Nanoporous Thulium(III)–Organic Framework for High Catalytic Performance on the CO2-Epoxide Cycloaddition DOI
Fei Yang, Yan-Peng Gao,

Meiyu Ren

и другие.

Crystal Growth & Design, Год журнала: 2024, Номер unknown

Опубликована: Дек. 8, 2024

Considering that the greenhouse effect is most concerning environmental issue globally, selective capture and resource utilization of CO2 have attracted widespread attention. Herein, we report a highly robust thulium(III)–organic framework {[Tm2(μ2-OH)(CPPDDA)(H2O)2]·3DMF·2H2O}n (NUC-108), which obtained from exquisite combination undocumented multifunctional clusters [Tm4(μ2-OH)2(COO)10(H2O)4] organic ligands 4,4′-(4-(4-carboxyphenyl)pyridine-2,6-diyl)diisophthalic acid (H5CPPDDA). NUC-108 possesses following unique merits: (i) functional tetranuclear rare-earth serve as nodes, in Tm3+ ions can be activated Lewis sites μ2-OH anions are base sites; (ii) high-porosity zeolite architecture contains three kinds channels: 12.29 × 9.74 Å2 8.92 4.97 along b axis 12.76 8.95 c axis; (iii) uncoordinated pyridine moieties further endow host with functionality; (iv) resistance to weak acidic alkaline aqueous solutions well various solvents. Notably, NUC-108a effectively separate binary CO2/CH4 mixture high adsorption selectivity, should due enough basic groups moieties. Furthermore, under mild conditions without any solvent, also used an effective recoverable catalyst facilitate cycloaddition epoxides aid tetrabutylammonium bromide. Hence, these findings beneficial for guiding development stable active catalysts carbon utilization.

Язык: Английский

Robust Fluorine-Functionalized {Ln5}-Organic Frameworks for Excellent Catalytic Performance on Cycloaddition of CO2 with Epoxides and Knoevenagel Condensation DOI
Chong Li, Hongxiao Lv, Kun Yang

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2023, Номер 15(29), С. 35052 - 35061

Опубликована: Июль 12, 2023

Lanthanide-organic frameworks (LnOFs) are a class of promising catalysts on large number organic reactions because the higher coordination Ln3+ ions, inspired by which exploratory preparation cluster-based LnOFs was carried out us. Herein, exquisite combination spindly [Ln5(μ3-OH)6(CO2)6(H2O)6] clusters (abbreviated as {Ln5}) and fluorine-functionalized tetratopic ligand 2',3'-difluoro-[p-terphenyl]-3,3″,5,5″-tetracarboxylic acid (F-H4PTTA) engendered two highly robust isomorphic nanoporous {[Ln5(FPTTA)2(μ3-OH)6(H2O)6](NO3)}n (NUC-61, Ln = Ho Dy). NUC-61 compounds rarely reported {Ln5}-based 3D with nano-caged voids (19 Å × 17 Å), shaped twelve [Ln5(μ3-OH)6(COO)8] eight completely deprotonated F-PTTA4- ligands. Activated NUC-61a characterized plentiful coexisted Lewis acid-base sites open LnIII sites, capped μ3-OH, -F. Judged ideal adsorbed solution theory (IAST), activated NUC-61Ho-a had high CO2/CH4 adsorptive selectivity value 12.7 (CO2/CH4 50/50) 9.1 5/95) at 298 K, could lead to high-purity CH4 (≥99.9996%). Furthermore, catalytic experiments exhibited that NUC-61Ho-a, representative, efficiently catalyze cycloaddition CO2 epoxides well Knoevenagel condensation aldehydes malononitrile. This work proves skeletons chemical stability, heterogeneity, recyclability an excellent bifunctional catalyst for some reactions.

Язык: Английский

Процитировано

43
Bifunctional two-dimensional copper-organic framework for high catalytic performance on cycloaddition of CO2 with epoxides and deacetalization-Knoevenagel condensation DOI
Chong Li,

Youbin Liu,

Tuoping Hu

и другие.

Journal of Molecular Structure, Год журнала: 2024, Номер 1306, С. 137849 - 137849

Опубликована: Фев. 22, 2024

Язык: Английский

Процитировано

13
Robust Nitro-Functionalized {Zn3}-Organic Framework for Excellent Catalytic Performance on Cycloaddition Reaction of CO2 with Epoxides and Knoevenagel Condensation DOI

Meiyu Ren,

Chong Li,

Tuoping Hu

и другие.

Crystal Growth & Design, Год журнала: 2024, Номер 24(8), С. 3473 - 3482

Опубликована: Апрель 8, 2024

Adjusting the Lewis acid–base sites in MOF-based catalysts to meet demand for catalytic CO2 chemical fixation is a huge challenge. Herein, highly robust rectilinear {Zn3}-based metal–organic framework of {[Zn3(TNTNB)2(4,4′-bip)(H2O)2]·5DMF·9H2O}n (NUC-80) was generalized from solvothermal condition (H3TNTNB = 1,3,5-tri(3-nitro-4-carboxyphenyl)-2,4,6-trinitrobenzene, 4,4′-bip 4,4′-bipyridine). Activated NUC-80a not only owns large void volume (58%) and two kinds solvent-accessible channels: rhombic-like (ca. 14.24 × 14.57 Å) along axis rectangular-like 11.72 14.48 b axis, but also functionalized by rich metal plentiful nitro groups on its inner surface. Performed experiments confirmed that could efficiently catalyze cycloaddition reaction with epoxides Knoevenagel condensations aldehydes malononitrile under mild conditions high turnover frequency (TOF). Hence, this work provides nitro-functionalized cluster-based nanoporous wide range potential applications such as catalysis, gas adsorption, separation.

Язык: Английский

Процитировано

9
NH2-Functionalized InIIIDyIII−Organic Frameworks for Efficient Catalytic Performance on Chemical Fixation of CO2 and Knoevenagel Condensation DOI

Meiyu Ren,

Fei Yang, Yan-Peng Gao

и другие.

Journal of Molecular Structure, Год журнала: 2025, Номер unknown, С. 141361 - 141361

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

1
Robust {Cd4}-Organic Framework for Efficiently Catalyzing CO2 Cycloaddition and Knoevenagel Condensation DOI
Shurong Liu,

Tuoping Hu,

Kun Yang

и другие.

Crystal Growth & Design, Год журнала: 2023, Номер 23(5), С. 3320 - 3329

Опубликована: Апрель 20, 2023

The high-value-added carbonates generated from CO2 have attracted the attention of more and researchers because which optimization metal–organic framework (MOF)-based catalysts has seen a considerable upsurge at present. scarcely reported cadmium(II)-based MOFs inspire us to explore CdOFs with excellent catalytic activity high reusability. Herein, unification unreported {Cd4(μ3-OH)2(CH3CO2–)} cluster 2,6-bis(2,4-dicarboxylphenyl)-4-(4-carboxylphenyl)pyridine (H5BDCP) led highly robust nanoporous crystalline material {(Me2NH2)5[Cd4(BDCP)2(μ3-OH)2(CH3CO2)(H2O)2]·3DMF·2H2O}n (NUC-67) 57.4% void volume. Structural analysis displays that inner surface channels in activated NUC-67a is functionalized by Lewis acid sites unsaturated Cd2+ ions base μ3-OH– groups, CH3CO2– anions, free pyridine, C═O groups. Under solvent-free conditions, exhibits performance on cycloaddition epoxides; for instance, conversion rate propylene oxide (PO) into carbonate (PC) 1 atm can reach 99% within 6 h 55 °C, resulting 660 turnover number 110 h–1 frequency. Moreover, Knoevenagel condensation reactions aldehydes malononitrile be efficiently catalyzed NUC-67a. Encouragingly, shows strong structural stability good reversible cyclicity above two organic metal leaching below 8 ppb. Hence, this work proves MOF-based should focus design selection ligands, plays decisive role regulation, such as cluster-based nodes, defect sites, unexpected insertion high-porosity channels.

Язык: Английский

Процитировано

20
Fe(III)-Anchored Porphyrin-Based Nanoporous Covalent Organic Frameworks for Green Synthesis of Cyclic Carbonates from Olefins and CO2 under Atmospheric Pressure Conditions DOI
Gulshan Singh, Kamal Prakash, C. M. Nagaraja

и другие.

Inorganic Chemistry, Год журнала: 2023, Номер 62(32), С. 13058 - 13068

Опубликована: Авг. 3, 2023

The utilization of carbon dioxide (CO2) as a C1 source coupled with olefins, readily accessible feedstocks, offers dual advantages mitigating atmospheric and green synthesis valuable chemicals. In this regard, herein we demonstrate the application Fe(III)-anchored porphyrin-based covalent organic framework (P-COF) promising recyclable catalyst for one-step generation cyclic carbonates (CCs), value-added commodity chemicals from olefins CO2, under mild pressure conditions. Moreover, one-pot was applied to transform various (aliphatic aromatic) into corresponding CCs in good yield selectivity. addition, Fe(III)@P-COF showed recyclability durability multiple reuse cycles without losing its catalytic activity. Notably, strategy presents an eco-friendly, atom-economic alternative conventional two-step process requiring epoxides. This work represents rare demonstration porphyrin COF-catalyzed CC by utilizing available at dioxide.

Язык: Английский

Процитировано

15
Ultrahigh Stable Heterometallic InCo-Organic Framework for Efficiently Catalyzing Cycloaddition of CO2 with Epoxides and Knoevenagel condensation DOI
Xiaotong Wang, Chong Li,

Tuoping Hu

и другие.

Journal of Molecular Structure, Год журнала: 2024, Номер 1318, С. 139223 - 139223

Опубликована: Июль 6, 2024

Язык: Английский

Процитировано

6
High‐Entropy Lanthanide‐Organic Framework as an Efficient Heterogeneous Catalyst for Cycloaddition of CO2 with Epoxides and Knoevenagel Condensation DOI

Siyang Jin,

Yu Fu, Kecheng Jie

и другие.

Chemistry - A European Journal, Год журнала: 2024, Номер 30(39)

Опубликована: Май 10, 2024

Multimetallic synergistic effects have the potential to improve CO

Язык: Английский

Процитировано

5
Robust {Pb10}-Cluster-Based Metal–Organic Framework for Capturing and Converting CO2 into Cyclic Carbonates under Mild Conditions DOI
Bo Zhao, Chong Li,

Tuoping Hu

и другие.

Inorganic Chemistry, Год журнала: 2024, Номер 63(30), С. 14183 - 14192

Опубликована: Июль 15, 2024

Developing a highly active catalyst that can efficiently capture and convert carbon dioxide (CO2) into high-value-added energy materials remains severe challenge, which inspires us to explore effective metal–organic frameworks (MOFs) with high chemical stability high-density sites. Herein, we report robust 3D lead(II)-organic framework of {(Me2NH2)2[Pb5(PTTPA)2(H2O)3]·2DMF·3H2O}n (NUC-111) unreported [Pb10(COO)22(H2O)6] clusters (abbreviated as {Pb10}) nodes (H6PTTPA = 4,4′,4″-(pyridine-2,4,6-triyl)triisophthalic acid). After thermal activation, NUC-111a is functionalized by the multifarious symbiotic acid–base sites open Pb2+ uncoordinated pyridine groups on inner surface void volume. Gas adsorption tests confirm displays higher separation performance for mixed gases f CO2 CH4 selectivity CO2/CH4 at 273 K 101 kPa being 31 (1:99, v/v), 23 (15:85, 8 (50:50, respectively. When temperature rises 298 K, 26 22 11 v/v). Moreover, activated exhibited excellent catalytic performance, stability, recyclability cycloaddition epoxides under mild conditions. Hence, this work provides valuable insight designing MOFs multifunctionality capture, separation, conversion.

Язык: Английский

Процитировано

5
Fluorine-Functionalized 2D Dysprosium(III)–Organic Framework for Highly Catalyzing the CO2-Epoxide Cycloaddition DOI

Meiyu Ren,

Kun Yang,

Liming Fan

и другие.

Journal of Molecular Structure, Год журнала: 2025, Номер 1336, С. 142068 - 142068

Опубликована: Март 14, 2025

Язык: Английский

Процитировано

0