APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Liqin Wang,Heqin Guo,Qilong Xie,Jungang Wang,Bo Hou,Litao Jia,Jinglei Cui,Debao Li
Furfural is one of the most valuable biomass platform compounds which is typically prepared from hemicellulose. Conversion of cellulose and its derived hexoses, which are the most abundant resource in nature, to furfural, is a big challenge. The amount of the reactive form (fructofuranose) which was beneficial to the formation of furfural and HMF, was increased when the solvent transformed from water to γ-butyrolactone (GBL)-water. The GBL promoted the adsorption of fructose on HY. The transfer of fructose from the solution to the channels of HY was enhanced with the introducing of GBL in solvent. The HY zeolite with apertures of 7.4 Å was found to promote the formation of acyclic fructose from cyclic fructose (8.6 Å) in the synergy with GBL. The Brønsted acid sites in the channels of HY favored the selective cleavage of the C C bond in acyclic fructose to xylose, and promoted the following dehydration of xylose to furfural, simultaneously. The furfural yield was increased while the 5-hydroxymethylfurfural (HMF) yield was decreased with the decrease of the Brønsted acid sites density. The maximum furfural yield was 37.8% over HY-3, while the maximum HMF yield was 69.2% over HY-1 in the conversion of fructose in GBL-water solvent. In addition, the etherification of HMF was the main factor for the low HMF yield and carbon balance in fructose conversion in GBL-water solvent.
研究领域:
化学工程
·
生物质转化
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Zhongwen Dong,Xinyi Wang,Weifeng Chu,Chuanyu Yang,Yanan Wang,Lin Mei,Dongpu Zhao,Wenjie Xin,Shenglin Liu,Hongxia Wang,Yongchen Shang,Longya Xu
A fast synthetic methodology of β-zeolite with the assistance of γ-butyrolactone (GBL) has been developed in this paper, and the synthetic parameters are systematically investigated to obtain β-zeolite efficiently. Compared to the conventional synthetic system with a crystallization time of 120 h, GBL promotes the crystallization of β-zeolite in a much shorter time of 24 h. An accelerated nucleation mechanism of β-zeolite assisted by GBL is unraveled by X-ray diffraction, scanning electron microscopy, thermogravimetry–differential thermal analysis, Fourier transform infrared spectroscopy, and NMR techniques. The results demonstrate that GBL can adjust the pH value of the initial gels and enhance the combination of TEA+ with aluminosilicate species; in the meantime, the Hoffmann degradation of TEAOH is suppressed. In addition, the β-catalyst obtained with the assistance of GBL exhibits both a higher selectivity of tert-butylbenzene and excellent catalytic stability in the alkylation of benzene with isobutylene compared with the commercial β-catalyst with a similar SiO2/Al2O3 molar ratio.
研究领域:
化学工程
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催化材料
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Zhenping Li,Hao Xu,Yukun Du,Zhongyu Huang,Jing Li,Lian Liu,Ying Dong,Xiao-Yu Yang
Gamma-hydroxybutyric acid (GHB), which is used in drug-facilitated sexual assault, is typically delivered in the form of gamma-butyrolactone (GBL) in beverage carriers. In response to the growing need of methods for rapid and on-site sensing of the drugs, we carried out an investigation aimed at developing a superwettable microchip for visual detection of the date-rape drug GBL in adulterated beverages. The superwettable microchip is comprised of Fe 3 O 4 nanoparticles which aggregate to form a reactive spot on a superhydrophobic fabric. The spot captures and confines microdroplets containing GBL on the superhydrophobic substrate. Fe(III), generated by HCl promoted reaction of the Fe 3 O 4 spot, then participates in a colorimetric reaction with GBL to form a naked eye observable colored complex. Quantitative determination of GBL in beverages is achieved by analyzing the red proportion of a smartphone camera derived image. The detection range of this assay protocol is ca. 0.1–10 mg mL −1 , which meets the requirements to detect potentially dangerous concentration of GBL in drinks. The detection stability of the superwettable microchip for GBL in water and common beverages is maintained over at least 30 cycles.
研究领域:
分析化学
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法医学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Haoyu Li,Pengfei Wu,Xianquan Li,Jifeng Pang,Shangru Zhai,Tao Zhang,Mingyuan Zheng
High-performance MFI zeolite supported nickel catalysts were prepared by the ammonia evaporation method for maleic anhydride (MA) conversion to γ-butyrolactone (GBL). According to comprehensive characterizations, the Ni catalysts possessed petal-like morphology and hierarchical structures with meso and micro pores. Nickel species were highly dispersed on the silica support and generated abundant Lewis acid sites (LAS), which effectively activated carbonyl groups in the reactant and accounted for the high activity in MA hydrogenation. Zr species hydrothermally introduced into the catalyst increased the number of LAS and decreased the apparent activation energy for the reaction. The highest GBL yield reached 95.6% over 40Ni-2Zr-MFI with the assistance of 3A zeolite to in-situ remove water byproduct. The catalyst showed reasonably good stability in five-cycle operation thanks to the strong interaction between Ni and support. The reaction route for MA hydrogenation was investigated, in which succinic anhydride (SA-A) served as the major reaction intermediate for GBL formation.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Siying Chong,Shuang Zhao,Jiaoyan Li,Gangwei Huang,Yajing Zhang,Ruirui Liu,Kangjun Wang
Gas-phase dehydrocyclization of biomass-derived 1,4-butanediol (BDO) to γ-butyrolactone (GBL) is a sustainable and environmentally friendly process conducted at atmospheric pressure. In the present work, a series of 15Cu/xMgO-yCeO 2 catalysts with different MgO: CeO 2 ratios were prepared by the ammonia vaporization method. The gas-phase dehydrocyclization of BDO to GBL was carried out over these Cu-based catalysts synthesized in a fixed-bed reactor. The physicochemical properties of the catalysts were investigated by XRD, SEM, TEM, FTIR, N 2 isothermal adsorption–desorption, H 2 -TPR, CO 2 -TPD, Raman, XPS, and EPR. The results indicated that the 15Cu/10MgO-90CeO 2 catalyst exhibited a smaller particle size, higher specific surface area, and increased oxygen vacancies than the 15Cu/CeO 2 catalyst. Operating conditions of 240 °C reaction temperature, 2.4 mL/h space velocity, and 98.92 % GBL yield from BDO dehydrogenation were achieved under 40 mL/min N 2 flow for 4 h. Density functional theory (DFT) calculations confirmed that the 15Cu/10MgO-90CeO 2 catalyst with more oxygen vacancies was more favorable for the adsorption and activation of BDO on the catalyst surface than 15Cu/CeO 2 , and its higher catalytic activity was attributed to the synergistic interaction between Cu + and oxygen vacancies on the catalyst surface.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiao Chen,Nannan Zhang,Huaming Wang,Ying Zhong,Tianming Lv,Changhai Liang
The continuous flow selective hydrogenation of maleic anhydride (MA) to γ-butyrolactone (GBL) over highly efficient and long-term stable catalysts is a considerable promising strategy for both lab-scale as well as industrial application. In this work, a PtPdCoNiCu/TiO 2 high-entropy alloy (HEA) catalyst is developed by the colloidal impregnation method, in which the HEA colloids are synthesized by lithium naphthalenide-driven reduction at mild conditions according to the redox potential of the various metals. The PtPdCoNiCu/TiO 2 catalyst exhibits highly efficient in the hydrogenation of MA with 91 % selectivity to GBL at full conversion of MA under the weighted hourly space velocity of 1.14 h −1 , 3 MPa H 2 , and 260 °C. Due to the present of oxygen vacancy in the TiO 2 support and the hydrogen spillover, the PtPdCoNiCu/TiO 2 HEA catalyst presents a low apparent activation energy (75 kJ mol −1 ), boosting the hydrogenolysis of C=O bonds for generating of GBL. The cocktail effect is presented in the PtPdCoNiCu/TiO 2 catalyst, and its catalytic activity is much better than that of corresponding monometallic and bimetallic catalysts. It realizes the reduction and substitution of precious metal catalysts. In addition, the PtPdCoNiCu/TiO 2 catalyst with sintering resistance and acid resistance shows excellent long-term stability within 132 h. This work is of great significance for understanding HEA catalysis at the atomic level and provides the possibility for developing low-cost and efficient precious metal industrial catalysts.
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
JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Ying Wei,Xin Guan,Sihan Feng,Qingguo Zhang,Dawei Fang,Xinyuan Zhang
Two functionalized ionic liquids , 1-cyanopropyl-3-methylimidazolium bistrifluoromethanesulfonimide ([C 3 CNmim][TFSI]) and 1-cyanopropyl-3-methylimidazolium trifluoromethanesulfonate ([C 3 CNmim][OTF]) were blended with γ-butyrolactone (GBL) under the full concentration range (molar fraction from 0 to 1) to form mixture systems, respectively. The densities and conductivities of pure ILs and their mixture systems were measured in the temperature range 288.15–343.15 K under normal pressure. The Vogel–Fulcher–Tammann (VFT) equation is employed to investigate the temperature dependence of conductivity. The volumetric properties of the mixture systems, excess molar volumes ( V E ) and apparent molar volumes ( V ϕ ), were calculated from the density data. The Redlich–Kister (R–K) polynomial equation and Redlich–Rosenfeld–Meyer (RRM) equation were used for the fittings of the V E and V ϕ , respectively. Further, the behaviors of intermolecular interactions in the mixture systems were explained by a combined analysis method composing of the assessment of the volumetric properties changes, the differential scanning calorimetry (DSC) analysis, the infrared (IR) spectrum shifts, and COSMO-RS methodology based on density functional theory (DFT) calculations. The stable optimized structures, H-bonding information, interaction energies, and charge distributions were consequently obtained. It can be found that the addition of the GBL weakened the hydrogen bonding interactions between the IL cations and anions. The [C 3 CNmim][TFSI] + GBL mixture system shows the lowest energy difference and it may give strong ion-solvent interactions when compare to [C 3 CNmim][OTF] mixture system.
研究领域:
物理化学
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材料科学
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 7
·070513
·
IF 3.721
Dandan Zhu,Yuhao Huang,Lei Zhang,Hui Fan,Hongyu Wang
PF6− intercalated graphite compounds have found promising applications in dual-ion batteries. However, the anion storage mechanisms of graphite positive electrode in different organic solvents have not been well understood yet, especially in the mixed solvents. In this report, PF6− storage behavior in graphite electrode in 1 M LiPF6-GBL/EMC solutions is studied by conventional electrochemical tests like galvano-static charge-discharge and cyclic voltammetry at first. Then the combined electrochemical in situ characterizations including both in situ X-ray diffraction and electrochemical quartz crystal balance on graphite electrodes are carried out to trace their changes of crystal structure and mass during the anion storage. It is discovered that with EMC addition in the solutions, EMC rather than GBL will preferentially solvate with PF6− anion as the intercalant species. Moreover, ionic conductivity values and NMR spectra of the solutions were measured to investigate the interactions between ions and solvents inside, and are correlated with the performance of graphite electrode.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 89
·56496-56508
·
IF 3.108
Yong-Ling Wu,Yan-Qing Gao,De-Long Wang,Chen-Quan Zhong,Jun-Tao Feng,Xing Zhang
In view of the great antifungal activities of sesquiterpene lactones and natural product Tulipalin A, 52 derivatives derived from α-methylene-γ-butyrolactone substructures were synthesized to study antifungal activities. In vitro and in vivo antifungal activity results revealed that compounds 2-25, which contain a γ-butyrolactone scaffold and cinnamic aldehyde moiety, have greater potent fungicidal activity than other compounds. The preliminary structure–activity relationships (SARs) demonstrated that compounds with electron-withdrawing groups and small steric hindrance would have more desirable potency. Meanwhile, the quantitative structure–activity relationship (QSAR) model (R2 = 0.947, F = 65.77, and S2 = 0.0028) revealed a convincing correlation of antifungal activity against B. cinerea with molecular structures of title compounds. The present study provided a more detailed insight into the antifungal activity of the α-methylene-γ-butyrolactone substructure, which provided a potential expectation for the exploration of α-alkenyl-γ-butyrolactone structures in agriculture.
研究领域:
植物化学
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药物化学
·
农业科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Chengliang Wang,Yin Zhang,Haitao Li,Feifan Zhang,Jie Wang,Wei Wei,Yongxiang Zhao
Core-shell Ni@C catalysts with a uniform grain size distribution were synthesised via a simple hydrothermal method followed by pyrolysis carbonisation, and their catalytic performance for the liquid-phase hydrogenation of maleic anhydride (MA) was investigated herein. When the pyrolysis temperature was 350 °C, the resulting Ni@C catalyst (Ni@C-350) possessed abundant Ni/NiO heterostructures and a carbon surface layer. Among the analysed catalysts, Ni@C-350 demonstrated the lowest apparent activation energy for the hydrogenation of C C bonds ( Ea = 34.3 KJ/mol) and C O bonds ( Ea = 65.18 KJ/mol), yielding an MA conversion of 100 % and a γ-butyrolactone (GBL) selectivity of 99.89 % under mild reaction conditions (200 °C, 3 MPa hydrogen pressure, and 0.05 g catalyst). Furthermore, the Ni@C-350 catalyst exhibited high stability, with the yield of GBL above 95 % after five consecutive usage cycles. Ni@C-350 significantly outperformed other previously reported catalysts for the liquid-phase hydrogenation of MA.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
Science China-Chemistry
·
2022
·Vol. 65
·期 5
·943-953
·
IF 10.138
Yan Yi-Teng,Wu Gang,Chen Si-Chong,Wang Yu-Zhong
The closed-loop recycling concept of the polymer wastes into building-block chemicals is attractive, but the closed-loop recycling of copolymers enabled by energy-efficient chemical recycling and cost-effective separations is still facing great challenges. Herein, for the first time, a one-pot sequential copolymerization of γ -butyrolactone ( γ -BL) and p -dioxanone (PDO) using an economical ureas/alkoxides catalytic system is conducted to synthesize biodegradable and chemically recyclable poly-( γ -butyrolactone)-block-poly( p -dioxanone) (P γ BL- b -PPDO) diblock copolymers with well-defined and controlled structures. The composition-dependent properties of P γ BL- b -PPDO copolymers, including thermal properties and crystallization behavior, are investigated. The results show that the thermal stability and crystalline ability of P γ BL are enhanced observably by introducing the PPDO block. Significantly, the P γ BL- b -PPDO copolymers can be depolymerized efficiently into the corresponding co-monomers with a yield of over 95% by simply low-temperature pyrolysis under vacuum. Moreover, γ -BL and PDO monomers are selectively separated with an isolated purity of about 99% based on the difference in their physicochemical properties. Subsequently, their repolymerization is realized to obtain the copolymers with nearly identical structures and thermostability, demonstrating the closed-loop recycling of copolymers, i.e. , polymerization-depolymerization-repolymerization. This research provides important guidance for the design of novel sustainable polymers towards more efficient chemical recycling, separation and regeneration.
研究领域:
材料科学
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环境科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2016
·Vol. 6
·期 7
·100
·
IF 2.964
Chi Zhang,Wenrong Cao,Hongye Cheng,Lifang Chen,Zhiwen Qi
The size of metal particles is an important factor to determine the performance of the supported metal catalysts. In this work, we report subnanometer Pd clusters supported on zirconia by the microwave-assisted hydrothermal method. The presence of subnanometer Pd clusters on the zirconia surface was confirmed by two-dimensional Gaussian-function fits of the aberration-corrected high-angle annual dark-field images. These subnanometer Pd catalysts exhibit high catalytic performance for the hydrogenation of biomass-derived succinic acid to γ-butyrolactone in water and avoid the formation of overhydrogenated products, such as 1,4-butanediol and tetrahydrofuran. The catalyst with an ultra-low Pd loading of 0.2 wt. % demonstrated high selectivity (95%) for γ-butyrolactone using water as a solvent at 473 K and 10 MPa. Moreover, it can be reused at least six times without the loss of catalytic activity, illustrating high performance of the small Pd clusters.Keywords:succinic acid hydrogenation;aqueous phase;subnanometer;Pd catalyst
研究领域:
催化化学
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生物质能转化
·
材料科学
✓ 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）