GREEN CHEMISTRY
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2019
·Vol. 21
·期 15
·4152-4158
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IF 9.405
Bernard Baffour Asare Bediako,Qingli Qian,Jingjing Zhang,Ying Wang,Xiaojun Shen,Jinbiao Shi,Meng Cui,Guanying Yang,Zhen Wang,Shengrui Tong,Buxing Han
Synthesis of ethanol from cheap and renewable CO2 is of great importance, but is still a challenge. Because it involves CO2 hydrogenation with simultaneous C–C bond formation, and the synergy of two or more transition metals is usually required for catalyzing the reaction effectively. Moreover, higher temperature is needed to drive the reaction. In this work, we found that the monometallic Ru3(CO)12 catalyst could efficiently catalyze the synthesis of ethanol from CO2, methanol and H2 in the ionic liquid, 1-butyl-3-methylimidazolium chloride ([bmim]Cl), using LiCl and LiI as promoters. Ethanol could form at 120 °C, which is among the lowest temperatures reported to date. A detailed study indicated that ionic liquids play an important role in monometallic catalysis. High ethanol selectivity and activity were obtained under optimized conditions. In addition, the catalyst could be easily recycled and the TON of ethanol reached 180 after five cycles. To our knowledge, this is the first time that an ionic liquid has been used as a reaction medium to produce ethanol using CO2 and H2.
研究领域:
化学
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可再生资源利用
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高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 6
·1651-1659
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IF 2.372
Bao Jingxian,Fan Yonghui,Zhang Shuyi,Zhong Liangshu,Wu Minghong,Sun Yuhan
Abstract An atomically economical green protocol for the hydrofunctionalization of olefins to higher aliphatic alcohols with 100% anti-Markovnikov regioselectivity was developed via visible-light photocatalytic coupling. This method employs cheap, readily available and abundant methanol as both the C1 feedstock and the hydrogen source under visible light irradiation over CdS photocatalyst. A wide scope of olefin substrates could be hydrofunctionalized successfully to the corresponding higher alcohols with high selectivity. Besides alcohol, acetone and acetonitrile can also couple with olefins to generate the corresponding hydrofunctionalization products, suggesting promising potential industrial application. Graphical Abstract Hydrofunctionalization of olefins to value-added chemicals with high selectivity was achieved via visible-light photocatalytic cross-coupling.
研究领域:
化学
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绿色化学
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光催化
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DOI
高影响因子
SOLAR ENERGY MATERIALS AND SOLAR CELLS
·
2015
·
IF 5.337
Zhao Li,Wei He,Jianjun Xu,Mengjin Jiang
In this study, an in situ grafting/crosslinking method was employed to prepare form stable thermal regulating fibers (TRFs). The fibers were made from polyvinyl alcohol (PVA, as fiber polymer), polyethylene glycol (PEG, as phase change material) and butane tetracarboxylic acid (BTCA, as crosslinking agent) and spun by dry spinning. The addition amount of BTCA and thermal treatment temperature for preparation were optimized by studying the reaction kinetics of PVA/BTCA and PEG/BTCA composite systems . The structures and properties of PEG/PVA/BTCA composite fibers were characterized by differential scanning calorimeter (DSC), two-dimensional wide angle X-ray diffraction (WAXD) and scanning electron microscope (SEM). Results show that small amounts of BTCA can form adequate chemical bonds to fix PEG in the PEG/PVA/BTCA composite at proper temperatures in the thermal treatment. In composite fibers, the crystallization of PVA promotes the phase separation between PVA and PEG, and the crosslinkages confine the crystallization of PEG. In the as-spun fiber, the crystallization of PEG occurred along the normal direction of the fiber axis . During the stretching, the original orientation of PEG crystals in fibers was destroyed and then new crystalline orientation formed along the fiber axis. The cross-sections of the composite fibers are almost round; after being extracted, the fibers crosslinked by BTCA are denser and have fewer defects than un-crosslinked PEG/PVA fiber, which demonstrated that the PEG can be fixed steadily in PVA fiber matrix by the in situ grafting/crosslinking method.
研究领域:
材料科学
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纺织工程
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DOI
高影响因子
RSC Advances
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2015
·Vol. 5
·期 77
·63044-63049
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IF 3.84
Hualei Hu,Jinghui Lyu,Jie Cen,Qunfeng Zhang,Qingtao Wang,Wenwen Han,Jiayao Rui,Xiaonian Li
The effect of MgO and Pd modification on the catalytic performance of hierarchical porous ZSM-5 for benzene alkylation with methanol was investigated. The results indicated that the introduction of MgO could reduce the Brönsted acid sites which suppressed the side reaction of methanol to olefins and in turn effectively promoted the alkylation of benzene. However, the single modification of MgO could not completely suppress the formation of ethylbenzene and coke. Doping a small amount of Pd had a positive effect on inhibiting the generation of ethylbenzene and coke, which could be attributed to the hydrogenation of ethylene into ethane on Pd. The dual modified catalyst (MgO and Pd) exhibited high benzene conversion (56%) and xylene selectivity (39.1%), and the lowest ethylbenzene selectivity (0.13%) and coke content (0.4 wt%).
研究领域:
催化化学
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材料科学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Jie Sun,Shaolong Wan,Fen Wang,Jingdong Lin,Yong Wang
A variety of catalysts for higher alcohol synthesis from syngas have been under development for potential commercial application, which are still facing challenges, including poor carbon efficiency due to low selectivity to desired products. In this contribution, we systematically studied the effects of temperature, loading of K and Cs, space velocity, and CO2 addition on the alkali-promoted Cu/ZnO/Al2O3 catalysts in order to achieve a high yield of desired higher alcohol products. Our particular focus was to maximize the carbon efficiency by restricting the amount of undesired byproducts, such as lower alkanes and CO2 that could be formed. Among K and Cs promoted Cu/ZnO/Al2O3 catalysts studied, Cs-promoted Cu/ZnO/Al2O3 catalysts exhibit better performance to higher alcohols and higher carbon efficiency than K-promoted counterparts under similar conditions studied. 1.64 mol % Cs-promoted Cu/ZnO/Al2O3 catalyst achieves the highest selectivity to higher alcohols (24.9%) at a CO conversion of 41.6% under 290 °C, 1875 mL g–1cat h–1, 5.4 MPa. The presence of a small amount of CO2 of 2.5 mol % in the feed has negligible effect on the productivity of higher alcohols but significantly suppresses the formation of CO2 byproduct. With the further increase of CO2 in the feed, the formation of CO2 can be further suppressed but at the expense of productivity loss of higher alcohols, which is probably due to the neutralization of surface Cs sites. The best carbon efficiency can be achieved at 8% mol CO2 in the feed.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2023
·Vol. 41
·期 24
·3618-3624
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IF 5.4
Sanyin Yang,Jun Bu,Rui Bai,Jin Lin,Siying An,Yafei Wu,Ying Guo,Jie Gao,Jian Zhang
Comprehensive Summary Alkenols are important intermediates for the industrial manufacture of various commodities and fine chemicals. At present, alkenols are produced via thermocatalytic semihydrogenation of corresponding alkynols using precious metal Pd-based catalysts in pressurized hydrogen atmosphere. In this work, we highlight an efficient electrocatalytic strategy for selectively reducing alkynols to alkenols under ambient conditions. Using 2-methyl-3-butyn-2-ol as a model alkynol, Cu 3 P nanoarrays anchored on Cu foam remarkably deliver an industrial-level partial current density of 0.79 A·cm –2 and a specific selectivity of 98% for 2-methyl-3-buten-2-ol in acidic solution. Over a 40-runs stability test, Cu 3 P nanoarrays maintain 90% alkynol conversion and 90% alkenol selectivity. Even in a large two-electrode flow electrolyser, the single-pass alkynol conversion and alkenol selectivity of Cu 3 P nanoarrays exceed 90%. Moreover, this selective electrocatalytic hydrogenation approach is broadly feasible for the production of various water-soluble alkenols. Electrochemical analyses, theoretical simulation and electrochemical in-situ infrared investigations together reveal that exothermic alkynol hydrogenation, facile alkenol desorption and formation of active H on Cu 3 P surfaces account for the excellent electrocatalytic performance.
研究领域:
化学工程
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电化学
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Xiaomeng Chang,Haoxu Yu,Ziai Liu,Zhen Yang,Faze Chen,Yanling Tian
Fluoroalkyl thiols and alkyl thiols are widely used as low surface energy reagents for the preparation of superhydrophobic surfaces and corrosion resistant surfaces. Although the corrosion resistance of thiol-induced superhydrophobic surfaces has been well addressed previously, few studies have devoted to revealing the difference of fluoroalkyl thiol and alkyl thiol modified surfaces towards anti-corrosion. In this work, two types of superhydrophobic surfaces were prepared by respectively coating self-assembled monolayers (SAMs) of 1 H,1 H,2 H,2 H-perfluorodecanethiol (PFDT) and 1-dodecanethiol (DDT) on femtosecond laser engineered copper substrates. The formation mechanism of the SAMs was explained by analyzing the surface chemical composition . The water contact angle of the PFDT and DDT modified surfaces were measured to be 157.7° and 154.6°, respectively. Electrochemical tests showed that both SAMs significantly reduced the corrosion current density ( I corr ) and corrosion rate of the copper surfaces, while simultaneously increased the charge transfer resistance ( R ct ) value by an order of magnitude compared to the pristine copper surface. The surface with PFDT SAM had the smallest I corr and its R ct value was about 1.5 times larger than that with the DDT SAM. These results confirmed that both the SAMs enhanced the anti-corrosion properties of the copper surfaces, and the PFDT SAM was proved to be more effective. Furthermore, the anti-corrosion durability of the PFDT and DDT modified surfaces were compared after exposing them to salt, acid, and alkali solutions for 12 h, and the results showed that the surfaces maintained to be hydrophobic and anti-corrosive, and the PFDT induced superhydrophobic surface indicated better durability. Our results demonstrated that thiols SAMs could significantly improve the anti-corrosion property of structured metal surfaces , and that fluoroalkyl thiol was more desired for long-term anti-corrosive applications in comparison with alkyl thiol.
研究领域:
材料科学
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腐蚀与防护
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表面工程
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DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2019
·
IF 2.298
Shenfeng Yuan,Yi Chen,Hong Yin,Zhirong Chen
In this work, the suitability or potential of ethanol aqueous solutions as a solvent for the extraction of alcohols from alcohol–alkane mixtures was studied. Experimental liquid–liquid equilibria (LLE) data of four quaternary systems {ethanol (1) + octanol (2) + dodecane (4) + water (6)}, {ethanol (1) + octanol (2) + tridecane (5) + water (6)}, {ethanol (1) + nonanol (3) + dodecane (4) + water (6)}, and {ethanol (1) + nonanol (3) + tridecane (5) + water (6)} were determined at T of 293.15, 298.15, and 303.15 K under atmospheric pressure. The nonrandom two-liquid model model was used to correlate binary interaction parameters. The parameters obtained from quaternary systems were used to predict six-component system LLE data. The predicted LLE data were in good agreement with the experimental data. The results showed that 75 wt % ethanol aqueous solution was suitable for separating octanol and nonanol from octanol + nonanol + dodecane + tridecane mixture and that 298.15 K was the suitable temperature.
研究领域:
化学工程
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物理化学
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热力学
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高影响因子
BIOTECHNOLOGY LETTERS
·
2020
·Vol. 42
·期 8
·1501-1511
·
IF 1.977
Chang Ya-Wen,Zhang Jian-Dong,Yang Xiao-Xiao,Li Jing,Gao Li-Li,Huang Shuang-Ping,Guo Xing-Mei,Zhang Cao-Feng,Chang Hong-Hong,Xu Jian-He
Objectives To screening of bacteria with cyclic amino alcohol deamination activity for enantioselective synthesis of chiral cyclic β-amino alcohols. Results A new strain named Arthrobacter sp. TYUT010-15 with the ( R )-selective deamination activity of cyclic β-amino alcohol has been isolated from nature via a high throughput solid-phase screening method. The reaction conditions of TYUT010-15 were optimized. Using the resting cell of TYUT010-15 as the catalyst, kinetic resolution of trans -2-aminocyclopentanol, trans -2-aminocyclohexanol and cis -1-amino-2-indanol was carried out to afford (1 S , 2 S )- trans -2-aminocyclopentanol, (1 S , 2 S )- trans -2-aminocyclohexanol and (1 R , 2 S )- cis -1-amino-2-indanol in > 99% ee and 49.6–50% conversion. Four aromatic β-amino alcohols and two amines were also resolved, ( S )-β-amino alcohols and ( R )-amines were obtained in > 99% ee. Preparation experiment was conducted with 200 mM (23.2 g L −1 ) racemic trans -2-aminocyclohexanol, yielding the desired (1 S , 2 S )- trans -2-aminocyclohexanol in 40% isolated yield, > 99% ee and 5.8 g L −1 d −1 space time yields. Conclusions This study provides a high throughput solid-phase method for screening of bacteria with cyclic amino alcohol deamination activity and a first example for practical preparation of chiral cyclic β-amino alcohol by Arthrobacter sp. TYUT010-15.
研究领域:
微生物学
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有机化学
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生物催化
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手性化学
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DOI
PubMed
高影响因子
METABOLIC ENGINEERING
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2019
·
IF 7.808
Wan-Ju Sun,Li Wang,Hao-Hao Liu,Yong-Jun Liu,Yu-Hong Ren,Feng-Qing Wang,Dong-Zhi Wei
The conversion of sterols to steroid synthons by engineered mycobacteria comprises one of the basic ways for the production of steroid medications in the pharmaceutical industry. Here, we revealed that high amounts of reactive oxygen species (ROS) generate during the conversion process of sterols, which impairs the cell viability of mycobacterial cells and thus hinders the conversion of sterols to steroid synthons. Accordingly, the endogenous antioxidants for detoxifying ROS in mycobacteria, ROS scavenging enzymes and low molecular weight thiols, were examined. The results revealed that three antioxidants, catalase (CAT), mycothiol (MSH), and ergothioneine (EGT), demonstrated efficacy toward neutralizing the excessive ROS produced during sterol metabolism . CAT overexpression or MSH or EGT augmentation enhanced the conversion of phytosterols to 22-hydroxy-23,24-bisnorchol-4-ene-3-one (4-HBC) by 18.9%, 23.8%, and 32.1%, respectively, and also enhanced the cell viability, indicating the benefits of these antioxidants in reducing ROS-induced stress. Further combinatorial augmentation of CAT, MSH, and EGT demonstrated enhanced effects toward intracellular ROS scavenging, resulting in 54.2% greater cell viability and 47.5% enhancement in 4-HBC production. These findings indicated that the excessive ROS induces cell stress, in turn limiting the conversion of sterols, whereas neutralization of the excessive ROS by combined control of CAT, MSH, and EGT serves as an effective strategy to boost the conversion productivity of sterols to steroid synthons.
研究领域:
药学
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微生物学
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生物技术
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生物化学
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Renren Sun,Haixia He,Lei Yuan,Jiao Sha,Liyuan Li,Zidan Cao,Gaoliang Jiang,Yu Li,Tao Li,Baozeng Ren
The solubility properties of dl-isoprenaline hydrochloride (dl-IPN) in four kinds of binary-solvents systems {( n -propanol, n -butanol, 2-propoxyethanol and 2-butoxyethanol) + methanol} at temperature range of 278.15–323.15 K under 101.3 kPa was further investigated using the laser monitoring technique. According to the result about solubility of dl-IPN in these chosen binary solvents, it is obvious that dl-IPN is more soluble at higher temperature. Additionally, the solubility values of dl-IPN, in all the investigated binary solvent mixtures, is improved with increasing mass fraction of co-solvent (methanol). The Hansen solubility parameters (HSPs) interpretate reasonably the order of dl-IPN solubility in these binary-solvents systems. Furthermore, the molecular dynamic (MD) simulation is employed to describe the molecular interactions of the types solute–solvent and solvent–solvent, and the obtained results confirm that solute–solvent and solvent–solvent molecular interactions have deep impact on the solubility of dl-IPN. The obtained experimental data about the solubility of dl-IPN is fitted by five models ( λh equation, Apelblat equation, Jouyban-Acree-Apelblat (J-A-A) model, Ma model and Sun model). The analysis of thermodynamic properties was based on the values of the calculated thermodynamic parameters. It can be concluded that the dl-IPN dissolution process is entropy-motivated and endothermal in all the investigated binary-solvents systems, and that the main contribution to Δ dis G o is due to enthalpy.
研究领域:
物理化学
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药学
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热力学
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分子模拟
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DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2022
·
IF 3.119
Guang Yang,Shaoming Fang,Jianqiang Zhang,Ruijuan Wang,Ruixue Liu,Renjie Xu,Chunjuan Huang
The solubility of 2-amino-3-chloropyrazine (ACPY) in some binary cosolvent mixtures of (methanol, isopropyl alcohol, ethylene glycol (EG), N,N-dimethylformamide (DMF)) plus water and the experimental solubility of 2-amino-3,5-dibromopyrazine (ADPY) in (ethanol + water), (isopropyl alcohol + water), (EG + water), and (PG + water) were all determined by the isothermal saturation method from 278.15 K to 323.15 K at 101.2 kPa. The trend of the system temperature and the change of the solvent partner are both factors that affect the dissolution. As the temperature goes higher, the amount of dissolution follows, but the higher is the water content of the solvent, the less solute will be dissolved. The combination of DMF and water is best for the dissolution of ACPY, and the addition of ethanol to water shows an advantage of dissolving ADPY over other combinations. The experimentally obtained dissolution data were then calculated by using three models for the two miscible solvent systems. For ADPY, RAD and RMSD maximums were 2.63 × 10–2 and 2.10 × 10–5. For ACPY, RAD and RMSD were no greater than 6.55 × 10–2 and 6.83 × 10–4.
研究领域:
物理化学
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化工
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药学
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DOI
高影响因子
危险品化学品经营许可证（带存储）