INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Li Cui,Yimin Wang,Zhen Yuan,Xiaoli Zhang,Yuewen Chen,Xiya Zhang,Yihu Ke,Zhile Xiong,Hai Liu
Oxidizing glycerol (the primary by-product of biodiesel production) into 1,3-dihydroxyacetone (DHA) can significantly boost the economic feasibility of the biodiesel industry, but the catalyst deactivation remains a significant challenge. Herein, we present a novel approach that achieves a breakthrough in the conversion of glycerol to DHA through the integration of porous zeolite platform (bio-ZSM-5), derived from corn straw templates, with the traditional Au/CuO catalyst via mechanical milling. Under alkali-free conditions, the synthesized Au/CuO@bio-ZSM-5 catalyst exhibits remarkable glycerol conversion rate of 97.3% and DHA selectivity of 92.2%. Notably, the catalyst retains its efficacy with a glycerol conversion of 89.7% and DHA selectivity of 90.3% even after three regeneration cycles, surpassing all previously documented catalysts for this specific reaction. Serial characterizations and density-functional theory (DFT) calculations reveal that the incorporation of bio-ZSM-5 can modify the electronic structure of surface Au, reduce the adsorption energy of glycerol, and elevate the reduction temperature. This work is expected to provide an effective perspective for the design of catalysts with high cyclic stability.
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ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Li Cui,Ren Gao,Qiaowei Zhang,Kun Jiang,Hongyan He,Wei-Lu Ding,Fangqin Cheng
Crown ethers (CEs) are promising materials for lithium isotope (6Li and 7Li) separation for their unique cavity structure and size effect, but the low partitioning of Li+ makes the practical implementation not applicable. The loss of CE molecules is also a critical problem. In this work, benzo-15-crown-5 functionalized imidazolium ionic liquids with different alkyl chain lengths ([Cn(B15C5)mim][NTf2], n = 6, 8, 10) are synthesized. The association constants of [Cn(B15C5)mim][NTf2] and Li+, Li+ partition, and the separation factor of 6Li and 7Li using [Cn(B15C5)mim][NTf2] were investigated. Compared with the B15C5 monomer, the covalent bonding of B15C5 onto the cation of imidazolium ILs contributes to the dramatic increase of binding ability toward Li+. The association constants of [Cn(B15C5)mim][NTf2] with Li+ increase with the elevation of the alkyl chain length due to the flexibility changes. However, [C8(B15C5)mim][NTf2] delivers the most outstanding partition coefficient of Li+ up to 7.59 with a separation factor of 1.033 (273 K), exceeding those reported for CE-based materials. The increased hydrophobicity of [Cn(B15C5)mim][NTf2] enables sustainable and robust use in the separation process. Both molecular dynamics simulations and interfacial tension experiments confirm that [C8(B15C5)mim][NTf2] exhibits the best affinity to the interfaces of dichloroethane/water. The coordination environment of Li+ can be tuned by regulating the length of the alkyl chains, resulting in different isotopic effects. This study offers a promising system for the effective and sustainable separation of 6Li and 7Li.
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ANALYST
·
2024
·Vol. 149
·期 4
·1271-1279
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IF 3.6
Aiwen Su,Dan Luo,Shixuan Li,Yanli Zhang,Hongbin Wang,Lijuan Yang,Wenrong Yang,Pengfei Pang
T4 polynucleotide kinase helps with DNA recombination and repair. In this study, an electrochemical biosensor was developed for a T4 polynucleotide kinase activity assay and inhibitor screening based on phosphate pillar[5]arene and multi-walled carbon nanotube nanocomposites. The water-soluble pillar[5]arene was employed as the host to complex thionine guest molecules. The substrate DNA with a 5′-hydroxyl group initially self-assembled on the gold electrode surface through chemical adsorption of the thiol group, which was phosphorylated in the presence of T4 polynucleotide kinase. Titanium dioxide nanoparticles served as a bridge to link phosphorylated DNA and phosphate pillar[5]arene and multi-walled carbon nanotube composite due to strong phosphate-Ti4+-phosphate chemistry. Through supramolecular host–guest recognition, thionine molecules were able to penetrate the pillar[5]arene cavity, resulting in an enhanced electrochemical response signal. The electrochemical signal is proportional to the T4 polynucleotide kinase concentration in the range of 10−5 to 15 U mL−1 with a detection limit of 5 × 10−6 U mL−1. It was also effective in measuring HeLa cell lysate-related T4 polynucleotide kinase activity and inhibitor screening. The proposed method offers a unique sensing platform for kinase activity measurement, holding great potential in nucleotide kinase-target drug development, clinical diagnostics, and inhibitor screening.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Mingfu Li,Liyuan Huai,Yingchuan Zhang,Hongli Ma,Pingjun Zhang,Feixiang Xu,Jian Zhang,Liqun Jiang
The green synthesis of 5-hydroxymethylfurfural (HMF) from biomass feedstocks is a crucial step for the development of sustainable fuels, resins and plastics. Here, a novel binary catalytic system was developed with metal–organic frameworks (MOFs) and deep eutectic solvents (DESs), which synergically exhibited a superior fructose dehydration efficiency with a HMF yield of 98.5% within 40 min. The replacement from terephthalic acid to 2,5-furandicarboxylic acid as the organic ligand in MOFs catalysts altered the coordination microenvironment of metal nodes, resulting in remarkably enhanced fructose conversion rates. The formation of hierarchical porous structures and moderated Brønsted acid sites in sulfonated MOFs further promoted the HMF production. Notably, HMF could be readily separated from the MOFs-DESs system and the MOF catalyst maintained stable performance after six recycles. Theoretical calculations clarified a positive correlation between the hydrogen bond interaction (between fructose and DESs components) energy and reaction efficiency. This study provided a new strategy to couple hierarchical solid acid catalysts with functional solvents binary towards effective and sustainable upgrading of biomass-derived molecules.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lingwu Meng,Maosheng Lin,Qirui Guo,Longzhao Zhang,Xiangyu Huang,Shule Zhang,Weihua Ma
Stabilizing metal species at the atomic level and tuning their catalytic properties is a significant challenge. Herein, an N-doped Fe x O y -N-ZSM-5 catalyst with layered and chain-like graphene structures is reported. The catalyst can selectively catalyze the oxidation of triethylamine (TEA) with an efficiency of 99.7 % at 240 °C, and maintain an N 2 yield of 97.6 % over the reaction temperature range of 240–360 °C. The results indicate that the layered graphene in the catalyst provide anchor sites for active Fe, while the abundant chain-like graphene act as connectors between ZSM-5 and the layered graphene, offering ample opportunities for TEA and its intermediates to contact the catalyst surface. This increases the number of active sites on the catalyst, thereby enhancing the catalytic performance of Fe x O y -N-ZSM-5. Notably, due to the interaction between FeO x and FeN x species, Fe x O y -N-ZSM-5 exhibits excellent thermal stability and water resistance, demonstrating promising potential for practical.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
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IF 2.843
Changsheng Zhang,Qinming Wu,Chi Lei,Shuxiang Pan,Chaoqun Bian,Liang Wang,Xiangju Meng,Feng-Shou Xiao
Large crystalline particles of ZSM-5 zeolites (S-ZSM-5) have been successfully synthesized by adjusting crystallization time and Si/Al ratios in the starting solid mixtures in the absence of water solvent. Catalytic tests in the methanol-to-olefins (MTO) reaction show that these S-ZSM-5 zeolites obtained from the solvent-free route exhibit superior catalytic properties including excellent propylene selectivity and extraordinarily long life in the MTO reaction. Particularly, when the crystallization time is 30 h and the Si/Al ratio in the starting solid mixture is adjusted at 150 under the solvent-free conditions, the S-ZSM-5-30h-150 catalyst with the large particle sizes (10–20 μm) gives propylene selectivity as high as 50.0% and catalyst life as long as 9 h, which are much better than those (propylene selectivity at 38.9% and catalyst life of 3 h) of the conventional ZSM-5 zeolite with smaller crystals (ca. 5 μm) synthesized from the hydrothermal route. High-resolution TEM images of these S-ZSM-5 zeolites demonstrate that there is mesoporosity in the samples. More interestingly, these mesopore size distributions could be adjusted by the crystallization time during the solvent-free synthesis. Obviously, the presence of mesoporosity is very favorable for the mass transfer, and an appropriate Si/Al ratio in the zeolite framework could offer suitable acidic density for the catalytic conversion, which should be responsible for the superior catalytic properties in the MTO over the S-ZSM-5-30h-150 catalyst. The features of mesoporosity in the S-ZSM-5 crystals and sustainability for the solvent-free synthesis could be potentially important for wide applications of these S-ZSM-5 zeolites in the future.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2025
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IF 6.2
Jihang Zhang,Xiao Zhang,Jinming Zhang,Jinglan Wu,Pengpeng Yang,Chenglun Tang,Fengxia Zou,Hanjie Ying,Wei Zhuang
Interfacial modulation of protein microenvironments plays a pivotal role in enhancing enzyme immobilization and catalysis. In this study, we proposed a polyethylenimine (PEI)-assisted strategy that combines electrostatic and affinity interactions to improve the performance of Cytidine 5′-Monophosphate (CMP) conversion by uridine-cytidine kinase (UCK). The PEI-modified interface creates an optimal local microenvironment that maintains a balanced charge distribution, stabilizes UCK’s conformation, and prevents denaturation. Electrostatic interactions promote product adsorption, enhance diffusion, and reduce substrate accumulation, boosting reaction efficiency. The kinetic assays revealed an increase in the maximum reaction rate from 16.8 to 113.2 μM·min–1 with a remarkable increase in substrate affinity and enzyme activity. The relative enzyme activity at the optimal substrate concentration increased from 70.4 to 106.9%, and by 113.3% under conditions of substrate inhibition. This study provides theoretical and technical support for the efficient production of CMP with promising applications in food, feed, and medical fields.
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PubMed
高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
·
2024
·
IF 6
Tianyue Xu,Ke Wang,Junjie Zhang,Yongzhi Cheng,Jiale Wei,Rui Duan
6S-5-methyltetrahydrofolate calcium salt crystal form C (MTHF-CAC) is a stable form of active folate. Compared with folic acid, MTHF-CAC is unaffected by the polymorphism of genes for folate-metabolizing enzymes and can be directly absorbed by the human body. In this study, MTHF-CAC was characterized by XRD, FTIR, DSC, and TGA. The effects of temperature, light, pH, and freeze–thaw cycles on the stability of MTHF-CAC solution were studied. The protective effects of ascorbic acid (AA) and cysteine (Cys) on MTHF-CAC were investigated by HPLC. The retention rate of MTHF-CAC solution was 82.6% after 6 days of storage at 4 °C but only 0.8% after heating at 75 °C for 330 min. Under UHT conditions, AA and Cys exerted protective effects on MTHF-CAC. 120 μg/mL of AA and Cys increased the retention of MTHF-CAC by 89.9% and 85.3%, respectively. The protective effect of AA was better than that of Cys. The research on the characterization and stability of MTHF-CAC provided the basic information for its application in the food industry.
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
·
2024
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IF 3.3
Lu Wang,Mingchun Wen,Yu Zhou,Liang Zhang
BACKGROUND Roasting is an essential step in making roasted teas, and its role in producing flavors has been widely studied. However, the variation of potential hazardous compounds during the tea roasting process is still vague. The present study established an effective method based on liquid chromatography-triple quadrupole-tandem mass spectrometry to simultaneously determine the variation of acrylamide (AA), 5-hydroxymethylfurfural (5-HMF), and free amino acids during the tea roasting process. Meanwhile, the effects of several tea polyphenols on the formation of AA and 5-HMF were investigated by a wet-to-dry thermal model reaction. RESULTS Medium-temperature roasted teas had the highest levels of AA and 5-HMF, with ranges of 0.13–0.15 μg g −1 and 68.72–123.98 μg g −1 , respectively. Quantitative results showed that the levels of monosaccharides and amino acids decreased during roasting, which might contribute to the formation of 5-HMF and AA. Meanwhile, the decrease of epigallocatechin gallate (EGCG), epigallocatechin (EGC), and epicatechin (EC) might be related to their inhibitory effects on 5-HMF and AA. Thermal model reaction results showed that EGCG and EC significantly inhibited 5-HMF formation with a decline rate of 33.33% and 72.22%, respectively, mainly by trapping glucose. Gallic acid (GA) also had an inhibitory effect on the formation of AA (decreased by 92.86%) and 5-HMF (44.44%), mainly through impeding the preliminary reaction of asparagine and glucose. CONCLUSION The roasting temperature determined the levels of AA and 5-HMF in teas. Catechins inhibited the formation of 5-HMF and AA mostly through trapping monosaccharides, while the inhibitory effect of GA was achieved by impeding the reaction. © 2024 Society of Chemical Industry.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Jinmiao Tian,Lichao Zhang,Xiaoqin La,Yuxuan An,Xiaxia Fan,Zhuoyu Li
Chemoresistance is one of the difficulties in the treatment of colorectal cancer (CRC), and the enhanced stemness of tumor cells is the underlying contributing factor. Leucine-rich repeat-containing G-protein-coupled receptor 5 (LGR5) is a classical marker of CRC stem cells and can be an important potential target for CRC chemotherapy. Quinoa, a protein-rich plant, offers potential as a source of high-quality active peptides. Novelly, the study obtained quinoa protein hydrolysate (QPH) from whole quinoa grains by simulated digestion. In vivo experiments revealed that the tumor volume in the 5-FU+QPH group decreased from 145.90 ± 13.35 to 94.49 ± 13.05 mm3 in the 5-FU group, suggesting that QPH enhances the chemosensitivity of CRC. Further, the most effective peptide QPH-FR from 631 peptides in QPH was screened by activity prediction, molecular docking, and experimental validation. Mechanistically, QPH-FR competitively suppressed the formation of the LGR5/RSPO1 complex by binding to LGR5, causing RNF43/ZNRF3 to ubiquitinate the FZD receptor, thereby suppressing the Wnt/β-catenin signaling pathway and exerting stemness inhibition. In summary, the study proposes that a novel peptide QPH-FR from quinoa elucidates the mechanism by which QPH-FR targets LGR5 to enhance chemosensitivity, providing theoretical support for the development of chemotherapeutic adjuvant drugs based on plant peptides.
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高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2025
·
IF 2.1
Ruojing Song,Yuxi Sun
A hydrazone compound 4-hydroxy-N’-(2-hydroxy-5-methylbenzylidene)benzohydrazide (HL) was prepared from the condensation reaction of 5-methylsalicylaldehyde with 4-hydroxybenzohydrazide. The compound was characterized by IR, UV-Vis, 1H NMR, and 13C NMR spectra. Reaction of HL with copper nitrate and copper chloride, respectively, afforded two new copper(II) complexes, [Cu2L2(CH3OH)2]·2NO3 (1) and [CuL(DMF)]·Cl (2). The complexes were characterized by IR and UV-Vis spectra. Structures of HL and the complexes were confirmed by single-crystal X-ray determination. The powder X-ray diffraction was performed to verify the purity of the bulk samples of the complexes. The hydrazone compound coordinates to the Cu atoms through phenolate oxygen, imino nitrogen, and carbonyl oxygen. The Cu atoms in complex 1 are in square pyramidal coordination, while that in complex 2 is in square planar coordination. The antibacterial study using the free hydrazone compound and the two copper complexes against both Gram-positive and Gram-negative bacteria are performed, the two complexes showed antibacterial activity against both Gram-positive and Gram-negative bacteria, whereas the free ligand shows no activity.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xinluona Su,Qihang Gong,Peikai Luo,Jian Li,Jingrong Li,Tingting Xiao,Haiyang Cheng,Fengyu Zhao
The selective hydrogenation of 5-hydroxymethylfurfural (HMF) is crucial for sustainable energy and chemical production. In this study, Ni-based catalysts with Ni nanoparticles supported on Al 2 O 3 , ZSM-5 and SiO 2 were investigated for the selective conversion of HMF. Notably, by precisely tuning the surface Ni-acid bifunctional sites, high yields (>88.9 %) of various products such as 2,5-bis(hydroxymethyl)furan, 2,5-bis(hydroxymethyl)tetrahydrofuran, 2,5-dimethylfuran and 2,5-dimethyltetrahydrofuran were achieved, respectively. Comprehensive catalyst characterization revealed that the surface Ni active sites and Brønsted acid sites along with their synergistic interaction play a crucial role in selectively activating C O and C C bonds. Metallic Ni species was identified as the primary active site for hydrogenation, and the Ni terrace sites were responsible for C C bonds activation in furan rings; while the Brønsted acid sites facilitated C O bonds cleavage. The kinetic experiments and H 2 temperature programmed desorption results suggest that increasing Brønsted acid sites enhanced the migration of H* migration, thereby accelerating C O bond cleavage and improving hydrodeoxygenation efficiency. This work presents a simple and effective strategic for the targeted synthesis of high-value chemicals from HMF, offering valuable insights for green synthesis and catalytic study.
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