CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Chanjuan Yang,Shoukang Xiao,Liyu Chen,Yingwei Li,Kui Shen
γ-Valerolactone (GVL) as an important high-value chemical can be readily produced through the catalytic hydrogenation of renewable levulinic acid (LA). However, high reaction temperatures (70–240 ℃) and H 2 pressures (0.5–6 MPa) are usually required to achieve full LA conversion and desired GVL yield in previous studies. Herein, we report, for the first time, the ambient-condition upgrading of LA to GVL by rationally constructing a series of metallic–acidic Ru x Pt y /MIL-101 catalysts comprising RuPt-alloyed nanoparticles (NPs) and Lewis-acid sites within a chromium-based MOF (namely MIL-101). Benefiting from the favorable synergy between Ru and Pt in their alloyed NPs and abundant Lewis-acid sites in MIL-101, the best Ru 4 Pt 1 /MIL-101 featuring an optimized Ru/Pt molar ratio of 4:1 shows a complete LA conversion with > 99.9 % yield of GVL under unprecedented ambient temperature and pressure, affording a high turnover frequency (TOF) of 1480.5h −1 , which is 15.1 and 10.1 times that of its monometallic Pt/MIL-101 (98.3 h −1 ) and Ru/MIL-101 (146.7 h −1 ) counterparts, respectively. Detailed experiments and density functional theory (DFT) calculations suggest the RuPt-alloyed effect and Lewis-acid sites in Ru 4 Pt 1 /MIL-101 can optimize the adsorption energy of 4-hydroxyvaleric acid (HPA) to remarkably boosting its catalytic performance for this reaction.
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Chemistry-An Asian Journal
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2025
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IF 3.3
Xiaoqing Jia,Yingfeng Wei,Xinyuan Zhang,Qiuping Gu,Youshun Liu,Shige Wang,Chunping Zhu
A dual-drug-loaded γ-polyglutamic acid (γ-PGA) hydrogel was synthesized, integrating third-generation dendrimers (G3) as cross-linkers for the simultaneous encapsulation of hydrophilic doxorubicin (DOX) and hydrophobic camptothecin (CPT). This hydrogel, formed via an efficient EDC/NHS-mediated reaction, demonstrated a biocompatible, porous, and pH-responsive network. The hydrophobic core of G3 significantly enhanced CPT loading, while γ-PGA facilitated effective DOX incorporation. Controlled drug release was observed, with DOX releasing faster in acidic tumor-like environments, optimizing therapeutic impact at the tumor site. In vitro studies highlighted the hydrogel's high biocompatibility and synergistic anticancer efficacy, reducing CT26 colon cancer cell viability more effectively than single-drug systems. In vivo experiments confirmed substantial tumor suppression, prolonged survival, and the absence of systemic toxicity in murine models. These results underscore the potential of this dual-drug delivery platform as a robust, multifunctional system for cancer therapy. The biocompatibility, degradability, and tailored drug release characteristics make this hydrogel a promising candidate for clinical translation, offering a novel solution for enhancing cancer treatment efficacy while minimizing side effects.
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FOOD RESEARCH INTERNATIONAL
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2025
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IF 8
Kangyu Zhao,Mengfei Xie,Xin Long,Ping Lan,Zizhe Cai,Yong Wang
The Maillard reaction during the foods processing and hot-pressed oils period generates potential antioxidant compounds that, along with endogenous antioxidants, enhance oxidation stability of oil. This study specifically investigated the interaction between 1-(1 H -imidazole [4,5-C]pyridine-4-yl) ethenone (IMPE), a Maillard reaction product (MRP) isolated from a fructose-histidine system, and γ-tocopherol, the primary endogenous antioxidant in flaxseed oil. The results revealed a significant synergistic antioxidant effect between IMPE and γ-tocopherol. Accelerated oxidation tests (Schaal oven, Rancimat analyses) demonstrated that IMPE/γ-tocopherol mixture exhibited an extended oxidation induction period (7.84 h), substantially exceeding the additive effect expected from IMPE (4.12 h) and γ-tocopherol (5.01 h) individually, resulting in a synergistic degree (SD) of 1.25. Furthermore, density functional theory (DFT) calculations at the B3LYP/6–311+G(d,p) level revealed that the primary mechanism underlying this synergy is the regeneration of γ-tocopherol by IMPE, a finding corroborated by experimental degradation assays. These results elucidate a molecular mechanism for MRP-endogenous antioxidant interactions and provide valuable insights for designing effective composite antioxidant systems, particularly for enhancing the stability of hot-pressed oils.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Xiao Chen,Nannan Zhang,Huaming Wang,Ying Zhong,Tianming Lv,Changhai Liang
The continuous flow selective hydrogenation of maleic anhydride (MA) to γ-butyrolactone (GBL) over highly efficient and long-term stable catalysts is a considerable promising strategy for both lab-scale as well as industrial application. In this work, a PtPdCoNiCu/TiO 2 high-entropy alloy (HEA) catalyst is developed by the colloidal impregnation method, in which the HEA colloids are synthesized by lithium naphthalenide-driven reduction at mild conditions according to the redox potential of the various metals. The PtPdCoNiCu/TiO 2 catalyst exhibits highly efficient in the hydrogenation of MA with 91 % selectivity to GBL at full conversion of MA under the weighted hourly space velocity of 1.14 h −1 , 3 MPa H 2 , and 260 °C. Due to the present of oxygen vacancy in the TiO 2 support and the hydrogen spillover, the PtPdCoNiCu/TiO 2 HEA catalyst presents a low apparent activation energy (75 kJ mol −1 ), boosting the hydrogenolysis of C=O bonds for generating of GBL. The cocktail effect is presented in the PtPdCoNiCu/TiO 2 catalyst, and its catalytic activity is much better than that of corresponding monometallic and bimetallic catalysts. It realizes the reduction and substitution of precious metal catalysts. In addition, the PtPdCoNiCu/TiO 2 catalyst with sintering resistance and acid resistance shows excellent long-term stability within 132 h. This work is of great significance for understanding HEA catalysis at the atomic level and provides the possibility for developing low-cost and efficient precious metal industrial catalysts.
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Journal of Water Process Engineering
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2025
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IF 6.7
Bo Tian,Wenze Li,Jianwei Zhang,Jinfeng Li,Na Zhou,Wa Gao,Nan Zhang,Hongtao Zhao
With the advancement of nuclear energy, the recovery and reuse of uranium pose extremely challenging tasks. This paper commences by toughening polyacrylamide (PAM) with nanorubber polybutadiene (PB) through the radiation-induced graft polymerization (RIGP) method, and diaminomaleonitrile (DAMN) is introduced and amidoximated, giving rise to a three-dimensional network hydrogel named as bis-amidoxime (AO) -based three-dimensional hydrogel uranium adsorbent based on nano-rubber toughening (PAM/PB/DAMN-AO). This hydrogel not only retains the favorable hydrophilicity and chemical stability of PAM but also experiences a significant enhancement in mechanical properties due to the addition of nanorubber PB. In the tests of 10 cyclic compressions (with a strain of ε = 80 %), the compressive strength remains nearly unchanged, indicating a stable structure. During the amidoximation reaction and uranium-adsorption process, the pore structure of the hydrogel has been modified, evolving into a structure more conducive to uranium adsorption. In a 100 ppm uranium solution, the adsorption capacity reaches 154.4 mg·g −1 . The kinetic and isotherm models are evaluated, and the adsorption process is found to be more consistent with the pseudo-second-order kinetic model ( R 2 = 0.992) and the Langmuir adsorption isotherm model ( R 2 = 0.997). It exhibits high selectivity in the presence of competing ions and can still maintain an adsorption efficiency of over 90 % after 4 adsorption-desorption cycles, demonstrating excellent recyclability. The prepared hydrogel has a high adsorption capacity for uranyl ions and rapid adsorption kinetics, showing potential application prospects in the fields of nuclear wastewater treatment and uranium resource recovery.
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CONSTRUCTION AND BUILDING MATERIALS
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2025
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IF 8
Rong Pengjie,Tang Pei,Chen Wei
The effects of different ammonium salts (ammonium carbonate, diammonium hydrogen phosphate, ammonium sulfate, and ammonium chloride) on the carbonation mineralization performance of γ-C 2 S were investigated. Various analytical techniques were employed to characterize the mechanical properties, carbonation product compositions, morphology and pore structure of the hardened matrix. The results indicate that the performance of the hardened matrix after carbonation curing is closely related to the mineralization degree, the types of formed products, and the calcium carbonate structure. The introduction of ammonium salts altered the carbonation products and microstructure of the materials, reducing the Q 4 /Q 3 content of the silica gel and modifying the formation of vaterite, particularly in the systems containing ammonium sulfate, diammonium hydrogen phosphate, and ammonium carbonate. These changes consequently affected the pore structure. Among the different salts, the use of a 2 mol/L ammonium chloride solution showed the most significant improvement in the performance of the hardened material. Compared to the control group, the compressive strength and carbonation degree increased by 42.04 % and 7.33 %, respectively. This enhancement was primarily attributed to the increased calcium carbonate content, which reduced harmful pores and led to a more regular and stable structure of calcite particles. This study identifies key factors influencing the performance changes of γ-C 2 S-based carbonated materials under different ammonium salt dosages, providing new possibilities for the development of high-performance carbon-cured cementitious materials.
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Acta Pharmaceutica Sinica B
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2025
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IF 14.6
Qian Jing,Mengnan Zhao,Yan Tang,Tao Chen,Mingyan Sun,Dandan Mi,Lan Zou,Rujing Wang,Jun Lu,Sanjun Shi
Interference with calcium homeostasis provokes tumor cell death and immune response, providing a novel direction for tumor immunotherapy as a promising cancer treatment strategy. Nevertheless, most reported Ca 2+ -overloaded nanoinducers encounter challenges such as intricate preparation procedures, safety concerns arising from inorganic material input, and limited anti-tumor efficiency. Herein, we synthesized a biocompatible and pH-sensitive Ca-doped cyclodextrin metal-organic framework (Ca/K-MOF) as a carrier, which was then loaded with photosensitizer hypericin (HY) via a simple one-pot synthesis to form HY@Ca/K-MOF. To enhance the stability both in vitro and in vivo , we coated HY@Ca/K-MOF with a hydrophilic layer of PEG ( PEG HY@Ca/K-MOF). When exposed to 590 nm photoirradiation, PEG HY@Ca/K-MOF, with its pH-responsive dissociation, the Ca 2+ and HY mediators released at the tumor site share the responsibility of triggering intracellular Ca 2+ disturbances, which amplified the production of reactive oxygen species (ROS) and led to mitochondrial calcium overload through modulating mitochondrial MICU1 function. Under photocontrol, this interplay between ROS generation and mitochondrial calcium overload created a bidirectional amplification effect, where each process reinforced the other, subsequently eliciting a pyroptosis-evoked immune response. Significantly, this newly constructed delivery platform effectively suppressed both primary and distant tumors without the need for additional immunological interventions. In summary, this Ca 2+ -doped MOF-based nanomaterial provides a promising approach for efficient tumor photo-controlled mitochondrial Ca 2+ overload-pyroptosis immunotherapy.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2024
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IF 5.4
Xiaowei Ding,Xuerong Luo,Imran Mahmood Khan,Lin Yue,Yin Zhang,Zhouping Wang
Geraniol (Ger) is an essential oil molecule with excellent biological activity. High hydrophobicity and volatility limit its practical application. Cyclodextrins (CDs) are water-soluble cyclic oligosaccharides with hydrophobic cavities. Physical encapsulation of CDs to improve the solubility and stability of essential oil molecules is not satisfactory. Therefore, this study synthesized the γ-CD derivative (γ-CD-Ger) by grafting Ger onto γ-CD using a bromide-mediated method. Compared to the inclusion complexes (γ-CD/Ger) formed by both, the derivatives exhibit better solubility and thermal stability. The derivative has better antibacterial activity when the ratio of γ-CD to Ger was 1:2. In addition, the derivatives did not exhibit cytotoxic and hemolytic properties. These results indicate that this research provides a water-soluble antibacterial agent with a wide range of promising applications and offers new ideas for the application of alcohol hydrophobic molecules in aqueous systems.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Tingting Ma,Yijia Guan,Yanru Zhang,Jinlun Feng,Yue Yang,Junying Chen,Wenjie Guo,Jianguo Liao
Magnesium oxychloride cement (MOC) has the advantage of high early strength. However, it has the defect of poor water resistance. Considering this performance, we use γ-polyglutamic acid (γ-PGA) and chitosan (CS) to modify MOC. The effects of γ-PGA and CS such as strength, in vitro degradation and in vitro bioactivity of MOC were studied. Based on the preparation of γ-PGA and CS modified MOC (γ-PGA/CS-MOC) composite bone cement, the strontium ranelate (SrR) was loaded on. The results showed that the softening coefficient of γ-PGA/3 wt.% CS-MOC after soaking in SBF for 28 d reached 0.48, while that of control group (without CS and γ-PGA) was only 0.35; Cell experiments indicated that SrR could promote differentiation into osteoblasts. After the γ-PGA/CS-MOC composite bone cement containing SrR was implanted into the osteoporotic bone defect for 12 w, it was found that the material was gradually absorbed and the new bone tissue grew. The results showed that SrR/γ-PGA/CS-MOC composite bone cement had a potential application prospect in the repair of osteoporotic bone defects.
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ACS Nano
·
2025
·
IF 16
Jingjing Cao,Wenji Zhan,Meng Ren,Yao Wang,Haifei Wang,Ni Zhang,Yuetian Chen,Tianfu Wang,Yanfeng Miao,Yixin Zhao
The application of promising perovskite light-emitting diodes (PeLEDs) faces a significant challenge known as efficiency roll-off, which refers to the decline in external quantum efficiency (EQE) at high current densities. This issue arises mainly from high trap densities in perovskite films and imbalanced carrier injection, which limit improvements in brightness and stability of PeLEDs. Here, we develop a green solvent strategy using γ-valerolactone (GVL) to suppress efficiency roll-off in PeLEDs. This strategy effectively slows down the crystallization kinetics, yielding cubic-phase formamidinium lead triiodide (α-FAPbI3) films with reduced trap states, enhanced charge carrier injection, and suppressed Auger recombination. As a result, we achieve a record radiance of 1411 W sr–1 m–2 for GVL-based PeLEDs. These PeLEDs exhibit a substantially reduced efficiency roll-off, maintaining an EQE above 20% even at a high current density of 900 mA cm–2. Our findings highlight the potential of the green solvent approach for developing high-brightness, high-efficiency PeLEDs for practical applications.
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ACTA PHARMACOLOGICA SINICA
·
2024
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IF 6.9
Hu You-tian,Liu Zhi-wei,Zhang Tong-hui,Ma Yu-e,He Lei,Zhang Jie,Zhou Yue-yang,Vidal-Puig Antonio,Pan De-jing,Wu Fang
Thymic egress is a crucial process for thymocyte maturation, strictly regulated by sphingosine-1-phosphate lyase (S1PL). Recently, cystathionine γ-lyase (CSE), one of the enzymes producing hydrogen sulfide (H 2 S), has emerged as a vital immune process regulator. However, the molecular connection between CSE, H 2 S and thymic egress remains largely unexplored. In this study, we investigated the regulatory function of CSE in the thymic egress of immune cells. We showed that genetic knockout of CSE or pharmacological inhibition by CSE enzyme inhibitor NSC4056 or D , L -propargylglycine (PAG) significantly enhanced the migration of mature lymphocytes and monocytes from the thymus to the peripheral blood, and this redistribution effect could be reversed by treatment with NaHS, an exogenous donor of H 2 S. In addition, the CSE-generated H 2 S significantly increased the levels of S1P in the peripheral blood, thymus and spleen of mice, suppressed the production of proinflammatory cytokines and rescued pathogen-induced sepsis in cells and in vivo. Notably, H 2 S or polysulfide inhibited S1PL activity in cells and an in vitro purified enzyme assay. We found that this inhibition relied on a newly identified C 203 XC 205 redox motif adjacent to the enzyme’s active site, shedding light on the biochemical mechanism of S1PL regulation. In conclusion, this study uncovers a new function and mechanism for CSE-derived H 2 S in thymic egress and provides a potential drug target for treating S1P-related immune diseases.
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RADIATION PHYSICS AND CHEMISTRY
·
2025
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IF 3.3
Jinfeng Li,Nan Zhang,Qianwen Wang,Jianwei Zhang,Bo Tian,Zhigang Li,Haifeng Gu,Hongtao Zhao
The research for highly removal of uranium from nuclear waste is of significance for radionuclide remediation and environment. Herein, a robust pyrazolate-based metal-organic framework (NiBTP) is prepared by γ-irradiation through complexation between 1,3,5-tris(1H-pyrazol-4-yl) benzene (H 3 BTP) and Nickel (II) and presents efficient U(VI) adsorption performance. The synthesized NiBTP is characterized by XRD, FTIR, SEM, TEM, XPS and N 2 adsorption–desorption isotherm analysis. Structural characterizations demonstrate that NiBTP prepared by γ-irradiation possesses decreased BET surface area with hierarchical pore structure, but also has excellent crystallinity and high chemical stability. Batch experiments reveal that NiBTP adsorbent displays high adsorption capacity of uranium and excellent selectivity for UO 2 2+ ion in the presence of competing K + , Cs + , Sr + , Co 2+ , Mg 2+ , Ca 2+ , La 3+ and Eu 3+ ions. Thermodynamic investigation shows the adsorption process is endothermic and spontaneous. In addition, the adsorption mechanism of UO 2 2+ ion onto NiBTP is attributed to the hierarchical pore architecture as well as complexation. This study presents a simpler and more efficient alternative method for the preparation of pyrazolate MOFs and highlights the power of robust pyrazolate MOFs in sequestrations of radioactive pollutants from water environment.
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