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Novel sustainable carbon dot as dual replacements for emulsion stabilizers and Photoinitiators in macroporous polymerized high internal phase emulsion fabrication 新型可持续碳点在大孔聚合高内相乳液制备中作为乳液稳定剂和光引发剂的双重替代品。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-05 DOI: 10.1016/j.jcis.2026.139838
Woming Gao , Zeming Cheng , Nicholas T.H. Farr , Cornelia Rodenburg , Frederik Claeyssens
Both emulsion stabilizers and photoinitiators are essential components in preparing photocurable water-in-oil (w/o) Polymerized High Internal Phase Emulsions (PolyHIPEs). Conventional stabilizers like Hypermer B246 and photoinitiators like 2,4,6-Trimethylbenzoyldiphenylphosphine oxide (TPO) pose environmental and biological hazards, requiring careful removal before use in bioengineering applications. Furthermore, PolyHIPEs prepared with traditional surfactants often feature narrow pores and pore throats, limiting effective fluid and cell infiltration. As a class of easy-synthesizing and biocompatible nanoparticles, carbon dots (CDs) exhibit potential for use as emulsion stabilizers and photoinitiators. Herein, novel amphiphilic carbon dots (GW CDs) were synthesised from Gromwell root waste, a byproduct of shikonin extraction, as sustainable alternative. GW CDs demonstrated excellent emulsion-stabilizing ability, effective photoinitiating performance and superior biocompatibility. GW CDs were employed to stabilize the emulsions and successfully crosslink them under UV light to fabricate 2-ethylhexyl acrylate (EHA)- isobornyl acrylate (IBOA)- trimethylolpropane triacrylate (TMPTA) PolyHIPEs. The pore size and pore throat formation of the resulting PolyHIPEs could be effectively tuned by adjusting the GW CDs content. Compared to PolyHIPEs prepared using Hypermer B246 and TPO, the GW CD-stabilized counterparts exhibited significantly larger pore sizes and pore throats, improving fluid and cell permeability for tissue engineering applications. Additionally, GW CDs possess upconversion luminescence, pH sensitivity, and cell-imaging capabilities, further highlighting their potential in biomedical engineering and environmental science applications.
乳液稳定剂和光引发剂是制备光固化油包水(w/o)聚合高内相乳液(PolyHIPEs)的重要组成部分。传统的稳定剂如Hypermer B246和光引发剂如2,4,6-三甲基苯甲酰二苯基氧化膦(TPO)会对环境和生物造成危害,在生物工程应用中使用前需要仔细去除。此外,用传统表面活性剂制备的PolyHIPEs通常具有狭窄的孔隙和孔喉,限制了流体和细胞的有效渗透。碳点作为一类易于合成且具有生物相容性的纳米颗粒,在乳状液稳定剂和光引发剂方面具有潜在的应用前景。本文以紫草素提取的副产物葛伦韦根废料为原料,合成了新型两亲性碳点(GW CDs)。GW CDs具有优异的乳液稳定性能、有效的光引发性能和良好的生物相容性。利用GW CDs稳定乳液,并在紫外光下成功交联制备了2-乙基丙烯酸己酯(EHA)-丙烯酸异鸟酯(IBOA)-三甲基丙烷三丙烯酸酯(TMPTA) PolyHIPEs。通过调整GW CDs的含量,可以有效地调节PolyHIPEs的孔径和孔喉形成。与使用Hypermer B246和TPO制备的PolyHIPEs相比,GW cd稳定的对应物具有更大的孔径和孔喉,提高了流体和细胞的渗透性,可用于组织工程。此外,GW CDs具有上转换发光,pH敏感性和细胞成像能力,进一步突出了其在生物医学工程和环境科学应用中的潜力。
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引用次数: 0
Robust self-healing superhydrophobic coating for anti-icing 坚固的自修复超疏水涂层,用于防冰
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-05 DOI: 10.1016/j.jcis.2026.139836
Yutao Wang, Yuechang Lian, Mingxuan Zhang, Shengyuan Zhao, Yuhang Li, Shengyang Tao, Wendong Liu
Superhydrophobic surfaces are prone to structural damage and degradation of low-surface-energy substances, which significantly affects their long-term stability and performance in anti-/de-icing applications. Inspired by the self-recovery capability of lotus leaves, a migration of low-surface-energy substance-mediated self-healing superhydrophobic coating was fabricated by spraying a mixture of silicone nanofilaments (Si NFs), liquid paraffin-loaded hollow silica microspheres (LP/H-MPs), trimethoxy (1H, 1H, 2H, 2H-heptadecafluorodecyl) silane (TMHFDS), and epoxy resin (E51). The coating demonstrated significant robustness, achieving a hardness of 2H and outstanding superhydrophobicity, characterized by a water contact angle (CA) exceeding 161° and a sliding angle (SA) below 2°. The preserved liquid paraffin also endowed the hybrid coating with a self-healing ability. Consequently, when the surface is mechanically damaged or chemically degraded, the superhydrophobicity can rapidly recover upon heating at 200 °C, and the self-healing is repeatable. After nine cycles of O2 plasma etching and self-healing, the coating maintained its liquid repellency, with a significant CA exceeding 164°. When exposed to a cold, high-humidity atmosphere, the self-healing superhydrophobic coating significantly delayed ice formation to 1105 s, enabling frost prevention. The synergistic effects of its robustness, superhydrophobicity, and self-healing properties indicate that the as-prepared self-healing superhydrophobic coating has great potential in wind power generation, transportation, and other fields.
超疏水表面容易受到低表面能物质的结构破坏和降解,这严重影响了其在防冰/除冰应用中的长期稳定性和性能。受荷叶自修复能力的启发,通过喷涂有机硅纳米丝(Si NFs)、液体石蜡负载的中空二氧化硅微球(LP/H-MPs)、三甲氧基(1H, 1H, 2H, 2H-十六氟癸基)硅烷(TMHFDS)和环氧树脂(E51)的混合物,制备了低表面能物质介导的自修复超疏水涂层。该涂层具有显著的鲁棒性,硬度达到2H,具有优异的超疏水性,其水接触角(CA)超过161°,滑动角(SA)低于2°。保存的液体石蜡也使混合涂层具有自愈能力。因此,当表面受到机械损伤或化学降解时,在200℃加热后超疏水性可以迅速恢复,并且自我修复是可重复的。经过9个O2等离子体刻蚀和自愈循环后,涂层保持了良好的拒水性,CA显著超过164°。当暴露在寒冷、高湿度的大气中时,自修复的超疏水涂层显着将冰的形成延迟到1105秒,从而实现防霜。其鲁棒性、超疏水性和自愈性的协同效应表明,制备的自愈性超疏水涂层在风力发电、交通运输等领域具有巨大的应用潜力。
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引用次数: 0
Spatial localization immobilization of metals and enzymes at Pickering emulsion droplet interfaces for chemo-enzymatic cascade catalysis 化学-酶级联催化中金属和酶在Pickering乳剂液滴界面的空间定位固定化。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-05 DOI: 10.1016/j.jcis.2026.139840
Geling Kuang , Jinchao Hou , Zichen Wang , Lixue Zhao , Yuxiao Feng , Hongwu Wang , Jiandong Cui
Developing chemo-enzymatic cascade catalysis in catalytic asymmetric synthesis is of utmost significance, but such processes often suffer from low reaction efficiency because of incompatible reaction environments and suppressed intermediate transportation. Herein, a novel compartmentalised metal–enzyme microcapsule nanohybrid, Candida antarctica lipase B@Pd(II)-loaded hydrophobic mesoporous silica nanoparticles (CALB@Pd(II)/HB-MSNs), was fabricated by spatially localizing Pd(II) active sites and CALB at the outer and inner interfacial layers of Pickering emulsion droplets, respectively. Benefiting from the localization of two catalysts in their preferred reaction microenvironments, nanoscale proximity of each other, and interfacial activation of lipase, the CALB@Pd(II)/HB-MSNs exhibited 60-fold higher activity than traditional random co-immobilized metal-enzyme catalysts (Pd(II)/HB-MSNs/CALB). Furthermore, the conversion of rac-1-phenylethanol catalyzed by CALB@Pd(II)/HB-MSNs reached 47.92 %, compared to only 4 % for the randomly co-immobilized catalyst Pd(II)/HB-MSNs/CALB, with a product enantiomeric excess of≥99 % in the cascade reaction of 4-pentynoic acid cycloisomerisation and racemic 1-phenylethanol chiral resolution. Our study offers a platform for the design of efficient chemoenzymatic catalytic cascades for the synthesis of fine chemicals.
在催化不对称合成中发展化学-酶级联催化具有重要意义,但由于反应环境不相容和中间体运输受到抑制,导致反应效率低。本文通过将Pd(II)活性位点和CALB分别定位于Pickering乳剂液滴的内外界面层,制备了一种新型的区隔化金属-酶微胶囊纳米复合物,即负载南极假丝酵母脂肪酶B@Pd(II)的疏水介孔二氧化硅纳米颗粒(CALB@Pd(II)/HB-MSNs)。得益于两种催化剂在其首选反应微环境中的定位,彼此的纳米级接近以及脂肪酶的界面激活,CALB@Pd(II)/HB-MSNs的活性比传统随机共固定化金属-酶催化剂(Pd(II)/HB-MSNs/CALB)高60倍。此外,CALB@Pd(II)/HB-MSNs催化的racc -1-苯乙醇的转化率达到47.92%,而随机共固定催化剂Pd(II)/HB-MSNs/CALB的转化率仅为4%,在4-戊酸环异构化和外消旋1-苯乙醇手性分解的级联反应中,产物对映体过量≥99%。我们的研究为设计用于精细化学品合成的高效化学酶催化级联提供了一个平台。
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引用次数: 0
A unique scandium oxide-doped cobalt oxide nanosheet array for coupling hydrogen evolution with catalytic conversion of polyethylene terephthalate into formate 一种独特的氧化钪掺杂氧化钴纳米片阵列,用于耦合析氢和催化聚对苯二甲酸乙酯转化为甲酸酯。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-04 DOI: 10.1016/j.jcis.2026.139831
Huiling Lu , Min Liu , E. Namila , Xin Liu , Menghe Baiyin
Upgrading polyethylene terephthalate (PET) plastic waste into value-added chemicals through electrocatalysis is an effective way to alleviate environmental pollution and the energy crisis. Herein, we developed a unique scandium oxide-doped cobalt oxide nanosheet array loaded on foam nickel ((ScCo)Ox/NF), which synergistically promotes both the hydrogen evolution reaction (HER) and the ethylene glycol oxidation reaction (EGOR), thereby enabling the integrated production of green H2 and upgrading of plastic waste. Benefiting from the unique interfacial effects, the cathodic (ScCo)Ox/NF catalyst achieves a current density of 10 mA cm−2 at an overpotential as low as 79 mV. The anodic (ScCo)Ox/NF catalyst exhibited an electrode potential of 1.23 V (vs. RHE) at a current density of 10 mA cm−2. Under the condition of applying an electric potential of 1.5 V, the Faradaic efficiency of formate production reached 92.8 %. Density functional theory (DFT) calculations highlight the synergistic interaction between Sc2O3 and Co3O4, which effectively lowers the reaction barrier and thereby enhances the catalytic activity in EGOR. This study successfully developed a novel bifunctional catalyst through the strategic design of doping scandium into cobalt oxide, offering a green and sustainable approach for the high-value conversion of PET.
利用电催化技术将聚对苯二甲酸乙二醇酯(PET)塑料废弃物转化为增值化学品是缓解环境污染和能源危机的有效途径。在此,我们开发了一种独特的氧化钪掺杂氧化钴纳米片阵列,负载在泡沫镍((ScCo)Ox/NF)上,协同促进析氢反应(HER)和乙二醇氧化反应(EGOR),从而实现绿色H2的综合生产和塑料废物的升级。得益于独特的界面效应,阴极(ScCo)Ox/NF催化剂在过电位低至79 mV时实现了10 mA cm-2的电流密度。阳极(ScCo)Ox/NF催化剂在电流密度为10 mA cm-2时的电极电位为1.23 V (vs. RHE)。在施加1.5 V电势的条件下,甲酸酯的法拉第效率达到92.8%。密度泛函理论(DFT)计算强调了Sc2O3和Co3O4之间的协同作用,有效地降低了反应势垒,从而提高了EGOR中的催化活性。本研究通过战略性设计将钪掺杂到氧化钴中,成功开发出一种新型双功能催化剂,为PET的高价值转化提供了绿色可持续的途径。
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引用次数: 0
A density functional theory-driven multifunctional design of metal-organic framework decorated glass fiber filters for efficient air purification 密度功能理论驱动的金属有机框架装饰玻璃纤维过滤器的多功能设计,用于高效空气净化
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-04 DOI: 10.1016/j.jcis.2026.139833
Chen Chen , Shijun Xing , Junjie Yu , Keneshbekova Aruzhan , Shaowei Wang , A.V. Rogachev , Urol K. Makhmanov , Wenping Li , Jiazhi Yang , Xiaohong Jiang
Advanced air filtration systems have attracted significant attention due to their high efficiency, broad application scope and long-term reliability in removing air pollutants. Density functional theory (DFT) has played a crucial role in exploring the removal mechanisms for air pollutants at the atomic level, thereby enabling the rational optimization of material properties to enhance air filters performance. Herein, a multifunctional air filter (GF/CS/ZIF-8) featuring a three-dimensional interconnected network was rationally fabricated by integrating glass fiber (GF), chitosan (CS), and zeolitic imidazolate framework-8 (ZIF-8), guided by DFT simulations. The resulting composite exhibits outstanding particulate matter (PM) removal performance, achieving an efficiency of 99.56 ± 0.41 % for PM0.3, along with a high-quality factor of 0.037 ± 0.0011 Pa−1 under optimized composition (50 % GF content and 7.38 wt% ZIF-8 loading). The strong interfacial binding between CS and ZIF-8, as quantitatively confirmed by DFT calculations, underpins remarkable stability. The filter maintained high performance (98.42 ± 0.026 % for PM0.3 removal efficiency and a pressure drop of 156.7 ± 1.24 Pa) during 12 h continuous filtration, with no observable shedding of ZIF-8. In addition, the composite demonstrates exceptional volatile organic compounds (VOCs) adsorption capability, with removal efficiencies exceeding 94 %. DFT simulations further verified the feasibility of VOCs desorption, confirming the regeneration potential of the filter. Importantly, by exploiting the pH-responsive behavior of ZIF-8, the composite exhibits selective and robust antibacterial activity while maintaining excellent biosafety. Overall, the as-prepared air filter combines high PM removal efficiency, excellent VOCs adsorption capacity and superior antibacterial activity, providing a promising strategy for efficient air purification systems.
先进的空气过滤系统以其高效、广泛的应用范围和长期可靠的去除空气污染物而备受关注。密度泛函理论(DFT)在探索空气污染物在原子水平上的去除机制方面发挥了至关重要的作用,从而使材料性能的合理优化能够提高空气过滤器的性能。在DFT模拟的指导下,将玻璃纤维(GF)、壳聚糖(CS)和沸石咪唑酸骨架-8 (ZIF-8)有机结合,合理制备了具有三维互联网络的多功能空气过滤器(GF/CS/ZIF-8)。所得到的复合材料具有出色的颗粒物(PM)去除性能,在优化的成分(GF含量为50%,ZIF-8负载为7.38 wt%)下,PM0.3的去除效率为99.56±0.41%,高质量因子为0.037±0.0011 Pa−1。DFT计算定量证实,CS和ZIF-8之间的强界面结合支撑了显著的稳定性。在连续过滤12 h的过程中,过滤器保持了良好的性能(PM0.3去除率为98.42±0.026%,压降为156.7±1.24 Pa), ZIF-8无明显脱落。此外,该复合材料具有优异的挥发性有机化合物(VOCs)吸附能力,去除效率超过94%。DFT模拟进一步验证了VOCs解吸的可行性,证实了过滤器的再生潜力。重要的是,通过利用ZIF-8的ph响应行为,复合材料具有选择性和强大的抗菌活性,同时保持良好的生物安全性。总体而言,制备的空气过滤器结合了高PM去除效率,优异的VOCs吸附能力和优异的抗菌活性,为高效空气净化系统提供了一个有前途的策略。
{"title":"A density functional theory-driven multifunctional design of metal-organic framework decorated glass fiber filters for efficient air purification","authors":"Chen Chen ,&nbsp;Shijun Xing ,&nbsp;Junjie Yu ,&nbsp;Keneshbekova Aruzhan ,&nbsp;Shaowei Wang ,&nbsp;A.V. Rogachev ,&nbsp;Urol K. Makhmanov ,&nbsp;Wenping Li ,&nbsp;Jiazhi Yang ,&nbsp;Xiaohong Jiang","doi":"10.1016/j.jcis.2026.139833","DOIUrl":"10.1016/j.jcis.2026.139833","url":null,"abstract":"<div><div>Advanced air filtration systems have attracted significant attention due to their high efficiency, broad application scope and long-term reliability in removing air pollutants. Density functional theory (DFT) has played a crucial role in exploring the removal mechanisms for air pollutants at the atomic level, thereby enabling the rational optimization of material properties to enhance air filters performance. Herein, a multifunctional air filter (GF/CS/ZIF-8) featuring a three-dimensional interconnected network was rationally fabricated by integrating glass fiber (GF), chitosan (CS), and zeolitic imidazolate framework-8 (ZIF-8), guided by DFT simulations. The resulting composite exhibits outstanding particulate matter (PM) removal performance, achieving an efficiency of 99.56 ± 0.41 % for PM<sub>0.3,</sub> along with a high-quality factor of 0.037 ± 0.0011 Pa<sup>−1</sup> under optimized composition (50 % GF content and 7.38 wt% ZIF-8 loading). The strong interfacial binding between CS and ZIF-8, as quantitatively confirmed by DFT calculations, underpins remarkable stability. The filter maintained high performance (98.42 ± 0.026 % for PM<sub>0.3</sub> removal efficiency and a pressure drop of 156.7 ± 1.24 Pa) during 12 h continuous filtration, with no observable shedding of ZIF-8. In addition, the composite demonstrates exceptional volatile organic compounds (VOCs) adsorption capability, with removal efficiencies exceeding 94 %. DFT simulations further verified the feasibility of VOCs desorption, confirming the regeneration potential of the filter. Importantly, by exploiting the pH-responsive behavior of ZIF-8, the composite exhibits selective and robust antibacterial activity while maintaining excellent biosafety. Overall, the as-prepared air filter combines high PM removal efficiency, excellent VOCs adsorption capacity and superior antibacterial activity, providing a promising strategy for efficient air purification systems.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"708 ","pages":"Article 139833"},"PeriodicalIF":9.7,"publicationDate":"2026-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145922896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the dual mechanisms of lattice distortion and electron transfer in alkaline-earth doped FeCoNiHPO4 for enhanced oxygen evolution reaction: experimental insights and density functional theory simulations 揭示碱土掺杂FeCoNiHPO4中晶格畸变和电子转移的双重机制:实验见解和密度泛函理论模拟
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-04 DOI: 10.1016/j.jcis.2026.139832
Linxiong Tan , Rui Xu , HuanHuan Li , Tao Wang , Ning Ma , Lengyuan Niu , Yinyan Gong , Can Li
Alkaline-earth elements possess atomic radii and electronegativities that differ significantly from those of Fe, Co, and Ni, thereby inducing substantial modulation of the catalytic properties in FeCoNi-based catalysts. In this study, a series of alkaline-earth (Ca, Mg and/or Ba) doped (FeCoNi)HPO4 samples are synthesized, and their oxygen evolution reaction (OER) electrocatalytic performance is investigated via experimental characterizations and theoretical calculations. Results reveal that dopant-induced lattice distortion and electron redistribution effectively modulate the local coordination environment and electronic structure of Fe, Co and Ni sites. By regulating the nature and concentration of dopants, the optimized S-FeCoNi-Ca1.0 sample exhibits outstanding OER performance, achieving overpotentials of only 218/273 mV at current densities of 10/100 mA/cm2. Concurrently, it displays favorable reaction kinetics, with a Tafel slope of 52 mV dec−1 and a low charge-transfer resistance of 2.31 Ω. Notably, the catalyst maintains excellent operational stability and achieves a turnover frequency 2.2 times higher than that of the undoped material. These findings offer valuable insights into the rational design of cost-effective, high-performance FeCoNi-based electrocatalysts through the strategic incorporation of alkaline-earth elements for advanced energy conversion applications.
碱土元素的原子半径和电负性与Fe、Co和Ni的原子半径和电负性有很大的不同,从而诱导了基于fecni的催化剂的催化性能的实质性调节。本研究合成了一系列碱土(Ca, Mg和/或Ba)掺杂的(FeCoNi)HPO4样品,并通过实验表征和理论计算研究了它们的析氧反应(OER)电催化性能。结果表明,掺杂剂诱导的晶格畸变和电子重分布有效地调节了Fe、Co和Ni位点的局部配位环境和电子结构。通过调节掺杂剂的性质和浓度,优化后的S-FeCoNi-Ca1.0样品表现出出色的OER性能,在电流密度为10/100 mA/cm2时,过电位仅为218/273 mV。同时,它表现出良好的反应动力学,塔菲尔斜率为52 mV dec−1,电荷转移电阻为2.31 Ω。值得注意的是,该催化剂保持了良好的运行稳定性,周转频率是未掺杂材料的2.2倍。这些发现为合理设计具有成本效益的高性能feconi电催化剂提供了有价值的见解,通过战略性地结合碱土元素用于先进的能量转换应用。
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引用次数: 0
A smartphone-integrated electrochemical biosensor based on engineered laccase-mimicking nanozymes for epinephrine detection in metabolic stress 基于工程漆酶模拟纳米酶的智能手机集成电化学生物传感器用于代谢应激中肾上腺素的检测
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-04 DOI: 10.1016/j.jcis.2025.139817
Sivaguru Jayaraman , Thenmozhi Rajarathinam , Jinyong Park , Duwon Jung , Amir Humayun , Prabakar Kandasamy , Jang-Hee Yoon , Jaewon Lee , Seung-Cheol Chang
A highly sensitive and selective electrochemical biosensor was developed based on Cu- and O-vacancy–engineered, laccase-mimicking mesoporous carbon (MC) nanozymes for epinephrine (EP) detection. N-doped MC was synthesized via a hydrothermal method, followed by immobilization of CuZn bimetallic nanoparticles through wet impregnation, and the resulting Cu–Zn–MC composite was drop-cast onto a disposable electrode strip. The N functionalities, dispersed Cu and Zn atoms, and Cu and O vacancies emulated the Cu active sites and CuN coordination environment of laccase enzyme. The porous Cu–Zn–MC nanozymes facilitate adsorption, electron transfer, and oxidation of EP to adrenochrome, which is measurable by differential pulse voltammetry. The biosensor exhibited a well-defined oxidation peak at +0.195 V (vs. Ag/AgCl), with the detection limit of 10 nM, and rapid detection capability when interfaced with a smartphone-operated miniaturized potentiostat. The enhanced electrochemical performance was attributed to accelerated electron hopping mediated by Cu centers and dual semiconducting pathways, involving p-type CuO behavior induced by Cu vacancies and n-type ZnO conductivity associated with O vacancies. Practical feasibility was confirmed through EP analysis in ex-vivo tissues from a metabolic stress-induced mouse model, yielding satisfactory recoveries (91.9–102.2 %) and high precision (RSD < 5.6 %).
基于Cu-和o -空位工程,模拟漆酶的介孔碳纳米酶(MC)开发了一种高灵敏度和选择性的肾上腺素(EP)电化学生物传感器。采用水热法合成n掺杂MC,湿浸渍法固定CuZn双金属纳米颗粒,将所得Cu-Zn-MC复合材料滴铸在一次性电极条上。N官能团、分散的Cu和Zn原子以及Cu和O空位模拟了漆酶酶的Cu活性位点和Cu配位环境。多孔Cu-Zn-MC纳米酶促进EP的吸附、电子转移和氧化成肾上腺素色素,这可以用差分脉冲伏安法测量。该生物传感器在+0.195 V (vs. Ag/AgCl)下表现出清晰的氧化峰,检测限为10 nM,与智能手机操作的微型恒电位器接口时具有快速检测能力。电化学性能的增强归因于Cu中心介导的加速电子跳变和双半导体途径,包括Cu空位诱导的p型CuO行为和O空位相关的n型ZnO电导率。通过代谢应激诱导小鼠模型离体组织的EP分析,证实了该方法的可行性,回收率(91.9 - 102.2%)令人满意,精密度(RSD < 5.6%)较高。
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引用次数: 0
A carrier-free nanomedicine targeting vascular remodeling and oxidative stress for enhanced pulmonary arterial hypertension therapy 一种靶向血管重构和氧化应激的无载体纳米药物用于增强肺动脉高压治疗
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-03 DOI: 10.1016/j.jcis.2025.139821
Jingjing Zhou , Yicheng Yang , Huiyu Zou , Xiaolian Jiang , Wuming Wu , Wenjie Yan , Songren Shu , Qiaoxi Yang , Peizhi Wang , Zhiling Luo , Yihua He , Changming Xiong , Chunyan Deng
Pulmonary arterial hypertension (PAH) is a life-threatening disease characterized by progressive pulmonary vascular remodeling and inflammation. Current therapies primarily focus on vasodilation and short-term symptom management, with limited efficacy in reversing vascular remodeling, suppressing oxidative stress, or modulating immune-inflammatory responses. To address this, we developed epigallocatechin gallate/manganese dioxide core-shell nanoparticles (EM NPs) as a carrier-free nanomedicine for PAH therapy, designed to simultaneously target key pathological processes for synergistic therapeutic effects. Our results demonstrated that EM NPs effectively scavenged reactive oxygen species, protected pulmonary artery smooth muscle cells (PASMCs) from oxidative damage, considerably improved hemodynamic parameters (reduced right ventricular systolic pressure (RVSP), mean pulmonary arterial pressure (mPAP), and right ventricular hypertrophy index (RVHI)), and attenuated pulmonary vascular remodeling without inducing hepatorenal toxicity. Concurrently, EM NPs markedly modulated inflammatory responses, indicated by the suppression of key pro-inflammatory mediators (CC Motif Chemokine Ligand 5 (CCL5), macrophage inflammatory protein-3 alpha (MIP-3α), monocyte chemoattractant protein-1 (MCP-1), interleukin (IL)-18 and the elevation of anti-inflammatory cytokines (IL-4, IL-13). Furthermore, the core-shell structure significantly enhanced the stability and bioavailability of natural polyphenol, thereby improving its in vivo therapeutic efficacy. Analysis of RNA sequencing data indicated that EM NPs suppressed immune activation in lung tissues by downregulating key pro-inflammatory genes and pathways. With their ability to concurrently target oxidative stress, vascular remodeling, and inflammation in PAH, EM NPs emerge as a promising nanotherapeutic candidate, demonstrating considerable clinical translation potential.
肺动脉高压(PAH)是一种以进行性肺血管重构和炎症为特征的危及生命的疾病。目前的治疗主要集中在血管舒张和短期症状管理,在逆转血管重构、抑制氧化应激或调节免疫炎症反应方面疗效有限。为了解决这个问题,我们开发了表没食子儿茶素没食子酸酯/二氧化锰核壳纳米颗粒(EM NPs)作为一种无载体纳米药物用于治疗PAH,旨在同时靶向关键病理过程以实现协同治疗效果。我们的研究结果表明,EM NPs有效地清除活性氧,保护肺动脉平滑肌细胞(PASMCs)免受氧化损伤,显著改善血流动力学参数(降低右心室收缩压(RVSP),平均肺动脉压(mPAP)和右心室肥厚指数(RVHI)),减轻肺血管重塑,而不引起肝肾毒性。同时,EM NPs通过抑制关键促炎介质(CC Motif趋化因子配体5 (CCL5)、巨噬细胞炎症蛋白-3α (MIP-3α)、单核细胞趋化蛋白-1 (MCP-1)、白细胞介素(IL)-18)和抗炎细胞因子(IL-4、IL-13)的升高,显著调节炎症反应。此外,核壳结构显著增强了天然多酚的稳定性和生物利用度,从而提高了其体内治疗效果。RNA测序数据分析表明,EM NPs通过下调关键促炎基因和通路抑制肺组织的免疫激活。EM NPs具有同时靶向PAH中的氧化应激、血管重构和炎症的能力,是一种有前途的纳米治疗候选药物,显示出相当大的临床转化潜力。
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引用次数: 0
MXene/Fe2O3 composite synthesized by electrostatic adsorption method as a high-performance anode material for Li-ion batteries 采用静电吸附法制备MXene/Fe2O3复合材料作为高性能锂离子电池负极材料。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-02 DOI: 10.1016/j.jcis.2026.139827
Ziwei Zhang, Yulei Sui, Zhihao Shi, Xiaoping Zhang, Yutong Fu, Ling Wu
The creation of anode materials with high capacity and stability is vital for next-generation lithium-ion batteries. Although Fe2O3 has a high theoretical capacity, its practical use is limited by significant volume expansion during cycling and low electrical conductivity. To address these challenges, a MXene/Fe2O3 composite is designed and prepared synthesized through a simple yet effective electrostatic adsorption strategy. Density Functional Theory (DFT) analysis indicates that polydiallyldimethylammonium chloride (PDADMAC) effectively anchors itself to the surfaces of both MXene and Fe2O3 through the quaternary ammonium cations located at each end, thereby serving as an efficient bridge between MXene and Fe2O3. Kinetics analysis reveals that the incorporation of MXene establishes an efficient conductive network that facilitates charge transfer and ion transport. MXene can also mitigate the aggregation and volume expansion of Fe2O3. As a result, the optimal MXene/Fe2O3 composite anode delivers a remarkable reversible capacity of 600 mAh g−1 after 3500 cycles at 5 A g−1, demonstrating improved cycling stability. This study proposes a versatile approach to designing MXene-supported composites incorporating metal oxides for use in high-performance energy storage systems.
制造高容量、高稳定性的负极材料对下一代锂离子电池至关重要。虽然Fe2O3具有很高的理论容量,但其实际应用受到循环过程中显着的体积膨胀和低导电性的限制。为了解决这些挑战,设计并制备了MXene/Fe2O3复合材料,通过简单而有效的静电吸附策略合成。密度泛函理论(DFT)分析表明,聚二烯基二甲基氯化铵(PDADMAC)通过位于两端的季铵阳离子有效地将自身锚定在MXene和Fe2O3的表面,从而成为MXene和Fe2O3之间的有效桥梁。动力学分析表明,MXene的加入建立了一个有效的导电网络,促进了电荷转移和离子传输。MXene还能减缓Fe2O3的聚集和体积膨胀。因此,最佳的MXene/Fe2O3复合阳极在5a g-1下循环3500次后提供了600 mAh g-1的显着可逆容量,显示出更好的循环稳定性。这项研究提出了一种通用的方法来设计含有金属氧化物的mxene支撑复合材料,用于高性能储能系统。
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引用次数: 0
Regulating the interaction between Zr-based support and Pt for enhanced room-temperature hydrogen elimination 调节zr基载体与Pt之间的相互作用以增强室温消氢。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-02 DOI: 10.1016/j.jcis.2026.139824
Yong Liu , Zexu Wang , Chenxu Liu , Guodong Miao , He Zhang , Changchun Wang , Ping Li , Xuanhui Qu
Hydrogen leakage safety concerns and the limited performance of conventional oxide-supported Pt catalysts have motivated the development of Pt-based catalysts supported on Zr-based multi-component alloys. In this study, a series of Pt-based catalysts (Pt/γ-Al2O3, Pt/ZrFe, Pt/ZrVFe, and Pt/ZrVFeTi) were synthesized via chemical reduction method. The phase structure, surface morphology, redox properties, and surface chemical states of the catalysts were characterized using various analytical techniques. Their hydrogen elimination performance was evaluated in a fixed-bed reactor under simulated operating conditions. The results indicate that Zr-based alloy-supported Pt catalysts exhibit superior catalytic activity for hydrogen elimination. Among them, Pt/ZrVFeTi catalyst demonstrates the highest performance, achieving a dynamic H2 conversion rate of 96.8 %, compared to 92.9 % for Pt/γ-Al2O3. In static tests, Pt/ZrVFeTi achieves a hydrogen elimination initiation threshold below 0.5 vol%, an initiation time of merely 2 mins, and a hydrogen elimination rate of 5.22 g H2·(kg·min)−1 highlighting its exceptional performance under ambient conditions. To unveil the underlying mechanism, density functional theory calculations were employed to analyze hydrogen adsorption energy, the Pt 3d orbital density of states, and interfacial charge transfer behavior. The calculations indicate that the enhanced performance of Pt/ZrVFeTi arises from the multi-component synergy of the ZrVFeTi support, which optimizes metal-support interaction, improves Pt dispersion, facilitates H2 adsorption, and promotes interfacial electron transfer, collectively leading to superior catalytic activity.
对漏氢安全性的担忧和传统氧化负载Pt催化剂性能的限制,促使了zr基多组分合金负载Pt催化剂的发展。本研究采用化学还原法制备了Pt/γ-Al2O3、Pt/ZrFe、Pt/ZrVFe和Pt/ZrVFeTi系列Pt基催化剂。采用各种分析技术对催化剂的相结构、表面形貌、氧化还原性能和表面化学状态进行了表征。在模拟操作条件下,在固定床反应器中对其除氢性能进行了评价。结果表明,zr基合金负载Pt催化剂具有较好的消氢活性。其中,Pt/ZrVFeTi催化剂表现出最高的性能,达到96.8%的动态H2转化率,而Pt/γ-Al2O3催化剂的动态H2转化率为92.9%。在静态测试中,Pt/ZrVFeTi的氢消除起始阈值低于0.5 vol%,起始时间仅为2 min,氢消除速率为5.22 g H2·(kg·min)-1,突出了其在环境条件下的优异性能。为了揭示其潜在机理,采用密度泛函理论计算分析了氢吸附能、Pt三维轨道态密度和界面电荷转移行为。计算表明,Pt/ZrVFeTi的性能增强是由于ZrVFeTi载体的多组分协同作用,优化了金属-载体相互作用,改善了Pt的分散,促进了H2的吸附,促进了界面电子转移,共同导致了优异的催化活性。
{"title":"Regulating the interaction between Zr-based support and Pt for enhanced room-temperature hydrogen elimination","authors":"Yong Liu ,&nbsp;Zexu Wang ,&nbsp;Chenxu Liu ,&nbsp;Guodong Miao ,&nbsp;He Zhang ,&nbsp;Changchun Wang ,&nbsp;Ping Li ,&nbsp;Xuanhui Qu","doi":"10.1016/j.jcis.2026.139824","DOIUrl":"10.1016/j.jcis.2026.139824","url":null,"abstract":"<div><div>Hydrogen leakage safety concerns and the limited performance of conventional oxide-supported Pt catalysts have motivated the development of Pt-based catalysts supported on Zr-based multi-component alloys. In this study, a series of Pt-based catalysts (Pt/γ-Al<sub>2</sub>O<sub>3</sub>, Pt/ZrFe, Pt/ZrVFe, and Pt/ZrVFeTi) were synthesized via chemical reduction method. The phase structure, surface morphology, redox properties, and surface chemical states of the catalysts were characterized using various analytical techniques. Their hydrogen elimination performance was evaluated in a fixed-bed reactor under simulated operating conditions. The results indicate that Zr-based alloy-supported Pt catalysts exhibit superior catalytic activity for hydrogen elimination. Among them, Pt/ZrVFeTi catalyst demonstrates the highest performance, achieving a dynamic H<sub>2</sub> conversion rate of 96.8 %, compared to 92.9 % for Pt/γ-Al<sub>2</sub>O<sub>3</sub>. In static tests, Pt/ZrVFeTi achieves a hydrogen elimination initiation threshold below 0.5 vol%, an initiation time of merely 2 mins, and a hydrogen elimination rate of 5.22 g H<sub>2</sub>·(kg·min)<sup>−1</sup> highlighting its exceptional performance under ambient conditions. To unveil the underlying mechanism, density functional theory calculations were employed to analyze hydrogen adsorption energy, the Pt 3d orbital density of states, and interfacial charge transfer behavior. The calculations indicate that the enhanced performance of Pt/ZrVFeTi arises from the multi-component synergy of the ZrVFeTi support, which optimizes metal-support interaction, improves Pt dispersion, facilitates H<sub>2</sub> adsorption, and promotes interfacial electron transfer, collectively leading to superior catalytic activity.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"708 ","pages":"Article 139824"},"PeriodicalIF":9.7,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145916515","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Journal of Colloid and Interface Science
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