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Heterophase CuO/Cu/Fe nanoparticle incorporated polyurethane coating for combating catheter-induced infection 掺入聚氨酯涂层的异相氧化铜/铜/铁纳米粒子用于抗导管引起的感染
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1016/j.matchemphys.2024.130154
Ludmila Ivanova, Olga Bakina, Nikolay Rodkevich, Marat Lerner
To combat biofilm formation on the surface of medical devices, a new coatings based on polyurethane filled with heterophase nanoparticles CuO/Cu/Fe composition have been developed. Due to the synergistic antibacterial effect of the nanoparticle constituents, the obtained coatings demonstrated exceptional antibacterial activity. Thus the coating containing 5 % wt. or more of the CuO/Cu/Fe nanoparticles was at least 99.99 % against bacteria S. aureus, A. bumannii, K. pneumonia, P. aeruginosa. For this coating, the value of surface energy was maximum, indicating an increase in its hydrophobicity. The operational life of the catheter samples was more than 30 days, which exceeds the operational life of standard urinary catheters. Based on the results obtained, the application of the developed coating is a promising strategy for solving the catheter-associated urinary tract infection problem. Good biocompatibility was determined in vitro using 3T3 fibroblast cell culture, which is highly sensitive to toxic effects. Compared to other strategies of catheter surface modification, the use of polyurethane coating with nanoparticles of complex composition has a number of advantages: high antibacterial activity of nanoparticles due to the synergistic effect of constituents; biocompatibility of the coating provided by the use of biometals; long-term service life due to good adhesion of the coating to the standard silicon Foley catheter. Thus, the proposed coating containing nanoparticles effectively prevents bacterial colonization on catheters or other implants, thereby reducing the risk of postoperative catheter-induced infection.
为了防止医疗器械表面生物膜的形成,我们开发了一种基于聚氨酯的新型涂层,其中填充了异相纳米粒子 CuO/Cu/Fe。由于纳米粒子成分的协同抗菌作用,所获得的涂层显示出卓越的抗菌活性。因此,含 5% 或更多重量 CuO/Cu/Fe 纳米粒子的涂层对金黄色葡萄球菌、布曼氏杆菌、肺炎双球菌和绿脓杆菌的抗菌率至少为 99.99%。这种涂层的表面能值最大,表明其疏水性增强。导尿管样本的使用寿命超过 30 天,超过了标准导尿管的使用寿命。根据所获得的结果,应用所开发的涂层是解决导尿管相关尿路感染问题的一种可行策略。利用对毒性高度敏感的 3T3 成纤维细胞进行体外培养,确定了该涂层具有良好的生物相容性。与导尿管表面改性的其他策略相比,使用含有复杂成分的纳米颗粒的聚氨酯涂层具有许多优点:由于各种成分的协同作用,纳米颗粒具有很高的抗菌活性;由于使用了生物金属,涂层具有生物相容性;由于涂层与标准硅Foley导尿管具有良好的粘附性,因此使用寿命长。因此,含有纳米粒子的涂层能有效防止导管或其他植入物上的细菌定植,从而降低术后导管引发感染的风险。
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引用次数: 0
Probing the effect of electrolyte ions on the electrochemical performance of nickel-based metal-organic frameworks 探究电解质离子对镍基金属有机框架电化学性能的影响
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1016/j.matchemphys.2024.130144
Shiwani Khokhar , Prakash Chand , Hardeep Anand
Understanding the influence of electrolyte ions dimension on electrochemical performance is essential for advancing the development of superior MOF-based devices. Nanosheet-type nickel metal-organic frameworks (Ni-BDC) have emerged as exceptional materials for next-generation supercapacitors. To address this, we investigate the energy storage performance of nickel-1,4-benzene dicarboxylate (Ni-BDC) via an elementary solvothermal approach. The primary objective of the present investigation was to elucidate the influence of distinct cationic components within aqueous electrolytes on the electrochemical efficiency of Ni-BDC. The electrochemical examination was performed using a three-electrode setup in different aqueous electrolytes, comprising LiOH, NaOH, and KOH, each with a concentration of 2 M. The calculated specific capacitance value of Ni-BDC increases in the order of 204 F/g (for LiOH) < 290 F/g (for NaOH) < 1526 F/g (for KOH) at 1 A/g due to the lowest hydration sphere radius, greater ionic mobility of K+ ion. The material performed better electrochemically in KOH electrolyte with 87 % capacitance preservation. Additionally, an asymmetric supercapacitor (ASSC) device was built using activated carbon (AC) as the negative electrode and nanosheet-like Ni-BDC as the positive electrode. The device, operating within a 1.4 V potential window, demonstrated a capacitance of 39.4 F/g at a current density of 1 A/g. The ASSC device maintained 85 % of its cyclic stability over 4000 charge-discharge cycles at a current density of 8 A/g. This study underscores the vital importance of selecting the optimal electrolyte to significantly enhance the electrochemical performance of Ni-BDC electrode material.
了解电解质离子尺寸对电化学性能的影响对于推动基于 MOF 的卓越装置的开发至关重要。纳米片型镍金属有机框架(Ni-BDC)已成为下一代超级电容器的特殊材料。为此,我们通过基本溶热法研究了 1,4-苯二甲酸镍(Ni-BDC)的储能性能。本研究的主要目的是阐明水性电解质中不同阳离子成分对 Ni-BDC 电化学效率的影响。Ni-BDC 的计算比电容值在 1 A/g 时依次增加了 204 F/g(LiOH)< 290 F/g(NaOH)< 1526 F/g(KOH),这是因为水合球半径最小,K+ 离子的离子迁移率更大。该材料在 KOH 电解液中的电化学性能更好,电容保持率达 87%。此外,还利用活性炭(AC)作为负极,纳米片状 Ni-BDC 作为正极,构建了一个不对称超级电容器(ASSC)装置。该装置在 1.4 V 电位窗口内工作,在电流密度为 1 A/g 时的电容为 39.4 F/g。在 8 A/g 的电流密度下,ASSC 器件在 4000 次充放电循环中保持了 85% 的循环稳定性。这项研究强调了选择最佳电解质对显著提高 Ni-BDC 电极材料电化学性能的重要性。
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引用次数: 0
Lac-based-biosynthesis of zinc–copper mixed metal oxide nanoparticles and evaluation of their antifungal activity against A.alternata and F. oxysporum 基于 Lac 的锌铜混合金属氧化物纳米粒子的生物合成及其对交替孢霉和氧孢霉抗真菌活性的评估
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1016/j.matchemphys.2024.130152
Sarla Yadav , Jigyasa Pathak , Purusottam Majhi , Sandeep Kaushik , A.K. Shukla , Raminder Kaur , Ravinder Kumar , Poonam Singh
The use of animal-based sources for biosynthesis resonates with the growing market for sustainable and eco-friendly materials, but remains severely unexplored in comparison to plant-based and microbial sources. In this purview, shellac, a bioresin obtained from the Kerria lacca insect, is emerging as an ideal candidate for nanomaterial fabrication due to its abundant availability and anti-microbial properties. It is commonly available in the form of raw seed lac, (SL) and in the processed button lac (BL) form. Therefore, in the current study, the potential of shellac as a green agent for the synthesis of zinc-copper mixed metal oxide nanoparticles, and the anti-fungal activitiy of synthesized nanoparticles was investigated. Two types of zinc copper oxide nanoparticles were synthesized using button lac (ZnCu(BL)O) and seed lac (ZnCu(SL)O), and they were characterised using various techniques such as Powder X-Ray Diffraction (PXRD), Fourier Transform Infrared spectroscopy (FTIR) and Scanning Electron Microscopy-Energy Dispersive X-Ray (SEM-EDX) spectroscopy. PXRD pattern confirmed the hexagonal wurtzite structure of crystalline ZnCuO NPs. FTIR analysis elucidated the presence of functional groups that were potentially involved in the synthesis of MMO nanoparticles, and the formation of Zn–O and Cu–O bonds was suggested by appearance of bands at 559 cm−1 and 555 cm−1. The morphology and elemental composition of the MMONPs were examined using SEM-EDX techniques that revealed the formation of biosynthesized ZnCuO NPs as spherical agglomerates having uniform distribution of Zn, Cu, C and O throughout the material. Further, the antifungal activity of synthesized NPs was evaluated against F. oxysporum and A. alternata fungal pathogens. It was found that the biosynthesized nanoparticles exhibited significant fungicidal potential against both F. oxysporum and A. alternata. Furthermore, the antifungal results indicated that ZnCuSL-(O) NPs exhibited higher antifungal activity against both fungal strains than ZnCuBL-(O) NPs and chemically synthesized ZnCu-O NPs. Thus, ZnCuSL-(O) NPs and ZnCuBL-(O) NPs prepared using shellac may be considered as cost-effective and eco-friendly substitutes over traditional fungicides.
使用动物来源进行生物合成与日益增长的可持续和生态友好型材料市场产生了共鸣,但与植物和微生物来源相比,动物来源的生物合成仍严重不足。在这一领域,从 Kerria lacca 昆虫中提取的生物树脂--虫胶,因其丰富的可获得性和抗微生物特性,正在成为纳米材料制造的理想候选材料。它通常以原种虫胶(SL)和加工后的钮扣虫胶(BL)的形式存在。因此,本研究考察了虫胶作为绿色制剂合成锌铜混合金属氧化物纳米粒子的潜力,以及合成的纳米粒子的抗真菌活性。使用钮扣漆(ZnCu(BL)O)和种子漆(ZnCu(SL)O)合成了两种类型的氧化锌铜纳米粒子,并使用粉末 X 射线衍射(PXRD)、傅立叶变换红外光谱(FTIR)和扫描电子显微镜-能量色散 X 射线(SEM-EDX)光谱等多种技术对它们进行了表征。PXRD 图谱证实了 ZnCuO NPs 晶体的六方菱面体结构。傅立叶变换红外光谱分析阐明了 MMO 纳米粒子合成过程中可能涉及的官能团的存在,559 cm-1 和 555 cm-1 处出现的条带表明 Zn-O 和 Cu-O 键的形成。利用 SEM-EDX 技术对 MMONPs 的形态和元素组成进行了检测,结果表明生物合成的 ZnCuO NPs 为球形团聚体,整个材料中 Zn、Cu、C 和 O 分布均匀。此外,还评估了合成的氮氧化物对 F. oxysporum 和 A. alternata 真菌病原体的抗真菌活性。结果发现,生物合成的纳米粒子对 F. oxysporum 和 A. alternata 都具有显著的杀真菌潜力。此外,抗真菌结果表明,与 ZnCuBL-(O) NPs 和化学合成的 ZnCu-O NPs 相比,ZnCuSL-(O) NPs 对这两种真菌菌株具有更高的抗真菌活性。因此,使用虫胶制备的 ZnCuSL-(O) NPs 和 ZnCuBL-(O) NPs 可被视为传统杀真菌剂的经济、环保型替代品。
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引用次数: 0
Radiation-thermal modification of fluoroplastic composite and evaluation of its radiation-protective characteristics 氟塑料复合材料的辐射热改性及其辐射防护特性评估
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1016/j.matchemphys.2024.130162
Vyacheslav Ivanovich Pavlenko , Vitaliy Valerievich Kashibadze , Anton Valerievich Noskov , Roman Vladimirovich Sidelnikov , Daria Aleksandrovna Ryzhikh , Sergey Viktorovich Serebryakov
In the work the composite on the basis of fluoroplastic with filler WO3 is studied and its efficiency for protection against X-ray and gamma radiation is proved. The technological scheme of composite production has been developed and its physical and mechanical characteristics have been studied. The composite with 60 wt% of WO3 content has the following properties: density 3.35 ± 0.02 g/cm3, Vickers microhardness (at 300 g load) 5.38 ± 0.32 HV, flexural strength 18.86 MPa. The γ-radiation sources used were E(207Bi) = 0.570 MeV with an activity of 50 kBq, E(137Cs) = 0.662 MeV with an activity of 9 kBq, and E(60Co) = 1.252 MeV with an activity of 100 kBq. The X-ray radiation sources were isotopes 241Am (half-life T1/2 = 432.1 years; photon energy E = 59.5 keV; radioisotope activity 46 μCi) and 109Cd (half-life T1/2 = 461.4 years; photon energy E = 88 keV; radioisotope activity 15 μCi). It is shown that for reduction of gamma radiation with energy 1.252 MeV by 50 % a screen from pure fluoroplastic with thickness of 6.301 ± 0.654 cm is required, and for composite with 60 wt% WO3 the thickness of screen is 1.5 times less (4.077 ± 0.509 cm). Comparison of the linear attenuation coefficient at energy 0.662 MeV with modern analogs confirmed the high efficiency of radiation protection of the developed material. Radiation-thermal modification of the samples was carried out, which allowed to increase their radiation resistance to gamma radiation many times. After radiation-thermal modification the radiation resistance increased up to 1 ± 0.1 MGy and 4.5 ± 0.2 MGy for fluoroplastic and composite with 60 wt% WO3 content, respectively. And the initial bending strength increased in both materials by 15 % and more.
在这项工作中,研究了以氟塑料为基础、填充物为 WO3 的复合材料,并证明了其对 X 射线和伽马射线辐射的防护效率。开发了复合材料的生产技术方案,并对其物理和机械特性进行了研究。WO3 含量为 60 wt% 的复合材料具有以下特性:密度 3.35 ± 0.02 g/cm3、维氏显微硬度(300 g 负载时)5.38 ± 0.32 HV、抗弯强度 18.86 MPa。使用的 γ 辐射源为 E(207Bi) = 0.570 MeV,活度为 50 kBq;E(137Cs) = 0.662 MeV,活度为 9 kBq;E(60Co) = 1.252 MeV,活度为 100 kBq。X 射线辐射源是同位素 241Am(半衰期 T1/2 = 432.1 年;光子能量 E = 59.5 keV;放射性同位素活度 46 μCi)和 109Cd(半衰期 T1/2 = 461.4 年;光子能量 E = 88 keV;放射性同位素活度 15 μCi)。结果表明,要将能量为 1.252 MeV 的伽马射线减少 50%,需要使用厚度为 6.301 ± 0.654 厘米的纯氟塑料滤网,而对于含有 60 wt% WO3 的复合材料,滤网的厚度要小 1.5 倍(4.077 ± 0.509 厘米)。能量为 0.662 MeV 时的线性衰减系数与现代类似材料的比较证实了所开发材料的高效辐射防护性能。对样品进行辐射热改性后,其抗伽马射线辐射的能力提高了许多倍。经过辐射热改性后,氟塑料和 WO3 含量为 60 wt% 的复合材料的抗辐射能力分别提高到 1 ± 0.1 MGy 和 4.5 ± 0.2 MGy。两种材料的初始弯曲强度都提高了 15% 或更多。
{"title":"Radiation-thermal modification of fluoroplastic composite and evaluation of its radiation-protective characteristics","authors":"Vyacheslav Ivanovich Pavlenko ,&nbsp;Vitaliy Valerievich Kashibadze ,&nbsp;Anton Valerievich Noskov ,&nbsp;Roman Vladimirovich Sidelnikov ,&nbsp;Daria Aleksandrovna Ryzhikh ,&nbsp;Sergey Viktorovich Serebryakov","doi":"10.1016/j.matchemphys.2024.130162","DOIUrl":"10.1016/j.matchemphys.2024.130162","url":null,"abstract":"<div><div>In the work the composite on the basis of fluoroplastic with filler WO<sub>3</sub> is studied and its efficiency for protection against X-ray and gamma radiation is proved. The technological scheme of composite production has been developed and its physical and mechanical characteristics have been studied. The composite with 60 wt% of WO<sub>3</sub> content has the following properties: density 3.35 ± 0.02 g/cm<sup>3</sup>, Vickers microhardness (at 300 g load) 5.38 ± 0.32 HV, flexural strength 18.86 MPa. The γ-radiation sources used were E(<sup>207</sup>Bi) = 0.570 MeV with an activity of 50 kBq, E(<sup>137</sup>Cs) = 0.662 MeV with an activity of 9 kBq, and E(<sup>60</sup>Co) = 1.252 MeV with an activity of 100 kBq. The X-ray radiation sources were isotopes <sup>241</sup>Am (half-life T<sub>1/2</sub> = 432.1 years; photon energy E = 59.5 keV; radioisotope activity 46 μCi) and <sup>109</sup>Cd (half-life T<sub>1/2</sub> = 461.4 years; photon energy E = 88 keV; radioisotope activity 15 μCi). It is shown that for reduction of gamma radiation with energy 1.252 MeV by 50 % a screen from pure fluoroplastic with thickness of 6.301 ± 0.654 cm is required, and for composite with 60 wt% WO<sub>3</sub> the thickness of screen is 1.5 times less (4.077 ± 0.509 cm). Comparison of the linear attenuation coefficient at energy 0.662 MeV with modern analogs confirmed the high efficiency of radiation protection of the developed material. Radiation-thermal modification of the samples was carried out, which allowed to increase their radiation resistance to gamma radiation many times. After radiation-thermal modification the radiation resistance increased up to 1 ± 0.1 MGy and 4.5 ± 0.2 MGy for fluoroplastic and composite with 60 wt% WO<sub>3</sub> content, respectively. And the initial bending strength increased in both materials by 15 % and more.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"330 ","pages":"Article 130162"},"PeriodicalIF":4.3,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721718","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic effects of Carbon@MoS2 core-shell nanostructures on charge dynamics for future optoelectronic applications 碳@MoS2 核壳纳米结构对未来光电应用中电荷动力学的协同效应
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1016/j.matchemphys.2024.130147
Shreya, Soumya Rai, Peeyush Phogat, Ranjana Jha, Sukhvir Singh
The pursuit of advanced materials for enhancing optoelectronic device performance has led to significant interest in core-shell structures, which combine the unique properties of different materials to achieve superior functionality. This study investigates the hydrothermal synthesis of a series of core-shell Carbon@MoS2 materials with varying carbon concentrations, aiming to identify the optimal carbon content for enhanced optoelectronic applications. XRD analysis revealed the formation of new crystallographic phases, with crystallite sizes ranging from 1.39 nm to 23.1 nm, indicating significant structural modifications. UV–Vis analysis highlighted an expanded light absorption range and a reduction in bandgap up to 0.92 eV, particularly in carbon-loaded samples. Morphological analysis by FESEM and HRTEM confirmed the successful formation of core-shell nanospheres with well-defined MoS2 layers enveloping carbon cores. Electrochemical studies, including CV and PEIS, demonstrated that the sample CM4, with an optimal carbon concentration, exhibited balanced redox behavior, lower charge transfer resistance of 2860 Ω, and pronounced Warburg diffusion, marking it as the most effective composition for improving optoelectronic performance in future.
为了提高光电器件的性能,人们对先进材料的追求使得核壳结构备受关注,这种结构结合了不同材料的独特性能,从而实现了卓越的功能。本研究调查了一系列不同碳浓度的核壳 Carbon@MoS2 材料的水热合成,旨在确定增强光电应用的最佳碳含量。XRD 分析显示形成了新的结晶相,结晶尺寸从 1.39 纳米到 23.1 纳米不等,表明结构发生了显著变化。紫外可见光分析显示,光吸收范围扩大,带隙减小到 0.92 eV,特别是在碳负载样品中。利用 FESEM 和 HRTEM 进行的形貌分析证实,成功地形成了核壳纳米球,并在碳核外包覆了定义明确的 MoS2 层。包括 CV 和 PEIS 在内的电化学研究表明,具有最佳碳浓度的 CM4 样品表现出平衡的氧化还原行为、较低的电荷转移电阻(2860 Ω)和明显的沃伯格扩散,使其成为未来提高光电性能的最有效成分。
{"title":"Synergistic effects of Carbon@MoS2 core-shell nanostructures on charge dynamics for future optoelectronic applications","authors":"Shreya,&nbsp;Soumya Rai,&nbsp;Peeyush Phogat,&nbsp;Ranjana Jha,&nbsp;Sukhvir Singh","doi":"10.1016/j.matchemphys.2024.130147","DOIUrl":"10.1016/j.matchemphys.2024.130147","url":null,"abstract":"<div><div>The pursuit of advanced materials for enhancing optoelectronic device performance has led to significant interest in core-shell structures, which combine the unique properties of different materials to achieve superior functionality. This study investigates the hydrothermal synthesis of a series of core-shell Carbon@MoS<sub>2</sub> materials with varying carbon concentrations, aiming to identify the optimal carbon content for enhanced optoelectronic applications. XRD analysis revealed the formation of new crystallographic phases, with crystallite sizes ranging from 1.39 nm to 23.1 nm, indicating significant structural modifications. UV–Vis analysis highlighted an expanded light absorption range and a reduction in bandgap up to 0.92 eV, particularly in carbon-loaded samples. Morphological analysis by FESEM and HRTEM confirmed the successful formation of core-shell nanospheres with well-defined MoS<sub>2</sub> layers enveloping carbon cores. Electrochemical studies, including CV and PEIS, demonstrated that the sample CM4, with an optimal carbon concentration, exhibited balanced redox behavior, lower charge transfer resistance of 2860 Ω, and pronounced Warburg diffusion, marking it as the most effective composition for improving optoelectronic performance in future.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"329 ","pages":"Article 130147"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142663138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Assessing the heat storage potential of zeolitic imidazolate frameworks (ZIFs) using water and ethanol as working fluids
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1016/j.matchemphys.2024.130143
Ciara Byrne , Matjaž Mazaj , Nataša Zabukovec Logar
Zeolitic imidazolate frameworks (ZIFs) are comprised of transition metal cations such as Zn(II) and imidazolate-based ligands. Due to their inherent properties, including large surface areas, well-defined and stable porous structure, ZIFs hold significant promise for adsorption applications. Sorption-based heat storage and transformation with porous materials and water as working fluid has been recently recognized as one of the most promising approaches to address more efficient use of energy. In this study, we examined seven different ZIFs (ZIF-8, ZIF-62, ZIF-71, ZIF-74, ZIF-76, ZIF-90 and ZIF-93) and their heat storage potential using water and ethanol as working fluids. It has been demonstrated that storage performance is governed by several factors, including pore dimensions, type and distribution of functional groups on imidazolate ligands, chemical stability of the framework as well as the type of the working fluid. Ethanol sorption data demonstrates inflection points in sorption isotherms at lower relative pressures, enhancement of uptakes for ZIFs with hydrophobic properties, but lower desorption enthalpies if compared to water sorption. We found that ZIF-93 was the most promising material for both working fluids.
{"title":"Assessing the heat storage potential of zeolitic imidazolate frameworks (ZIFs) using water and ethanol as working fluids","authors":"Ciara Byrne ,&nbsp;Matjaž Mazaj ,&nbsp;Nataša Zabukovec Logar","doi":"10.1016/j.matchemphys.2024.130143","DOIUrl":"10.1016/j.matchemphys.2024.130143","url":null,"abstract":"<div><div>Zeolitic imidazolate frameworks (ZIFs) are comprised of transition metal cations such as Zn(II) and imidazolate-based ligands. Due to their inherent properties, including large surface areas, well-defined and stable porous structure, ZIFs hold significant promise for adsorption applications. Sorption-based heat storage and transformation with porous materials and water as working fluid has been recently recognized as one of the most promising approaches to address more efficient use of energy. In this study, we examined seven different ZIFs (ZIF-8, ZIF-62, ZIF-71, ZIF-74, ZIF-76, ZIF-90 and ZIF-93) and their heat storage potential using water and ethanol as working fluids. It has been demonstrated that storage performance is governed by several factors, including pore dimensions, type and distribution of functional groups on imidazolate ligands, chemical stability of the framework as well as the type of the working fluid. Ethanol sorption data demonstrates inflection points in sorption isotherms at lower relative pressures, enhancement of uptakes for ZIFs with hydrophobic properties, but lower desorption enthalpies if compared to water sorption. We found that ZIF-93 was the most promising material for both working fluids.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"332 ","pages":"Article 130143"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142743728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nitrogen, phosphorous co-doped carbon quantum dots as glucose and lactate sensor 作为葡萄糖和乳酸传感器的氮磷共掺杂碳量子点
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1016/j.matchemphys.2024.130149
H.J. Yashwanth , M. Madhukara Naik , M.S. Dileep , Murthy Muniyappa , M. Navya Rani
The present work emphases on the development of a sensor constructed based on the carbon quantum dots (CQDs) doped with heteroatoms such as nitrogen and phosphorous (NPCQDs) by one step microwave radiation assisted method. Cyclic voltammetry and chronoamperometry are used to investigate and compare the sensing performance of CQDs, nitrogen doped CQDs (NCQDs), phosphorous doped CQDs (CQDs) and NPCQDs towards glucose and lactate. It is observed that NPCQDs shows enhanced current response compared to CQDs, NCQDs and PCQDs due to the injection of extra electrons by dopants. Further, NPCQDs sensor exhibited good stability over 5000 s which is excellent in its class.
本研究通过一步微波辐射辅助法,重点开发了一种基于掺杂氮和磷等杂原子的碳量子点(CQDs)的传感器。利用循环伏安法和计时电流法研究和比较了 CQDs、掺氮 CQDs(NCQDs)、掺磷 CQDs(CQDs)和 NPCQDs 对葡萄糖和乳酸盐的传感性能。与 CQDs、NCQDs 和 PCQDs 相比,由于掺杂剂注入了额外的电子,NPCQDs 显示出更强的电流响应。此外,NPCQDs 传感器在 5000 秒内表现出良好的稳定性,在同类产品中非常出色。
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引用次数: 0
Thermal/pressure-induced transformation of C60(CF2) C60(CF2) 的热/压诱导转化
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1016/j.matchemphys.2024.130142
Victor A. Brotsman , Natalia S. Lukonina , Andrei A. Eliseev , Ilya N. Ioffe , Alexey A. Goryunkov , Fedor S. Khorobrykh , Sergei A. Klimin , Boris A. Kulnitskiy , Elena A. Skryleva , Igor B. Kutuza , Pavel V. Zinin , Mikhail Yu Popov
Homofullerenes are the class of fullerene derivatives where all fullerene carbon atoms remain in the sp2-state. This is facilitated by cleavage of the skeletal C–C bonds between the adjacent sites of attachment of divalent addends, e.g. certain types of >CX2 groups. Homofullerenes rarely reveal any important differences in optical and chemical properties compared to pristine fullerenes. Here we report an important novel example of such rare differences: formation of new fullerene polymer phases under thermal and high-pressure treatment as evidenced by the in situ and ex situ studies by means of Raman spectroscopy, HRTEM and XPS. Initially, C60(CF2) molecules undergo dimerization yielding double-caged multiply linked [C60(CF2)]2 dimers. High-pressure treatment of C60(CF2) with additional shear stress leads to phase transitions observed up to 27 GPa yielding high-pressure phases (IV and V) with partial defluorination. This behavior is qualitatively similar to that of pristine C60, but due to the presence of the CF2 moiety, the pressures required are 5–8 GPa higher compared to pristine C60. While the shear loads distort the crystal lattice of the C60(CF2) sample, interplane distances are preserved, indicatively of the lack of long polymeric fullerene chains typical of pristine C60. Most importantly, high-pressure phase V of C60(CF2) demonstrates a transition at 45 GPa yielding an even harder phase which remains stable under 45–80 GPa loads.
同富勒烯是一类富勒烯衍生物,其中所有富勒烯碳原子都保持在 sp2 状态。二价附加物(如某些类型的 CX2 基团)的相邻连接点之间的骨架 C-C 键的裂解促进了这种状态的形成。与原始富勒烯相比,同富勒烯很少在光学和化学性质上显示出重要差异。在此,我们报告了此类罕见差异的一个重要新实例:通过拉曼光谱、HRTEM 和 XPS 进行原位和非原位研究,证明在热处理和高压处理下形成了新的富勒烯聚合物相。最初,C60(CF2) 分子发生二聚化,产生双笼型多链路 [C60(CF2)]2 二聚体。用额外的剪切应力对 C60(CF2) 进行高压处理会导致相变,最高可观察到 27 GPa 的相变,产生具有部分脱氟的高压相(IV 和 V)。这种行为在性质上与原始 C60 相似,但由于 CF2 分子的存在,所需的压力比原始 C60 高 5-8 GPa。虽然剪切载荷会扭曲 C60(CF2) 样品的晶格,但平面间的距离保持不变,这表明原始 C60 中缺乏典型的长聚合物富勒烯链。最重要的是,C60(CF2) 的高压相 V 在 45 GPa 时发生了转变,产生了一种在 45-80 GPa 负载下保持稳定的更坚硬的相。
{"title":"Thermal/pressure-induced transformation of C60(CF2)","authors":"Victor A. Brotsman ,&nbsp;Natalia S. Lukonina ,&nbsp;Andrei A. Eliseev ,&nbsp;Ilya N. Ioffe ,&nbsp;Alexey A. Goryunkov ,&nbsp;Fedor S. Khorobrykh ,&nbsp;Sergei A. Klimin ,&nbsp;Boris A. Kulnitskiy ,&nbsp;Elena A. Skryleva ,&nbsp;Igor B. Kutuza ,&nbsp;Pavel V. Zinin ,&nbsp;Mikhail Yu Popov","doi":"10.1016/j.matchemphys.2024.130142","DOIUrl":"10.1016/j.matchemphys.2024.130142","url":null,"abstract":"<div><div>Homofullerenes are the class of fullerene derivatives where all fullerene carbon atoms remain in the <em>sp</em><sup>2</sup>-state. This is facilitated by cleavage of the skeletal C–C bonds between the adjacent sites of attachment of divalent addends, e.g. certain types of &gt;CX<sub>2</sub> groups. Homofullerenes rarely reveal any important differences in optical and chemical properties compared to pristine fullerenes. Here we report an important novel example of such rare differences: formation of new fullerene polymer phases under thermal and high-pressure treatment as evidenced by the <em>in situ</em> and <em>ex situ</em> studies by means of Raman spectroscopy, HRTEM and XPS. Initially, C<sub>60</sub>(CF<sub>2</sub>) molecules undergo dimerization yielding double-caged multiply linked [C<sub>60</sub>(CF<sub>2</sub>)]<sub>2</sub> dimers. High-pressure treatment of C<sub>60</sub>(CF<sub>2</sub>) with additional shear stress leads to phase transitions observed up to 27 GPa yielding high-pressure phases (IV and V) with partial defluorination. This behavior is qualitatively similar to that of pristine C<sub>60</sub>, but due to the presence of the CF<sub>2</sub> moiety, the pressures required are 5–8 GPa higher compared to pristine C<sub>60</sub>. While the shear loads distort the crystal lattice of the C<sub>60</sub>(CF<sub>2</sub>) sample, interplane distances are preserved, indicatively of the lack of long polymeric fullerene chains typical of pristine C<sub>60</sub>. Most importantly, high-pressure phase V of C<sub>60</sub>(CF<sub>2</sub>) demonstrates a transition at 45 GPa yielding an even harder phase which remains stable under 45–80 GPa loads.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"331 ","pages":"Article 130142"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A DFT and cluster expansion study of (Fe,Ni)9S8 pentlandite and unravelling doping with Mn, Co, Cu and precious metals 对(Fe,Ni)9S8戊兰特的 DFT 和聚类展开研究,以及对锰、钴、铜和贵金属掺杂的揭示
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1016/j.matchemphys.2024.130146
Kgwajana B. Molala, Peace P. Mkhonto, Mofuti A. Mehlape, Phuti E. Ngoepe
This study used density functional theory (DFT) adopting the universal cluster expansion (UNCLE) technique to generate different structures for (Fe,Ni)9S8 pentlandite and doped with Mn, Co, Cu and precious metals (Ru, Rh, Pd, Os, Ir and Pt) on the Ni and Fe tetrahedral (T) sites. The cluster expansion (CE) depicted the Fe-rich Fe5Ni4S8 structure with space-group of P42/nmc (tetragonal) as the most stable. The doped Fe5Ni4S8 structure on the Fe(T) with Mn, Cu, Rh, Pd, Ir and Pt changed from tetragonal to cubic structures, while doping with Co, Ru and Os remained tetragonal. Doping on the Ni(T) with Co, the structure changed from tetragonal to cubic, while doping with Mn, Cu, Ru, Rh, Pd, Os, Ir and Pt the structure remained tetragonal. It was found that doping with Pd on the Fe(T) generated the most thermodynamically stable compound (Fe3Pd2Ni4S8) with heats of formation of −130.24 meV. The density of states (DOS) showed that the Pd and Pt were the most preferred substitution of Fe(T) in the pentlandite structure, while the Co preferred the Ni(T) sites. In addition doping with Mn on Fe(T) and Ru doped on Ni(T) induced magnetism to the structure. This study predicted various compositions of dopants on pentlandite and laid a foundation for prediction of new mineral-compounds using DFT-CE method.
本研究利用密度泛函理论(DFT),采用通用聚类展开(UNCLE)技术,生成了(Fe,Ni)9S8戊土矿的不同结构,并在 Ni 和 Fe 的四面体(T)位上掺杂了 Mn、Co、Cu 和贵金属(Ru、Rh、Pd、Os、Ir 和 Pt)。团簇扩展(CE)显示,富含铁的 Fe5Ni4S8 结构最稳定,其空间群为 P42/nmc(四方)。在 Fe(T)上掺入 Mn、Cu、Rh、Pd、Ir 和 Pt 后,Fe5Ni4S8 结构从四方结构变为立方结构,而掺入 Co、Ru 和 Os 后则保持四方结构。在 Ni(T)中掺入 Co 后,其结构从四方结构变为立方结构,而掺入 Mn、Cu、Ru、Rh、Pd、Os、Ir 和 Pt 后,其结构仍为四方结构。研究发现,在铁(T)上掺入钯会产生热力学上最稳定的化合物(Fe3Pd2Ni4S8),其形成热为-130.24 meV。状态密度(DOS)显示,钯和铂是戊兰特结构中最优选的铁(T)取代位,而钴则优选镍(T)位。此外,在铁(T)上掺杂锰和在镍(T)上掺杂钌也会使结构产生磁性。这项研究预测了掺杂剂在戊兰特上的各种组成,为使用 DFT-CE 方法预测新的矿物化合物奠定了基础。
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引用次数: 0
Optimization of atomic layer deposited Pt-shell thickness of PtCu3@Pt/C catalyst for oxygen reduction reaction 优化用于氧还原反应的 PtCu3@Pt/C 催化剂的原子层沉积铂壳厚度
IF 4.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1016/j.matchemphys.2024.130145
Xuankai Zhao, Zhejie Ma, Xueru Li, Yujie Guo, Ping Li
A series of PtCu3@Pt/C catalysts with core@shell structure applicable to oxygen reduction reaction (ORR) were successfully synthesized by combining wet chemistry method for supported PtCu3/C preparation and atomic layer deposition (ALD) technique for Pt-shell covering PtCu3 nanoparticles. The oxygen adsorption energy on the surface of model PtCu3@Pt(111) based on density functional theory calculation revealed that the optimal oxygen adsorption strength suitable for ORR appears on the PtCu3@Pt(111) having few layers of Pt-shell. For this purpose, the Pt-shell thickness was precisely adjusted by varying the number of ALD cycles between 1 and 6, and four ALD cycles were found to deposit approximately one layer of Pt atoms on the surface of PtCu3 nanoparticles. In-depth investigation through material characterization verified the formation of PtCu3 alloy and the adjustability of Pt-shell thickness. Strain effect and electronic effects were observed between the PtCu3 core and Pt-shell, manifested as lattice compression of the Pt-shell and electron transfer from Pt band to Cu, both of which can downshift d-band center of the Pt-shell thus weakening the adsorption of oxygen species. The electrocatalytic performance of various PtCu3@PtALD-n/C (n = 1–6) catalysts was tested in the ORR process using rotating disk electrode approach. PtCu3@PtALD-4/C exhibited the maximum mass and specific activity among all catalysts, being 3.2 and 2.6 times higher than a commercial Pt/C catalyst, and much better as well than the PtCu3/C without Pt-shell. The durability of the PtCu3@PtALD-4/C catalyst was also superior to that of the PtCu3/C and Pt/C catalysts.
通过湿化学法制备支撑型PtCu3/C和原子层沉积(ALD)技术制备铂壳覆盖型PtCu3纳米颗粒,成功合成了一系列适用于氧还原反应(ORR)的核@壳结构PtCu3@Pt/C催化剂。基于密度泛函理论计算的模型 PtCu3@Pt(111) 表面的氧吸附能表明,适合 ORR 的最佳氧吸附强度出现在铂壳层数较少的 PtCu3@Pt(111) 上。为此,通过改变 1 至 6 次 ALD 周期来精确调节铂壳厚度,结果发现 4 次 ALD 周期可在 PtCu3 纳米粒子表面沉积约一层铂原子。通过材料表征进行的深入研究验证了 PtCu3 合金的形成和铂壳厚度的可调性。在 PtCu3 内核和 Pt 壳之间观察到了应变效应和电子效应,表现为 Pt 壳的晶格压缩和电子从 Pt 带转移到 Cu,这两种效应都会使 Pt 壳的 d 带中心下移,从而削弱对氧物种的吸附。采用旋转盘电极法测试了各种 PtCu3@PtALD-n/C(n = 1-6)催化剂在 ORR 过程中的电催化性能。在所有催化剂中,PtCu3@PtALD-4/C 的质量活性和比活性最高,分别是商用 Pt/C 催化剂的 3.2 倍和 2.6 倍,也远远优于不含铂壳的 PtCu3/C。PtCu3@PtALD-4/C 催化剂的耐久性也优于 PtCu3/C 和 Pt/C 催化剂。
{"title":"Optimization of atomic layer deposited Pt-shell thickness of PtCu3@Pt/C catalyst for oxygen reduction reaction","authors":"Xuankai Zhao,&nbsp;Zhejie Ma,&nbsp;Xueru Li,&nbsp;Yujie Guo,&nbsp;Ping Li","doi":"10.1016/j.matchemphys.2024.130145","DOIUrl":"10.1016/j.matchemphys.2024.130145","url":null,"abstract":"<div><div>A series of PtCu<sub>3</sub>@Pt/C catalysts with core@shell structure applicable to oxygen reduction reaction (ORR) were successfully synthesized by combining wet chemistry method for supported PtCu<sub>3</sub>/C preparation and atomic layer deposition (ALD) technique for Pt-shell covering PtCu<sub>3</sub> nanoparticles. The oxygen adsorption energy on the surface of model PtCu<sub>3</sub>@Pt(111) based on density functional theory calculation revealed that the optimal oxygen adsorption strength suitable for ORR appears on the PtCu<sub>3</sub>@Pt(111) having few layers of Pt-shell. For this purpose, the Pt-shell thickness was precisely adjusted by varying the number of ALD cycles between 1 and 6, and four ALD cycles were found to deposit approximately one layer of Pt atoms on the surface of PtCu<sub>3</sub> nanoparticles. In-depth investigation through material characterization verified the formation of PtCu<sub>3</sub> alloy and the adjustability of Pt-shell thickness. Strain effect and electronic effects were observed between the PtCu<sub>3</sub> core and Pt-shell, manifested as lattice compression of the Pt-shell and electron transfer from Pt band to Cu, both of which can downshift d-band center of the Pt-shell thus weakening the adsorption of oxygen species. The electrocatalytic performance of various PtCu<sub>3</sub>@Pt<sub>ALD-n</sub>/C (n = 1–6) catalysts was tested in the ORR process using rotating disk electrode approach. PtCu<sub>3</sub>@Pt<sub>ALD-4</sub>/C exhibited the maximum mass and specific activity among all catalysts, being 3.2 and 2.6 times higher than a commercial Pt/C catalyst, and much better as well than the PtCu<sub>3</sub>/C without Pt-shell. The durability of the PtCu<sub>3</sub>@Pt<sub>ALD-4</sub>/C catalyst was also superior to that of the PtCu<sub>3</sub>/C and Pt/C catalysts.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"329 ","pages":"Article 130145"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142663139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","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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Materials Chemistry and Physics
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