Nature Communications
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2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Liu Meihuan,Su Hui,Liu Xuanzhi,He Xiaorong,Tan Pengfei,Liu Feng,Pan Jun
The interfacial electron interactions in heterogeneous catalysts are critical in determining the adsorption strengths and configurations of reaction intermediates, which are essential for the efficiency of multistep tandem catalytic processes. Amorphous-crystalline (a-c) heterostructures have garnered significant interest due to their unusual atomic arrangements, adaptable electron configurations, and exceptional stability. Here, we introduce a mesoporous a-c heterojunction catalyst featuring enriched amorphous-crystalline Ni(OH) 2 /Pt boundaries (ac-Ni(OH) 2 @m-Pt), designed for efficient acidic oxygen reduction reaction (ORR). This catalyst enables electron redistribution at the heterogeneous interface, thereby enhancing both catalytic activity and durability. As anticipated, the ac-Ni(OH) 2 @m-Pt delivers a high mass activity (MA) of 0.95 A mg Pt − 1 and maintains good durability (89.8% MA retention) over 15000 cycles. Advanced characterization and theoretical calculations reveal that the catalyst’s high performance stems from the dynamic heterogeneous-interface electron redistribution at the a-c interface. This dynamic-cycling electron transfer, driven by the applied potential, promotes O 2 activation and accelerates the protonation of *O intermediate during ORR. This work offers a promising avenue for improving the design of electrocatalysts using a-c interface engineering.
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Journal of Orofacial Orthopedics-Fortschritte der Kieferorthopadie
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2024
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IF 1.3
Pang Huiqi,Ding Luhua,Che Xiaoxia
Purpose We aimed to investigate early effects of regulating alpha‑7 nicotinic acetylcholine receptor (α7nAChR) agonists and antagonists on maxillary expansion in mice. Methods We allocated 36 six-week-old male C57BL/6J mice into three group: 1) expansion alone, 2) expansion plus the α7nAChR-specific agonist 3‑(2,4-dimethoxybenzylidene)-anabaseine dihydrochloride (GTS-21), and 3) expansion plus alpha-bungarotoxin (α-BTX), a competitive antagonist of α7nAChR. The groups were daily injected with saline, GTS-21 (4 mg/kg/day) or α‑BTX (1 mg/kg/day), respectively, from days 0–7. In addition, a mouse model of maxillary expansion was established. Masson’s trichrome staining was used to observe morphological changes and immunohistochemistry was performed to analyze α7nAChR, interleukin (IL)-1β, IL‑6, tumor necrosis factor (TNF)-α, runt-related transcription factor 2 (RUNX2), and osteocalcin (OCN) expression in the midpalatal suture. Microcomputed tomography was used to measure midpalatal suture and palatal basal bone widths. We assessed the normal distribution of our data using the Kolmogorov–Smirnoff test and evaluated the homogeneity of variance by Levene’s test, followed by a two-way ANOVA and Bonferroni tests at a significance level of P < 0.05. Results In the GTS-21+expansion group, osteogenesis was more active in the middle palatine suture. New bone was calcified and deposited in the suture and we observed decreased IL-1β, IL‑6, and TNF‑α expression ( P < 0.05). In the α‑BTX+expansion group, we observed increased proinflammatory cytokine and decreased RUNX2 and OCN expression and increased midpalatal suture and palatal basal bone widths ( P < 0.05). Conclusion Using α7nAChR agonists and antagonists to regulate the cholinergic anti-inflammatory pathway, the secretion of inflammatory factors and osteoblast markers during maxillary expansion were altered, indicating the potential for clinical modulation of maxillary palatal suture expansion.
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CELLULOSE
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2024
·Vol. 31
·期 10
·6141-6153
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IF 4.9
Song Jun,Wang Linfeng,Shan Jicheng,Li Chuanmeng,Wang Mengdie
Cellulose liquid crystal solutions have been extensively studied, and the methylene length of mesogenic units has a significant influence on the properties of cellulose liquid crystal solutions. In this study, 4-(ω-(methylimidazole)alkyloxy)-4’-(cyano)-biphenyl (CBP-n) with 4–7 methylene lengths were synthesized as mesogenic units to prepare cellulose side chain liquid crystal in 1-Allyl-3-methylimidazolium chloride (AMIMCl). And their liquid crystal properties were studied by differential scanning calorimetry (DSC), in-situ infrared spectrometer (IR), torque rheometer, and polarizing microscope (POM). The results showed that CBP-n with 4–7 methylene lengths were thermotropic liquid crystal, and the cellulose/CBP-n/AMIMCl solutions were lyotropic liquid crystal when the concentration of cellulose is 6wt% and the concentration of CBP-n with methylene length 4 and 6 is 3wt%. In-situ IR proved that the liquid crystal formation of cellulose/CBP-n/AMIMCl solution was caused by the hydrogen bonding formed between cellulose and CBP-n. And the solutions have a fewer entanglement number and lower viscosity than those of methylene length 5 and 7, indicating that the hydrogen bonding interaction between CBP-n with even methylene length and cellulose molecule is stronger than that of odd methylene length. This study provides a new approach to produce cellulose fibers using cellulose/CBP-n/AMIMCl as a new renewable resource.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2024
·Vol. 35
·期 11
·1-8
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IF 2.8
Liu Juan,Liu Bing,Song Kai Xin
The effects of cold sintering assisted two-step sintering on the structural evolution and microwave dielectric properties of Al 2 O 3 ceramics are systematically investigated in this work. XRD analysis reveals that the crystal structure remains stable throughout the cold sintering and following high-temperature sintering processes. Rietveld refinement confirms the trigonal Al 2 O 3 configuration and the absence of impurities. Increasing cold sintering pressure results in improved relative density, reaching over 94% after post-sintering at 1575 °C. Additionally, the sintering temperature of Al 2 O 3 ceramics via cold-sintering assisted two-step sintering route is 100 °C lower than that via direct conventional sintering. The microwave dielectric properties, including ε r and Qf , exhibit enhancements with increasing cold sintering pressure and post-sintering temperature. The measured ε r closely aligns with the theoretical value, indicating a successful densification. Qf achieves its peak of 100,220 GHz at 1575 °C under 375 MPa, nearly 2 times higher than the value obtained at 125 MPa (53,280 GHz). The optimal microwave dielectric properties ( ε r = 9.67, Qf = 100,220 GHz, and τ f = − 54.5 ppm/°C) are achieved at a cold sintering pressure of 375 MPa and post sintering temperature of 1575 °C.
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Journal of Inorganic and Organometallic Polymers and Materials
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2025
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IF 4.9
Bao Xuemei,Yang Yongcong,Zhao Tianjing,Liu Song,Zhou Wenyao,Liu Qianqian,Yu Fengjiao,Yang Yang
A modified polysulfone (PSF) ultrafiltration (UF) membrane is designed by grafting phytic acid/silver ion (PA-Ag I ) complex aggregates on the membrane surface for achieving improved separation and anti-biofouling performance. We demonstrate that PA molecules directly grafted on the PSF membrane surface through hydrogen bonding offer a suitable coordinating ability to immobilize Ag ions to form hydrophilic aggregates. One-cycle sequential assembly reinforced by a high concentration of PA is confirmed optimal for generating a compact grafting layer with better water affinity and properly narrowing the pore aperture. This modification results in a reasonable permeation flux (313.3 L m –2 h –1 bar –1 ), a high BSA rejection (93.2%) and a good antifouling property. Moreover, the PA-Ag I /PSF membrane displays excellent antibacterial and anti-adhesion properties against E. coli and B. subtilis , attributed to the gradual release of Ag ions from the moderately stable PA-Ag I complexes in a favorable aqueous environment. The PA-Ag I /PSF membrane keeps over 83% of water flux after incubation of bacteria culture for 48 h, presenting outperforming anti-biofouling durability. The low dosage of Ag ions from the PA-Ag I /PSF membrane has merits of low consumption, optimization of release profile, and alleviated environmental concerns.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ren Yuqi,Fu Yiwei,Li Naixu,You Changjun,Huang Jie,Huang Kai,Sun Zhenkun,Zhou Jiancheng,Si Yitao,Zhu Yuanhao,Chen Wenshuai,Duan Lunbo,Liu Maochang
H 2 O dissociation plays a crucial role in solar-driven catalytic CO 2 methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO 2 catalyst with single-atom Ni anchored around its surface V o sites by replacing Ce atoms to promote H 2 O dissociation and achieve effective photothermal CO 2 reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH 4 production and prevents V o from depletion. The defects coordinated with single-atom Ni, significantly promote the capture of charges and local phonons at the Ni d -impurity orbitals, thereby inducing more effective H 2 O activation. The catalyst presents a CH 4 yield of 192.75 µmol/cm 2 /h, with a solar-to-chemical efficiency of 1.14% and a selectivity ~100%. The mechanistic insights uncovered in this study should help further the development of H 2 O-activating catalysts for CO 2 reduction and thereby expedite the practical utilization of solar-to-chemical technologies.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Zhang Zhen,Xing Zhenyu,Luo Xianglin,Cheng Chong,Liu Xikui
Dual-atom catalysts featuring synergetic dinuclear active sites, have the potential of breaking the linear scaling relationship of the well-established single-atom catalysts for oxygen reduction reaction; however, the design of dual-atom catalysts with rationalized local microenvironment for high activity and selectivity remains a great challenge. Here we design a bisalphen ladder polymer with well-defined densely populated binuclear cobalt sites on Ketjenblack substrates. The strong electron coupling effect between the fully-conjugated ladder structure and carbon substrates enhances the electron transfer between the cobalt center and oxygen intermediates, inducing the low-to-high spin transition for the 3 d electron of Co(II). In situ techniques and theoretical calculations reveal the dynamic evolution of Co 2 N 4 O 2 active sites and reaction intermediates. In alkaline conditions, the catalyst exhibits impressive oxygen reduction reaction activity featuring an onset potential of 1.10 V and a half-wave potential of 1.00 V, insignificant decay after 30,000 cycles, pushing the overpotential boundaries of ORR electrocatalysis to a low level. This work provides a platform for designing efficient dual-atom catalysts with well-defined coordination and electronic structures in energy conversion technologies.
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INTERNATIONAL JOURNAL OF THERMOPHYSICS
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2025
·Vol. 46
·期 3
·1-20
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IF 2.9
Jin Guofan,Shi Jianrong,Wang Xiaopo
Both polyoxymethylene dimethyl ethers (OME n ) and biodiesel are considered as promising alternatives or additives to traditional fuels. The addition of OMEs to biodiesel can realize complementary advantages. The physical properties of OME n , biodiesel, or OME n /biodiesel blends are decisive for the performance of internal combustion engines. In this work, density and viscosity of mixtures of OME n with three typical components of biodiesel (methyl decanoate, methyl dodecanoate, and methyl tetradecanoate) were measured from 303.15 K to 333.15 K at atmospheric pressure. The vibrating-tube method and capillary-tube method were used for the present density and viscosity measurement, respectively. The combined relative uncertainty is 0.1% for density and 1.5% for viscosity ( k = 2). The experimental results were fitted by Jouyban-Acree model and McAllister model. Moreover, the excess properties of each mixture including excess molar volume and viscosity deviations were discussed.
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Nature Chemistry
·
2025
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IF 20.2
Wen Ping,Huang Hanwei,Zhang Ruizhe,Zheng Hanqi,Liang Tingxizi,Zhuang Chuyue,Wu Qing,Wang Junxia,Liu Feng,Zhang Ke,Wu Wei,He Kaixin,Liu Funan,Li Hongjun,Gu Zhen
Vesicles play critical roles in cellular materials storage and signal transportation, even in the formation of organelles and cells. Natural vesicles are composed of a lipid layer that forms a membrane for the enclosure of substances inside. Here we report a coacervate vesicle formed by the liquid–liquid phase separation of cholesterol-modified DNA and histones. Unlike a phospholipid-based membrane-bounded vesicle, a coacervate vesicle lacks a membrane structure on the surface and is organized with a high-density liquid layer and a water-filled cavity. Through a straightforward coacervation process, we demonstrate that various biological agents, including virus particles, mRNA, cytokines and peptides, can be innocuously and directly enriched in the liquid phase. In contrast to the droplet-like coacervates that are prone to aggregation challenges, coacervate vesicles display superior kinetic stability, positioning them as a versatile delivery vehicle for biopharmaceuticals. We validate that incorporating oncolytic viruses into these coacervate vesicles endows them with potent oncolytic efficacy and elicits robust anti-tumour immune responses in mouse models.
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JOURNAL OF POROUS MATERIALS
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2024
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IF 2.5
Liang Ni,Wang Haiyan,Wang Yujia,Kang Lei,Bai Yingzhi,Sun Na
A strategy was devised for the synthesis of SAPO-34, which involved a concentrated gel system-assisted two-step crystallization method. This strategy effectively controlled the size and morphology of SAPO-34. The successful synthesis of SAPO-34 crystals with micron-scale cubic morphology and nano-scale sheets were achieved using triethylamine as a low-cost template. The paper thoroughly examined the growth evolution that occurs during the crystallization process, and it delved into the factors such as gel concentration and crystallization conditions in the synthesis. Furthermore, potential theories regarding nucleation and growth mechanisms were suggested. A systematic study was conducted to examine how the morphology and acidity of SAPO-34 zeolites impact their catalytic performance. The results confirmed that the SAPO-34 with low silicon content and lamellar structure was successfully synthesized through a two-step crystallization within a gel system of H 2 O/Al 2 O 3 = 30, with a thickness of approximately 50–300 nm. SAPO-34 nanosheets demonstrated a substantial enhancement in catalytic performance, with a catalytic life of 370 min and an 84.1% selectivity towards light olefins.
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CATALYSIS LETTERS
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2024
·
IF 2.3
Zhao Xiao-Ting,Li Wen-Dian,Tao Fei-Yan,Wang Na
Pictet-Spengler reaction is one of the main ways to synthesize spiroindolones, which widely exists in natural products and pharmaceutical agents. We accidentally discovered bovine serum albumin (BSA) had catalytic activity for Pictet-Spengler reaction previously. After a series of exploratory experiments around the catalytic process, it was found that some amino acids played a key role. It is worth noting that, Pictet-Spengler reaction catalyzed by amino acids has been rarely described. Herein, we report the cysteine-catalyzed Pictet-Spengler reaction between tryptamine and isatin under metal-free and convenient conditions. The catalytic performance of amino acid was optimized through screening reaction conditions such as time, temperature, solvent, molar ratio and catalyst amount and a series of spiroindolones can be obtained in moderate to excellent yields. The present investigation featured relatively mild reaction conditions with good functional group tolerance and provided an alternative method for preparation of spiroindolones. Graphical Abstract
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CELLULAR AND MOLECULAR LIFE SCIENCES
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2024
·Vol. 81
·期 1
·1-17
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IF 6.2
Li Long,Liu Huimin,Chai Quanyou,Wei Junyi,Qin Yuqiao,Yang Jingyao,Liu He,Qi Jia,Guo Chunling,Lu Zhaoyang
Vascular calcification is a complication that is frequently encountered in patients affected by atherosclerosis, diabetes, and chronic kidney disease (CKD), and that is characterized by the osteogenic transdifferentiation of vascular smooth muscle cells (VSMCs). At present, there remains a pressing lack of any effective therapies that can treat this condition. The sodium-glucose transporter 2 (SGLT2) inhibitor dapagliflozin (DAPA) has shown beneficial effects in cardiovascular disease. The role of this inhibitor in the context of vascular calcification, however, remains largely uncharacterized. Our findings revealed that DAPA treatment was sufficient to alleviate in vitro and in vivo osteogenic transdifferentiation and vascular calcification. Interestingly, our study demonstrated that DAPA exerts its anti-calcification effects on VSMCs by directly targeting SGLT2, with the overexpression of SGLT2 being sufficient to attenuate these beneficial effects. DAPA was also able to limit the glucose levels and NAD + /NADH ratio in calcified VSMCs, upregulating sirtuin 1 (SIRT1) in a caloric restriction (CR)-dependent manner. The SIRT1-specific siRNA and the SIRT1 inhibitor EX527 attenuated the anti-calcification effects of DAPA treatment. DAPA was also to drive SIRT1-mediated deacetylation and consequent degradation of hypoxia-inducible factor-1α (HIF-1α). The use of cobalt chloride and proteasome inhibitor MG132 to preserve HIF-1α stability mitigated the anti-calcification activity of DAPA. These analyses revealed that the DAPA/SGLT2/SIRT1 axis may therefore represent a viable novel approach to treating vascular calcification, offering new insights into how SGLT2 inhibitors may help prevent and treat vascular calcification. Graphical abstract Dapagliflozin attenuated vascular smooth muscle cells osteogenic transdifferentiation and vascular calcification through the SIRT1-mediated deacetylation and degradation of HIF-1α in a manner dependent on caloric restriction.
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