Chemical Science
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2022
·Vol. 13
·期 19
·5693-5700
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IF 9.969
Ya-Jie Liu,Yinghua Yu,Yi-Fan Sun,Wei-Hui Fang,Jian Zhang
Heterometallic cluster-based framework materials are of interest in terms of both their porous structures and multi-metallic reactivity. However, such materials have not yet been extensively investigated because of difficulties in their synthesis and structural characterization. Herein, we reported the designable synthesis of atomically precise heterometallic cluster-based framework compounds and their application as catalysts in aldol reactions. By using the synergistic coordination protocol, we successfully isolated a broad range of compounds with the general formula, [Al4M4O4(L)12(DABCO)2] (L = carboxylates; DABCO = 1,4-diazabicyclo[2.2.2]-octane; M2+ = Co2+, Mn2+, Zn2+, Fe2+, Cd2+). The basic heterometallic building blocks contain unprecedented main-group γ-alumina moieties and surrounding unsaturated transition metal centers. Interestingly, the porosity and interpenetration of these frameworks can be rationally regulated through the unprecedented strategy of increment of the metal radius in addition to general introduction of sterically bulky groups on the ligand. Furthermore, these porous materials are effective catalysts for aldol reactions. This work provides a catalytic molecular model platform with accurate molecular bonding between the supporters and catalytically active metal ions.
研究领域:
材料化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
·
2015
·
IF 2.515
Jiexuan Song,Haiyang Zhang,Jianping Deng
This article reports on the preparation of a novel category of optically active magnetic microspheres (OAMMPs) consisting of Fe 3 O 4 nanoparticles and helical substituted polyacetylene bearing pendent prolineamide groups and the use of them for asymmetric direct Aldol reactions. The microspheres (200–300 μm in diameter) were prepared by using chiral acetylenic monomer and alkynyl-Fe 3 O 4 nanoparticles via suspension polymerization approach. They were obtained in high yield (> 99%) with regular spheric morphology and exhibited noticeable optical activity, according to circular dichroism spectra and specific optical rotation measurements. The microspheres further served as chiral catalyst for performing direct Aldol reactions between acetone and p -nitrobenzaldehyde, providing the product in moderate yield (68%) and ee (75%). The magnetic microspheres can be easily recycled and reused. Mechanism for the asymmetric catalysis of Aldol reaction was further proposed.
研究领域:
材料科学
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有机化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 25
·12318-12323
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IF 3.925
Wei Xiao,Zihao Wang,Jinxiang Yang,Tianyou Chen,Changfeng Yi,Zushun Xu
Aldol reaction in water can effectively limit the formation of Schiff bases that deactivate active amine sites. To date, regulation of cooperative behaviors and morphologies of polymer-supported acid–base catalysts remains a challenge. Here, we develop a controllable strategy for engineering polystyrene-supported acid–base catalysts by using nanoprecipitation in water. Benzylamine-containing copolymers and catechol-containing copolymers were synthesized and used for nanoprecipitation. Because of the hydrophobic nature of the polystyrene chains, coil-globule collapse not only constructs hydrophobic environments but also brings catechol groups and benzylamine groups in close proximity to enable the synergistic effect. The influence of polymer compositions and effective constituent ratios on catalytic performance was investigated to understand the structure-activity relationships. A postulated catalytic mechanism for polystyrene-supported acid–base catalysts was proposed. Our results demonstrate that this strategy provides access to more efficient polymer-supported acid–base catalysts and has the potential for the construction of other bifunctional catalytic systems in aqueous media.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2025
·
IF 3.9
Dancheng Zhu,Yuchen Cao,Yuchen Qian,Weijie Yu,Yuxuan Xu,Hao Xu,Jun Qiao,Chao Shen,Jiabin Shen
Graphical This study develops amino-modified Ti 3 C 2 /Mg 3 Al-LDH composites as solid base catalysts for aldol reactions. The composite reduces surface agglomeration, enhances active site exposure, and increases basicity, achieving 99% product yield under optimized conditions (60 °C, 30 min). It retains > 91% efficiency over five cycles, demonstrating superior stability and catalytic performance compared to non-modified LDHs. Aldol reaction is an important class of industrially catalyzed reactions for synthesizing high-value fine chemicals. Traditionally conducted under alkaline conditions, these reactions often utilize liquid alkali catalysts, which present challenges such as difficult separation and recovery and undesirable side reactions promoted by the catalyst. Solid base catalysts have received much attention and research in recent years to address these issues. In this study, magnesium–aluminum layered double hydroxides (MgAl-LDHs) were synthesized using magnesium chloride hexahydrate, aluminum chloride hexahydrate, and anhydrous sodium carbonate. These were subsequently combined with amino-modified Ti 3 C 2 to form composite materials. Characterization of the prepared Mg 3 Al-LDH/Ti 3 C 2 -NH 2 composites was conducted using X-ray diffractometer (XRD), scanning electron microscope (SEM), infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS) confirming the successful preparation of the composite material. The prepared Mg 3 Al-LDH/Ti 3 C 2 -NH 2 was applied as a catalyst in the aldol condensation reaction. Key factors such as catalyst dosage, reaction time, acetone amount, and temperature were investigated to optimize catalytic efficiency. Under optimal conditions—100 mg Mg 3 Al-LDH/Ti 3 C 2 -NH 2 , a reaction time of 0.5 h, 200 mg of p -nitrobenzaldehyde, 1 mL of acetone, and a reaction temperature of 60 °C—a yield of 99% was achieved. The result demonstrates that Mg 3 Al-LDH/Ti 3 C 2 -NH 2 exhibits excellent catalytic activity and holds promising potential for application in solid base catalysis.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RUSSIAN JOURNAL OF ORGANIC CHEMISTRY
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2025
·Vol. 61
·期 2
·338-345
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IF 0.9
Li Chonglong,Lai Caiyun,Zhan Murong,Zhao Xiaona,Dong Wenyuan,Liu Jiaqi,Wang Peibiao
A novel helical poly(phenyl isocyanide) bearing an ( R,R )-(‒)-1,2-diaminocyclohexane pendant (poly- 2 200 ) was designed and synthesized. Helical poly- 2 200 showed an excellent catalytic performance in the asymmetric aldol reaction between cyclohexanone and 2-(trifluoromethyl)benzaldehyde in ethanol: the reaction product had an enantiomeric excess ( ee ) of 87.8%.
研究领域:
有机化学
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催化化学
✓ 已验证
DOI
高影响因子
MACROMOLECULAR RAPID COMMUNICATIONS
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2012
·Vol. 33
·期 8
·652-657
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IF 4.596
Dongyue Zhang,Chonglei Ren,Wantai Yang,Jianping Deng
This Communication reports optically active helical substituted polyacetylenes which solely catalyzed asymmetric Aldol reaction between cyclohexanone and p-nitrobenzaldehyde; more importantly the helical structures are found to play crucial roles in the asymmetric catalysis, with a remarkable yield and ee (both up to 80%). A synergic effect is observed between the helical structures in the polymer main chains and the pendent prolinamide moieties for successfully catalyzing the asymmetric reaction. The role of the helical polymer backbones is further verified by tuning the relative helical structure content.
研究领域:
有机化学
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高分子化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
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2020
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IF 3.687
Yang Zhong,Bo Zhou,Lijun Wang
Fe/FeO x embedded in LDH was prepared by reducing the pre-synthesized [Fe(C 2 O 4 ) 3 ] 3− anions intercalated LDH and used as a multi-functional catalyst for synthesis of C7-C9 compound via transfer hydrogenation between furfural (C5) and short-chain alcohols (C2-C4) and a subsequent aldol reaction of furfural with intermediate short-chain aldehydes in the absence of a homogeneous base with furfuryl alcohol as a byproduct. Screening reaction conditions, evaluation and improvement of the cyclic catalytic performance, and determination of catalytically active components were performed, and the results demonstrated that both high conversion and high selectivity to the C C bond forming product can be obtained under a non-oxidizing atmosphere of Ar or H 2 /Ar mixed gas, a reaction temperature of 140 °C and a reaction time of 4 h; the catalyst was easily deactivated during the cycle experiments, however, its catalytic stability can be effectively improved by depositing Ni with weak reducibility on the surface of Fe nanoparticles at the cost of reducing partial catalytic activity. Fe/FeO x together with LDH as a whole proved to be effective in catalyzing the transfer hydrogenation reaction and the support LDH imparted basic catalytic function to the composite realizing the aldol reaction in the absence of a homogeneous base.
研究领域:
催化化学
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材料科学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）