FUEL
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2025
·
IF 7.5
Jianping Ding,Xiaoyan Zhou,Zhengzheng Yang,Changgeng Liu,Mingchao Sun,Congling Yang,Lu Fan
In this study, a novel strategy was proposed for synthesizing dual single-atom Ce-Ti catalysts supported on γ-Fe 2 O 3 via ball milling and calcination. Compared to γ-Fe 2 O 3 and single-atom Ce/γ-Fe 2 O 3 and Ti/γ-Fe 2 O 3 catalysts, the Ce-Ti/γ-Fe 2 O 3 catalyst exhibits superior NO conversion rates and significantly enhanced tolerance to H 2 O and SO 2 at 200–240 °C. These advancements are attributed to the synergistic interactions between Ce and Ti, which enhance redox properties, increase Lewis acid site density, and facilitate the Langmuir-Hinshelwood reaction pathway. In-situ DRIFTS and density functional theory (DFT) analyses revealed the mechanistic role of surface-active oxygen species and intermediate formation in promoting the SCR reaction. The findings provide valuable mechanistic insights and establish a scalable approach for the development of high-performance, environmentally friendly catalysts for industrial NO x removal.
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JOURNAL OF CHROMATOGRAPHY A
·
2025
·
IF 4
Wenbin Zhang,Yuzeng Li,Nurimangul Muntiza,Wenquan Ji,Zhen Fan,Qinran Li,Jin Zhao,Hongfeng Zhang,Qiliang Deng,Donglan Sun,Tianjun Liu
A dual-epitopes imprinted strategy for cytochrome c selective recognition assisted with γ-cyclodextrin host-guest interaction via N-terminal and C-terminal epitope's simultaneous imprinting and reversible addition-fragmentation chain transfer (RAFT) polymerization was developed. N-terminal and C-terminal nonapeptides of Cyt c (GI-9 and AE-9) were used simultaneously as the epitope to achieve collaborative recognition for cytochrome c. As a supramolecule, γ-cyclodextrin can encapsulate the aromatic functional groups of amino acid residues to capture the peptide and improve the corresponding spatial orientation for epitope or cytochrome c recognition by host-guest interaction. After the γ-cyclodextrin modification and dual-epitopes immobilization, the imprinted polymer was synthesized by RAFT polymerization with 4-cyano-4-(phenyl-carbonothioylthio) pentanoic acid as a chain transfer agent. After the template removal, the obtained dual-epitopes imprinted particles showed well binding ability to AE-9 (26.50 mg·g −1 , IF= 4.13), GI-9 (7.36 mg·g −1 , IF= 2.18) and cytochrome c (79.56 mg·g −1 , IF= 3.27). With the successive addition of RAFT agent, the imprinting factor rising of epitope peptide and cytochrome c further illustrated the regulation of imprinted polymer chains. The imprinted particles had the advantage for cytochrome c recognition compared to other proteins and good reusability with 82.60 % repeated reproduction rate after six cycles of adsorption and desorption. Furthermore, the selective recognition for cytochrome c in bovine serum proved its potentiality to be applied in complex biological samples. It indicated that the combination of dual-templates epitope imprinting, γ-CD host-guest interaction and RAFT polymerization provided an efficient method for collaborative protein recognition with well selectivity, reusability and stability.
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高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 3.8
Wenyu Gao,Guanying Shi,Lihua Zhang,Zhaogai Wang,Wei Zong
γ-glutamyl transpeptidase (GGT, E.C.2.3.2.2) has great applications in the food industry, but there is no commercially available bacterial GGT on the market. In this paper, response surface methodology was used to optimize the yield of Bacillus licheniformis GGT ( Bl GGT). The enzyme was extracted and used to catalyze the synthesis of volatile sulfur compounds (VSCs) in Toona sinensis (TS). The results showed that the optimal conditions for fermentation of GGT production were: lactose 8 g/L, tryptone: soybean meal (1:1) 15 g/L, MgSO 4 ·7 H 2 O 0.5 g/L, K 2 HPO 4 1 g/L, inoculum volume of 5 % v/v, initial pH 8.0, loading volume of 50 mL, and fermentation temperature of 37.0 ℃. Under this condition, the enzyme activity of GGT reached 918.38 ± 0.012 U/L, which was 19 times higher than the activity under the initial medium conditions. In addition, when the GGT was added to the precursor extract from TS, it was noteworthy that VSCs in TS were regained, with the total amount reaching 30.38 μg/mL. The optimization of the fermentation medium to increase the yield of Bl GGT may also provide valuable data for the large-scale production of GGT. The results of this study provide an effective pathway for the synthesis of unique VSCs in TS.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Xueting Liu,Yajing Zhu,Yutong Jing,Yuheng Zhu,Lichuan Wu,Wenqian Nong
Bacteria deep in the wound can cause prolonged inflammation and dysfunctional angiogenesis, impeding healing and potentially leading to chronic conditions, disability, or even death. To address this, we developed a double-layer metal-organic framework (MOF) microneedle (MN) patch system (GCM-MN-CSH), designed to accelerate the healing of infected wounds through programmed therapy. The GCM-MN-CSH system consists of a hydrocaffeic acid-modified chitosan (CSH) hydrogel patch and a metformin (Met)-loaded Ga-Car-MOF (GCM)-based γ-polyglutamic acid matrix MN array (GCM-MN). The GCM nanoparticles were incorporated in the MN tips. The deep, localized penetration of GCM-MN, combined with the multifunctional activity of GCM, enables effective delivery of GCM nanoparticles into the dermis. These nanoparticles acid-response release Ga 3+ ions and benzylpenicillin carboxylate, which possess antimicrobial activity, as well as Met, which promotes tissue regeneration. The adhesive CSH patch not only helps create a controlled, moist environment at the wound site but also provides antimicrobial properties on the surface. Together, the components of the GCM-MN-CSH system work synergistically to control infection, reduce inflammation, stimulate tissue proliferation, support tissue remodeling, and ultimately enable programmed wound healing. This advanced system offers a promising therapeutic platform for the management of infected wounds.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Gouda Helal,Zhenhang Xu,Wei Zuo,Jun Qian,Gongzhen Cheng,Pingping Zhao
Transition metal-based electrocatalysts undergo electrochemical surface reconstruction to generate metal oxy-hydroxide-based hybrids, which regard the actual active sites for the oxygen evolution reaction (OER). Many efforts have been devoted to understanding the electrochemical surface reconstruction, but there is rare research to identify the origin of improved OER performance derived from the substrate. Herein, we reported the electrochemical synthesis of an amorphous γ-NiOOH surface layer on NiFealloy/NiFeN pre-catalysts for efficient water oxidation. However, the conversion of β-NiOOH to γ-NiOOH is a thermodynamically unfavorable process, resulting in much higher applied potential to drive the reaction and subsequently catalyze OER.We identified that the NiFe-bimetallic active sites can promote the OER catalytic activity more than the Ni-monometallic active sites. Besides, nitrogen can reduce the potential required to generate γ-NiOOH OER-active sites from β-NiOOH and generate the NO3- anion, which promotes the formation of γ-NiOOH. The electrochemical analysis and in situ spectroscopic approaches, including cyclic voltammetry (CV), linear sweep voltammetry (LSV), and Raman, reveal that Ni species in NiFealloy/NiFeN are more thermodynamically favorable to form γ-NiOOH than in Nialloy/NiN and NiFeLDH. Beside the electrochemical behavior, X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), and bode plots further demonstrate that Fe doping and nitrogen significantly increase the electrochemically active sites. Additionally, DFT calculation results show that the electronic structure of the catalysts is modulated by Fe doping, and the surface reconstruction optimized the adsorption energy of oxygen-containing species and enhanced the OER catalytic activity. This work provides a new design for constructing transition metal-based electrocatalysts for water oxidation.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 6
·1504-1510
·
IF 5.726
Shanshan Yu,Peiyuan Yao,Jinlong Li,Jinhui Feng,Qiaqing Wu,Dunming Zhu
Nitrilase-catalysed desymmetrization of 3-substituted glutaronitriles to optically active 3-substituted 4-cyanobutanoic acid offers an attractive approach to access chiral β-substituted γ-amino acids, an important moiety in pharmaceuticals. In this study, we employed enzyme-substrate docking and alanine scanning to determine the key amino acid residues which have a positive effect on the activity and stereoselectivity of a nitrilase from Synechocystis sp. PCC6803 (SsNIT). Then, site-saturation mutagenesis and combinatorial mutagenesis of the positive amino acid residues (H141, P194, M197, I201 and F202) were performed, and a double mutant (P194A/F202V) and a triple mutant (P194A/I201A/F202V) with high activity and stereoselectivity were identified for desymmetrization of 3-substituted glutaronitriles to afford (S)-3-substituted-4-cyanobutanoic acids with a high space–time productivity of up to 488 g L−1 d−1. Molecular calculation suggests that the enzymatic activity improvement may be due to the enlargement of the substrate binding cavity. It is interesting that the stereoselectivity is enhanced simultaneously.
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Catalysts
·
2018
·Vol. 8
·期 12
·642
·
IF 3.465
Yan Gao,Tao Luan,Mingyang Zhang,Wenke Zhang,Wenchen Feng
A series of Mn−Fe−Ce−Ox/γ-Al2O3nanocatalysts were synthesized with different Mn/Fe ratios for the catalytic oxidation of NO into NO2and the catalytic elimination of NOxvia fast selective catalytic reduction (SCR) reaction. The effects of Mn/Fe ratio on the physicochemical properties of the samples were analyzed by means of various techniques including N2adsorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature-programmed reduction (TPR), NH3-temperature-programmed desorption (TPD) and NO-TPD, meanwhile, their catalytic performance was also evaluated and compared. Multiple characterizations revealed that the catalytic performance was highly dependent on the phase composition. The Mn15Fe15−Ce/Al sample with the Mn/Fe molar ratio of 1.0 presented the optimal structure characteristic among all tested samples, with the largest surface area, increased active components distributions, the reduced crystallinity and diminished particle sizes. In the meantime, the ratios of Mn4+/Mnn+, Fe2+/Fen+and Ce3+/Cen+in Mn15Fe15−Ce/Al samples were improved, which could enhance the redox capacity and increase the quantity of chemisorbed oxygen and oxygen vacancy, thus facilitating NO oxidation into NO2and eventually promoting the fast SCR reaction. In accord with the structure results, the Mn15Fe15−Ce/Al sample exhibited the highest NO oxidation rate of 64.2% at 350 °C and the broadest temperature window of 75–350 °C with the NOxconversion >90%. Based on the structure–activity relationship discussion, the catalytic mechanism over the Mn−Fe−Ce ternary components supported byγ-Al2O3were proposed. Overall, it was believed that the optimization of Mn/Fe ratio in Mn−Fe−Ce/Al nanocatalyst was an extremely effective method to improve the structure–activity relationships for NO pre-oxidation and the fast SCR reaction.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Yu Tian,Haodi Yang,Fei Wang,Ping Ning,Kunlin Li,Kai Li
Increasing the oxygen vacancy (Ov) content and inducing lattice oxygen activation are critical for enhancing the oxidation performance of transition metal oxides. However, precisely regulating these properties remains a significant challenge. In this study, a stepwise pyrolysis method was employed on a colloidal complex formed by citric acid coordinated with Fe(NO 3 ) 3 ·9H 2 O to synthesize Fe 2 O 3 -X catalysts comprising a mixture of α- and γ-Fe 2 O 3 characterized by abundant surface oxygen vacancies and activated lattice oxygen. The resulting Fe 2 O 3 -1 presented excellent low-temperature H 2 S selective catalytic oxidation (H 2 S-SCO) performance, achieving selective oxidation of H 2 S at 130°C with removal efficiency and sulfur selectivity exceeding 95 % and 85 %, respectively, within 60 h. Characterization results show that the γ-Fe 2 O 3 induced by citric acid forms a crystal interface with the α-Fe 2 O 3 . At the interface, the asymmetrically coordinated lattice oxygen is more likely to be released from the catalyst, thereby enhancing the oxidation ability of the catalyst. Furthermore, the synthesis method effectively modulates the catalyst’s surface basicity, resulting in an optimal distribution of basic sites that mitigates catalyst poisoning and deactivation. This study presents a straightforward approach for synthesizing Fe 2 O 3 catalysts with enhanced oxidation ability, offering valuable insights for developing more efficient transition metal catalysts.
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CHEMOSPHERE
·
2018
·
IF 4.427
Zhuangpeng Huang,Zhiping Chen,Yuancai Chen,Yongyou Hu
Iron-copper bimetal supported on mesoporous γ-Al 2 O 3 with different Fe/Cu ratios was prepared via a modified evaporation-induced self-assembly method and employed to degrade 4-chlorophenol (4-CP) in a Fenton-like process. The X-ray photoelectron spectroscopy, X-ray diffraction spectrum and UV–vis diffuse reflectance spectroscopy results confirmed the co-doping of Fe 2+ /Fe 3+ and Cu + /Cu 2+ into the lattice of γ-Al 2 O 3 through the bonds of Al O Fe and Al O Cu. With the iron and copper co-doped in γ-Al 2 O 3 , three-fold oxygen vacancies (V 0 ) could be achieved compared with that of non-metal catalysts, which was favorable for the reduction of iron and copper species. The 1Fe3Cu-γ-Al 2 O 3 with a Fe/Cu mass ratio of 1:3 exhibited the highest activity on Fenton-like degradation of 4-CP due to the synergistic effects of Fe and Cu by facilitating the electron transfer in the recycles of Cu + /Cu 2+ and Fe 2+ /Fe 3+ based on the results of X-ray photoelectron spectroscopy, cyclic voltammetry and electro paramagnetic resonance analysis. The utilization efficiency of H 2 O 2 was as high as 86.0% when 4-CP almost disappeared (i.e., 99.7 percent of 0.78 mM 4-CP) at 240 min and pH 7.0, additionally, their dechlorination and TOC removal efficiencies were 92.0% and 81.6%, respectively. The catalyst also displayed a good performance after 5th cycles. Furthermore, a possible mechanism for activation of OH on the catalyst surface was also proposed.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Xueyin Ru,Wanli You,Jinglin Zhang,Feng Xu,Zhengguo Wu,Peng Jin,Yonghua Zheng,Shifeng Cao
The effects of γ-aminobutyric (GABA) on enzymatic browning , storage quality, membrane and reactive oxygen species (ROS) metabolism in fresh-cut stem lettuce were investigated. The results illustrated that GABA treatment delayed browning degree, polyphenol oxidase (PPO) activity and the expression of LsPPO . Meanwhile, higher chlorophyll and ascorbic acid contents were exhibited in GABA-treated stem lettuce, as well as the slower microbial propagation. Further investigation revealed that exogenous GABA application declined malondialdehyde content, electrolyte leakage and the enzyme activities of membrane metabolism, and the expression levels of related genes were also downregulated. In addition, GABA treatment scavenged ROS and strengthened the enzyme activities of ROS metabolism, as well as the expression levels of corresponding genes. Taken together, these findings implied that the repressed enzymatic browning and microbial propagation in GABA-treated stem lettuce were due to the inhibition of ROS accumulation, enhancement of membrane stability and increased resistance to oxidation .
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JOURNAL OF ORGANIC CHEMISTRY
·
2020
·
IF 4.335
Ling Tang,Qin Yang,Jianfang Zhang,Guisheng Deng
A regioselective reverse strategy for the construction of eight-membered sulfur-containing heterocycle-fused γ-pyrones and 2-(1,4-dithianyl)-4-pyrones starting from 2-diazo-γ-pyrones and dithioacetals was achieved for the first time. The process combines C–S bond formation via sulfur ylides and C–C bond formation via electron transfer to afford the target molecules in a facile manner with 100% regioselectivity and in excellent isolated yields (up to 90%).
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POLYMER COMPOSITES
·
2025
·
IF 4.7
Xinyue Hu,Hong Ruan,Yuqi Li
The synthesis of polyimides with low dielectric constants, high wear resistance, and excellent mechanical properties is crucial to expanding their applications in aerospace and microelectronics. This study employed γ-aminopropyl triethoxysilane to modify the surface of silica, yielding a modified silica/polyimide nanocomposite (KSPI). Molecular dynamics simulations were conducted to evaluate the performance of the KSPI, incorporating the microstructural morphology and interface interaction energy changes. Results demonstrated that adding 0.5 wt.% APS-modified silica improved interfacial bonding, as well as mechanical and tribological properties. Compared with pure polyimide, the tensile strength of KSPI increased by 35.99%, whereas the dielectric loss and wear rate decreased by 52.4% and 54.03%, respectively. Simulations comparing KSPI and silica/polyimide systems revealed a 24.15% reduction in the solubility parameter similarity coefficient R and a 77.02% decrease in the free volume for KSPI, indicating superior compatibility owing to its reaction with silica hydroxyl groups to form Si O Si bonds, reduce hydrophilicity, and inhibit agglomeration. γ-aminopropyl triethoxysilane modification improves silica dispersion, enhancing the thermal resistance, tensile mechanical properties, and dielectric properties of the KSPI. This study established a robust preparation method for high-performance polyimide composites and elucidated how interface compatibility regulates polyimide composite performance employing combined theoretical analysis and experimental validation. Highlights γ-aminopropyl triethoxysilane enhances silica and polyimide compatibility. Interface regulation simultaneously improves polyimide mechanical properties. Molecular simulations revealing correlations between interface and performance. The modified composite exhibits higher thermal stability and lower dielectric loss.
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