CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Xin Li,Yue Ma,Xuning Wang,Jianguo Wu,Dong Cao,Daojian Cheng
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd 0 /Pd 2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C 3 N 4 –300 catalyst with a Pd 0 /Pd 2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd 0 and Pd 2+ in Pd/g–C 3 N 4 –300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Ruixue Zhang,Weiyao Yang,Hongda Zhang,Le Sang,Zhiping Zhao
This work presents the efficient, safe, and continuous production of 5-hydroxymethylfurfural (HMF) and levulinic acid (LA) from inulin in micropacked bed reactors (μPBRs) over HND-580. Through optimization reaction conditions, the highly selective production of fructose and LA from aqueous inulin and HMF from an inulin DMSO-water mixed solution can be achieved with respect to other reactor technologies. The highest yields of 89% for fructose, 81% for HMF, and 84% for LA can be obtained within a reaction time of 7.26 min. Polysaccharide inulin is used as the reaction substrate, and the space-time yield (STY) of HMF and LA in μPBRs is at least an order higher than that in conventional batch reactors. Subsequently, an intrinsic kinetic model for inulin conversion is established. The most predicted values show good agreement with the experimental results with a relative error of ±20%.
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APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Qiang Fang,Lu Hao,Tao Zhao,Jiahui Li,Genyan Hao,Guang Liu,Dazhong Zhong,Jinping Li,Qiang Zhao
The electrocatalytic production of 2,5-furandicarboxylic acid (FDCA) via the 5-hydroxymethylfurfural oxidation reaction (HMFOR) is an effective and more suitable alternative to the oxygen evolution reaction (OER) in electrocatalytic water splitting. High-valence Ni(III) is critical for the HMFOR, but the formation is greatly limited by the difficult in situ self-oxidation. In this study, the pre-oxidization-derived amorphous NiO x H y nanosheet presents more accessible Ni(III) for efficient HMFOR. In addition, NiO x H y /NF exhibits a low onset potential of 1.35 V, a high FDCA yield of 98.5 %, and a high Faradaic efficiency of 98.3 % for the HMFOR in 0.1 M KOH with 10 mM HMF. In situ Raman spectroscopy results indicate that Ni(III)OOH is an active intermediate in the electrochemical HMFOR. This work provides a strategy for promoting the formation of high-valence Ni(III) and boosting biomass oxidation.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Yingyang Song,Junyu Lang,Qingrui Zeng,Jinping Cheng,Mingce Long
Monoethanolamine (MEA)-based carbon dioxide absorption is one of the effective carbon capture, utilization, and storage (CCUS) technologies but is significantly restricted by the high energy consumption in the regeneration of rich amine solution. Solid acid catalysts have the potential to reduce energy consumption, while the exploration of highly active catalysts with abundant Bro̷nsted and Lewis acid sites remains needing. We developed an efficient solid acid catalyst, niobium-modified HZSM-5 (Nb/HZ), to facilitate CO2 desorption from the CO2-captured MEA solutions. The Nb/HZ catalysts with various niobium loadings were synthesized by using an impregnation method. HZSM-5 retained its pore structure and large surface area after niobium incorporation. The catalyst with 4% Nb (4.0-Nb/HZ) has the highest activity and stability, with 61% increase in the desorption rate, 50% increase in the desorbed CO2 amount, and 37% reduction of relative heat duty. According to theoretic calculations and experimental analyses, the Nb/HZ catalyst provides abundant Bro̷nsted and Lewis acid sites to facilitate carbamate adsorption, proton transfer, and carbamate breakdown, thus reducing the activation energy for CO2 desorption. This work provides a valuable solid acid catalyst for amine-based CO2 capture and also brings insights for the development of a novel solid acid for diverse catalysis.
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Journal of Neuroinflammation
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2025
·Vol. 22
·期 1
·1-16
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IF 10.1
Ding Peng-Fei,Zhang Jia-Tong,Zhu Xiao-Long,Cui Yue,Chen Chun-Lei,Liu Xun-Zhi,Shen Jun-Da,Zou Le-Xuan,Lu Yue,Zhuang Zong,Hang Chun-Hua,Li Wei
Background
Subarachnoid hemorrhage (SAH) is a common acute condition in neurosurgery, with microglial function playing a crucial role in determining patient outcomes. However, the involved mechanisms are complex and demand thorough investigation. In our study, we combined transcriptomic and metabolomic approaches to identify key regulators of microglial function, offering novel insights for potential therapeutic strategies in SAH treatment.
Methods
The neurological function of SAH mice was evaluated using the open field test, rotarod test, and nissl staining. In an in vitro SAH model, key pathways and genes that regulate microglial function were identified through the integration of transcriptomics and metabolomics. Enzyme-Linked Immunosorbent Assay, Immunofluorescence, Western blot, Real-Time PCR, pHrodo, and Lyso-Tracker were employed to assess lysosomal and microglial function.
Results
In SAH mice, both neurological and microglial functions were significantly impaired on the first day but showed recovery over time. The combined results from transcriptomics and metabolomics identified 5-lipoxygenase (5-LOX) as a key target in regulating microglial function post-SAH. Administering resolvin D1 (RvD1) exogenously to inhibit 5-LOX nuclear translocation or directly supplementing lipoxin A4 (LXA4) to adjust the leukotriene B4 (LTB4)/LXA4 ratio, can improve lysosomal acidification, mitigate impaired lysosomal function, and enhance phagocytosis while reducing the inflammatory response. Protecting microglial function can also be achieved through JNJ or P2X purinoceptor 7 (P2X7) siRNA, which inhibit calcium/calmodulin-dependent protein kinase II (CaMKII) activation, prevent 5-LOX nuclear translocation, and improve lysosomal function. Furthermore, P2X7 siRNA also improved neurological function, lysosomal function and microglial function in SAH mice.
Conclusion
Activation of P2X7-CaMKII after SAH promotes 5-LOX nuclear translocation, increases the LTB4/LXA4 ratio, elevates intracellular Ca2+ concentration, and impairs lysosomal and microglial function.
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JOURNAL OF GASTROENTEROLOGY
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2025
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IF 5.5
Ren Bingyu,Li Han,Liu Shenglu,Huang Zhiwei,Bai Junjie,Jiang Zhonghao,Xu Tongjie,Gu Boyuan,Yu Wenhao,Sun Lei,Tan Peng,Fu Wenguang
Background and Aims Inflammatory cell infiltration in the liver is a hallmark of metabolic dysfunction-associated fatty liver disease (MAFLD). However, the pathological events that trigger the infiltration of inflammatory cells to mediate MAFLD pathogenesis remains poorly understood. This study aims to investigate the function and mechanism of Hic-5 on hepatic inflammation of MAFLD. Methods MAFLD animal models were fed a methionine- and choline-deficient (MCD) diet in Hic-5 knockout mice. Liver tissues were analyzed by immunohistochemical staining, immunofluorescence and flow cytometry, with a particular focus on the impact on the immune microenvironment. Results Hic-5 deficiency alleviates the severity of MAFLD, particularly the inflammation response. Gain- and loss-of-function experiments revealed that Hic-5 deficiency results in decreased neutrophil proliferation and increased apoptosis, as well as impaired migration. Conversely, Hic-5 overexpression had the opposite effects. This study confirmed that METTL3-mediated methylation of m 6 A stabilizes Hic-5 mRNA and promotes its expression, which in turn regulates the infiltration of neutrophils by the CXCL1-CXCR2 axis. Conclusions The study reveals the role of Hic-5 in regulating neutrophils and indicates that it may be a potential therapeutic target for MAFLD.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Jing Wang,Xin Xu,Wanqing Wei,Wei Song,Jian Wen,Guipeng Hu,Xiaomin Li,Cong Gao,Xiulai Chen,Liming Liu,Jing Wu
Pyridoxal 5′-phosphate (PLP) is highly valuable in food and medicine. However, achieving the efficient biosynthesis of PLP remains challenging. Here, a salvage pathway using acid phosphatase from Salmonella typhi (StAPase) and pyridoxine oxidase from Escherichia coli (EcPNPO) as pathway enzymes was established for the first time to synthesize PLP from pyridoxine (PN) and pyrophosphate (PPi). StAPase was identified as a rate-limiting enzyme. Two protein modification strategies were developed based on the PN phosphorylation mechanism: (1) improving the binding of PN into StAPase and (2) enhancing the hydrophobicity of StAPase’s substrate binding pocket. The kcat/Km of optimal mutant M7 was 4.9 times higher than that of the wild type. The detailed mechanism of performance improvement was analyzed. Under the catalysis of M7 and EcPNPO, a PLP high-yielding strain of 14.5 ± 0.55 g/L was engineered with a productivity of 1.0 ± 0.02 g/(L h) (the highest to date). The study suggests a promising method for industrial-scale PLP production.
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ChemCatChem
·
2025
·
IF 3.9
Xinyu Xiao,WEIWEI ZHAO,Mingyue Li,Guangmeng Chen,Wenjie Yu,Weihua Zhou,Xiaoqing Liu
The electrooxidation of 5-hydroxymethylfurfural (HMF) has emerged as a promising way to generate high-value-added bio-based products. However, improving catalyst selectivity for HMF and inhibiting competitive oxygen evolution reaction (OER) in a limited potential range remain long-term targets. In this work, the self-supported LIG-NiCuP electrode, utilizing porous laser-induced graphene (LIG) skeleton as the substrate and loaded with NiCuP compound, is designed for the efficient and highly selective electrooxidation of HMF to 2,5-furandicarboxylic acid (FDCA). The surface reconstruction of electrode forms a LIG-NiCuP/NiCu(OH)x heterostructure, demonstrating high activity (HMF conversion 99.7%, FDCA yield 92.6%) for HMF oxidation reaction (HMFOR). Studies indicate that the low activity of Cu for OER allows it to function as a co-catalyst, enhancing the selectivity of Ni-based primary catalyst for HMF. In addition, the pine needle-like structure of Cu can optimize the morphology of catalyst deposited on LIG skeleton, increasing the contact area with HMF. On the other hand, in terms of the substrate to support metal catalysts, LIG fabrication combines the characteristics of rapidity, simplicity, scalability, and low cost, therefore, holding high promise in practical applications. Overall, the material system and processing method in this work present a significant step toward developing efficient catalyst electrodes for biomass conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Junpu An,Hongchen Liu,Fan Yang,Kexin Wei,Chunhui Yu,Siyuan Sun,Yang Sun,Qing Guo,Jianfeng Wang,Chenlin Wang,Jiahui Liu,Kuobo Wang,Yongfeng Li
Nickel-based catalysts show great potential as promising candidates for the electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF). However, the limited adsorption capacity of nickel-based catalysts for OH – and HMF limits their further development. In this study, amorphous Fe/NiOOH-SO x was generated from nanosheets (Fe/NiOOH-Ni 3 S 2 ), which was pre-fabricated on nickel foam via pre-reconstruction and anionic regulation strategy. The optimized catalyst Fe/NiOOH-Ni 3 S 2 demonstrated exceptional activity in the HMF oxidation reaction (HMFOR) with a current density of 10 mA cm −2 at 1.32 V vs RHE, accompanying with the 98.9 % HMF conversion, 97.8 % 2,5-Furandicarboxylic acid (FDCA) selectivity, 96.8 % Faraday efficiency, and stability for ten cycles. The incorporating amorphous FeOOH reduces the electron density around Ni, promoting the formation of high-valent Ni spices. Meanwhile, the SO x combined with amorphous hydroxy nickel oxide provides unsaturated sites, which enhances the adsorption capacity of HMF. Density functional theory (DFT) computations reveal that the designed amorphous Fe/NiOOH and surface-adsorbed SO x collectively modulate the electronic structure of the catalyst, causing an upwards shift of the NiOOH d-band center and enhancing adsorption capacities for both HMF and OH – . This study proposes the adsorption enhancement mechanism of regulating electronic structure and offers a rational strategy for HMFOR electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Junru Li,Si Li,Shuhan He,Heng Zhang,Hengwei Lin,Peng Wang
Chiral nanomaterials with biomimetic catalytic properties hold significant potential for applications in asymmetric catalysis, chiral synthesis, and regulation of biological activity. However, further research remains necessary to advance synthetic methodologies and practical implementations of these materials. In this study, L - and D -V 2 O 4/5 nanoparticles (NPs) were successfully synthesized with pronounced chiral optical activity from ultraviolet to near-infrared regions via an in-situ etching-regrowth approach, exhibiting an enantioselective oxidase-like catalytic activity toward chiral molecules. Specifically, L -V 2 O 4/5 displayed a preference toward L -epinephrine ( L -EP) with a selectivity factor of 1.40, for L -norepinephrine ( L -NE) with a selectivity factor of 1.34. During the catalytic oxidation of d -Glucose ( D -Glu), the produced H 2 O 2 byproduct degraded the chiral surface configuration of chiral V 2 O 4/5 NPs, significantly diminishing their chiroptical signals in the visible range. This effect enabled the development of a novel self-feedback D -Glu sensing platform. The comparative analysis demonstrated that D -V 2 O 4/5 NPs exhibited 1.80 times greater detection sensitivity than L -V 2 O 4/5 NPs for D -Glu detection, attributed to their superior ability to recognize chiral molecules. These findings highlight the significant impact of nanomaterial chirality on the ultrasensitive detection of chiral substances and underscore the promising applications of rationally designed chiral nanomaterials in enantioselective biomimetic catalysis and biosensing.
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Journal of the Taiwan Institute of Chemical Engineers
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2025
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IF 6.3
Jun-Feng Lu,Huan Wang,Yi Zhou,Xue-Ying Mao,Xiao-Qian Feng,Shuang Wang,Yong-Hua Zhao
Background Rhodamine B (RhB) poses a significant threat to aquatic ecosystems. While Fenton oxidation process is promising approach for RhB degradation, the conventional Fenton reaction has the narrow pH range and poor reusability. To overcome these, this study developed Fenton-like system with Fe-Cu/HZSM-5 catalyst for effective RhB degradation. Methods A series of Fe x Cu 5-x /HZSM-5 catalysts (x represents the molar ratio of Fe to Cu) were prepared by impregnation. These catalysts were integrated with H 2 O 2 to construct Fenton-like system for the degradation of RhB. The catalysts were characterized by XRD, NH 3 -TPD, XPS, FT-IR, and N 2 adsorption-desorption at low temperature techniques. Significant findings Among the tested catalysts, Fe 3 Cu 2 /HZSM-5 exhibited optimal performance, achieving near-complete RhB degradation (∼100%) under the condition of 45 °C, 5.3 mM/L H 2 O 2 , 3.0 g/L catalyst dosage, and broad pH range (2–5). Mechanistic studies confirmed that hydroxyl radicals (·OH) were the primary oxidants responsible for RhB degradation in Fenton-like system. Under ·OH attacking, RhB underwent a series of reactions such as N-deethylation and disruption of the conjugated structure and was eventually mineralized into CO 2 and H 2 O. Overall, a novel Fe-Cu/HZSM-5 catalyst was developed to address the limitations of the traditional Fenton reaction, providing valuable insights for future research in this field.
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高影响因子
FUEL
·
2025
·
IF 7.5
Xiaohui Wang,Zhilong Cheng,Bingrong Liu,Huiyi Liu,Xin Fang,Ruiqi Chai,Lishuang Ma,Yuchao Lyu,Jianye Fu,Xinmei Liu
Methane dehydroaromatization (MDA) was a promising technology for the synthesis of high value-added aromatics through natural gas. Fe/ZSM-5 catalysts were widely used in MDA reaction. However, its catalytic mechanism remained ambiguous. In this work, a novel one-pot strategy was developed for the preparation of Fe/ZSM-5 catalysts, which can delicately control the iron species and acidic property of Fe/ZSM-5 catalysts. In-situ DRIFTS and DFT calculation demonstrated that MDA followed a bifunctional mechanism and the second C–H bond breaking process of CH 4 was the rate-determining step, where methane underwent coupling and dehydrogenation at the iron active sites to generate intermediate species (ethylene), and Brønsted acid sites played a key role in determining the selectivity of aromatics. Moreover, CO-pulse chemisorption revealed the quantitative synergistic effect between metal active sites and Brønsted acid sites. Catalysts with highly dispersed iron oxide and proper density of Brønsted acid sites exhibited the best catalytic performance. This study elucidated the catalytic roles of iron species and Brønsted acid sites in Fe/ZSM-5 catalysts in MDA and provided guidance for the future development of highly active MDA catalysts.
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