A Biomass‐Ligand‐Based Ru(III) Complex as a Catalyst for Cycloaddition of CO<sub>2</sub> and Epoxides to Cyclic Carbonates and a Study of the Mechanism

Mao, Haifang; Guo, Manli; Fu, Hong-Qing; Yin, Kun; Jin, Miaomiao; Wang, Chaoyang; Zhao, Yun; Dong, Zhenbiao; Liu, Jibo

doi:10.1002/ejic.202200624

Cited by 4 publications

(3 citation statements)

References 60 publications

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“…According to the experimental results and combined with previous reports, − the mechanism of the formation of cyclic carbonate catalyzed by ZnBr 2 -CP from CO 2 with epoxide was proposed, as shown in Figure . Both Lewis acid center Zn 2+ and the proton on the imidazole ring connected first to the O atom on the epoxide, resulting in C–O bond polarization to decrease the bond energy.…”

Section: Resultssupporting

confidence: 68%

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO₂ Fixation

Gu,

Zhao,

Liang

et al. 2023

ACS Appl. Polym. Mater.

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The development of efficient catalysts for the catalytic conversion of CO 2 is extremely important in the process of CO 2 chemistry. In this work, a Zn-based coordination polymer (ZnBr 2 -CP) was synthesized from a tridentate pyridine ligand bearing an imidazolium salt ligated with ZnBr 2 . It possesses not only the high activity of homogeneous catalysts but also the recoverable features of heterogeneous catalysts. More importantly, configured double active sites allow the catalyst ZnBr 2 -CP to exhibit excellent activity in the cycloaddition of CO 2 with epoxides under solvent-and co-catalyst-free conditions, achieving yields as high as 99% for a variety of cyclic carbonates at 80 °C for 24 h. This study provides insight into the design of efficient catalysts for conversion of CO 2 .

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Section: Resultssupporting

confidence: 68%

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO₂ Fixation

Gu,

Zhao,

Liang

et al. 2023

ACS Appl. Polym. Mater.

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“…(b) Conversion–time curve of CO 2 cycloaddition with 1a . (c) Comparison of TON and TOF values among various catalysts (1, NU-1000-RX; 2, Zn(dibpca)(OAc); 3, Cu-MOF; 4, {2Cu(L)(A)·3H 2 O} n ; 5, [Th 48 Ni 6 ]-MOF; 6, [Zn 3.5 (PDC) 2 (H 2 O) 10 ]; 7, (Me 2 NH 2 ) 1.5 [In 1.5 L 2 ]·2DMF·2H 2 O; 8, HKUST-1; 9, PCN-224(Co)-BPDC-CH 2 NBu 3 Br; 10, NUC-82a; 11, Zn-MOF-184; 12, SalRu). (d) Catalytic performance of catalyst 1 being used six consecutive times.…”

Section: Resultsmentioning

confidence: 99%

Metal Hydrogen-Bonded Organic Frameworks as Open Lewis Acid Catalysts for Two Types of CO₂ Transformations

Liu,

Zheng,

Zhang

et al. 2024

Inorg. Chem.

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Efficient and multiple CO2 utilization into high-value-added chemicals holds significant importance in carbon neutrality and industry production. However, most catalysis systems generally exhibit only one type of CO2 transformation with the efficiency to be improved. The restricted abundance of active catalytic sites or an inefficient utilization rate of these sites results in the constraint. Consequently, we designed and constructed two metal hydrogen-bonded organic frameworks (M-HOFs) {[M3(L3–)2(H2O)10]·2H2O} n (M = Co (1), Ni (2); L = 1-(4-carboxyphenyl)-1H-pyrazole-3,5-dicarboxylic acid) in this research. 1 and 2 are well-characterized, and both show excellent stability. The networks connected by multiple hydrogen bonds enhance the structural flexibility and create accessible Lewis acidic sites, promoting interactions between the substrates and catalytic centers. This enhancement facilitates efficient catalysis for two types of CO2 transformations, encompassing both cycloaddition reactions with epoxides and aziridines to afford cyclic carbonates and oxazolidinones. The catalytic activities (TON/TOF) are superior compared with those of most other catalysts. These heterogeneous catalysts still exhibited high performance after being reused several times. Mechanistic studies indicated intense interactions between the metal sites and substrates, demonstrating the reason for efficient catalysis. This marks the first instance on M-HOFs efficiently catalyzing two types of CO2 conversions, finding important significance for catalyst design and CO2 utilization.

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“…Cyclic carbonates possess desirable properties such as non-toxicity, flame retardancy, high dipole moment, and a high boiling point. They can be utilized as effective clean polar solvents, battery electrolytes [5], antifreeze additives [6], and reaction intermediates [7,8].…”

Section: Introductionmentioning

confidence: 99%

Ring-Opening Polymerization of Cyclohexene Oxide and Cycloaddition with CO2 Catalyzed by Amine Triphenolate Iron(III) Complexes

Li,

Dai

et al. 2024

Molecules

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A series of novel amine triphenolate iron complexes were synthesized and characterized using UV, IR, elemental analysis, and high-resolution mass spectrometry. These complexes were applied to the ring-opening polymerization (ROP) of cyclohexene oxide (CHO), demonstrating excellent activity (TOF > 11050 h−1) in the absence of a co-catalyst. In addition, complex C1 maintained the dimer in the presence of the reaction substrate CHO, catalyzing the ring-opening polymerization of CHO to PCHO through bimetallic synergy. Furthermore, a two-component system consisting of iron complexes and TBAB displayed the ability to catalyze the reaction of CHO with CO2, resulting in the formation of cis-cyclic carbonate with high selectivity. Complex C4 exhibited the highest catalytic activity, achieving 80% conversion of CHO at a CHO/C4/TBAB molar ratio of 2000/1/8 and a CO2 pressure of 3 MPa for 16 h at 100 °C, while maintaining >99% selectivity of cis-cyclic carbonates, which demonstrated good conversion and selectivity.

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A Biomass‐Ligand‐Based Ru(III) Complex as a Catalyst for Cycloaddition of CO₂ and Epoxides to Cyclic Carbonates and a Study of the Mechanism

Cited by 4 publications

References 60 publications

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO₂ Fixation

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO₂ Fixation

Metal Hydrogen-Bonded Organic Frameworks as Open Lewis Acid Catalysts for Two Types of CO₂ Transformations

Ring-Opening Polymerization of Cyclohexene Oxide and Cycloaddition with CO2 Catalyzed by Amine Triphenolate Iron(III) Complexes

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A Biomass‐Ligand‐Based Ru(III) Complex as a Catalyst for Cycloaddition of CO2 and Epoxides to Cyclic Carbonates and a Study of the Mechanism

Cited by 4 publications

References 60 publications

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO2 Fixation

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO2 Fixation

Metal Hydrogen-Bonded Organic Frameworks as Open Lewis Acid Catalysts for Two Types of CO2 Transformations

Ring-Opening Polymerization of Cyclohexene Oxide and Cycloaddition with CO2 Catalyzed by Amine Triphenolate Iron(III) Complexes

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A Biomass‐Ligand‐Based Ru(III) Complex as a Catalyst for Cycloaddition of CO₂ and Epoxides to Cyclic Carbonates and a Study of the Mechanism

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO₂ Fixation

A Zn-Based Coordination Polymer with Homogeneous Catalyst Properties for Efficient CO₂ Fixation

Metal Hydrogen-Bonded Organic Frameworks as Open Lewis Acid Catalysts for Two Types of CO₂ Transformations