CATALYSIS LETTERS
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2021
·Vol. 152
·期 8
·2293-2301
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IF 3.186
Liu Xueping,Shi Shengbin,Yang Su,Gu Liuyu,Gao Lijing,Zhang Jin,Xiao Guomin
Using etherification to convert glycerol into biofuel additives is an effective way to solve the current problem of excess glycerol. In this study, a series of environmentally friendly (x)HPW/ZrO 2 catalysts were synthesized for the etherification of glycerol and tert-butyl alcohol (TBA). The internal microstructure and acidity analysis of the synthesized samples were derived from BET, XRD, Raman spectroscopy, FTIR, SEM, NH 3 -TPD and Py-FTIR. The results revealed that the synthesized catalysts retained the complete Keggin structure of phosphotungstic acid (HPW) which supported on it. The (15)HPW/ZrO 2 catalyst with suitable structure and acidity had an excellent catalytic effect on the etherification reaction. Driven by the (15)HPW/ZrO 2 catalyst, the optimal reaction conditions were determined from parameters of reaction temperature, time, molar rate of glycerol and TBA, and catalyst dosage. 93.2% glycerol conversion and 42.5% selectivity of multi-substituted tert-butyl glycerol ethers (DTBG + TTBG) were obtained under optimal conditions. In addition, even after a total of four consecutive reactions, (15)HPW/ZrO 2 catalyst still demonstrated relatively good catalytic activity. Graphic Abstract
研究领域:
催化化学
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可再生能源
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 21
·5828-5840
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IF 9.405
Xinli Tong,Pengfei Guo,Shengyun Liao,Song Xue,Haigang Zhang
The selective transformation of the aldehyde group (–CHO) in multifunctional oxygenates is a key challenge in the development of sustainable biomass feedstock. Herein, a smart Ni-MFC catalyst was developed from a 2D Ni-based metal–organic framework (MOF), which efficiently promoted the transformation of –CHO in the presence of H2 to a methyl group (–CH3) via the reductive etherification and hydrogenolysis of the C–O ether bond in methanol. Moreover, the catalytic process could be controlled to directionally produce methyl ether (–CH2OR) using the reductive etherification protocol. For the catalytic reduction of vanillin, the Ni-MFC-700 catalyst guaranteed the full conversion of vanillin and 96.5% yield of the desired 2-methoxy-4-methylphenol (MMP), while the Ni-MFC-500 catalyst afforded about 82.7% yield of 4-(methoxymethyl)-2-methoxyphenol in methanol solvent. This is a novel and promising approach for the valorization of multifunctional oxygenates and biomass-derived platform compounds.
研究领域:
化学催化
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生物质转化
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有机合成
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
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2018
·Vol. 8
·期 9
·383
·
IF 3.465
Wenting Fang,Hualei Hu,Zhongsen Ma,Lei Wang,Yajie Zhang
The revealing mechanism of side reactions is crucial for obtaining theoretical yield in industrialization when 2,5-bis(methoxymethyl)furan (BMMF) yield is above 95%. By-products catalyzed by the conventional ZSM-5 (C-ZSM-5) and hierarchical porous ZSM-5 (HP-ZSM-5) catalytic systems were different, and some key by-products were identified. Thus, possible pathways were proposed, which helps to further improve BMMF selectivity. Additionally, HP-ZSM-5 exhibited quicker reaction rate, higher BMMF yield and selectivity, and slower deactivation process. The relatively weak acidity of HP-ZSM-5 suppresses the ring-opening reaction and subsequent side reactions, and introduction of mesopores improves mass transport and slightly increases hydration of 2,5-bis(hydroxymethyl)furan (BHMF).Keywords:etherification;furanic diether;heterogeneous catalysis;side reaction;ZSM-5
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
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2023
·Vol. 13
·期 6
·969
·
IF 3.9
Srinivasan Vinju Vasudevan,Jin Cai,Junming Xu,Hongjian Lin,Hongliang Wang,Quan Bu
In this work, the microwave-assisted reaction of 5-hydroxymethylfurfural (5-HMF) into valuable ether and acylated production formation was investigated with the help of molybdophosphoric acid encapsulated dendritic fibrous silica (KCC-1) as a catalyst. XRD, N2adsorption-desorption, SEM, FT-IR, NH3-TPD, and TEM were used to analyze the physicochemical and structural properties of the synthesized catalysts. The microwave etherification of 5-HMF with ethanol was tested using synthesized catalysts. The effects of the reaction temperature, reaction time, catalytic amount, and microwave power were investigated. The resulting MPA-KCC-1 and IMPA-KCC-1 catalysts demonstrated excellent activity for the etherification of 5-HMF with ethanol, producing 5-(hydroxymethyl) furfural diethyl acetal (HMFDEA) and 5-(ethoxymethyl)furfural diethyl acetal (EMFDEA) products selectively. The significant advantages of the work are the selective production of EMFDEA at 82%, the catalyst can be easily removed via filtration, and the catalyst activity remains nearly intact even after five reaction cycles.Keywords:biomass;acetylation;5-HMF;etherification;heteropolyacid;fibrous silica
研究领域:
化学工程
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
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2024
·
IF 9.7
Mingyuan Liu,Yuchen Meng,Xinyang He,Jiatai Gu,Zhen Li,Shu Yang,Yue Zhang,Maorong Zheng,Liming Wang,Xiaohong Qin
The utilization of starch to treat sewage that received widespread attention has become one of the promising ways to purify water due to the advantages of low cost and biodegradability. However, the poor purification capacity for wastewater and difficult liquid phase dispersion of natural starch severely hindered its application in wastewater treatment and limited the development of starch materials. Hence, a series of cationic starches with different particle sizes were fabricated by controlling the acidification time and combining starch with N-2,3-epoxy-propyl trimethyl ammonium chloride to improve the dispersion and purification effect of starch in water. Acid hydrolysis could destroy the spatial structure of starch, which improved the etherification property to enhance the purification property of starch to different pollutants and the dispersed stable state in water. The maximum adsorption capacities of the optimal functional agents were 43.2 mg/g (methyl orange), and 236.8 mg/g (acid black) and the optimal penetration rate of the treated kaolin solution was 94.6%. The working behavior of cationic starch could be composed of rapid, stable, and equilibrium stages, and the working process of HS-g-GTA conformed to the pseudo-second-order dynamic model. This work provides a simple and low-energy pretreatment method for preparing cationic starch, which has important application value in removing anionic substances from wastewater.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
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2020
·Vol. 10
·期 14
·4684-4692
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IF 5.721
Pilan Zhang,Jie Yang,Hualei Hu,Danxin Hu,Jiang Gan,Yexin Zhang,Chunlin Chen,Xiaoqiang Li,Lei Wang,Jian Zhang
The self-etherification of 5-hydroxymethylfurfural (HMF) to 5,5′(oxy-bis(methylene))bis-2-furfural (OBMF) was investigated on ZSM-5, MCM-22, beta and hierarchical micro–mesoporous ZSM-5 (HMZ) catalysts. The hierarchically structured zeolites exhibited a superior intrinsic activity and good resistance to carbonaceous deposit; the latter could be ascribed to the lower mass transfer barrier in the mesopores of the HMZ catalysts. The structure–activity correlation showed that the catalytic activity mainly originated from one or several specific Brønsted acid sites, providing key clues to design efficient zeolite catalysts for producing OBMF.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Huan Wang,Weitao Wang,Yihong Ma,Jiaqi Zhu,Zhen-Hong He,Zhao-Tie Liu,Buxing Han
5-Hydroxymethylfurfural (HMF) can be upgraded to ether as fuel or fuel additives through conversion of the hydroxyl and aldehyde groups. The two groups are always involved in different catalytic reactions, such as etherification, acetalization, hydrogen transfer reduction, and even ring-opening reactions. This makes the etherification upgrading of HMF with high selectivity to desired product a great challenge. In the present wok, transformation of HMF in isopropanol was systematically investigated over different catalysts with Brønsted acid and Lewis acid sites. The effect of catalytic sites on product distribution and selectivity was studied. Moreover, several products, such as 5-isopropoxymethylfurfural, 5-isopropoxymethylfurfuryl alcohol, 5-isopropoxymethylfurfuryl alcohol, and 2,5-furandimethanol, were obtained with high selectivity, and the conversion pathway of HMF with alcohols on different catalytic sites was revealed under different catalytic conditions. The transformation of HMF to furan triether products over multi-site catalyst was realized for the first time based on the proposed reaction pathway with excellent activity and selectivity.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
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2019
·Vol. 22
·期 5
·945-954
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IF 3.382
Lanjian Xu,Yangyang Yuan,Jie Zhang,Yanfei Zhang,Xiaomin Zhang,Lei Chen,Lei Xu
A green, cost-effective and facile steam-assisted crystallization (SAC) strategy was developed to synthesize core–shell-structured zeolite composites with different frameworks between the core and shell. Chemical incompatibility from different structures has been circumvented by dip-coating Silicalite-1 seeds and an in situ transformation process. Beta@Silicalite-1 zeolites with a nanoscale polycrystal Silicalite-1 shell wrapped around the monocrystal Beta core was synthesized. The crystallization process and synthetic parameters, such as the composition of the core, crystallization temperature and gel composition of the seed solution, were investigated. The results revealed the importance of stability of the core and the crystallization rate of the Silicalite-1 shell. Interestingly, a trace amount of aluminum in the core zeolite could help resist corrosion during crystallization. Further investigation on alkylation and etherification reactions over Beta@Silicalite-1 demonstrated the advantage in selectivity control toward self-etherification versus alkylation.
研究领域:
化学工程
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催化材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 18
·14799-14808
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IF 3.289
Ximing Yan,Ming Ke,Zhaozheng Song,Qingzhe Jiang,Pei Yu
Lanthanum ion exchange, low-temperature steam treatment and La/steam combined modification were used to modify Hβ zeolite, and then comparative studies were performed on the influences of single and compound modified methods on the etherification activity. XRD, XRF, BET, FETEM-EDS, FTIR, OH-FTIR, NH3-TPD and Py-IR analysis methods were used to characterize the catalysts. The evaluation results show that the best modification method is lanthanum ion exchange followed by low-temperature steam treatment; the highest conversion of isoamylene was 67.72% and the yield of TAME was 65.63%. The characterization results implied that large pore sizes, high acidity, moderate acid strength and a suitable Brønsted acid proportion are all favourable for etherification.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2023
·
IF 4.7
Feng Du,Mengyu Wang,Libin Wang,Yushan Li,Yuangao Wang,Wenan Deng,Wenjuan Yan,Xin Jin
Catalytic conversion of waste polyoxymethylene plastics to renewable and value-added chemicals represents a promising area in green chemistry. Previous studies in both academia and industry have focused on thermal depolymerization under harsh operating temperature and pressure. In this work, we have investigated the detailed reaction mechanism for cascade depolymerization and etherification of polyoxymethylene with bio-derived polyols into valuable oxygenates. As one of the highlights in this work, we proposed and validated a two-step mechanism involving depolymerization and nucleophilic attack C O C bond. Kinetic modeling, IR and NMR spectra revealed mechanistic information for solvent-enhancement: the synergism of cation (Bi 3+ ), anion (OTf - ) and 1,4-dioxane (1) induces formation of intermolecular H bonding thus activating C O H bond in polyol molecules, and (2) facilitates nucleophilic attack on carbocation in polyoxymethylene. The outcome of this work will provide useful fundamental data for rational design of industrial processes involving atomic efficient conversion of various polymers into value-added products.
研究领域:
绿色化学
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催化反应工程
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
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2024
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IF 5.8
Jian Xiong,Liying Li,Xuebin Lu,Lei Ye,Zhihao Yu,Wei Li,Ming Zhang,Yiming Li,Jiao Tao,Rui Zhang,Yina Qiao
The biomass-derived furan compound furfuryl alcohol can be utilized to produce fuel substitutes, furfuryl ethers, through etherification reactions with short-chain monohydric alcohols. In order to solve the problems of high reaction temperature and poor product selectivity in this research, a porous carbon-based material with adjustable acidic strength and content, and acid species ratio was synthesized and prepared in this work. Zirconium was employed as Lewis acid and adjusting its loading was the key method to drive the etherification reaction. The physicochemical properties of the material were confirmed based on BET, FTIR, XRD, NH 3 -TPD and other characterization methods. The active sites of the catalysts were identified by poisoning experiments, and the kinetics of the catalytic reactions were designed and discussed. The apparent activation energy of Zr5-ST-C was calculated according to the Arrhenius equation. This study provides an effective solution for the efficient synthesis and industrial application of furfuryl ethers.
研究领域:
化学工程
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材料科学
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可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2024
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IF 4.3
Yikun Wang,Yuanmeng Wang,Xiangyuan Li,Jingbo Zhao
Biobased polyphenols have been widely studied for their renewable and non-toxic properties, and their thermoplastic/thermosetting materials have also been reported. However, most biobased polyphenols have high melting points and resistance to common solvents, which greatly hinder their applications in organic reactions and material synthesis. Herein, a trihydroxyethyl resveratrol (TER) with a relatively low melting point was prepared by an etherification of biobased resveratrol with ethylene carbonate, and TER trimethacrylate (TTM) was synthesized further from TER and methacryloyl chloride in the presence of triethylamine. TER and TTM were characterized by FTIR, NMR, ESI-MS, and DSC. Free radical curing reaction of TTM was conducted at different initiator dosages, and three crosslinked networks (TER-Ans) were obtained. The conversion rate, crosslinking density, T g , T α , mechanical properties, and contact angles were influenced highly by the initiator dosages. At the best initiator dosage of 1 wt% BPO, TER-A2 with the highest crosslinking density (42129.3 mol/m 3 ) and the maximum tensile strength (14.3 MPa) was obtained. Green etherification and hydroxylethylation were established to prepare sustainable crosslinked polymethacrylate materials from biobased resveratrol.
研究领域:
材料科学
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有机化学
✓ 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）