‐Organic Frameworks for CO₂ Chemical Transformations

Metal‐Organic Frameworks for CO₂ Chemical Transformations