CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jieqiong Wang,Fei Li,Zhengwei Xu,Mingsong Zang,Shengda Liu,Tianhe Li,Jiayun Xu,Hongcheng Sun,Shuangjiang Yu,Junqiu Liu
Bacterial infection is one of the most serious physiological conditions threatening human health. There is an increasing demand for selective antibacterial therapy through noninvasive approaches recently years. Herein, a novel strategy for fabrication of positively charged, monolayered nanosheets (P5PD) bearing perylene diimide derivative (DAPDI) was reported through covalent self-assembly with laterally-brominated pillar[5]arene (LBP5). Mannose derivative (Man-HQA) was further immobilized to P5PD nanosheets (named as mP5PD) through host–guest complexation with LBP5 for improving biocompatibility and recognition with microbes. It was found that the mP5PD nanosheets could be converted to radical anions in the presence of E. coli in terms of their excellent reductive surroundings, which showed excellent photothermal conversion efficiency under the 0.5 W/cm 2 of 808 nm laser irradiation. Moreover, the selective photothermal antibacterial activity could be realized by the different ability of amplifying radical anions for facultative anaerobic E. coli and aerobic B. subtilis . Importantly, the mP5PD nanosheets exhibited excellent biocompatibility to mammalian cells even at high concentration, which held great potential for developing intelligent photothermal nanomaterials in future biomedical fields.
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ADVANCED POWDER TECHNOLOGY
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2024
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IF 4.2
Hu Wen,Yuxin Li,Haitao Yin,Wei Wang,Zhengchao Jin,Shunyu Han,Nanzhe Jiang
The conversion of natural clay to crystalline zeolites has been the subject of considerable interest from both academic and industrial circles. We present an effective strategy for converting kaolin to ZSM-5 zeolite, addressing the issue of reduced mesopore formation in conventional nano-ZSM-5 aggregates due to close-packing. This strategy utilizes kaolin as the sole source of silicon and aluminum, and by decoupling the nucleation and growth of ZSM-5 crystals, loosely stacked nano-H-ZSM-5 aggregates with high crystallinity crystals can be synthesized in a solid-like system by employing a tiny amount of TPAOH (TPAOH/SiO 2 = 0.064). The resulting nano-H-ZSM-5 aggregates exhibited high specific surface area (405.66 m 2 /g), high mesopore volume (0.64 cm 3 /g), and superior catalytic activity. This strategy offers a novel approach to the cost-effective synthesis of nano-H-ZSM-5 aggregates suitable for industrial applications.
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GREEN CHEMISTRY
·
2025
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IF 9.2
Ke Liu,Ling Jiang,Lun Wang,Qunfeng Zhang,Li-Rong Yang,Jianping Wu,Haoran Yu
2,5-furandicarboxylic acid (FDCA) is a potential platform chemical from renewable feedstocks to make various polymers and high-value compounds. Bioconversion of 5-hydroxymethylfurfural (HMF) to FDCA by biocatalysts has the advantages of high selectivity, cost-effectiveness, and eco-friendliness. However, the full oxidation of HMF often requires a combination of two or three enzymes, as the production of FDCA involves three consecutive oxidation steps. In this study, we identified a pyrroloquinoline quinone (PQQ) and lanthanide-dependent alcohol dehydrogenase, PedH, capable of directly converting HMF to FDCA, representing a rare and intriguing discovery. We then engineered the enzyme for improved thermostability and activity against HMF to improve FDCA yield. Using computational design method, the thermostability was first significantly improved, with the 4M variant obtained showing a Tm value increased by 9.6 oC, and a half-life improved by 10.3-fold compared to wild type. With the 4M as the template, potential mutation sites for engineering enzyme activity were identified based on calculation of binding free energy and a deep learning model MutCompute. An automatic high-throughput platform for site-saturation mutagenesis library construction and screening was developed and applied to the identified mutation targets. After five rounds evolution, a variant was obtained that produced FDCA at a yield 474-fold higher than that of 4M. Under optimized reaction conditions, the optimal variant achieved a FDCA yield of 96.4% with 40 mM HMF as the substrate. Molecular dynamics simulations revealed that the mutations expanded the substrate binding pocket and shortened the reaction distances between substrate and cofactors. This study provides a highly efficient evolution approach for PedH, and several variants that are potentially used for high yield production of FDCA in industrial fields.
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Royal Society Open Science
·
2024
·Vol. 11
·期 8
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IF 2.9
Junchi Zheng,Zhifeng Wang,Qiulan Shi,Lipeng Jiang,Cuiping Yang,Yuan Zhang,Jianbo Zhao
Trivalent ruthenium (Ru) can catalyse the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). However, the structure of Ru itself is unstable and is prone to aggregation and oxidation, leading to a decrease in catalytic activity. Therefore, it is necessary to prepare a stable, reliable, Ru-based catalyst. Based on the catalytic properties of trivalent Ru, a stable spinel structure with zinc ferrite was designed and loaded onto different carbon supports to prepare a homogeneous and stable Ru-based catalyst. The structure and physico-chemical properties were characterized through scanning electron microscopy, X-ray diffraction, transmission electron microscopy and other techniques, and the catalyst was applied to the oxidation of HMF for the preparation of FDCA. The results show that the prepared magnetic activated carbon-supported Ru-based catalyst has a concentrated particle size distribution in the range of 5–8 nm, with a loading amount of 3.61 at%. It exhibits strong soft magnetism, which is beneficial for Ru loading. Additionally, it can be reused in the oxidation of HMF to prepare FDCA over 10 cycles, with the product yield remaining essentially unchanged. The catalyst prepared in this study is characterized by recyclability and structural stability, making it promising for practical applications.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuan Bao,Weijia Pu,Yiwei Zhang,Yahui Xiao,Yong Liu
Ni-Co nano-alloys confined by in-situ formed N-doped porous carbon overlayer have been prepared through chelation of metal cations with citric acid and urea followed by carbonization for hydrodeoxygenation of 5-hydroxymethylfurfural (HMF) into 2, 5-dimethylfuran (DMF). The results indicated that the Ni-Co nano-alloys were formed and homogeneously distributed within the N-doped porous carbon overlayer. The electronic effect of the Ni-Co nano-alloys significantly boosted hydrodeoxygenation activity of the Co 2 Ni 1 @NC catalyst and simultaneously inhibited further hydrogenation and opening of furan ring. The N-doped porous carbon overlayer around Ni-Co nano-alloys not only facilitated to disperse and stable Ni-Co nano-alloys through strong metal-support interaction, but also protected the Ni-Co nano-alloys from aggregation. Therefore, the Co 2 Ni 1 @NC catalyst offered superior catalytic performance with the HMF conversion of 100 % and DMF selectivity of 93.0 %. Moreover, the Co 2 Ni 1 @NC catalyst displayed excellent stability without significant activity loss after five recycles due to the spatial confinement of N-doped carbon overlayer.
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ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Shiling Zhao,Kaizhi Wang,Shaoqi Mao,Beibei Yang,Yu Zhao
In the pursuit of high-selective oxidation of 5-hydroxymethylfurfural (HMF) to valuable derivatives such as 5-hydroxymethylfuroic acid (HMFCA), 5-formyl-2-furanoic acid (FFCA), and furan-2,5-dicarboxylic acid (FDCA), we have developed a diethylenetriamine pentaacetic acid (DTPA)-assisted strategy to construct a highly effective photothermal catalyst with maximized Ag–CeO2 interfaces and rich oxygen vacancies. Under optimal reaction conditions, this catalyst achieves remarkable yields of 99% for HMFCA, 99% for FFCA with a turnover frequency (TOF) of 163 h–1, and 98% for FDCA. Combined theoretical calculations and a series of characterization analyses reveal that the superior performance is due to the unique properties of the maximized Ag–CeO2 interfaces and the rich oxygen vacancies, which enhance electron transport and synergistically enhance the catalytic activity of silver clusters. In contrast to other photocatalytic oxidation systems for HMF, this work showcases high selectivity in the oxidation of HMF to HMFCA, FFCA, and FDCA. These findings not only elucidate the mechanisms behind selective oxidation but also offer a promising approach for the directional photosynthesis of high-purity chemicals in related applications.
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Frontiers in Bioscience-Landmark
·
2024
·Vol. 29
·期 9
·325
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IF 3.3
Ziwei Guo,Sixu Bao,Zehui Shi,Xuejiao Li,Peijin Li,Bin Zhong,Ming Zhang,Qiyong Wu
Background: Platelets have the hemostatic function, and their aberrant activation is associated with occlusive thrombus formation. Plasma exosomes are rich in platelets containing ubiquitin-specific peptidase 15 (USP15). Herein, we aim to explore the effect of USP15 on thrombosis, as well as expounding whether USP15 acts as an upstream target of FK506 binding protein 5 (FKBP5) to regulate occlusive thrombus formation. Methods: Washed human platelets were treated with thrombin for measurement of USP15 and FKBP5 expressions. USP15 loss/gain-of-function variant in HEK293 cells was performed by cell transfection, and the interaction between USP15 and FKBP5 was examined using immunoprecipitation and ubiquitination assays. Mice with USP15-knockout platelets (Plt USP15-/-) were modeled, and subjected to calculation of bleeding time, artery thrombosis imaging and clot retraction assay. FKBP5 expression and the inhibitor of nuclear factor kappa B kinase subunit epsilon (IKBKE)/phosphatidylinositol 3-kinase (PI3K)/Rap1 pathway in wild-type and Plt USP15-/- mice-derived platelets were detected using Western blot. The activation of αIIbβ3 in washed platelets was analyzed using flow cytometry. Results: USP15 and FKBP5 expressions were upregulated in platelets after thrombin treatment. Following transfection of USP15 knockdown and USP15 overexpression plasmids into HEK293 cells, FKBP5 protein expression was downregulated by USP15 knockdown while being upregulated by USP15 overexpression. USP15 bound to FKBP5 and protected FKBP5 against ubiquitination. Knockdown of platelet USP15 prolonged bleeding time, inhibited arterial thrombosis and delayed clot retraction in mice. Knockdown of platelet USP15 also decreased protein expressions of FKBP5, IKBKE and Rap1, p-PI3K/PI3K ratio, and activation of αIIbβ3 in mice. Conclusion: USP15 knockdown in platelets affects thrombosis in mice by promoting the instability of FKBP5 to repress the activation of IKBKE/PI3K/Rap1 pathway-mediated αIIbβ3.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Qisong Yi,Lu Lin,Huawei Geng,Shaohua Chen,Yuanchao Shao,Ping He,Zhifeng Liu,Haimei Xu,Tiehong Chen,Yuanshuai Liu,Valentin Valtchev
The hydrothermal stability of zeolites is essential for their potential applications in biomass conversion, especially in processes involving elevated temperatures alongside the use or generation of H 2 O. In this study, we employed F - ions as mineralizers to synthesize hydrothermally stable ZSM-5 zeolites under acidic conditions. The acidic synthesis system promotes zeolites with fewer silanol-terminated lattice defects (ZSM-5(A)) compared to the traditional basic conditions (ZSM-5(B)), endowing materials with substantially higher structural integrity and hydrophobicity. After 10 days of autoclave treatment at 200 °C in aqueous phase, H-ZSM-5(A) demonstrated nearly unchanged reaction rates in the dehydration of cyclohexanol, while H-ZSM-5(B) lost > 50% of the dehydration activity. Additionally, H-ZSM-5(A) delivered higher initial dehydration rates compared to H-ZSM-5(B). The different measured activation energies further revealed variations in reaction pathways during cyclohexanol dehydration, i.e., the monomer- or dimer-mediated routes depending on the concentration of alcohol molecule within zeolite pores, providing additional evidence for the strengthened hydrophobic nature of H-ZSM-5(A). Beyond this, the zeolite surface properties and the strength of cyclohexanol-zeolite interactions may impose additional transport/adsorption barriers attributed to multi-phase phenomena on the more polar H-ZSM-5(B) zeolite surfaces. More importantly, the hydrothermal treatment did not induce significant desilication and dealumination in H-ZSM-5(A), thereby preserving its active acid sites and ensuring exceptional hydrothermal stability. The present work fundamentally studies the synthesis of hydrothermally stable zeolites in an acidic medium using fluorides and expands the understanding of polar interactions in catalysis, characterized by the dehydration of cyclohexanol, for future application in biomass conversion.
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ACS Catalysis
·
2025
·
IF 13.1
Rong Shang,Hao Zhang,Yulong Li,Bang Gu,Qinghu Tang,Feng Qiu,Qiu-E Cao,Wenhao Fang
The synthesis of primary amines from renewable biobased carbonyl compounds via reductive amination has received much attention. Modifying the surface structure of a heterogeneous catalyst may offer prospects to address selectivity maneuvering in this complex amination process. In this work, a metal–organic framework (MOF)-derived carbon-coated strategy was adopted to prepare the Ni@C catalysts with different thicknesses of carbon shells. This type of Ni catalyst achieved 98% yield of (5-(aminomethyl)furan-2-yl)methanol (AMF) at 100 °C under 2 bar of H2 from reductive amination of 5-hydroxymethylfurfural (HMF, an important cellulose-derived platform molecule) with NH3·H2O. In comparison, a Ni-NiO catalyst obtained by reducing NiO with H2 would mainly overhydrogenate AMF to (5-(aminomethyl)tetrahydrofuran-2-yl)methanol (THAMF, 52% in yield) as a byproduct. The modification of the electronic structure of Ni0 active sites with a carbon shell was elucidated, demonstrating electron-rich Ni0 sites for H2 activation. Moreover, different HMF adsorption modes on Ni-NiO and Ni@C surfaces were illustrated, significantly affecting the product distribution. Subsequently, distinctive NH3·H2O activation processes were proposed for both Ni catalysts to understand selective conversion of the Schiff base (i.e., the critical reaction intermediate). The developed Ni@C catalyst with suitable carbon thickness, abundant Ni0 centers, and defective carbon species showed high AMF yield under mild reaction conditions, facile separation–regeneration, and satisfying reusability. In addition, this Ni catalyst can also provide a relatively good substrate scope toward bioamine synthesis via reductive amination.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Wei Lv,Yao Wang,Hong Chen,Yongqi Tang,Yongdan Li
Nitrogen atom-doped biomass carbon prepared from corn stover is a newly discovered metal-free catalyst that shows good activity on the selective oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-diformylfuran (DFF). Here, the presence of graphitic nitrogen on the catalyst surface activated the oxygen adsorbed on the carbon sites next to the graphitic nitrogen in the carbon material and promoted the formation of oxygen radicals on the surface-active sites, improving the HMF oxidation process. The results show that the catalyst NC-800 reacted with acetonitrile as the reaction solvent at 110 °C and 1.0 MPa O 2 for 8 h to obtain 93.0 % HMF conversion and 94.4 % DFF selectivity, and the 5-HMF conversion and DFF selectivity were maintained at more than 85 % after five cyclic tests, with excellent cyclic stability. One of the main factors influencing the material flaws is the variation in pyrolysis temperature. Using maize stover, a readily available and renewable biomass, in the catalytic oxidation of biomass platform compounds may improve biomass utilization more extensively.
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RENEWABLE ENERGY
·
2025
·
IF 9.1
Congcong Zhao,Jian Zhang,Guo Qiu,Yan Sun,Yongguo Liu,Hongyu Tian
5-Hydroxymethylfurfural (5-HMF), as an important biomass derivative, has received widespread attention due to its ability to be converted into numerous high value-added chemicals. In this work, a low-cost and efficient vanadium-loaded montmorillonite (V-Mont) catalyst for the transformation of glucose and fructose to 5-HMF was prepared using the ion exchange method, possessing both strong Brønsted acid and Lewis acid sites. The highest 5-HMF yields of 63.33 % and 70.02 % with almost complete conversion were obtained from glucose at 160 °C for 2 h and from fructose at 170 °C for 20 min, respectively. The V-Mont catalyst in saturated salt water system also achieved a satisfactory result in 5-HMF synthesis and was recycled for four times with no obvious loss of activity. The mechanism was speculated and validated using density functional theory (DFT) calculations, indicating that among the three calculation models, the energy barrier crossed by the [VO(OH) 2 ] + catalytic reaction was the lowest, further demonstrating the mononuclear pentavalent [VO(OH) 2 ] + as a dominant species could accelerate the synergetic proton transfer in the glucose isomerization process and promote the positive progression of chemical equilibrium. This study provides a novel and green strategy to further design efficient catalytic system for 5-HMF production.
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Innovative Food Science & Emerging Technologies
·
2025
·
IF 6.8
Lijun Tan,Shasha Zheng,Yong Xie,Wendi Zhang,Baocai Xu
Photodynamic inactivation (PDI) is a promising non-thermal antimicrobial technology known for broad-spectrum efficacy and low resistance potential. However, conventional PDI face limitations in bactericidal efficacy due to the short-lived and poorly diffusing reactive oxygen species (ROS). This study proposes a novel food-grade PDI strategy that incorporates disodium 5′-inosinate (IMP) into a vitamin B2 (VB2)-mediated system, significantly enhancing H 2 O 2 production. Acting as an electron donor, IMP promotes type I photochemical reactions, enabling sustained H 2 O 2 generation and achieving >6 log CFU/mL inactivation of Bacillus safensis , a spoilage bacterium often overlooked in cooked meat products. Mechanistic analyses showed that H 2 O 2 oxidized key phospholipids in the cell membrane, increased permeability, caused membrane potential hyperpolarization and ion leakage, and ultimately disrupted multiple membrane domains. Moreover, this strategy also exhibited persistent antimicrobial activity, effectively delaying spoilage in cooked meat products stored at 4 °C and 25 °C. Overall, this study introduces a safe and effective non-thermal sterilization method with promising industrial potential and offers a novel pathway to enhance PDI efficacy via intensified type I ROS mechanisms.
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