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POLYHEDRON · 2024 · IF 2.4

Interior precisely designed metal–organic framework for light hydrocarbons separation

Meng Zhao,Yun Yang,Xue-Song Gu,Lanlan Sun

The separation and purification of light hydrocarbons are performed by energy-intensive distillation processes. Microporous metal–organic framework based absorbents acting as alternative technology gains focus. Open metals sites (OMSs) enriched MOF-74 show great potential in light hydrocarbons but its separation selectivity is low and difficult to regenerate. To address this issue, we introduced N -donor ligands into open sites of Co-MOF-74 by post modification. Structure was determined by powder X-ray diffraction, element analysis, infrared spectroscopy and thermogravimetric analyses. As-synthesized modified Co-MOF-74 display potential in C 2 H 4 /C 2 H 6 , C 3 H 6 /C 3 H 8 , C 3 H 8 /CH 4 and C 2 H 6 /CH 4 separation for N -donor ligands placeholder.

CAS / MDL: 290-37-9 100-48-1
研究领域: 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Preparation of a novel silica-based N-donor ligand functional adsorbent for efficient separation of palladium from high level liquid waste

Hefang Liu,Shunyan Ning,Zengyuan Li,Shichang Zhang,Lifeng Chen,Xiangbiao Yin,Toyohisa Fujita,Yuezhou Wei

In this work, a novel silica-based N-donor ligand functional adsorbent (SiVpC) is prepared by in situ polymerization for the efficient separation of palladium from high level liquid waste (HLLW). The as-prepared SiVpC adsorbent is characterized by SEM-EDS, TGA, and BET. The effects of nitric acidity, SiVpC adsorbent dosage, time, temperature, and palladium ion concentration on the adsorption are investigated. Among the 12 typical fission product metal ions (Ru, Rh, La, Y, Pr, Ce, Sm, Nd, Gd, Eu, Zr, Mo) existing in HLLW, SiVpC adsorbent can selectively adsorb palladium ( SF Pd/other metals  = 137.6) in 0.5 M HNO 3 solution. The adsorptio kinetics of Pd(II) are consistent with the pseudo-second-order model, reaching equilibrium within 120 min. The maximum adsorption capacity is 38.4 mg/g in 0.5 M HNO 3 , and the adsorption process is consistent with the Langmuir model. The adsorbed palladium can be completely desorbed with 0.5 M HNO 3 -0.5 M Thiourea. Furthermore, SiVpC adsorbent remains good performance after five adsorption–desorption cycles, which indicates good reusability. The adsorption mechanism of SiVpC adsorbent on palladium is analyzed by FT-IR and XPS that N-containing functional groups on the ligand are coordinated with palladium, which is also further verified by DFT calculations. In addition, through the column chromatography separation system, SiVpC adsorbent can efficiently adsorb palladium from HLLW and the adsorbed palladium can be desorbed with 0.5 M HNO 3 -0.5 M thiourea solution, which has great application potential.

研究领域: 化学工程 · 环境科学
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CRYSTAL GROWTH & DESIGN · 2020 · IF 4.089

N-Donor Auxiliary Ligand Influence on the Coordination Mode Variations of V-Shaped Triazole Dicarboxylic Acid Ligand Affording Seven New Luminescent Zn(II) Compounds with Variable Structural Motifs

Jin-Xia Yang,Xin Zhang,Ye-Yan Qin,Yuan-Gen Yao

A 2D network of {[Zn(Hbcpt)(H2O)3]·7H2O} (1) was hydrothermally synthesized and structurally characterized. By employing different N-donor ligands into the system of 3,5-bis(4′-carboxyl-phenyl)-1,2,4-triazole (H3bcpt) and Zn(II) cations, six novel entangled coordination polymers, namely, {[Zn2(bcpt)(μ2-OH)(H2O)]·(py)·4H2O} (2), {[Zn2(Hbcpt)2(bpa)2]·2H2O} (3), {[Zn(Hbcpt)(bpp)]·[Zn(Hbcpt)(bpp)]·2.5H2O} (4), {[Zn5(bcpt)2(biimpy)2(μ2-OH)4]·5H2O} (5), {[Zn2(bcpt)(bib)(μ2-OH)]·H2O} (6), and {[Zn2(bcpt)(bix)4(μ2-OH)]·3H2O} (7) (H3bcpt = 3,5-bis(4′-carboxyl-phenyl)-1,2,4-triazole, bpa = 1,2-bis(4-pyridyl)ethane, bpp = 1,3-bi(4-pyridyl)propane, biimpy = 2,6-bis(imidazole-1-yl)pyridine, bib = 1,4-bis(N-imidazolyl)butane, bix = 1,4-bis(imidazol-1-ylmethyl)-benzene, py = pyridine), were obtained. Single-crystal X-ray diffraction analysis reveals that, with the different N-donor ligands, the resulting compounds present entangled structures with different topologies. Compound 1 shows a 2D (4, 4) network, and the adjacent sheets are extended into a 3D supramolecular framework via hydrogen-bonding interactions. Interesting, by introducing a series of ditopic N-donor ligands into the reaction system, compounds 2–7 with entangled structures were harvested. Compound 2 exhibits a 3D self-penetrating network with an 8-connected bcu topology. Compound 3 features an 8-fold dia network showing an unusual [4 + 4] mode of interpenetration. Compound 4 is comprised of two parts of undulated 2D 44-sql networks, and the adjacent undulated layers are parallel interpenetrated to each other to give a 2D → 3D polycatenated framework. Compound 5 presents an unusual 3D self-penetrating network with a novel 4,6,6-connected trinodal network with the point symbol of (32·4·52·6)(32·4·56·66}{32·56·66·7}. Compound 6 shows a 2-fold interpenetrating 3D architecture with 6-connected sxd topology. Compound 7 displays an unprecedented self-penetration derived from abnormal [3 + 2] 5-fold interpenetrating dia subnets. Structural diversity of these compounds suggests that different N-donor ligands can induce the organic ligand to present different conformations and coordination modes, and the influence on the final structures. Furthermore, the luminescent properties of compounds 1–7 have been investigated in the solid state.

CAS / MDL: 553-26-4 80-05-7
研究领域: 配位化学 · 材料科学 · 晶体学
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JOURNAL OF MOLECULAR STRUCTURE · 2020 · IF 2.463

Luminescence and catalytic properties of two nickel(II)-organic frameworks constructed by 5-substituted isophthalate and N-donor mixed ligands

Fenglan Liang,Deyun Ma

Two nickel (II) based metal-organic frameworks, [Ni(1,4-bib) 1.5 (NO 2 -BDC) (H 2 O)] n ( 1 ) and [Ni(1,4-bimb) (CH 3 O-BDC)] n ( 2 ) (1,4-bib = 1,4-bis(1-imidazolyl)benzene, NO 2 -BDC = 5-nitroisophthalate, 1,4-bimb = 1,4-bis(imidazole-1-ylmethyl)benzene, and CH 3 O-BDC = 5-methoxyisophthalate) have been synthesized and were structurally characterized. Complex 1 is a three-fold interpenetrated 3D framework with 5-connected pcu topology and is comprised of Ni-1,4-bib layers further pillared by 5-nip approximately in the b direction. Complex 2 shows a 2D (4,4) sql network when dinuclear nickel ions and ligands are regarded as nodes and linkers, respectively. Furthermore, the luminescence and catalytic properties of 1 – 2 for the degradation of methyl orange in a Fenton-like process have also investigated.

研究领域: 材料科学 · 化学 · 催化
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CRYSTENGCOMM · 2016 ·Vol. 18 ·期 8 ·1363-1375 · IF 3.849

Structural diversity of a series of coordination polymers built from 5-substituted isophthalic acid with or without a methyl-functionalized N-donor ligand

De-Yun Ma,Liang Qin,Jia-Mei Lei,Yun-Qiu Liang,Wei-Jie Lin,Jing-Jing Yan,Wan-Qiu Ding,Hai-Fu Guo,Yun Ling

The reaction of X-H2BDC (X = H, Br, NO2 and CH3) and methyl-functionalized dmbpy ligands with metal salts under different solvent media conditions generates nine structurally diverse zinc(II)/cadmium(II)-based coordination polymers (CPs), {[Zn2(BDC)2(DMF)3]·DMF}n (1), [Zn(BDC)2(dmbpy)]n (2), {[(Me2NH2)2Zn3(Br-BDC)4]·3DMF·3H2O}n (3), [Zn2(Br-BDC)2(dmbpy)]n (4), {[Zn13(NO2-BDC)8(μ3-OH)2(μ2-OH)6(H2O)4]·12H2O·2NO3}n (5), [Zn2(NO2-BDC)2(dmbpy)(H2O)2]n (6), {[Cd(NO2-BDC)(dmbpy)0.5(H2O)]·(ACN)·H2O}n (7), [Zn(CH3-BDC)(dmbpy)0.5(H2O)]n (8), and [Zn(CH3-BDC)(dmbpy)0.5]n (9) (H2BDC = isophthalic acid, Br-H2BDC = 5-bromoisophthalic acid, NO2-H2BDC = 5-nitroisophthalic acid, CH3-H2BDC = 5-methylisophthalic acid, dmbpy = 2,2′-dimethyl-4,4′-bipyridine, DMF = N,N-dimethylformamide, ACN = acetonitrile). All the compounds are synthesized using dual linkers (X-H2BDC and dmbpy). 1 and 7–8 show a 2D (4,4) network when dinuclear metal ions and ligands are regarded as nodes and linkers, respectively. 2 is a wave-like chain with BDC ligands alternately pointing up and down. CPs 3–6 and 9 all exhibit 3D networks with 5-connected sqp, 6-connected jsm, 6-connected pcu, (3,4)-connected dmc and 6-connected jsm topologies, respectively. Furthermore, luminescence, thermogravimetric and chemical stability properties of these CPs were investigated. The results suggest that both organic ligands and solvent media influence the final resulting CPs.

CAS / MDL: 10022-68-1 10196-18-6
研究领域: 无机化学 · 材料科学 · 晶体学
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FUEL · 2022 · IF 8.035

N-donating and water-resistant Zn-carboxylate frameworks for humid carbon dioxide capture from flue gas

Yi-Ming Gu,Ya-Hui Wang,Sheng-Sheng Zhao,Hong-Jun Fan,Xiao-Wei Liu,Zhiping Lai,Shu-Dong Wang

Carbon capture from flue gases is one of the crucial routines for reducing current CO 2 emissions and mitigating the greenhouse effect. Metal-organic frameworks (MOFs) have received a lot of interest as efficient solid adsorbents for CO 2 /N 2 separation in flue gas treatment. However, many MOF materials are susceptible to the presence of water vapor, which has a significant impact on their adsorption efficacy and moisture stability. Here in this work, we reported two pillar-layered Zn-MOFs with N -donors, i.e., Zn 2 (TRZ) 2 (Fuma) and Zn 2 (TRZ) 2 (BDC), which demonstrated high CO 2 uptakes (3.92 and 1.52 mmol/g) and CO 2 /N 2 (132 and 20.5) adsorption selectivities at 298 K and 101 kPa, among the best comprehensive results reported by far. After seven days of exposure to a 100 % RH environment, it was found that, the Zn-N pillar contributes to the robust structure of MOFs . Furthermore, in-depth theoretical calculations indicated the guest-framework interactions, and dynamic sorption tests confirmed high working capacities (2.78 and 1.14 mmol/g), sufficient water stability and remarkable cycling performance of the studied MOFs under humid ambient conditions. We believe this work provides a routine to prepare robust and promising candidates to address the challenge in carbon capture under humid conditions.

研究领域: 材料科学 · 环境科学 · 化学工程
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