CHEMISTRY & BIODIVERSITY
·
2024
·Vol. 21
·期 6
·e202400150
·
IF 2.3
Long Ren,Yupu Xu,Wenjun Chen,Changsen Zhang
Experiments were conducted in this study on the co-hydropyrolysis of three components of biomass (cellulose, hemicellulose, and lignin) and HDPE by using SR-Pd/Trap-HZ-5 as catalyst. To control the variable, we use the same experiment conditions in co-hydropyrolysis: Si/Al ratio of 50, Pd load 1 %, catalyst to reactant ratio of 1 : 10, 1 MPa, 400 °C, reaction time 1 h. Use XRD, TEM, BET, and NH 3 -TPD to confirm catalyst successful synthesis; use pine sawdust (PW) co-hydropyrolysis with HDPE to analyse catalytic activity; and use GC/MS to characterize the chemical composition of the bio-oil from the co-hydropyrolysis of biomass components and HDPE. The results show that cellulose has a significant synergistic effect with aromatic hydrocarbon production, whose selectivity was 93.3 %; hemicellulose has a synergistic effect; aromatic selectivity can reach 75.1 %; and a negative synergistic effect between lignin and HDPE was shown as the selectivity of aromatic hydrocarbons decreased from 62.1 % to 15.6 %. Graphical
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BIOMASS & BIOENERGY
·
2024
·
IF 5.8
Yong Liu,Jirong Long,Zhijiao Huang,Lungang Chen,Chenguang Wang,Xinghua Zhang,Longlong Ma
Direct production of 2,5-dimethylfuran (DMF) from fructose is crucial for developing biomass-derived fuels, yet it presents significant challenges due to the need for multifunctional active sites for dehydration and hydrodeoxygenation. Meanwhile, the disposal of wine lees, a major winemaking by-product, incurs substantial costs. Herein, a hybrid catalyst system of sulfonated wine lees carbon (WLC-SO 3 H) and PtFe/C was introduced, achieving a DMF yield of 66.4 % directly from fructose. WLC-SO 3 H, with enhanced Brønsted acidity, demonstrated high activity in dehydrating fructose to 5-hydroxymethylfurfural (HMF) with a 98.2 % yield. PtFe/C effectively catalyzed the hydrodeoxygenation of HMF to DMF, driven by the strong interaction between Pt and Fe species. This interaction was confirmed through in situ DRIFTS and theoretical calculations, highlighting the system's superior catalytic performance.
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AICHE JOURNAL
·
2024
·
IF 3.5
Yanru Zhu,Zhen Zhang,Yunfei Zou,Jian Zhang,Zhe An,Xin Shu,Hongyan Song,Jing He
Catalytic conversion of biomass-derived 5-(hydroxymethyl)furfural (5-HMF) into carbon-increased hydrocarbons as drop-in energy-rich biofuels has received a great deal of concern for the development of sustainable chemical industry. Here, we demonstrate a one-pot conversion of 5-HMF into C 9 -alkanes on one single catalyst, acidic–basic layered double oxides (Mg(Al)(Zr)O) supported CuCo alloy. The well-defined multifunctional catalytic sites with harmonious combination carry out cascade catalysis, affording C 9 -alkanes (including 30% of more value-added branched-cycloalkanes) in 83% yield. The basic–acidic sites on Mg(Al)(Zr)O show high activity for aldol condensation of 5-HMF and acetone, producing 4-[5-(hydroxymethyl)-2-furanyl]-3-buten-2-one (HAc) in a yield of >99%. The engineered Co–Cu–Co linkages on supported CuCo perform efficient hydrodeoxygenation, affording C 9 -alkanes in a selectivity of 96% from HAc. C 9 -cycloalkanes are generated from the cyclization of the corresponding monohydric alcohol intermediates by the synergy of acidic and CuCo sites in the hydrodeoxygenation reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Minlei Yin,Shiyin Huang,Yuxin Lin,Xuanjie Chen,Zhaoyang Qi,Jie Chen,Ting Qiu
Effective removal of acetaldehyde and propionaldehyde from propylene oxide is important for polyether industry but remains a significant challenge due to their similar molecular sizes and relatively close volatilities. Herein, we studied flexible molecular materials, perethylated pillar[n]arene crystals (n = 5, 6), which can be used to separate acetaldehyde and propionaldehyde in propylene oxide. Through a space size matching effect, perethylated pillar[5]arene demonstrates excellent adsorption selectivity of 95 % and 100 % for aldehydes in ternary mixture and binary mixture of propylene oxide, acetaldehyde and propionaldehyde, respectively. These impressive selective adsorption is achieved based on their differential host–guest interactions. Density functional theory calculations provide a comprehensive explanation of the adsorption process, revealing that the adsorption mechanisms of perethylated pillar[5]arene for acetaldehyde and propionaldehyde primarily involve C-H···O hydrogen bonding and C-H···π interactions. This study also provides a novel method for achieving one-step purification of propylene oxide in industrial applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Mingfu Li,Shuanglan Hu,Yingchuan Zhang,Jiannan Qin,Douyong Min,Chunlin Chen,Pingjun Zhang,Liqun Jiang,Jian Zhang
The green oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a crucial step in the development of sustainable and degradable plastics. Here, a series of MnCO 3 -Mn x Co 3-x O 4 -Ov composite oxides are synthesized by a simple solid-state grinding and carbonization method, exhibiting a 100 % HMF conversion rate and 98.7 % FDCA yield directly using air as the oxygen source. Physicochemical characterizations indicate that the introduced carbon promotes the diffusion of Mn species and reduction of Co 3 + /Co 4+ , resulting in more unsaturated coordination of Co–O and the enhanced formation of oxygen vacancies (O v ). The kinetic analysis suggests that the oxidation of HMF to FDCA can be effectively promoted by regulating the O v content in the catalyst after changing the Mn/Co ratio. Moreover, density functional theory (DFT) calculations demonstrate the crucial role of O v in reducing the adsorption energy of HMF on the catalyst surface and activation of O 2 molecules to replenish lattice oxygens during the completion of the catalytic cycle. This work provides a promising strategy to engineer transition metals as alternatives to noble metal-based catalysts towards catalytic oxidation for the production of biofuels and bioplastics.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Le Xu,Peng Guo,Jie Xu,Boxiong Shen,Zhong Zhao
TiO 2 has been widely studied in photocatalytic VOCs oxidation but its photocatalytic activity is still unsatisfied due to poor visible light absorption, serious charge recombination and weak toluene adsorption . Herein, a composite catalyst (TiO 2 /ZSM-5) was constructed between TiO 2 and hierarchical ZSM-5 by ball milling for photocatalytic toluene oxidation. The optimal composite catalyst exhibited the toluene degradation efficiency of 91.08 %, which was 2.7 and 1.3 times than those of TiO 2 and TiO 2 /commercial ZSM-5. It showed that the strong interaction between TiO 2 and hierarchical ZSM-5 was established via the formation of Ti-O-Si bond, which decreased the band gap from 3.08 to 0.55 eV when compared with TiO 2 and was helpful for the enhanced charge separation. In addition, the mesoporous volume of hierarchical ZSM-5 was regulated by a dual-template method, making the mesoporous volume increased from 0.23 to 0.38 cm −3 g −1 when compared with TiO 2 /commercial ZSM-5, which improved the toluene adsorption capacity from 0.12 to 0.16 cm −3 g −1 . DFT calculation further indicated that the energy barrier of toluene oxidation and ring-opening reaction was reduced in the presence of hierarchical ZSM-5. This work provided a new catalyst design method to improve the photocatalytic activity by the synergy action of TiO 2 and ZSM-5.
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ADVANCED POWDER TECHNOLOGY
·
2024
·
IF 4.2
Han Hao,Tiantian Ren,Cuilu Quan,Wei Guo,Jing Wang
Pharmaceutical cocrystal is an emerging strategy not only to improve physicochemical properties, but also to generate synergistic effects. In this work, a novel cocrystal composed by 5-fluorouracil (5-FU) and sarcosine (SAR) was successfully assembled by wet powder grinding method. The cocrystal was characterized by single crystal X-ray diffraction (SCXRD), powder X-ray diffraction (PXRD), differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR) and Raman spectra. The differences of 1 H NMR spectroscopy between 5-FU/SAR physical mixture (PM) and cocrystal hinted the existence of supramolecular interactions between 5-FU and SAR in solid and solution. Bioavailability of cocrystal was increased than 5-FU. Most importantly, the weak interactions between 5-FU and SAR in cocrystal solution induced the superior cellar inhibition activity on 4T1 and BEL-7402 cells compared than 5-FU and PM. Cocrystal can interfere with the stability of methionine cycle and tetrahydrofolate (FH 4 ) level through the SAR-Gly-Met pathway, enhance the inhibition of thymidylate synthase (TS) compared to 5-FU, thereby interfering with cell cycle and inducing cell apoptosis. The results provided the novel strategy to develop the cocrystal drugs using bioactive amino acids as precursors to enhance the efficacy.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zhen-Qiang Yu,Yao-Xin Xiao,Dong Liang,Che Zhao,Zhen Huang,Gang-Qi Cheng,Rui Shan,Hao-Ran Yuan,Yong Chen
The chemical upgrade of the waste polyester coating on the surface of aluminum cans to value-added products can not only decrease the release of toxic substances, but also improve the quality of aluminum in the recycling process. In this study, different types of zeolite molecular sieve catalysts loaded with Ni, Mo and Co were synthesized, and utilized in the rapid catalytic pyrolysis of polyester coating. Among them, the Ni/ZSM-5 achieved the maximum aromatic compounds yield of 68.43 % at 600 ℃. A series of characterization results demonstrated that the embedding of transition metals (like Ni) could promote the cyclization and aromatization of products through deoxidation and dehydrogenation reactions by changing the pore structure and increasing total acid content (Brønsted and Lewis acids) of the ZSM-5 molecular sieve. Meanwhile, the thermodynamics of polyester coating during catalytic pyrolysis was studied by thermogravimetric method. The average activation energy of Ni/ZSM-5 catalytic pyrolysis of polyester coating is 238.65 kJ/mol. Furthermore, even after being reused for over 5 cycles, the catalyst can still maintain a relatively high yield of aromatic compounds (exceeding 60 %). Finally, the mechanism for aromatic compounds formation from Ni-modified ZSM-5 in-situ catalyzed polyester coating pyrolysis was proposed. This work provided useful ideas for the subsequent treatment of solid wastes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Chenhui Xu,Yang Yang,Chengyang Hui,Pengfei Tang,Genlei Zhang,Jialun Liu,Zhenzhen Yang
Highly efficient synthesis of 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) or fructose has attracted much attention in recent years. Herein, one-dimensional MoO2@a-NCx core–shell nanorods that oxygen vacancy-rich molybdenum dioxide (MoO2) coated with porous amorphous nitrogen-doped carbon layer (a-NC) are synthesized via pyrrole polymerization followed by pyrolysis, using orthorhombic molybdenum trioxide (α-MoO3) nanorods as a precursor. Benefiting from the well-engineered architecture and the strong interfacial interaction between MoO2 and surface carbon, the optimized MoO2@a-NC9 with an a-NC layer thickness of ∼9 nm exhibits considerable catalytic activity and stability in oxidation of HMF/fructose to DFF. Under optimal reaction conditions, MoO2@a-NC9 achieves nearly quantitative DFF yield of 99.1% with complete HMF conversion (100%) in the aerobic oxidation of HMF. A possible reaction mechanism involving a Mo4+/Mo3+ redox cycle is proposed for MoO2@a-NC9-catalyzed oxidation of HMF to DFF, based on experimental and characterization results. Furthermore, MoO2@a-NC9 served as a bifunctional catalyst for direct conversion of fructose to DFF via a “one-pot, two-step” approach, achieving a high DFF yield of 82.5%. Notably, this catalyst exhibits excellent recyclability, maintaining its catalytic performance over at least six reaction cycles without significant activity decay.
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Materials
·
2025
·Vol. 18
·期 16
·3780
·
IF 3.2
Lei Yang,Anbang Duan,Zhanyin Liu,Tingying Wei,Chunzhao Liu
Aiming to address the key challenges of poor enzyme stability, difficult recovery, and difficult synergistic optimization of catalytic efficiency in high-value conversion of biomass, this study utilizes mineralization self-assembly technology to combine laccase with Fe3O4@SiO2-PMIDA-Cu2+composite, constructing magnetic laccase nanoflower (MLac-NFs) materials with a porous structure and superparamagnetism. This synthetic material can efficiently catalyze the selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). The characterization results indicated that MLac-NFs exhibit optimal catalytic activity (63.4 U mg−1) under conditions of pH 6.0 and 40 °C, with significantly enhanced storage stability (retaining 94.26% of activity after 30 days of storage at 4 °C). Apparent kinetic analysis reveals that the substrate affinity and maximum reaction rate of MLac-NFs were increased by 38.3% and 439.6%, respectively. In the laccase–mediator system (LMS), MLac-NFs mediated by 30 mM TEMPO could achieve complete conversion of HMF to FDCA within 24 h. Moreover, due to the introduction of magnetic nanoparticles, the MLac-NFs could be recovered and reused via an external magnetic field, maintaining 53.26% of the initial FDCA yield after six cycles.
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RENEWABLE ENERGY
·
2025
·
IF 9.1
Liqiang Zhang,Ningmin Zhu,Yuxiang Liu,Honglei Shi,Yiya Wang,Ruiqi Liu,Riyi Lin
A two-stage co-pyrolysis approach was developed for the efficient utilization of marine waste plastics and biomass, with a focus on the influence of biomass components. HZSM-5 was modified with Cu via wet impregnation and applied in the catalytic co-pyrolysis of Enteromorpha and polypropylene under varying catalyst-to-feedstock ratios. The Cu/HZSM-5 catalyst was characterized using X-ray diffraction (XRD), N 2 adsorption, and scanning electron microscopy (SEM). The results showed that Cu modification preserved the HZSM-5 framework while increasing pore size, enhancing catalytic cracking efficiency. Thermogravimetric and kinetic analyses revealed that Cu/HZSM-5 lowered the pyrolysis temperature, reduced residues, improved synergy, and decreased activation energy without altering the reaction mechanism. The catalyst significantly reduced oxygenated compounds and enhanced the formation of aromatic hydrocarbons in the oil products, reaching a maximum aromatic content of 90.20 % at a 6:5 catalyst-to-feedstock ratio in the second stage. Under the same conditions, hydrogen production in the gas phase also peaked at 47.91 %. Increased catalyst dosage decreased carbon and hydrogen content in the char while raising oxygen and nitrogen levels, with a higher H/C ratio mitigating char aromatization and densification. A reaction mechanism for Enteromorpha and polypropylene over Cu/HZSM-5 was proposed. This study provides insights into the catalytic co-pyrolysis of marine waste plastics and biomass with complex compositions.
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JOURNAL OF FOOD SCIENCE AND TECHNOLOGY-MYSORE
·
2025
·
IF 3.3
Ma Shutian,Shi Zhuang,Yang Yi,Zhang Jinglin,Zou Hongyu,Diao Enjie,Zhang Liming
Solo-bulb black garlics (SBBG) are novel foods rich in nutritional and functional ingredients. However, certain process contaminants formed during thermal processing of SBBG raise safety concerns. This study investigated the formations of 5-hydroxymethyl-2-furfural (5-HMF) and acrylamide, as well as the browning degree of SBBG during a 12-day aging period. Both 5-HMF and acrylamide contents exhibited exponential increases, with their formations well simulated by pseudo-first-order kinetic models. 5-HMF formation showed a significant positive correlation with fructose content ( p < 0.05), while acrylamide formation was strongly associated with asparagine content ( p < 0.01). Browning degree correlated significantly with acrylamide accumulation and asparagine content ( p < 0.01), but not with 5-HMF ( p > 0.05). These results indicate that fructose and asparagine accumulations play critical roles on 5-HMF and acrylamide formations in SBBG, respectively, and acrylamide accumulation promotes SBBG browning. Notably, acrylamide level in SBBG exceeded those reported in some commonly consumed foods, which is a concern considering the daily consumption of this food.
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