JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 38
·e55968
·
IF 2.7
Meili Li,Xiancheng Meng,Zaizai Tong
Poly( L -lactic acid) (PLLA), as a green, biodegradable polymer material, has garnered considerable attention due to its ease of processing and exceptional properties. However, the inherent slow crystallization rate and brittleness of PLLA substantially restrict its extensive applications across various domains. In present work, PLLA and poly( D -lactide) (PDLA)-modified cellulose nanocrystals (CNCs), referred as CNC- g -L and CNC- g -D, are serving as nano-fillers to enhance the crystallization rate of PLLA. Our findings demonstrate that both nano-fillers could enhance the crystallization rate of PLLA, but the CNC- g -D shows a more efficient nucleation agent compared with its counterpart, CNC- g -L. Isothermal crystallization analysis indicates that CNC- g -D substantially increases nucleation density of PLLA, with pronounced crystallization at an elevated temperature of 155°C as confirmed by differential scanning calorimetry (DSC) and polarized optical microscopy (POM). Wide-angle x-ray diffraction (WAXD) analysis shows the preformation of stereocomplex crystals on the CNC- g -D surface may result in a fast crystallization rate. Meanwhile, after incorporation of different nano-fillers, the toughness property of PLLA has also been significantly enhanced. Our result has shown the CNC- g -D could serve as an efficient nucleation agent toward PLLA and also facilitate to aiding in establishing comprehensive structure–property relationships of polymer materials.
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Cell Death & Disease
·
2025
·Vol. 16
·期 1
·1-11
·
IF 9.6
Chu Xiufeng,Zhang Ting,Bukhari Ihtisham,Hu Mei,Xu Jixuan,Xing Yamin,Liang Xinfeng,Zhang Zisen,Zheng Pengyuan
Gasdermin D (GSDMD) is a critical pyroptosis mediator, consisting of one N-terminal pore-forming domain and one C-terminal auto-inhibitory domain. The free N-terminal domain (GD-NT), which is released through caspase-1/11 cleavage, exhibits distinct features from the full-length GSDMD (GD-FL), including oligomerization, membrane translocation, and pore-formation. However, the underlying mechanisms are not well elucidated. Here, we found that GD-NT, but not GD-FL, was massively ubiquitinated in cells. The K63-linked polyubiquitination of GD-NT at Lys236/237 (human/mouse), catalyzed by TRAF1, directly prompted its membrane translocation and pore-formation during pyroptosis. Inhibition of GD-NT ubiquitination via site-directed mutations or the UBA1 inhibitor PYR-41 suppressed cell death in several pyroptosis cell models. Additionally, applying PYR-41 in septic mice efficiently suppressed the release of IL-18 and TNFα. Thus, GD-NT ubiquitination is a key regulatory mechanism controlling its membrane localization and activation, which may provide a novel target for modulating immune activity in pyroptosis-related diseases.
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IMMUNITY
·
2025
·
IF 26.3
Qianzhou Yu,Danlu Jiang,Tianming Zhao,Yuelin Guan,Jian Zhang,Dehang Yang,Ruya Sun,Weiwei Yu,Zhen Wang,Sheng Chen,Mobai Li,Tianyi Hu,Qiqi Deng,Xiaoyang Lu,Yidong Yang,Mengfei Chang,Liheng Du,Xue Zhang,Zhexu Chi,Di Wang
The small intestine (SI) absorbs nutrients and acts as a barrier against pathogens. Diet enables the absorptive function of the SI while maintaining immune homeostasis. But how the SI transmits nutritional signals to the immune response and adapts to dietary intake remains unclear. Here, we demonstrated that epithelial gasdermin D (GSDMD) in the SI facilitated the absorptive function of enterocytes, subsequently empowering an epithelial-immune cooperation to modulate host defense. Unlike its pyroptotic function, GSDMD determines the absorptive versus the defensive zonation of enterocytes and promotes brush border assembly. This diet-induced, GSDMD-mediated adaptation promoted lipid absorption and subsequently rewired enterocyte metabolism to support intraepithelial γδ T lymphocytes (γδ T-IELs), thereby enhancing barrier function. Impairment of this GSDMD-mediated circuit exacerbated barrier-dysfunction-associated enteritis. Our results reveal how epithelial cells and lymphocytes co-adapt to nutrient signals in the SI, thereby adjusting the equilibrium between nutrient uptake and host defense in response to environmental change.
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Biology-Basel
·
2025
·Vol. 14
·期 3
·226
·
IF 3.5
Zonghan Jiang,Leisheng Sun,Yuanyuan Li,Haoyu Li,Yu Fu,Jiyun Li,Zhiliang Sun
Simple SummaryEscherichia coliis a ubiquitous pathogen, with certain strains causing severe diarrhea and intestinal illnesses, which pose significant health risks to both children and animals. As antimicrobial resistance continues to rise, traditional antibiotics are increasingly ineffective, highlighting the urgent need for novel therapeutic strategies. In this study, we investigated the antimicrobial peptide D-CONGA-Q7, aiming to evaluate its efficacy and underlying mechanism against drug-resistantE. colistrains. Our results demonstrate that D-CONGA-Q7 effectively disrupts bacterial cell membranes, leading to bacterial death, and exhibits comparable activity against polymyxin- and meropenem-resistant strains. In vivo experiments revealed that D-CONGA-Q7 significantly alleviated intestinal inflammation, reduced inflammatory cytokine levels, and promoted the repair of damaged intestinal tissues. Furthermore, D-CONGA-Q7 displayed good stability. These findings suggest that D-CONGA-Q7 not only represents a promising new approach to combat drug-resistant bacterial infections but also holds potential for clinical application.Escherichia coli(E. coli) is a zoonotic bacterium widespread in the environment, highly transmissible, and responsible for significant economic losses and millions of cases of illness annually. The rise of multidrug-resistant (MDR) strains has rendered last-line antibiotics such as polymyxin and meropenem ineffective, making the development of new antibiotics urgent. Although D-CONGA-Q7 has broad-spectrum bactericidal activity, its underlying mechanism remains poorly understood. In this study, we used in vitro and in vivo experiments to demonstrate that D-CONGA-Q7 effectively kills both antibiotic-sensitive and multidrug-resistant strains ofE. coli. D-CONGA-Q7 disrupts the cell membranes of Gram-negative bacteria, and the treatment ofE. colistrainLN175with D-CONGA-Q7 resulted in a significant up-regulation of theMlacgene, suggesting that D-CONGA-Q7 may interact with phospholipids in the cell membrane. Furthermore, in treatingK88-induced bacterial enteritis in the small intestine, D-CONGA-Q7 significantly reduced intestinal inflammation. In conclusion, this study provides a novel approach to combat drug-resistantE. coli.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Meilan Xue,Xuehan Zhang,Yifan Zhou,Jiayi Yan,Haiqi Gao,Yixian Bai,Jing Shi,Yuhan Liu,Yan Xu,Nan Zhang,Lu Li,Shaobo Shi,Hui Liang
This study was aimed to reveal the neuroprotective effect of sulfated fucooligosaccharides (FOS) in an aging mouse model induced by d-galactose. The results showed that FOS treatment ameliorated inflammation, improved behavioral decline in memory and cognition, and exerted neuroprotective effects. FOS reduced microglia activation by decreasing the expression of P38 mitogen-activated protein kinase (P38 MAPK), cyclic-AMP response binding protein (CREB), cyclooxygenase-2 (COX-2), and prostaglandin E2 (PGE2). In addition, FOS improved intestinal mucosal barrier damage and reduced the release of lipopolysaccharide. FOS increased the diversity of the gut flora and promoted a significant enrichment of the Akkermansia genus. FOS also increased the butyric acid level and reduced the expression of histone deacetylase 3 (HDAC3), Toll-like receptor 4 (TLR4), and nuclear factor kappa-B (NF-κB). Fecal microbiota transplantation from the FOS-treated mice showed a similar effect to FOS treatment in inhibiting neuroinflammation and reduced d-galactose-induced cognitive dysfunction. The results suggested that FOS supplementation ameliorated d-galactose-induced neuron damage and exerted neuroprotective effects through the gut–brain axis.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Liu Hong-Zhi,Shu Xiao-Xuan,Huang Mingjie,Wu Bing-Bing,Chen Jie-Jie,Wang Xi-Sheng,Li Hui-Lin,Yu Han-Qing
Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d -band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding strength for peroxymonosulfate through d -band center modulation. A 100% polymerization transfer ratio is achieved by lowering the d -band center. This work presents a paradigm to dynamically modulate the electronic structure of high-valent metal-oxo species and optimize pollutant removal from wastewater via polymerization.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Shaorou Ke,Yajing Zhao,Xin Min,Xinyu Zhu,Xin Li,Bozhi Yang,Fan Yang,Xiaowen Wu,Ruiyu Mi,Yangai Liu,Zhaohui Huang,Minghao Fang
Platinum-based bimetallic catalysts exhibit superior hydrogen evolution reaction performance compared to single platinum catalysts. Most studies on platinum bimetallic catalysts have focused on changing the metals used, with not much attention on how the d-band theory affects the catalyst's performance. Herein, we investigated the additional of different transition metals alters the d-band center for better hydrogen evolution. A method combining the ultrasound processing and in-situ reduction was designed, resulting in the alloys with different stacking orders. As the d-band of transition metal elements in the alloy shifts upwards, the lower the energy of the alloy's d-band center, the better the stability of the adsorption bonding exhibited by the alloy. The PtCu/C, with a hexagonal-close-packed structure and a d-band center at −1.823 eV, has an 84 mV overpotential at 100 mA cm −2 , lower than PtNi/C (89 mV) and PtCo/C (91 mV). It also has 4.75 times the mass activity of commercial Pt/C. As a cathode catalyst, PtCu/C provides improved water-splitting at 2.31 V vs. 2.55 V for commercial Pt/C (at 1 A cm −2 ). This analytical strategy through the d-band center advances the design of platinum-based bimetallic catalysts and offers a new direction for the optimization and development of hydrogen evolution reaction electrocatalysts.
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CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Detao Li,Zichen Ning,Feiqiang He,Zhi Gao,Limin Zhou,Li Xu,Zhijian Zheng,Jerry Heng,Shichao Du,Jinbo Ouyang
To enable efficient separation of chiral drugs and enhance their practical utility, this study investigates cocrystallization as a novel separation and purification strategy. Using R/S-mandelic acid and d/l-prolinamide as model compounds, we screened potential cocrystal/salt coformers and successfully synthesized seven novel chiral salts. The proton transfer was elucidated by analyzing molecular electrostatic potential differences at the hydrogen-bonding sites. Moreover, the formation mechanism of salts was explored through structural analyses, such as Hirshfeld surface calculations, energy framework assessments, and crystal void analysis. Considering the distinct properties of various chiral salts, we conducted competitive cocrystallization experiments, establishing a complementary chiral pairing principle that provides a theoretical foundation for cocrystallization-based chiral resolution. Based on these findings, we developed multiple processes for the separation of R- and S-mandelic acid as well as l- and d-prolinamide, achieving product purities exceeding 80%, which strongly demonstrate the feasibility of cocrystallization separation technology for chiral resolution. This work not only introduces a groundbreaking approach to chiral separation but also highlights the vast potential of cocrystallization technology in pharmaceutical purification and beyond.
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ACS Catalysis
·
2024
·
IF 11.3
Ruilin Liu,Chao Wang,Yong Yan,Ruzhi Wang,Ge Chen
The direct hydrogen peroxide (H2O2) product from H2 and O2 is a promising anthraquinone replacement because it is environmentally friendly and has a high atom efficiency. Experimental and theoretical studies have proven that optimizing the adsorption of the critical intermediate OOH* on the metal site significantly promotes the further protonation of this intermediate and inhibits the O–O bond cleavage, thus enhancing the activity and selectivity. Redistributing the charge density of active sites to tuning the d-band center of the metal could effectively modulate the intermediates adsorption, and thus regulate the catalytic efficiency. Herein, we show that a Lewis acid (ZnCl2 solution) induces abundant oxygen vacancies (Ovs) on the TiO2 surface, which results in a reversal of charge transfer from TiO2–Ov support to the Pd atom, generating an electron-rich Pd configuration. Compared with pristine Pd/TiO2, Pd/TiO2–Ov possesses higher H2O2 selectivity and productivity, with values of 80.7% and 186 mol kgcat–1 h–1, respectively. In addition, Pd/TiO2–Ov maintains stability during the six cycles reaction due to its high resistance to the leaching of Pd species. Theoretical calculations reveal that the reversed charge transfer downshifts the d-band center of Pd, which promotes O2 adsorption on the Pd surface and weakens the OOH* intermediates adsorption. Thus, the energy barrier for the hydrogenation of the OOH* intermediate is significantly decreased, and the O–O band cleavage is inhibited. This study reports a reversal of charge transfer tuning the d-band center of the active site for efficient direct H2O2 synthesis, which may provide insight for designing high-performance catalysts.
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PHYTOMEDICINE
·
2025
·
IF 8.3
Guifang Fan,Xiaojiaoyang Li,Fanghong Li,Ranyun Chen,Xiaoyong Xue,Le Wang,Qi Zheng,Shuni Duan,Ranyi Luo,Rong Sun,Runping Liu
Background : Radix Bupleuri (RB) and acetaminophen (APAP) are two popular medications having potential hepatotoxicity and substantial risks of irrational co-administration and excessive use, posing an overlooked danger of drug-induced liver injury (DILI). Autophagy is a protective mechanism against APAP-induced DILI, yet, saikosaponin d (SSd) in RB has been characterized to regulate autophagy, although the current findings are controversial. Purpose : We aim to elucidate whether SSd promoted APAP-induced liver injury by regulating autophagy. Methods : UPLC-MS analysis was employed to measure the hepatic abundance of APAP-cysteine protein adducts. Multiple techniques such as fluorescence probe, proteinase K protection assay, immunoprecipitation-coupled proteomic analysis, surface plasmon resonance, molecular docking and et.al were applied to evaluate the SSd on autophagy flux. Results : We discovered that, by inhibiting autophagy, SSd impaired the removal of APAP-cysteine protein adducts and delayed the compensation of damaged mitochondria. This ultimately potentiated the development of severe liver toxicity induced by subtoxic APAP. The use of autophagy probes, transmission electron microscopy, membrane curative assay, and protein K assay collectively revealed that SSd predominately disrupted autophagosome-lysosome fusion, without affecting other stages of autophagic flux. Immunoprecipitation-coupled proteomic analysis and surface plasmon resonance further found that SSd directly bound to GABARAP, thus preventing the recruitment and autoactivation of STX17 and the following assembly of STX17-SNAP29-VAMP8 complex. Conclusion : In conclusion, our findings not only highlight the significant risk of drug-induced liver injury associated with the co-administration of RB and APAP in clinical practice but also unveils that GABARAP-SNARE complex is a novel druggable target for the treatment of autophagy-related diseases.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Mubalake Rehemaitijiang,Gaosheng Li,Rongchao Zhu,Baiyi Zu,Xincun Dou,Zhi Su,Zhenzhen Cai
The rational design of the D-π-A chemodosimeter with a significant Stokes shift is of great importance for enhancing the visualization of optical sensing signals. Here, three D-π-A fluorescent chemodosimeters with 2-(3-cyano-4,5,5-trimethylfuran-2(5H)-ylidene) malononitrile (TCF) as the electron-withdrawing group are synthesized by precisely modulating the electron-releasing strength. By decreasing the ability of electron release, the electrophilicity of the recognition site is increased by 1.449 kcal/mol, the Stokes shift of the chemodosimeter is improved to 201 nm, and the sensing mode changes from fluorescence quenching to ratiometric fluorescence and finally to fluorescence on. Furthermore, the three D-π-A fluorescent chemodosimeters display superior sensing performance toward ClO–, including low limits of detection (LOD, 37.0, 5.1, and 1.0 nM), rapid response (<5 s), and great selectivity in the presence of 16 kinds of interferents. Moreover, the practicality of the chemodosimeters is further validated by a portable triple-standard quantitative array detection platform, which can quantitatively detect ClO– solutions. The proposed design and modulation strategy for chemodosimeters can provide a new pathway for the sensitive and visualized identification of oxidants and other hazardous chemicals.
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Polymers
·
2020
·Vol. 12
·期 9
·2053
·
IF 3.426
Chen Qi,Wenke Yang,Fuyan He,Jinshui Yao
Eight kinds of chiral diacid monomers were prepared with amino acids with different side groups or configurations. Polyester-imides (PEIs) were synthesized from these diacid monomers and diphenol monomers through polycondensation reaction, and the performances and properties were compared with the chiral polyamide-imides (PAIs) previously synthesized by our work group. Their thermal properties were analyzed by thermo gravimetric analysis (TGA) and dynamic thermomechanical analysis (DMA), and it was found that the glass transition temperature (Tg) of PEI was mainly affected by the volume of side groups. Their degradability was studied through buffer degradation experiments, and the changes in their water contact angle, molecular weight, structure and appearance during the degradation process were characterized by contact angle tester, gel permeation chromatography (GPC), Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). With degradation, the hydrophilicity of PEI was improved, and when amino acids with larger side groups or D configuration were introduced into the backbone of PEI, the degradability decreased.Keywords:chiral amino acids;polyester-imides (PEIs);degradation;thermal property
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