ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Chenguang Wang,Yong Liu,Zhibing Cui,Xiaohu Yu,Xinghua Zhang,Yuping Li,Qi Zhang,Lungang Chen,Longlong Ma
A facile approach was developed to directly synthesize carbon-supported metal nanoparticles with pomelo peel as the carbon source and metal nitrate solution as the metal source. Fe/C, Co/C, Ni/C, and Cu/C catalysts were prepared after calcination in N2 without further reduction. The metal nanoparticles and formation mechanism were investigated by multiple techniques such as XRD, HRTEM, XPS, FTIR spectra, SEM, and TG-MS thermal analysis. In the case of furfural hydrogenation, Cu/C catalyst exhibited the best activity and exclusive selectivity to produce furfuryl alcohol with complete conversion, and excellent selectivity can be maintained at a higher temperature of 240 °C. The particle size of Cu nanoparticles can be tuned by the calcination temperature and metal loading for improving catalytic activity. The excellent performance of Cu nanoparticles was also studied by density functional theory calculation, agreeing well with the experiments.
研究领域:
催化
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材料科学
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绿色化学
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纳米技术
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可再生能源
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Yuewen Shao,Kai Sun,Mengjiao Fan,Guoming Gao,Junzhe Wang,Lijun Zhang,Shu Zhang,Xun Hu
Copper-based catalysts are active for hydrogenation, while they are prone to sintering in hydrothermal conditions. In this study, alloying Cu with Ni and Zn was adopted to suppress sintering of copper species in the catalyzed conversion of furfural to cyclopentanone (CPO) and cyclopentanol (CPL) in the aqueous phase. The results indicated that Zn acted as a “glue” for aiding the formation of CuZn or CuNiZn alloy. The formation of the ternary CuNiZn alloy in CuNiZn/Al2O3 catalyst created the developed porous structure, induced the formation of abundant Lewis acidic sites and Brønsted acidic sites, and enhanced the dispersion and the total surface area of Cu species. These together rendered CuNiZn/Al2O3 with superior activity to monometallic or bimetallic Cu-based catalysts for the production of CPO and CPL (sum yield of 86% over Cu1.0Ni1.0Zn1.0/Al2O3), which was attributed to the synergy between CuNiZn alloy and Brønsted acidic sites. Alloying Ni with Cu and Zn weakened the adsorption of the C═C bond in the furan ring of furfural, while enhancing the activation of C═O and C–O–C bonds in furfural, avoiding the deep hydrogenation of the furan ring, facilitating the rearrangement of furfuryl alcohol to CPO, and improving the turnover frequency for the production of CPO from furfural remarkably (1011.3 h–1 over Cu1.0Ni1.0Zn1.0/Al2O3 vs 23.9 h–1 over Cu1.0/Al2O3). The formation of ternary CuNiZn alloy could not only suppress the sintering of metallic Cu species during the reduction in hydrogen but also effectively prevent the aggregation of Cu species in the aqueous phase, enhancing the catalytic stability under hydrothermal conditions.
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DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
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2020
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IF 2.888
Midong Shi,Wei Zeng,Shixian Song,Meiting Zhou,Wei Wang
Liquid-liquid equilibrium (LLE) data for {n-heptane + p-xylene (PX) + furfural/dimethyl sulfoxide (DMSO)} ternary systems were measured at 303.15 K and 323.15 K and atmospheric pressure. Extraction performance of furfural and DMSO were evaluated using distribution coefficient (D) and selectivity (S) according to the measured tie-line data. And the results showed that DMSO had better extraction performance than furfural for separation of n-heptane and PX. Both UNIQUAC and NRTL models were used to correlate the experimental LLE data, and relevant interaction parameters were obtained. Consistency between the measured LLE data and the calculated by these two models was well evaluated by RMSD and maximum absolute deviation. Moreover, reliability of binary interaction parameters was confirmed by topological analysis related to the Gibbs tangent plane test.
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高影响因子
JOURNAL OF CATALYSIS
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2018
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IF 6.759
Juan Du,Jiaren Zhang,Yong Sun,Wenlong Jia,Zhihao Si,He Gao,Xing Tang,Xianhai Zeng,Tingzhou Lei,Shijie Liu,Lu Lin
Catalytic transfer hydrogenation (CTH) of bio-derived furfural (FF) to furfuryl alcohol (FFA) was performed using the physically mixed CuO-Pd/C as catalyst and formic acid (FA) as hydrogen donor. The evolution investigation of Cu showed the precursor CuO firstly dissolved into Cu 2+ by FA and then formed coordination polymer-copper(II), which uniformly dispersed in reaction solution of 1, 4-dioxane. Subsequently the Cu 2+ was in-situ reduced and Cu-Pd alloys formed simultaneously. The in-situ prepared nano Cu-Pd/C catalyst exhibited the best performance with a complete FF conversion and FFA selectivity of 98.1%. Reaction conditions test suggested that the FFA selectivity was greatly dependent on the Cu content. The underlying mechanism revealed that the Pd in Cu-Pd alloys mainly promoted the FF conversion by enhancing hydrogen adsorption, while the nano Cu for increasing FFA selectivity; the Cu-Pd alloys functioned in synergistic way. Leaching and recycling tests demonstrated an excellent stability of the Cu-Pd/C catalyst.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2016
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IF 5.267
Xing-kang Li,Zhen Fang,Jia Luo,Tong-chao Su
In order to develop a process for the simultaneous production of furfural and easily hydrolyzable cellulose, the degradation of sugar cane bagasse in a single aqueous system and in a 2-methyltetrahydrofuran (MTHF)/aqueous AlCl3 biphasic system was studied. In single aqueous system, the influence of acid species (FeCl3, HCl, and AlCl3) on furfural production and cellulose degradation was investigated at 150 °C. FeCl3 and HCl promoted furfural production from hemicellulose but with severe cellulose degradation. AlCl3 decreased cellulose degradation with considerable furfural yield and high glucan content in solid residues. The role of NaCl in furfural production and cellulose decomposition was also investigated in the single aqueous system using different acids as catalysts. Addition of NaCl significantly promoted furfural yield but also accelerated cellulose decomposition when FeCl3 or HCl was used as catalyst. In the AlCl3-catalyzed system, NaCl had less influence on residue yield and its composition, although NaCl also promoted furfural production. The influence of MTHF on furfural yield, residue composition, and enzymatic hydrolysis of residue was also studied. Under the best conditions (0.45 g of bagasse, 9 mL of MTHF, 9 mL of water, 0.1 M AlCl3, 150 °C, 45 min, and 10 wt % NaCl), 58.6% furfural was obtained while more than 90% of cellulose remained in the residue. The organic phase was separated from the aqueous phase directly by decantation. After reuse of organic phase for 3 cycles, 11.5 g/L furfural was obtained. The catalyst-containing aqueous phase could be reused directly after decantation of the organic phase without loss of activity. The obtained residue was easy to hydrolyze and produced 89.3% glucose yield after 96-h enzymatic hydrolysis at low cellulase loading (30 FPU of cellulase/g glucan).
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
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IF 5.6
Haowen Cui,Xu Zhang,Haian Xia
Currently, the conversion of lignocellulosic biomass into furfural using deep eutectic solvents (DES) as the solvent and catalyst has many shortcomings including low furfural yields and inefficient resource utilization. To address these issues, a novel effective DES-methyl isobutyl ketone (DES-MIBK) reaction system was designed and used to catalyze the transformation of wheat straw to furfural and separate/recover cellulose and lignin in this work. The results showed that the DES-MIBK system could significantly improve furfural yield of up to 76.2 % at a mild condition (at 100 °C for 60 min). Furthermore, cellulose and lignin were fractionated and recovered from the reaction residues and the lignin yield reached 68.7 %. Moreover, the recovered cellulose exhibits high crystallinity (CrI=67.7 %). and the obtained lignin also has good uniformity with a small polydispersity index (PDI=2.36), and the results of FT-IR and 2 D NMR indicated that the obtained lignin retains its fundamental structure. This research highlights that the innovative DES-MIBK system has a high-efficient in the production of furfural and the recovery of lignin and cellulose, which could provide a novel strategy for the high-value and sustainable application of lignocellulose biomass.
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高影响因子
Molecular Catalysis
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2022
·
IF 5.089
Peng Zhang,Mingwei Ma,Pan Hou,Jingjie Cao,Qi Guo,Huijuan Yue,Ge Tian,Shouhua Feng
A series of ultrathin metal intercalated montmorillonite (Mont) nanosheet materials were prepared and characterized for the one-pot cascade conversion of furfural (FAL) to obtain γ-valerolactone (γ-GVL). The coordination of the intercalated metal ions and the hydroxyl groups between the montmorillonite layers leads to an increase in the specific surface area and pore volume of the material, which coupled with the acidity of the metal ions themselves improves the catalytic performance of the material. Thus Zr-Mont-0.1 exhibited optimal catalytic performance with 100% conversion of FAL and 50.4% yield of GVL under mild conditions, and more importantly, the catalyst maintained its good catalytic performance after the fourth use. Meanwhile the number of Lewis and Brønsted acid sites in the Zr-Mont catalyst can be varied by adjusting the zirconium ion concentration. The proposed reaction mechanism provides initial insights into the role of metal-functionalized montmorillonite in catalyzing the reaction. In addition, the ten-fold magnification reaction confirmed the potential industrial application of the catalyst.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Jie Yang,Liyuan Huai,Jiang Gan,Hualei Hu,Shenghu Zhou,Jian Zhang
The 5,5′(oxy-bis(methylene))bis-2-furfural (OBMF) formation from the 5-hydroxymethylfurfural (HMF) self-etherification over zeolites is an important reaction for the synthesis of value-added chemicals from biomass resources. However, there is still a lack of knowledge about the reaction mechanism and the roles of different acid sites that impedes the exploitation of zeolite catalysts for efficient OBMF production. In the present study, the ZSM-5 (HPZ) catalysts of four hierarchically micromesopores were successfully synthesized in different Si/Al ratios by adjusting the amount of Al in the solvent evaporation with the assistance of a dry gel conversion method. The kinetics of OBMF formation from HMF self-etherification was investigated. The apparent activation energy and the conversion reaction order were calculated to be 104.6 kJ/mol and 0.65, respectively. The intrinsic activity comparison of four catalysts and density functional theory (DFT) calculations showed that HMF adsorption and etherification benefit from Brønsted-acid sites. Besides, the DFT results suggested that the etherification proceeds via a concerted step, instead of the sequential pathways, thus leading to the high selectivity of OBMF on hierarchically micromesoporous ZSM-5 (HPZ) catalysts.
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DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 30
·16919-16928
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IF 3.049
Wenzhi Li,Mingxue Su,Tao Yang,Tingwei Zhang,Qiaozhi Ma,Song Li,Qifu Huang
Liquid fuel intermediates can be produced via aldol condensation reactions through furan aldehydes and ketones driven from biomass. It was found that cerous phosphate (CP) with two different crystal structures (hexagonal and monoclinic structure), which was tailored by different hydrothermal temperature (120 °C for the hexagonal structure and 180 °C for the monoclinic structure) and calcination temperature (900 °C for the monoclinic structure) as a solid acid catalyst, exhibit high catalytic performance in aldol condensation between furfural and acetone. The CP with hexagonal structure gave 89.1% conversion of furfural with 42% yield of 4-(2-furyl)-3-buten-2-one (FAc) and 17.5% of yield of 1,5-di-2-furanyl-1,4-pentadien-3-one (F2Ac), much higher than CP with monoclinic structure. However, both furfural conversion and aldol product yield increased from 82.3% to 96% and from 50.5% to 68.4%, respectively, for CP with the monoclinic structure after calcination owing to the higher amount of acid of catalyst after calcination but decreased continuously for CP with hexagonal structure after calcination because of its rapidly reduced BET surface area and total pore volume. The results indicated that calcination affects significantly the physical–chemical properties of CP catalysts, which influence subsequently the catalytic performance in the aldol condensation reaction. Recycling experiments showed that the catalytic performance after five number runs for CP with monoclinic structure after calcination was acceptable but was not ideal for CP with hexagonal structure owing to its poor hydrothermal stability.
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DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2019
·Vol. 9
·期 23
·6659-6668
·
IF 5.726
Jie Yang,Haochen Yu,Yanbing Wang,Fuyuan Qi,Haodong Liu,Lan-Lan Lou,Kai Yu,Wuzong Zhou,Shuangxi Liu
Four types of Ca–Mn oxides, CaMnO3, CaMn2O4, CaMn3O6 and Ca2Mn3O8, have been prepared and used as supports for Pd nanoparticles. The oxygen activation capacity of these oxides and the catalytic activity of the oxide supported Pd nanocatalysts have been investigated using the aerobic oxidation of 5-hydroxymethyl-2-furfural as a model reaction. It is found that the local coordination environment of lattice oxygen sites plays a crucial role on their redox properties and charge transfer ability from Pd nanoparticles to the support. In particular, the Ca–Mn oxide with lower oxygen coordination number, weaker metal–oxygen bonds and tunnel crystal structure, e.g. CaMn2O4, exhibits promoted oxygen activation capacity, and stronger electron transfer ability. Consequently, Pd/CaMn2O4 exhibits the highest catalytic activity among these catalysts, providing a promising yield of 2,5-furandicarboxylic acid. This work may shed light on future investigations on the design of local structure of active oxygen sites in oxides or oxide supported catalysts for redox reactions.
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高影响因子
FUEL
·
2024
·
IF 6.7
Wei Xue,Mingwei Ma,Pan Hou,Peng Zhang,Wenzheng Liu,Yongchen Liu,Huijuan Yue,Xiaofeng Wang,Ge Tian,Shouhua Feng
The one-pot tandem conversion of furfural (FUR) to γ-valerolactone (GVL) is desirable due to the high value of GVL and the efficiency of the synthesis process. While MOF-808 presented a good catalytic potential among Zr-MOFs, it lacked the necessary Brønsted acidity for the tandem conversion. In this study, Zr-based metal–organic framework (MOF-808) was modified with acids of different strengths (triflic acid, sulfuric acid, sulfamic acid, and trifluoroacetic acid) using a two-step post-synthesis impregnation method. EPR results revealed the appearance of coordinatively unsaturated sites of Zr (Zr-CUS) in the first step of HCl-treated Zr-808-HCl and their disappearance in the subsequent acid-modified catalysts, clarifying the impregnation process. These modified frameworks (Zr-808-TF, Zr-808-S, Zr-808-SN, and Zr-808-CF) were employed as catalysts for the tandem conversion of FUR to GVL. Zr 3d XPS and solid-state 31 P MAS NMR spectra of TMPO adsorbed on the catalysts proved that Zr-808-TF outperformed other catalysts in terms of both Brønsted/Lewis acid strength and ratio. With such catalytic active sites, Zr-808-TF exhibited superior catalytic activity, achieving 83% GVL yield over an 8-hour reaction period. The four acid-modified catalysts not only differed in Lewis/Brønsted acid sites, but also exhibited different catalytic performances in the tandem conversion. The in-depth insight into the relationship between the modified functional groups and the acid-base sites provides a new avenue to optimize the acid-base sites and expands the application of MOFs in cascade catalysis.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 31
·14958-14966
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IF 3.925
Liang Shi,Kun Lu,Xiao Kong,Licheng Li,Xiaoli Gu,Junmeng Cai,Xingguang Zhang
Supported Pt catalysts play an important role in selective hydrogenation reactions for upgrading bio-derived chemicals, and they are traditionally prepared by methods such as deposition–precipitation (DP), wet impregnation (WI) and chemical reduction (CR) using NaBH4 and H2 under thermal conditions. This study developed a new reduction method to produce supported Pt NPs on nanofibers, in which Ti3AlC2 (a typical MAX phase) and chloroplatinic acid (H2PtCl6) were employed as raw materials, using as-produced H2 as a reducing agent under hydrothermal synthetic conditions. In the selective hydrogenation of furfural to furfuryl alcohol, the newly-developed catalyst of Pt2.0/Ti3AlxC2Ty exhibited high furfural (FUR) conversion (86.3%) and excellent furfuryl alcohol (FA) selectivity (98.1%) under optimized reaction conditions of 600 rpm, 100 °C, 3 h, and 1 MPa H2 in aqueous media. Moreover, these fibrous catalysts exhibited strong reusability and recyclability for five runs without loss of activity and selectivity.
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高影响因子
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