949-97-3Relevant academic research and scientific papers
A Calix[4]resorcinarene-Based [Co12] Coordination Cage for Highly Efficient Cycloaddition of CO2 to Epoxides
Guo, Ting-Ting,Su, Xiao-Fang,Xu, Xianxiu,Yang, Jin,Yan, Li-Kai,Ma, Jian-Fang
, p. 16518 - 16523 (2019)
The design and synthesis of polynuclear metal cluster-based coordination cages is of considerable interest due to their appealing structural characteristics and potential applications. Herein, we report a calix[4]resorcinarene-based [Co12] coordination cage, [Co12(TPC4R-I)2(1,3-BDC)10(μ3-OH)4(H2O)10(DMF)2]·7DMF·23H2O (1), assembled with 2 bowl-shaped calix[4]resorcinarenes (TPC4R-I), 10 angular 1,3-benzenedicarboxylates (1,3-BDC), and 12 Co(II) cations. Remarkably, it is shown to be a highly efficient recyclable heterogeneous catalyst for CO2 conversion due to its exposed Co(II) Lewis acid sites.
Ultrastrong Alkali-Resisting Lanthanide-Zeolites Assembled by [Ln60] Nanocages
Dong, Jie,Cui, Ping,Shi, Peng-Fei,Cheng, Peng,Zhao, Bin
, p. 15988 - 15991 (2015)
Zeolites, as one of the most important porous materials, are most widely utilized in sorbents, catalysis, and ion-exchange fields. However, the multi-functional lanthanide-zeolites constructed exclusively by lanthanide ions and oxygen linkers are to our knowledge unknown hitherto. Herein, we, for the first time, report the unique structure and multifunctions of lanthanide zeolites (1·Gd, 1·Tb, 1·Dy), featuring 60 nuclear [Ln60] nanocages as building blocks and ultrastrong alkali-resisting. These compounds possess extremely high stability and still retain single crystallinity after treatment in boiling water, 0.1 M HCl, and 20 M NaOH aqueous solutions. Magnetic studies revealed 1·Gd has large magnetocaloric effect with -ΔSmmax = 66.5 J kg-1 K-1, falling among the largest values known to date. Importantly, these lanthanide-zeolites themselves can efficiently catalyze the cycloaddition of CO2 with epoxides under mild conditions. Our finding extends the conventional zeolites to lanthanide counterparts, opening a new space for seeking novel and/or multifunctional zeolites.
A Porphyrin-Based Porous rtl Metal–Organic Framework as an Efficient Catalyst for the Cycloaddition of CO2to Epoxides
Jiang, Wei,Yang, Jin,Liu, Ying-Ying,Song, Shu-Yan,Ma, Jian-Fang
, p. 16991 - 16997 (2016)
A porous rtl metal–organic framework (MOF) [Mn5L(H2O)6?(DMA)2]?5DMA?4C2H5OH (1?Mn) (H10L=5,10,15,20-tetra(4-(3,5-dicarboxylphenoxy)phenyl)porphyrin; DMA=N,N′-dimethylacetamide) was synthesized by employing a new porphyrin-based octacarboxylic acid ligand. 1?Mn exhibits high MnIIdensity in the porous framework, providing it great Lewis-acid heterogeneous catalytic capability for the cycloaddition of CO2with epoxides. Strikingly, 1?Mn features excellent catalytic activity to the cycloaddition of CO2to epoxides, with a remarkable initial turnover frequency 400 per mole of catalyst per hour at 20 atm. As-synthesized 1?Mn also exhibits size selectivity to different epoxide substrates on account of their steric hindrance. The high catalytic activity, size selectivity, and stability toward the epoxides on catalytic cycloaddition of CO2make 1?Mn a promising heterogeneous catalyst for fixation and utilization of CO2.
Potassium organoaluminate: Synthesis, structure, and catalytic activity for the conversion of CO2 into cyclic carbonates
Guo, Zhiqiang,Yan, Leilei,Liu, Yaoming,Wu, Xiaoqin,Wei, Xuehong
, (2020)
Potassium organoaluminate stabilized by bidentate pyrrolyl ligand [C4H3NH(2-CH2NHtBu)] was successfully synthesized and characterized. The solid state structure reveals it is a rare example of an alkyl-bridged K/Al complex, which is interlocked by bridging potassium ions to form a monodimensional polymeric array, and featured an unsupported bridging methyl interaction between potassium and aluminum metals lead to ultimate 2D supramolecular network structure. It was proved to an efficient catalyst for the conversion of CO2 into cyclic carbonates in good yields at 50 °C and 1 atm carbon dioxide pressure.
Shape-persistent octanuclear zinc salen clusters: Synthesis, characterization, and catalysis
Haak, Robert M.,Decortes, Antonello,Escudero-Adan, Eduardo C.,Belmonte, Marta Martinez,Martin, Eddy,Benet-Buchholz, Jordi,Kleij, Arjan W.
, p. 7934 - 7936 (2011)
We describe a selective and template-controlled synthesis of a series of Zn8 metal complexes based on a bis-nucleating salen ligand scaffold. Our results, a combination of X-ray analysis and solution studies, show that discrete, shape-persistent metal clusters can be prepared in high yield. Their activity in organic carbonate catalysis is a function of the metal-connecting fragment present in the exterior of the cluster complex. The high stability of the clusters has been confirmed by 1H, 13C (DEPTQ) and DOSY NMR, gel permeation chromatography, high-performance liquid chromatography, and mass spectrometry.
Catalytic CO2 Fixation over a Robust Lactam-Functionalized Cu(II) Metal Organic Framework
Ansari, Shagufi Naz,Kumar, Pawan,Gupta, Anoop K.,Mathur, Pradeep,Mobin, Shaikh M.
, p. 9723 - 9732 (2019)
A porous, Cu(II)-metal organic framework (Cu-MOF) constituted of a rigid lactam functionalized ditopic ligand (H2L) was synthesized at room temperature under slow evaporation conditions {H2L = (5-(1-oxo-2,3-dihydro-1H-inden-2-yl)isop
In situcleavage and rearrangement synthesis of an easy-to-obtain and highly stable Cu(ii)-based MOF for efficient heterogeneous catalysis of carbon dioxide conversion
Qin, Lan,Pan, Yu,Yu, Lei,Huai, Ranran,Yang, Lu,Dou, Yong,Zhou, Zhen
, p. 6307 - 6314 (2021)
Cycloaddition of carbon dioxide (CO2) with epoxides into cyclic carbonates has been attracted substantial attentions for metal-organic frameworks based catalysis of CO2chemical fixation, not only due to the contributions that solving the environmental issue of the excessive emission CO2, but also providing an effective pathway for the production of value-added fine chemicals. Herein, a Cu(ii)-based metal-organic framework (1) was synthesized by thein situcleavage and rearrangement of theN,N′-bis(4-picolinoyl)hydrazine ligand into an isonicotinate (INA) moiety as a connected nodeviasolvothermal synthesis in high yields. This three-dimensional framework possesses infinite one-dimensional Cu-O double chains in a ladder-like arrangement with exposed metal centres, and can be highly stable up to at least 240 °C and in various solvents. Gas adsorption experiments reveal the good adsorption ability of1towards CO2with a high value ofQst. Cycloaddition of CO2with epoxides could successfully occur by using1as an efficient heterogeneous catalyst, affording almost complete conversion and selectivity under solvent free conditions.
Wheel-like Ln18 Cluster Organic Frameworks for Magnetic Refrigeration and Conversion of CO2
Song, Tian-Qun,Dong, Jie,Yang, An-Fei,Che, Xue-Jing,Gao, Hong-Ling,Cui, Jian-Zhong,Zhao, Bin
, p. 3144 - 3150 (2018)
Two isostructural 2D MOFs ([Ln7(CDA)6(HCOO)3(μ3-OH)6(H2O)8]n, abbreviated as 1-Gd and 2-Dy) were successfully synthesized under solvothermal conditions. The self-assem
High Uptake of ReO4? and CO2 Conversion by a Radiation-Resistant Thorium–Nickle [Th48Ni6] Nanocage-Based Metal–Organic Framework
Xu, Hang,Cao, Chun-Shuai,Hu, Han-Shi,Wang, Shi-Bin,Liu, Jin-Cheng,Cheng, Peng,Kaltsoyannis, Nikolas,Li, Jun,Zhao, Bin
, p. 6022 - 6027 (2019)
Assembled from [Th48Ni6] nanocages, the first transition-metal (TM)-thorium metal–organic framework (MOF, 1) has been synthesized and structurally characterized. 1 exhibits high solvent and acid/base stability, and resistance to 400 kGy β irradiation. Notably, 1 captures ReO4? (an analogue of radioactive 99TcO4?, a key species in nuclear wastes) with a maximum capacity of 807 mg g?1, falling among the largest values known to date. Furthermore, 1 can enrich methylene blue (MB) and can also serve as an effective and recyclable catalyst for CO2 fixation with epoxides; there is no significant loss of catalytic activity after 10 cycles. Theoretical studies with nucleus-independent chemical shifts and natural bond orbital analysis reveal that the [Th6O8] clusters in 1 have a unique stable electronic structure with (d–p)π aromaticity, partially rationalising 1′s stability.
3d-4f Heterometal-Organic Frameworks for Efficient Capture and Conversion of CO2
Qiao, Wan-Zhen,Xu, Hang,Cheng, Peng,Zhao, Bin
, p. 3128 - 3133 (2017)
Two novel three-dimensional 3d-4f heterometallic-organic frameworks {[TbZn(BPDC)2(μ2-H2O)Cl(H2O)3]·5H2O·0.5DMA}n (1) and {[TbCo(BPDC)2(μ2-H2O)Cl(H2O)3]·8H2O·0.5DMA}n (2) have been synthesized and structurally characterized. They are isostructural and exhibit irregular one-dimensional channels with a large potential pore volume. Importantly, both of them demonstrate excellent catalytic activity for the chemical fixation of CO2 into cyclic carbonates under mild conditions. Moreover, the catalytic recycling of compound 1 as a representative example was explored; it can be easily separated and reused for at least four times without significant reduction in catalytic ability.
