CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Linsong Yang,Yuting Liu,Yu Peng,Yu-Cai He,Cuiluan Ma
The feasibility of chemobiocatalytic production of furfuryl alcohol from biomass-derived D -xylose was investigated using a tandem catalysis with deep eutectic solvent betaine:benzenesulfonic acid (DES BE:BA) and recombinant Escherichia coli DCF cell. The DES BE:BA (2.5 wt%) was applied to catalyze D -xylose under 170 °C for 0.5 h, resulting in a furfural yield of 51.1%. Consequently, recombinant Escherichia coli DCF fully transformed D -xylose-derived furfural to furfuryl alcohol in DES BE:BA-water under pH 7.5 and 40 °C using HCOONa as cosubstrate. This eco-friendly chemobiocatalytic strategy was successfully applied for transforming D -xylose to furfuryl alcohol in DES BE:BA-water.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Luming Wang,Yuhang Bian,Zhenyu Wu,Zengxi Li,Gang Wang,Chunshan Li
Hydroesterification of ethylene with carbon monoxide (CO) and methanol (MeOH) for preparing methyl propionate (MP) has stimulated researcher’s attention in recent years. Herein, the palladium-phosphine catalyzed ethylene hydroesterification with the promotion of acidic poly ionic liquids (APILs) for direct MP synthesis was developed. Series of APILs samples having different anions and acid densities were prepared and their structural properties were characterized by employing NMR, FTIR, TG and XPS. The anion type and acid density in APILs shown great influence on the catalytic performance due to the electronic effect and proton supply capacity related to Pd-H species formation. The hydrogen bond formed through the interaction between the anion of APILs and methanol could effectively promote the ethylene hydroesterification. The substrate extension experiments revealed the polarity and steric hindrance of alcohol would impact ethylene conversion. The mechanistic studies using in-situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) unraveled that the hydroesterification started with the activation of palladium complex to Pd-H species by CO, followed by the sequential formation of Pd-C 2 H 4 , Pd-alkyl and Pd-acyl intermediate species and consequential product MP. As a result, 94.4 % ethylene conversion could be achieved with 100 % selectivity toward MP at 80 °C and 2 MPa. No obvious deactivation behavior was observed for this kind of palladium catalyst after ten recycling experiments. The kinetic studies revealed the activation energy of ethylene hydroesterification is 59.3 kJ/mol.
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WASTE MANAGEMENT
·
2019
·
IF 5.431
Yuanpeng Fu,Yaqun He,Lili Qu,Yi Feng,Jinlong Li,Jiangshan Liu,Guangwen Zhang,Weining Xie
Recycling of valuable metals from spent lithium ion batteries (LIBs) is of great significance considering the conservation of metal resources and the alleviation of potential hazardous effects on environment. Thus, the present work focuses on enhancing the efficiency of leaching process for the recovery of cobalt and lithium from the cathode active materials of spent LIBs. In this study, benzenesulfonic acid (C 6 H 5 SO 3 H) with a reducing agent hydrogen peroxide (H 2 O 2 ) was innovatively used as leaching reagents, and the operating variables were optimized to obtain higher leaching efficiencies. Results show the optimized leaching recovery of 99.58% Li and 96.53% Co was obtained under the conditions of 0.75 M benzenesulfonic acid, 3 vol% H 2 O 2 , a solid to liquid (S/L) ratio of 15 g/L, 500 rpm stirring speed, and 80 min leaching time at 90 °C. Moreover, a new kinetic model was introduced to describe the leaching kinetics of LiCoO 2 from the cathode material. The apparent activation energies E a for leaching of lithium and cobalt are 41.06 and 35.21 kJ/mol, respectively, indicating that the surface chemical reaction is the rate-controlling step during this leaching process. Further, the proposed recovery mechanism for spent cathode material was raised by analyzing the experimental results and characterizing the morphological and chemical state (i.e. SEM-EDS, XPS and XRD) of raw material and leaching residues. In comparison with the previous leaching process, this research was found to be efficient, low energy consumption, and environmental friendly.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Ruiyi Wang,Zhiwei Wu,Zhikai Li,Zhangfeng Qin,Chengmeng Chen,Zhanfeng Zheng,Guofu Wang,Weibin Fan,Jianguo Wang
Polyoxymethylene dimethyl ethers (PODE n , with the formula of CH 3 O–(CH 2 O) n –CH 3 ), as a promising environmentally benign diesel fuel or additive with an enormous potential in the reduction of soot and NO x emissions, can be efficiently synthesized from methanol derivatives such as dimethoxymethane (DMM) and trioxymethylene (TOM), which requests a proper catalyst of high performance. In this work, the catalytic performance of graphene oxide (GO) in the synthesis of PODE n as well as its relation to the catalyst structure was thoroughly investigated. The results indicate that GO is an excellent catalyst in the synthesis of PODE n from DMM and TOM; a TOM conversion of 94.6% and selectivity of 86.0% to PODE 2–8 are achieved under mild reaction conditions, which is superior to the majority of the state-of-the-art catalysts. Meanwhile, the active species and characteristic layer structure of GO sheets catalytically responsible for PODE n formation were discriminated through selectively removing certain surface functional groups, thermally annealing at different temperatures, and carefully comparing with a series of model compounds. The results illustrate that the superior catalytic performance of GO in the PODE n synthesis should be ascribed to a synergy between the surface sulfonyl, hydroxyl and carboxyl groups present on the GO surface and the unique layered structure of GO sheets, wherein the surface sulfonyl groups act as the main active sites. The insights shown in this work are beneficial to a deep understanding on the catalytic principle of GO and development of efficient catalyst for the synthesis of PODE n .
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Frontiers in Chemistry
·
2019
·
IF 3.782
Cai Guangming,Yang Shaoqi,Zhou Qing,Liu Lifei,Lu Xingmei,Xu Junli,Zhang Suojiang
In order to obtain the regularities of physicochemical properties of hydroxy protic ionic liquids (PILs) and broaden their potential application, a series of 2-hydroxyethylammonium sulfonate-based PILs were synthesized through proton transfer reaction and characterized by NMR and FT-IR and elemental analysis. Their phase transfer behavior (Tm) and initial decomposition point (Td) were characterized by differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA), respectively. Meanwhile, the regularities of density (ρ), viscosity (η) and electrical conductivity (σ) of synthesized PILs at different temperatures were measured. The results indicated that their physicochemical properties were tightly related with their structures and the interactions between cations and anions. In addition, the dissociation constants (pKa) of synthesized PILs were obtained by acid-base titration, which revealed that all synthesized PILs had pKa exceeding 7 and their cations were the crux of determining the pKa value. Moreover, several synthesized PILs with a low melting temperature also showed potential application in the deoxidation reaction of cyclohexanol, as they had conversion rates approximating 100% and the selectivity of cyclohexane or cyclohexene was about 80%.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2018
·
IF 2.196
Chen Meng-qi,Xu Jie,Wei Yan,Hao Shuang-hong
The primary aim of this study is to develop a recovery process for PhSO3K from the industrial waste of Qpe (quizalofop-p-ethyl) production. The solubility data for the PhSO3K–K2CO3–H2O system at 15, 25, 35, 45, and 55 °C were determined to obtain the phase diagram of the system. Moreover, the different crystallization fields in the phase diagram of 25 °C were analyzed. The separation technology of PhSO3K from the PhSO3K–K2CO3–H2O system was designed based on the phase diagram. Furthermore, the PhSO3K and K2CO3 in a wastewater from Qpe production were crystallized in sequence by evaporation according to the designed method. The organic impurities precipitated concomitantly with PhSO3K were washed out by ethanol. Finally, the purified PhSO3K was converted to (R)-ethyl O-bezenesulfonyl lactate, the intermediate of Qpe production.
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POLYMER COMPOSITES
·
2014
·Vol. 35
·期 10
·2056-2066
·
IF 1.455
Xiangming Hu,Yanyun Zhao,Weimin Cheng,Deming Wang,Wen Nie
In this study, phenol, urea, and paraformaldehyde were used as the monomers for the one-step synthesis of phenol-urea-formaldehyde (PUF) foaming resin that was used to block air leakage in mining. An orthogonal test was used to study the effects of urea amount, catalyst amount, reaction temperature, and reaction time on the foaming property of the resin. The results showed that the optimum parameters for synthesizing PUF resin are as follows: 1 mol phenol, 0.5 mol urea, 3 mol formaldehyde equivalents of paraformaldehyde, and 0.05 mol catalyst at 75°C for 3 h. The infrared and 13 C nuclear magnetic resonance spectra of the PUF resin showed that the chemical structure of the PUF resin was significantly different from that of phenol-formaldehyde resin, indicating that a copolymerization reaction has occurred among the three components, that is, phenol, urea, and paraformaldehyde. In this study, PUF foam was prepared from catalysts and PUF resin. The results showed that the foaming capacity and oxygen index of the PUF foam were significantly improved by using urea, whereas the shrinking percentage decreased with no change in compression strength. POLYM. COMPOS., 35:2056–2066, 2014. © 2014 Society of Plastics Engineers
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Wen Zhou,Fucheng Zhu,Yuanlin Li,Chen Liu,Jie Xu,Houmei Liu
Genotoxic impurities (GTIs), which are present at very small amounts in drugs, can cause severe toxicity. The existence of GTIs poses a significant risk to patients, pharmaceutical companies, and regulatory agencies. Sulfonate compounds, as a typical genotoxic impurity, present a challenge in quantitative analysis because of their low concentration and instability. In this work, by a green, simple and low-cost preparation strategy, a novel polymer was modified on the surface of silica by the reaction of two monomers (1,5-dihydroxynaphthalene and 1,3,5-trimethylhexahydro-1,3,5-triazine). By systematically optimizing the ratio and concentration between the two polymeric monomers and silica, the resultant adsorbent labeled as S-D 1 T 1 /20 was obtained and showed outstanding adsorption performance for sulfonate. Mechanism studies revealed that there are effective hydrogen bond and π-π stacking interactions between S-D 1 T 1 /20 and sulfonate. For the partial sulfonates which are easy to hydrolyze, we proposed to detect the concentration of their hydrolyzed forms. By optimizing the loading and eluting conditions, an SPE-HPLC-DAD method with high sensitivity was developed for the quantitative enrichment and determination of six sulfonates with a wide linear range (0.01 ∼ 3μg mL −1 ), low limits of detection (5 ∼ 25 ng mL −1 ), satisfied inter-day precision, and intra-day precision. Last, this method was successfully applied to various species and forms of commercial drugs and achieved satisfied sulfonate recoveries (91.2 % ∼ 105.8 %). This work provides a unique solution to the frontier scientific problem of accurate determination of trace sulfonate genotoxic impurities in drugs, which is of great significance for ensuring drug quality and clinical safety.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Na Zhang,Lei-qiang Liu,Yao Zhang,Jun Shen,Yu-gao Wang,Gang Liu,Yan-xia Niu
Coal tar pitch (CTP) is a carbon material with abundant yield in China, but the toxic polycyclic aromatic hydrocarbons (PAHs) contained in it have restricted its broader applications. In order to reduce the PAHs content, an alkylation method was developed in this study to modify CTP (MCTP) by using 1-dodecene as the alkylating reagent, and the optimal reaction conditions (temperature 170 °C, time 4 h, solvent dosage 60 times that of CTP, and alkylating reagent dosage 4 times that of CTP) for synthesizing the MCTP were determined by alkylation modification with model compounds. Compared with CTP, the content of PAHs in MCTP was reduced by 97.35 %. The mechanism of the reaction was explained by analyzing the types of alkylation products and combining structural analyses of CTP and MCTP. PAHs emissions from fumes and the toxic equivalent quantity (TEQ) among different environmental standards were greatly reduced, while MCTP demonstrated low cytotoxicity and ecotoxicity. The method can also be applied to the toxicity assessment of road materials such as alkylation by-products.
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ChemistrySelect
·
2025
·Vol. 10
·期 7
·e202405464
·
IF 2
Kun Jia,Peng Jia
Graphical The asymmetric activation of anhydrous methanol molecules is realized by exogenous protons, the position and protonation position of asymmetric activation are determined, and the C─H bonding energy and reaction activation energy of some methanol molecules are reduced, and the asymmetric regulation of the non-oxidation dehydrogenation reaction process of anhydrous methanol molecules was realized. The activation of C─H bonds under mild conditions is a crucial step in the conversion of organic molecules. However, the simultaneous activation of C─H bonds in methanol can result in excessive oxidation, thereby diminishing the selectivity for formaldehyde production. We achieved selective activation of the C─H bonds in methanol under mild conditions by adjusting the proton concentration in an anhydrous methanol solution, which significantly enhanced the dehydrogenation rate of methanol. Additionally, we constructed related molecular models to identify the sites of asymmetric oxidation, providing new insights for further studies on C─H bond activation.
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