DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 9
·4048-4053
·
IF 3.5
Lin Gao,Guoqiang Ding,Lei Zhu,Zhanqiu Yu,Hongju Li,Guoqiang Li,Yulei Zhu,Hongwei Xiang,Xiaodong Wen,Yong Yang,Yongwang Li
The dimethyl maleate hydrogenation activity of Cu, ZnO-X and physically mixed Cu+ZnO-X samples was systematically investigated to probe the essential role of ZnO in ester hydrogenation processes. Cu samples exhibited high CC bond hydrogenation ability with dimethyl succinate as the main product. Comparatively, ZnO was inactive in hydrogenation due to its weak ability to dissociate hydrogen while the CO group could be activated and adsorbed on the ZnO surface. Interestingly, physical mixing with ZnO significantly improved the CO hydrogenation activity of Cu samples. The H2-TPD results reveal the origin of “Cu–ZnO synergy”: hydrogen atoms formed on the copper surface can spill over to the ZnO surface and react with the adsorbed CO group.
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2023
·
IF 6.1
Dingkai Wang,Mingyu Cui,Wei Zhao,Yanjun Li,Shangshang Ma,Zhijie Jiang,Xutang Liu,Chong Liang,Rujuan Li,Long Ma,Yanmin Song,Xian-Yong Wei
Lignin, the second largest component of biomass, is considered as an important alternative source of fossil reserves for the production of fuels and chemicals. Here, we developed a novel method to oxidatively degrade organosolv lignin into value-added four-carbon esters, particularly diethyl maleate (DEM), with the cooperative catalyst consisting of 1-(3-sulfobutyl) triethylammonium hydrogen sulfate ([BSTEA]HSO4) and 1-butyl-3-methylimidazolium ferric chloride ([BMIM]Fe2Cl7). Under optimized conditions (1.00 MPa initial O2 pressure, 160 °C, 5 h), the lignin aromatic ring was effectively cleaved by oxidation to form DEM with a yield of 15.85% and a selectivity of 44.25% in the presence of the synergistic catalyst of [BMIM]Fe2Cl7-[BSMIM]HSO4 (1/3, mol/mol). The structure and composition analysis of lignin residues and liquid products confirmed that the aromatic units in lignin were effectively and selectively oxidized. Furthermore, the catalytic oxidation of lignin model compounds was explored for obtaining a possible reaction pathway of oxidative cleavage of lignin aromatic units to DEM. This study provides a promising alternative method for the production of traditional petroleum-based chemicals.
研究领域:
化学工程
·
生物质能
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
·
2012
·
IF 2.947
Xing Li,Jijuan Su,Honghong Chang,Gong Li,Yanwei Li,Wenlong Wei
A simple and efficient method has been developed which describes KOH-oriented catalytic regioselective ring-opening reactions of various N -tosylaziridines with malonates. In the presence of 20 mol% KOH, most N -tosylaziridines can smoothly react with malonates to give the corresponding products in good to excellent yields (up to 99%) and with good to excellent regioselectivity under mild experimental conditions.
研究领域:
有机化学
·
合成化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Qiuyan Ding,Zhengkun Hou,Xueli Geng,Guiyu Gao,Wenwei Dong,Hong Li,Yaohong Wang,Xibo Chen,Xin Gao
The new energy battery is currently a hot research topic, leading to an increase in the demand for malonic acid (MA) as a raw material. The objective of the present work is to find a potential reactive distillation (RD) process to solve the problem of low conversion and high energy consumption in hydrolytic system. In the meantime, the RD technology still faces the problem of how to distribute water in the RD column. Aiming at the problem, four different RD processes are proposed: RD combined water separation process (RDWS), RD combined with MA concentration process (RDMC), RD combined methanol separation process (RDMS), and single RD process (SRD). Beforehand, reaction kinetic of dimethyl malonate (DM) hydrolysis was investigated using the ion exchange resin catalysts, and the developed RD model was verified via pilot-scale RD experiments. Finally, the proposed RD process is analyzed from the aspects of economic and environmental and compared with the traditional reaction + distillation (R + D) process. Consequently, the proposed SRD process is a better economy-saving and environment-friendly technology, and has certain directive significance for the industrial production of MA.
研究领域:
化学工程
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能源材料
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产品关联
DOI
高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Qiang Yao,Jing Guo,Yuanfa Liu,Fucheng Guan,Shuxing Liu,Xuelin Huang,Xin Zhang,Qiang Yang
In this work, an organic phase change material-Bishexadecyl maleate was prepared by direct esterification of maleic anhydride (MA) and hexadecanol (HD). Then, in order to improve the crystalline phase of bishexadecyl maleate (MAHD), the synthesized MAHD was recrystallized with ethanol to prepare ethanol-bishexadecyl maleate (MAHD (E) ). Fourier transform infrared spectroscopy (FTIR), nuclear magnetic resonance (NMR), and x-ray diffraction (XRD) were used to characterize the chemical and crystalline structures of MAHD and MAHD (E) . Polarizing Light Microscopy (POM) for observation of phase transition behavior of MAHD/MAHD (E) . Differential scanning calorimetry (DSC), Variable temperature Fourier transform infrared spectroscopy (VT-FTIR), and thermo gravimetric analysis (TG) characterize the thermal properties and thermal stability of MAHD/MAHD (E) . The results display that MAHD/MAHD (E) have the same chemical structure, and no chemical change occurs within the phase transition temperature, but the crystallinity of MAHD (E) has increased. Compared with HD, the crystallization temperature and melting temperature of MAHD/MAHD (E) is significantly reduced, which effectively expands the application range of HD. POM was observed to have a melting-recrystallization-melting behavior during the heating of MAHD/MAHD (E) . This behavior was shown in the DSC curve as an unusual endothermic-exothermic-endothermic curve. After 100 thermal cycles, both MAHD and MAHD (E) exhibit good cycling stability. TG exhibits that the thermal stability of MAHD/MAHD (E) has been dramatically improved compared to HD, it has high application potential in phase change and energy storage. Therefore, MAHD/MAHD (E) is expected to be a substrate for new phase change materials , while the C C in the molecular chain provides potential reactivity with significant potential applications in the field of phase change energy storage.
研究领域:
材料科学
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化学工程
·
能源存储
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Gui Zhang,Lunkai Li,Yuqin Yang,Li Song,Guangrong Kuang,Yingzi Fu
Organic luminescent materials with unique photoelectric properties are as a kind of emerging luminophore at the forefront of research in biological detection on account of their facilely varied functional groups. However, most organic luminophores are aromatic compounds with certain biological toxicity to limit their application. Herein, we envisioned a green organic electrochemiluminescencence (ECL) luminophore without aromatic ring structure but electron-rich functional groups via in-situ growth of poly (ethylene maleate) (PEM) on nano-silica (NS). The experimental and theoretical modelling results indicate that ECL signal of PEM-NSs was enhanced by the spatial conjugation of ester groups (ester clusters), due to the contribution of smart bridging of NS with different sizes. The smaller the NS size is, the more growth of ester groups on the NS surface is, and the closer individual ester groups are linked via “through-space interaction” to form stable ester clusters with smaller energy gaps, thus achieving high ECL performance. For further application, PEM-NS-1 was selected as meaningful ECL luminophore, and integrated with exonuclease III-assisted catalytic hairpin assembly amplification strategy, an efficient platform for biomarkers (microRNA-21) detection was constructed with the detection limit of 2.73 fM (S/N = 3). This work sets the stage for strengthening ECL of electron-rich functional groups, and provides a way of thinking for low-toxicity organic luminophores.
研究领域:
分析化学
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生物医学工程
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材料科学
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产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·Vol. 50
·期 7
·3369-3389
·
IF 2.8
Wang Lu,Rehman Mooeez ur,Jiang Yong,Sun Fan,Zhao Yuanqi,Lu Xiyue,Zhang Zhijun,Liu Wei,Xu Yan,Zhai Yong,Zhao Yujun
With the growing global demand for biodegradable plastics, the hydrogenation of dimethyl maleate (DMM) to produce 1,4-butanediol (BDO), raw materials for poly(butylene succinate), has become one of the hot spots in chemical industry. In this work, we synthesized a series of Cu@C/ZnO–S x catalysts by the method of sorbitol modification for the liquid-phase hydrogenation of DMM. The modification with appropriate sorbitol led to a decoration of carbon on catalyst surface, which improved the copper dispersion and Cu + /(Cu 0 + Cu + ) molar ratio in the Cu@C/ZnO–S 0.08 catalyst. The carbon decoration not only promoted the formation of more copper species having stronger interaction with ZnO, but also enhanced the absorption of ester on catalyst surface. These distinctive properties contributed to the high performance of the Cu@C/ZnO–S 0.08 catalyst in DMM hydrogenation, achieving an excellent BDO yield of 98.4% and superior reusability. The insights into the roles of sorbitol modification could give valuable guidance to the further design of high performance catalysts for esters hydrogenation. Graphical abstract
研究领域:
化学工程
·
催化科学
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产品关联
DOI
高影响因子
JOURNAL OF PHYSICAL CHEMISTRY B
·
2015
·
IF 3.302
Dongdong Hu,Shaojun Sun,Peiqing Yuan,Ling Zhao,Tao Liu
Multiscale molecular modeling and dissolution behavior measurement were both used to evaluate the factors conclusive on the CO2-philicity of poly(vinyl acetate) (PVAc) homopolymer and poly(vinyl acetate-alt-maleate) copolymers. The ab initio calculated interaction energies of the candidate CO2-philic molecule models with CO2, including vinyl acetate dimer (VAc), dimethyl maleate (DMM), diethyl maleate (DEM), and dibutyl maleate (DBM), showed that VAc was the most CO2-philc segment. However, the cohesive energy density, solubility parameter, Flory–Huggins parameter, and radial distribution functions calculated by using the molecular dynamics simulations for the four polymer and polymer–CO2 systems indicated that poly(VAc-alt-DBM) had the most CO2-philicity. The corresponding polymers were synthesized by using free radical polymerization. The measurement of cloud point pressures of the four polymers in CO2 also demonstrated that poly(VAc-alt-DBM) had the most CO2-philicity. Although copolymerization of maleate, such as DEM or DBM, with PVAc reduced the polymer–CO2 interactions, the weakened polymer–polymer interaction increased the CO2-philicity of the copolymers. The polymer–polymer interaction had a significant influence on the CO2-philicity of the polymer. Reduction of the polymer–polymer interaction might be a promising strategy to prepare the high CO2-philic polymers on the premise that the strong polymer–CO2 interaction could be maintained.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhengkun Hou,Qiuyan Ding,Hongbin Wang,Yilai Jiao,Peng Jin,Hong Li,Xin Gao
In reactive distillation processes constrained by the efficiency of vapor–liquid mass transfer, reducing the physical dimensions of simultaneous reaction and separation operations can significantly enhance overall process efficiency. To achieve this, HY@SiC, a structured catalytic packing was developed, allowing for concurrent catalytic reactions and vapor–liquid mass transfer on its surface. This innovative catalytic packing was employed in a pilot reactive distillation column to experimentally investigate the production of dimethyl maleate via reactive distillation, marking the first validation of its performance. Additionally, a reactive distillation model incorporating HY@SiC structured catalytic packing was established. Ultimately, a new double-column reactive distillation process for producing dimethyl maleate was proposed, with plans for optimization aimed at minimizing total annual cost, which was 4.08 × 10 5 $/y, utilizing a sequential iterative algorithm as the core focus for design improvements, while achieving DMM yield and purity levels of 99.42 % and 99.0 wt%, respectively.
研究领域:
化学工程
·
工艺设计
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催化
·
反应精馏
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产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 13
·e55172
·
IF 2.7
Guochen Wang,Weiping Xu,Yanxin Zhang,Dong Chen,Yuhong Ma,Changtong Song,Wantai Yang
Dynamic B O bonds are often applied to fabricate reversible-cross-linking and reprocessable polymer networks due to their high thermodynamic stability and kinetic tunability. However, it is still difficult to tailor boronic ester polymers, which have both excellent mechanical and self-healing properties in the absence of external stimuli. To address the above challenge, a range of room-temperature self-healable vitrimers are prepared by the reactions of various poly(vinyl hydroxyalkyl ether- alt -dialkyl maleate) copolymers and 1,4-phenyldiboronic acid. The dynamic cross-linking networks offer the as-prepared vitrimers superior mechanical properties and thermostability. Because of the presence of dynamic boronic ester bonds, the networks also demonstrated self-healing (the tensile strength recovered to 83% after 3 days at room temperature) and reprocessing capabilities (no significant change in tensile strength after thrice process recycles). Moreover, the vitrimers have potential as promising damping materials with wide temperature windows around room temperature. For example, the vitrimer of poly(ethylene glycol monovinyl ether- alt -dibutyl maleate) and 1,4-phenyldiboronic acid demonstrates its tan δ max 1.18, T g = 6.2°C and effective damping temperature range is from −16.4 to 48.5°C.
研究领域:
材料科学
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高分子化学
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机械工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Lin Chen,Di Wang
A tunable cascade reaction of ureidomalonates and alkenyl azlactones was disclosed, which gave rise to the construction of N-aroyl α-amino acid ester and imide-functionalized hydantoins in moderate to good yields and with excellent diastereoselectivities. The reaction pathway was precisely manipulated by organocatalysis and phase-transfer/sunlight relay catalysis, respectively, to realize the divergent synthesis. The successful gram-scale preparation of representative products exhibited the application potential of this protocol. Mechanistic studies indicated that the exchange and phase transfer of ethoxy anion played a key role in altering the reaction pathway, and sunlight might accelerate the oxidation process at the late stage of the reaction triggered by phase-transfer catalysis.
研究领域:
有机化学
·
合成化学
·
催化
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Huashan Wang,Kaiyue Liu,Xing Chen,Meiyi Wang
A series of biodegradable copolyester of poly (butylene succinate-co-butylene malate) (P (BS-co-BM)) bearing hydroxyl groups were prepared by one-pot synthetic strategy without hydroxy-protection. The structure and properties of the P (BS-co-BM) were characterized by nuclear magnetic resonance ( 1 H NMR), thermogravimetry analysis (TGA), differential scanning calorimetry (DSC), polarized optical microscope (POM), contact angle tester and enzymatic degradation. The results showed that the P (BS-co-BM) manifested excellent thermal properties. The glass transition temperature (T g ) of the P (BS-co-BM) increased with malic acid units added, the crystallizability temperature (T c ) decreased from 72.6 °C to 21.7 °C, and the melting point temperature (T m ) decreased from 117.9 °C to 82.4 °C. The crystallization rate of poly(butylene succinate) (PBS) segment within P (BS-co-BM) was improved by the introduction of malic acid. The enzymatic degradation rate increased with hydrophilicity of the copolyester improving.
研究领域:
材料科学
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高分子化学
·
生物降解材料
·
热分析
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）