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Gd3+ engineered Co–Mn–Mg spinel nanoferrites for multifunctional theranostics: magnetic hyperthermia, antioxidant hepatoprotection, and antibacterial activity Gd3+工程Co-Mn-Mg尖晶石纳米铁素体用于多功能治疗:磁热疗,抗氧化肝保护和抗菌活性。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA08039H
M. Elansary, N. Bentarhlia, O. Oulhakem, Y. Mouhib, B. Salameh, A. M. Alsmadi, B. Kartah, H. Monfalouti, M. Belaiche and O. M. Lemine

We synthesized Co0.5Mn0.25Mg0.25Fe2−xGdxO4 (x = 0.00; 0.04; 0.06) nanoferrites using a sol–gel auto-combustion method and studied their structural, magnetic, and biological properties. XRD with Rietveld refinement confirmed the formation of a pure spinel structure with nanosized crystallites. FTIR and XPS analyses proved the presence of metal–oxygen bonds, mixed oxidation states of Fe and Co, and the successful incorporation of Gd3+. TEM images revealed nanometric particles with homogeneous elemental distribution. Magnetic measurements showed that Gd3+ doping modifies the saturation magnetization (Ms) and coercivity (Hc), with the best performance at x = 0.04 (Ms = 45.7 emu g−1, Hc = 427 Oe). Under an alternating magnetic field, the samples efficiently produced heat in the hyperthermia range, with a specific absorption rate (SAR) of about 34 W g−1 for x = 0.04. In vivo experiments in ethanol-induced liver injury models demonstrated that the x = 0.04 sample improved antioxidant activity (increased SOD and CAT levels) and restored important serum biochemical markers such as albumin, total protein, creatinine, urea, uric acid, and electrolytes. This indicates strong hepatoprotective and nephroprotective effects. Antibacterial studies further showed that the nanoferrites were more effective against Gram-positive bacteria (S. aureus, B. subtilis, B. licheniformis) than Gram-negative ones (E. coli, P. aeruginosa). Overall, our results show that Gd3+ substitution enhances both magnetic and biological properties. The x = 0.04 composition provides the best compromise between magnetic heating efficiency, antioxidant protection, and antibacterial activity, making these nanoferrites promising candidates for biomedical applications such as cancer hyperthermia therapy, antioxidant defense, and infection control.

采用溶胶-凝胶自燃烧法合成了Co0.5Mn0.25Mg0.25Fe2-x Gd x O4 (x = 0.00; 0.04; 0.06)纳米铁氧体,并对其结构、磁性和生物学性能进行了研究。XRD和Rietveld细化证实形成了具有纳米级晶粒的纯尖晶石结构。FTIR和XPS分析证实了金属-氧键的存在,Fe和Co的混合氧化态,以及Gd3+的成功掺入。TEM图像显示纳米颗粒具有均匀的元素分布。磁性测量结果表明,Gd3+的掺杂改变了饱和磁化强度(ms)和矫顽力(hc),在x = 0.04 (ms = 45.7 emu g-1, hc = 427 Oe)时表现最佳。在交变磁场作用下,样品有效地产生热疗范围内的热量,当x = 0.04时,比吸收率(SAR)约为34 W g-1。乙醇肝损伤模型的体内实验表明,x = 0.04的样品提高了抗氧化活性(SOD和CAT水平升高),恢复了重要的血清生化指标,如白蛋白、总蛋白、肌酐、尿素、尿酸和电解质。这表明其具有较强的保肝保肾作用。抗菌研究进一步表明,纳米铁氧体对革兰氏阳性菌(金黄色葡萄球菌、枯草芽孢杆菌、地衣芽孢杆菌)的抑菌效果优于革兰氏阴性菌(大肠杆菌、铜绿假单胞菌)。总的来说,我们的研究结果表明Gd3+取代提高了磁性和生物学性能。x = 0.04的组合物在磁加热效率、抗氧化保护和抗菌活性之间提供了最佳的折衷,使这些纳米铁氧体成为生物医学应用的有希望的候选者,如癌症热疗、抗氧化防御和感染控制。
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引用次数: 0
Reduced graphene oxide surface modification with nanoparticles and its efficiency in removing crystal violet and malachite green dyes from wastewater 纳米颗粒还原氧化石墨烯表面改性及其去除废水中结晶紫和孔雀石绿染料的效果。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA08749J
Sumood Al-Hadeethy, Aws Z. Abdulmajeed, Ali M. Alalusi, Alauddin M. Mahdi, Wassan N. Hussain and Ibraheem A. Alrazaq

Industrial dyes are among the most complicated contaminants, posing an increasing hazard to aquatic life if left untreated. Carbon nanoparticles are extremely effective in the adsorption process. As a result, the purpose of this study was to manufacture reduced graphene oxide from sunflower husks, an affordable raw material, and modify its surface with zinc oxide and copper oxide nanoparticles that were produced in an environmentally friendly method. This improved material was employed as a sustainable adsorbent to remove crystal violet and malachite green dyes from wastewater. The results revealed that the optimal medium for adsorption was basic, with an equilibrium time of 25 minutes at 35 °C. Kinetic experiments found that the adsorption follows pseudo-second-order kinetics and is consistent with the Langmuir-Isotherm model. The thermodynamic study showed that the process is spontaneous and endothermic, with increased system randomness. Crystal violet had a removal effectiveness of 95.6%, and malachite green had one of 96% from wastewater.

工业染料是最复杂的污染物之一,如果不加以处理,会对水生生物造成越来越大的危害。碳纳米颗粒在吸附过程中非常有效。因此,本研究的目的是利用向日葵壳(一种经济实惠的原材料)制造还原性氧化石墨烯,并用环保方法生产的氧化锌和氧化铜纳米颗粒修饰其表面。将该改性材料作为可持续吸附剂用于废水中结晶紫和孔雀石绿染料的脱除。结果表明,最佳吸附介质为碱性介质,35℃下吸附平衡时间为25分钟。动力学实验发现,吸附符合拟二级动力学,符合langmuir -等温线模型。热力学研究表明,该过程是自发的、吸热的,系统随机性增加。结晶紫和孔雀石绿对废水的去除率分别为95.6%和96%。
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引用次数: 0
Systematical synthesis of magnetic-layered core@shell supports for metalloporphyrin immobilization aiming catalysis 磁性层状core@shell催化金属卟啉固定化载体的系统合成。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA08288A
Everton Henrique dos Santos, Adriana Duarte Dalla Costa, Vanessa Prevot, Claude Forano and Shirley Nakagaki

Bioinspired catalytic systems based on metalloporphyrins have been extensively researched in recent years and, in many cases, have played a key role in the development of more efficient and selective catalysts. The immobilization of this family of catalyst species in robust supports can permit the preparation of recoverable and reusable catalyst solids. In this work, we present the systematic and comprehensive preparation of core@shell-like solids for catalyst immobilization based on magnetic particle, using microwave-assisted synthesis of magnetite, coated with a shell composed of two distinct LDH formulations: Mg3Al and Ni3Al, evaluating different LDH/magnetite molar ratios. Four different tetra-anionic metalloporphyrins (Na4[M(TDFSPP)], M = iron(III), manganese(III), zinc(II), or magnesium(II) ions) (MP) were immobilized in both prepared LDHs. The eight resulting solids were evaluated as catalysts in the model oxidation reaction of cyclooctene to cis-cyclooctene oxide, using iodosylbenzene (PhIO) as the oxidant.

近年来,基于金属卟啉的生物激发催化系统得到了广泛的研究,在许多情况下,在开发更高效、更有选择性的催化剂方面发挥了关键作用。固定化这一家族的催化剂物种在稳健的支持可以允许制备可回收和可重复使用的催化剂固体。在这项工作中,我们提出了系统和全面的制备core@shell-like固体催化剂固定化基于磁颗粒,使用微波辅助合成的磁铁矿,包覆由两种不同的LDH配方组成的壳:Mg3Al和Ni3Al,评估不同的LDH/磁铁矿的摩尔比。将四种不同的四阴离子金属卟啉(Na4[M(TDFSPP)], M =铁(iii),锰(iii),锌(ii)或镁(ii)离子)(MP)固定在两种制备的LDHs中。以碘基苯(iodosylbenzene, PhIO)为氧化剂,评价了所得到的8种固体在环烯氧化成顺式环烯氧化物模型反应中的催化作用。
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引用次数: 0
Synthesis of biocompatible gold nanoparticles for photothermal therapy by mineralization using peptides 利用多肽矿化合成用于光热治疗的生物相容性金纳米颗粒。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA08717A
Shuhei Yoshida, Koki Yoshida, Yoshiki Shitamukai, Makoto Ozaki, Takaaki Tsuruoka and Kenji Usui

Anisotropic gold nanostructures, such as rods and cubes, exhibit unique optical properties, including absorption in the near-infrared region, which makes them highly attractive for biomedical applications such as imaging and phototherapy. However, conventional synthesis methods often require toxic surfactants and strong reducing agents, limiting their biocompatibility. In this study, we developed a method for synthesizing biocompatible gold nanostructures suitable for photothermal therapy by mineralization using peptides. We designed peptides with different numbers of tryptophan (Trp) residues at N-terminal that can reduce gold ions and control nanoparticle growth. The peptides with fewer Trp residues were found to have a red-shifted maximum absorption wavelength at lower concentrations. A 2 : 1 ratio of gold ions to silver ions was optimal for the formation of anisotropic structures. The peptides successfully imparted high dispersibility to mineralized gold nanostructures. In addition, biocompatibility testing showed no toxicity in mineralized Au nanostructures. We studied the photothermal effect of visible light irradiation on the Au nanostructures, showing that they possessed high biotoxicity under light irradiation conditions. These results suggest that this method can be used for photothermal therapy. Our peptide-based approach offers a simple, safe, and biocompatible strategy to synthesize anisotropic gold nanostructures, which could be applied to the development of future nanomedical tools.

各向异性金纳米结构,如棒状和立方体,具有独特的光学特性,包括在近红外区域的吸收,这使得它们在成像和光疗等生物医学应用中具有很高的吸引力。然而,传统的合成方法往往需要有毒的表面活性剂和强还原剂,限制了它们的生物相容性。在这项研究中,我们开发了一种利用多肽矿化合成适合光热治疗的生物相容性金纳米结构的方法。我们设计了在n端具有不同数量色氨酸残基的肽,可以减少金离子并控制纳米颗粒的生长。在较低浓度下,具有较少色氨酸残基的肽具有红移的最大吸收波长。金离子与银离子的比例为2:1是形成各向异性结构的最佳条件。多肽成功地赋予矿化金纳米结构高分散性。此外,生物相容性测试表明,矿化金纳米结构没有毒性。我们研究了可见光照射对金纳米结构的光热效应,表明它们在光照射条件下具有很高的生物毒性。这些结果表明,该方法可用于光热治疗。我们基于肽的方法为合成各向异性金纳米结构提供了一种简单、安全、生物相容性好的方法,可应用于未来纳米医疗工具的开发。
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引用次数: 0
Fabrication and characterization of 3D-printed PLA-based composite filters for cationic dye removal 用于阳离子染料去除的3d打印pla基复合过滤器的制造和表征。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA08506C
Niyazi Erdem Delikanli

This study presents the fabrication and characterization of 3D-printed biodegradable composite filters for the removal of cationic dyes from aqueous solutions. Inspired by the hierarchical structure of tree leaves, the filters were produced using commercially available polylactic acid (PLA) and a PLA/wood composite filament containing 30% wood dust, via fused deposition modeling (FDM). Post-printing modification was performed by treating the filters with aqueous potassium hydroxide (KOH) solutions at varying concentrations (0.1, 0.2, and 0.4 M). The adsorption behavior was assessed using Crystal Violet (CV) as a model cationic dye at concentrations ranging from 10 to 200 mg L−1 under gravity driven filtration. KOH treatment significantly enhanced the dye adsorption capacity of PLA/wood composite filters, achieving removal efficiencies up to 97.5%. Surface characterization via SEM, FTIR, XRD, and pHpzc analysis confirmed that KOH activation increased surface roughness and introduced functional groups, leading to enhanced electrostatic interaction with cationic species. Moreover, the bioinspired filter geometry with hierarchical porosity contributed to improved mass transfer and dye retention. These findings demonstrate the synergistic effect of material composition, surface modification, and structural design in developing 3D-printed filtration media. The study offers a reproducible and scalable approach for designing polymer-based sorbents for potential applications in water purification.

本研究介绍了3d打印生物可降解复合过滤器的制造和表征,用于从水溶液中去除阳离子染料。受树叶分层结构的启发,过滤器使用市购的聚乳酸(PLA)和含有30%木粉的PLA/木材复合长丝,通过熔融沉积建模(FDM)生产。印后改性是用不同浓度(0.1,0.2和0.4 M)的氢氧化钾溶液处理过滤器。在重力驱动过滤条件下,以结晶紫(CV)为模型阳离子染料,在10 ~ 200mg L-1的浓度范围内对其吸附行为进行了评价。KOH处理显著提高了PLA/wood复合过滤器对染料的吸附能力,去除率高达97.5%。通过SEM, FTIR, XRD和pHpzc分析证实,KOH活化增加了表面粗糙度并引入了官能团,从而增强了与阳离子物种的静电相互作用。此外,具有分层孔隙度的仿生过滤器几何形状有助于改善传质和染料保留。这些发现证明了材料组成、表面改性和结构设计在开发3d打印过滤介质中的协同作用。该研究为设计聚合物基吸附剂在水净化中的潜在应用提供了一种可重复和可扩展的方法。
{"title":"Fabrication and characterization of 3D-printed PLA-based composite filters for cationic dye removal","authors":"Niyazi Erdem Delikanli","doi":"10.1039/D5RA08506C","DOIUrl":"10.1039/D5RA08506C","url":null,"abstract":"<p >This study presents the fabrication and characterization of 3D-printed biodegradable composite filters for the removal of cationic dyes from aqueous solutions. Inspired by the hierarchical structure of tree leaves, the filters were produced using commercially available polylactic acid (PLA) and a PLA/wood composite filament containing 30% wood dust, <em>via</em> fused deposition modeling (FDM). Post-printing modification was performed by treating the filters with aqueous potassium hydroxide (KOH) solutions at varying concentrations (0.1, 0.2, and 0.4 M). The adsorption behavior was assessed using Crystal Violet (CV) as a model cationic dye at concentrations ranging from 10 to 200 mg L<small><sup>−1</sup></small> under gravity driven filtration. KOH treatment significantly enhanced the dye adsorption capacity of PLA/wood composite filters, achieving removal efficiencies up to 97.5%. Surface characterization <em>via</em> SEM, FTIR, XRD, and pHpzc analysis confirmed that KOH activation increased surface roughness and introduced functional groups, leading to enhanced electrostatic interaction with cationic species. Moreover, the bioinspired filter geometry with hierarchical porosity contributed to improved mass transfer and dye retention. These findings demonstrate the synergistic effect of material composition, surface modification, and structural design in developing 3D-printed filtration media. The study offers a reproducible and scalable approach for designing polymer-based sorbents for potential applications in water purification.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":" 56","pages":" 48381-48392"},"PeriodicalIF":4.6,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12683515/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145712630","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Structure-dependent pyrolysis mechanisms of tobacco carbohydrates: from monosaccharides to polysaccharides under programmed and fast pyrolysis conditions 烟草碳水化合物的结构依赖热解机制:在程序化和快速热解条件下从单糖到多糖。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA07210G
Yuhan Peng, Xiaopeng Shi, Xiaodong Tang, Lu Dai, Depo Cao, Qingxiang Li, Fangqi Du, Kaige Wang and Yiming Bi

This study systematically investigates the pyrolysis mechanisms of typical carbohydrates in tobacco under both fast pyrolysis (500 °C) and temperature-programmed conditions (50–500 °C), with a focus on their structural influences on product distributions and reaction pathways. Comparing the fast and temperature-programmed pyrolysis experiments reveals the pyrolysis pathways and product distributions of different structural sugars. Using Py-GC/MS analysis, we demonstrate that small-molecule sugars exhibit distinct pyrolysis behaviors: glucose favors diversified products through 1,2-enolization, while fructose preferentially forms furans via 2,3-enolization due to its ketose configuration. Macromolecular sugars display structure-dependent mechanisms: cellulose yields anhydrosugars through β-1,4-glycosidic cleavage; amylose's α-1,4-linked helical structure enhances anhydrosugar production (62.21%); and xylan's pentose units promote furfural selectivity (46.6%). The Maillard reaction with proline significantly alters pyrolysis pathways, introducing nitrogenous heterocycles and suppressing anhydrosugars while enhancing the ester formation. These findings elucidate the structure–activity relationships governing tobacco carbohydrate pyrolysis, offering a theoretical foundation for optimizing pyrolysis processes and developing functional flavor compounds.

本研究系统研究了烟草中典型碳水化合物在快速热解(500°C)和程控温度(50-500°C)条件下的热解机理,重点研究了其结构对产物分布和反应途径的影响。通过快速热解实验和程序升温热解实验的对比,揭示了不同结构糖的热解途径和产物分布。通过Py-GC/MS分析,我们证明了小分子糖表现出不同的热解行为:葡萄糖通过1,2-烯醇化倾向于多种产物,而果糖由于其酮糖结构而优先通过2,3-烯醇化形成呋喃。大分子糖表现出结构依赖机制:纤维素通过β-1,4-糖苷裂解产生无水糖;直链淀粉的α-1,4链螺旋结构提高无水糖产量(62.21%);木聚糖的戊糖单元提高了糠醛的选择性(46.6%)。与脯氨酸的美拉德反应显著改变了热解途径,引入了含氮杂环,抑制了无水糖,同时促进了酯的形成。这些发现阐明了烟草碳水化合物热解的构效关系,为优化热解工艺和开发功能性风味化合物提供了理论基础。
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引用次数: 0
Hydrophobic alkyl-linked base-modified pyrimidine and 7-deazapurine 2′-deoxyribonucleoside phosphoramidites: synthesis and application in solid-phase synthesis of modified and hypermodified oligonucleotides 疏水烷基链基修饰嘧啶和7-去氮杂嘌呤2'-脱氧核糖核苷磷酰胺:合成及其在固相合成修饰和超修饰寡核苷酸中的应用。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA06147D
Ivana Jestřábová, Lucie Bednárová, Lenka Poštová Slavětínská and Michal Hocek

A series of 2′-deoxyribonucleoside 3′-phosphoramidites bearing hydrophobic alkyl-linked modifications at nucleobases was synthesized, namely 5-phenylethyluracil, 5-pentylcytosine, 7-(indol-3-yl)ethyl-7-deazaadenine, and 7-isopentyl-7-deazaguanine derivatives. These nucleoside phosphoramidites were used for solid-phase synthesis of modified and hypermodified oligonucleotides containing up to fifteen modified nucleotides in a row. Their hybridization with complementary non-modified or modified oligonucleotides and thermal stability of the resulting DNA duplexes was studied using UV-vis denaturing experiments and CD spectroscopy. The results indicate that the partially modified hydrophobic DNA can still retain B-conformation, although with lower thermal stability. On the other hand, the hypermodified ONs containing all four modified nucleotides did not hybridize to duplexes likely due to formation of aggregates as indicated by dynamic light scattering measurement. This work expands the toolkit of chemically modified nucleotides for applications in functional nucleic acids or nucleic acid therapeutics, but also shows the scope and limitations of the use of hydrophobic nucleotides in hypermodified oligonucleotides and DNA.

合成了一系列在核碱基上具有疏水性烷基连接修饰的2'-脱氧核糖核苷3'-磷酰胺,即5-苯基乙基尿嘧啶、5-戊基胞嘧啶、7-(吲哚-3-基)乙基-7-去氮杂腺嘌呤和7-异戊基-7-去氮杂胍衍生物。这些核苷磷酰胺被用于固相合成修饰和超修饰的寡核苷酸,其中含有多达15个修饰的核苷酸。利用紫外-可见变性实验和CD光谱研究了它们与互补的未修饰或修饰的寡核苷酸的杂交和所得到的DNA双链的热稳定性。结果表明,部分修饰的疏水DNA仍能保持b构象,但热稳定性较低。另一方面,动态光散射测量表明,含有所有四种修饰核苷酸的超修饰的离子没有杂交成双链,这可能是由于形成聚集体。这项工作扩展了化学修饰核苷酸在功能核酸或核酸治疗中的应用,但也显示了在超修饰寡核苷酸和DNA中使用疏水核苷酸的范围和局限性。
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引用次数: 0
Influence of laser ablation preparation of MgO and Bi2O3 nanoparticles on the optical and dielectric behavior of the PVA/PEO polymer blend 激光烧蚀制备MgO和Bi2O3纳米颗粒对PVA/PEO共混聚合物光学和介电行为的影响
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA08147E
I. S. Elashmawi and A. A. Menazea

This study aims to optimize the optical and electrical performance of polyvinyl alcohol/polyethylene oxide (PVA/PEO) incorporated with magnesium oxide (MgO) and bismuth(III) oxide (Bi2O3) nanoparticles synthesized by pulsed laser ablation over different durations. XRD revealed that the MgO nanoparticles acted as nucleating centers, increasing crystallinity. The incorporation of Bi2O3 resulted in sharper peaks and improved phase ordering with a prolonged ablation time. The FTIR spectra showed strong interactions between the PVA/PEO blend and nanoparticles, mediated by hydrogen bonding and novel vibrational modes between the metal and oxygen. UV-DRS showed optical modification and redshift of the absorption edge with a prolonged ablation time, indicating improved nanoparticle homogeneity, size growth, and crystallinity. TGA demonstrated an enhancement in the thermal stability of the Bi2O3/MgO double-filler composite. Dielectric and AC conductivity studies demonstrated a frequency behavior consistent with Maxwell–Wagner–Sillars interface polarization. Increasing the ablation time resulted in a decrease in the dielectric constant and conductivity, which was attributed to the small size and good dispersion of the nanoparticles and the restricted charge mobility due to the interface adhesion force.

本研究旨在优化聚乙烯醇/聚乙烯氧化物(PVA/PEO)与氧化镁(MgO)和氧化铋(Bi2O3)纳米颗粒在脉冲激光烧蚀不同持续时间下的光学和电学性能。XRD分析表明,MgO纳米颗粒作为成核中心,提高了结晶度。随着烧蚀时间的延长,Bi2O3的掺入使峰更清晰,相有序度提高。FTIR光谱显示PVA/PEO共混物与纳米颗粒之间存在强烈的相互作用,这种相互作用是由氢键和金属与氧之间的新型振动模式介导的。随着烧蚀时间的延长,UV-DRS的吸收边出现了光学修饰和红移,表明纳米颗粒的均匀性、尺寸增长和结晶度得到了改善。TGA表明Bi2O3/MgO双填料复合材料的热稳定性增强。介电和交流电导率研究表明,频率行为与麦克斯韦-瓦格纳-西拉界面极化一致。随着烧蚀时间的延长,纳米颗粒的介电常数和电导率下降,这主要是由于纳米颗粒的体积小、分散性好,以及界面附着力限制了电荷的迁移率。
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引用次数: 0
Machine learning-based prediction and mechanistic insight into PFAS adsorption on carbon-based materials 基于机器学习的PFAS在碳基材料上吸附的预测和机理研究。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA07898A
Yanliang Lu, Fangfang Ding, Guchun Wang, Yabin Li, Zhitao Guo, Peiyao Pang, Baojun Wang and Jue Liu

Carbon-based materials hold significant potential in environmental remediation, as they can effectively remove per- and polyfluoroalkyl substances (PFAS) through adsorption, thereby influencing their environmental behavior and associated risks. However, due to the complexity of the physicochemical properties of carbon-based materials, the molecular diversity of PFAS—including variations in chain length, functional groups, and degree of fluorination—as well as differences in environmental conditions, it remains challenging to fully elucidate the adsorption mechanisms solely through experimental approaches. In this study, a gradient boosting decision tree (GBDT) model was developed and optimized to systematically predict the adsorption performance of carbon-based materials toward PFAS. The GBDT model demonstrated excellent predictive accuracy on the test dataset, achieving an R2 of 0.96 and a root mean square error (RMSE) of 0.02. Model interpretation using Shapley additive explanations (SHAP) and partial dependence plots revealed that environmental conditions contributed the most to adsorption, followed by the physicochemical characteristics of carbon-based materials and the molecular features of PFAS. Specifically, solution pH, the number of fluorine atoms within PFAS molecules, temperature, and the pore structure of carbon-based materials were identified as the most influential factors, with electrostatic interactions and hydrophobic–hydrophilic character are likely the dominant mechanisms. This study provides a novel perspective that integrates machine learning with environmental chemistry to enhance understanding of PFAS–carbon interactions, offering valuable insights for environmental risk assessment and the rational design of functional materials.

碳基材料可以通过吸附有效去除全氟烷基和多氟烷基物质,从而影响其环境行为和相关风险,在环境修复中具有巨大的潜力。然而,由于碳基材料的物理化学性质的复杂性,pfas的分子多样性(包括链长、官能团和氟化程度的变化)以及环境条件的差异,仅通过实验方法充分阐明其吸附机制仍然具有挑战性。本研究建立并优化了梯度增强决策树(GBDT)模型,以系统地预测碳基材料对PFAS的吸附性能。GBDT模型在测试数据集上表现出出色的预测精度,r2为0.96,均方根误差(RMSE)为0.02。基于Shapley加性解释(SHAP)和部分依赖图的模型解释表明,环境条件对吸附的影响最大,其次是碳基材料的物理化学特性和PFAS的分子特性。其中,溶液pH、PFAS分子内氟原子数、温度和碳基材料的孔隙结构是影响PFAS性能的主要因素,静电相互作用和疏亲水性可能是主要机制。本研究提供了一个新的视角,将机器学习与环境化学相结合,以增强对pfas -碳相互作用的理解,为环境风险评估和功能材料的合理设计提供了有价值的见解。
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引用次数: 0
LiCl modified MOFs-derived porous carbon hollow spheres for efficient solar-driven atmospheric water harvesting LiCl改性mofs衍生的多孔碳空心球用于高效太阳能驱动的大气集水。
IF 4.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-08 DOI: 10.1039/D5RA04196A
Jiake Jin, Simiao Guo, Yue Hu, Yefeng Yang, Pingwei Ye and Xinsheng Peng

Developing adsorbents with excellent photothermal and water uptake properties for solar-driven sorption-based atmospheric water harvesting (SAWH) is full of challenging, which requires a balance between the adsorption capacity, hydrophilicity, and photothermal performance of adsorbent. In this work, a LiCl modfiied porous carbon hollow microspheres (CHM@LiCl) adsorbent with high adsorption capacity (2.07 g g−1) at 100% RH and enhanced low moisture adsorption performance was synthesized by loading LiCl hydrophilic adsorption sites into MOFs-derived hollow porous carbon. LiCl, as the main adsorption site, enhances the hydrophilicity of the CHM@LiCl adsorbent, and its water uptake capacity at 20% RH, 40% RH, 60% RH, and 80% RH are 0.25, 0.39, 0.60 and 1.04 g g−1, respectively. In addition, the hiearchical porous structure of the hollow carbon with mciroporus shell effectively suppresses the salt leakage during water adsorption. The sorbent exhibites stable performance for cycling water adsorption-release, indicating its long-term reliability. The excellent photothermal performance of CHM@LiCl adsorbent can quickly heat up to 67 °C under one sun irradiation, and completely desorb the adsorbed water within 30 minutes. The outdoor water harvesting experiment shows that the CHM@LiCl adsorbent holds great potential for practical solar-driven SAWH with a water collection capacity of 3.3 Lwater kgsorbent−1 day under RH 60%.

开发具有良好光热和吸水性的吸附剂用于太阳能驱动的大气集水(SAWH)是充满挑战的,这需要在吸附剂的吸附能力、亲水性和光热性能之间取得平衡。本研究通过将LiCl亲水吸附位点加载到mofs类中空多孔碳中,合成了LiCl改性多孔碳空心微球(CHM@LiCl)吸附剂,在100% RH下具有较高的吸附量(2.07 g g-1),并增强了低湿吸附性能。LiCl作为主要吸附位点增强了CHM@LiCl吸附剂的亲水性,在20% RH、40% RH、60% RH和80% RH条件下吸水性分别为0.25、0.39、0.60和1.04 g-1。此外,微孔壳中空碳的多孔结构有效地抑制了水吸附过程中盐的泄漏。该吸附剂具有稳定的循环水吸附-释放性能,具有长期的可靠性。优异的光热性能CHM@LiCl吸附剂在一次太阳照射下可快速加热至67℃,并在30分钟内将吸附的水完全解吸。室外集水实验表明,CHM@LiCl吸附剂在RH为60%的条件下,具有3.3 Lwater kkabsorb剂-1 d的集水能力,具有很大的实用潜力。
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