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Doping stimulated ferromagnetic ordering and tailoring of the dielectric properties of Ba1−xCexTiO3† 掺杂激发铁磁有序和定制 Ba1-xCexTiO3† 的介电性能
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1039/D4MA00593G
Rahul Sharma, Shreya Sinha, Rahul Singh, Saurabh Pathak, Barsha Borgohain, Noor Jahan and N. S. Negi

The concurrent integration of ferroelectricity and ferromagnetism in BaTiO3 (BT) introduces a promising paradigm for multifunctional applications. This study delves into the structural, magnetic, and dielectric characteristics of Ba1−xCexTiO3 (BCT) ceramics with Ce substitution varying from 0 to 2%. Notably, BT in its pristine state exhibited weak ferromagnetism at a lower applied magnetic field. However, the introduction of Ce3+ led to an augmentation in the Ms values, attributed to the elevated presence of oxygen vacancies. Rietveld analysis of the X-ray diffraction patterns and the Raman spectra of all the samples revealed the unaltered tetragonal structure of BT despite increasing the Ce content to 1.5%. Simultaneously, an increase in the unit cell volume and crystalline size was noted, whereas the tetragonality factor (c/a) diminished with increasing Ce substitution. Field emission scanning electron microscopy (FESEM) analysis highlighted a transition in the average grain size from 738 nm to 899 nm with increasing Ce content. The investigation of dielectric properties showed a proportional reduction in the dielectric constant with increasing Ce concentration. Additionally, dielectric measurements revealed that AC conductivity increased with frequency, and Ce doping further enhanced the conductivity by introducing additional charge carriers. Despite the reduction in the dielectric constant, the minimal dielectric loss made these materials highly suitable for high-frequency applications. This study underscores the significance of Ce incorporation into BT, introducing magnetic behaviour to an otherwise non-magnetic, lead-free BT system. The observed phenomena open avenues for exploring previously limited multiferroic and magnetoelectric properties of BT ceramics, a promising direction in the realm of lead-free ferroelectrics.

在 BaTiO3(BT)中同时集成铁电性和铁磁性为多功能应用引入了一种前景广阔的范例。本研究深入探讨了 Ba1-xCexTiO3 (BCT) 陶瓷的结构、磁性和介电特性,其中 Ce 的替代率从 0% 到 2%不等。值得注意的是,原始状态的 BCT 在较低的外加磁场下表现出弱铁磁性。然而,Ce3+ 的引入导致 Ms 值增加,这归因于氧空位的增加。对所有样品的 X 射线衍射图样和拉曼光谱进行的里特维尔德分析表明,尽管 Ce 的含量增加到了 1.5%,但 BT 的四方结构没有改变。同时,样品的单胞体积和结晶尺寸都有所增加,而四方系数(c/a)则随着铈取代量的增加而减小。场发射扫描电子显微镜(FESEM)分析显示,随着 Ce 含量的增加,平均晶粒尺寸从 738 纳米变为 899 纳米。介电性能调查显示,随着 Ce 浓度的增加,介电常数成比例地降低。此外,介电测量显示交流电导率随频率的增加而增加,而掺杂 Ce 则通过引入额外的电荷载流子进一步提高了电导率。尽管介电常数降低了,但最小的介电损耗使这些材料非常适合高频应用。这项研究强调了在 BT 中掺入 Ce 的重要性,它为原本无磁的无铅 BT 系统引入了磁性。所观察到的现象为探索 BT 陶瓷以前有限的多铁性和磁电性能开辟了道路,是无铅铁电领域中一个很有前途的方向。
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引用次数: 0
Eradication of planktonic bacteria by shape-tailored gold nanoparticle photothermia† 通过形状定制的金纳米粒子光热技术消灭浮游细菌†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1039/D4MA00821A
Zhendong Peng, Laurent Royon, Yun Luo, Philippe Decorse, Sarra Gam Derouich, Michaël Bosco, Christine Gravier-Pelletier, Romain Briandet, John S. Lomas, Claire Mangeney and Miryana Hémadi

Bacterial antimicrobial resistance (AMR) has emerged as a global challenge, exacerbated by the formation of biofilms. To address this issue, the bactericidal effect of gold nanoparticle photothermia has been explored. Gold nanoparticles with different morphologies: spherical (AuNSP), rods (AuNRO), stars (AuNST), and flower-shaped (AuNFL) were synthesised and characterised. Scanning and transmission electron microscopy images confirm the morphologies and give dimensions for the different types of nanoparticles in good agreement with those from dynamic light scattering measurements. Their photothermal capacities under irradiation at 808 and 1064 nm were assessed. The specific absorption rates were determined, and light-to-heat conversion efficiencies evaluated in the heating and cooling phases. Phothermally induced localized hyperthermia significantly increased the mortality rate of planktonic Escherichia coli in the stationary phase, approaching 100% for AuNRO, AuNST, and AuNFL, while AuNSP was ineffective. This demonstrates that bactericidal efficacy is highly dependent on nanoparticle morphology. These findings highlight the potential of shape-tailored gold nanoparticles for developing effective antibacterial treatments.

细菌的抗菌药耐药性(AMR)已成为一项全球性挑战,生物膜的形成更加剧了这一问题。为解决这一问题,人们探索了金纳米粒子光热的杀菌效果。研究人员合成并鉴定了不同形态的金纳米粒子:球形(AuNSP)、棒形(AuNRO)、星形(AuNST)和花形(AuNFL)。扫描和透射电子显微镜图像证实了这些形态,并给出了不同类型纳米粒子的尺寸,与动态光散射测量结果十分吻合。评估了它们在 808 和 1064 纳米波长照射下的光热能力。测定了比吸收率,并评估了加热和冷却阶段的光热转换效率。光热诱导的局部高热显著提高了静止期浮游大肠杆菌的死亡率,AuNRO、AuNST 和 AuNFL 的死亡率接近 100%,而 AuNSP 则无效。这表明杀菌效果与纳米粒子的形态有很大关系。这些发现凸显了形状定制金纳米粒子在开发有效抗菌疗法方面的潜力。
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引用次数: 0
ZnO vapor phase infiltration into photo-patternable polyacrylate networks for the microfabrication of hybrid organic–inorganic structures† 将氧化锌气相渗入可光图案化的聚丙烯酸酯网络,实现有机-无机混合结构的微细加工†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1039/D4MA00733F
Lisanne Demelius, Li Zhang, Anna Maria Coclite and Mark D. Losego

Photopatterning of polymers enables the microfabrication of numerous microelectronic, micromechanical, and microchemical systems. The incorporation of inorganics into a patterned polymer material can generate many new interesting properties such as enhanced stability, optical performance, or electrical properties. Vapor phase infiltration (VPI) allows for the creation of hybrid organic–inorganic materials by infiltrating polymers with gaseous metalorganic precursors. This study seeks to explore the potential of integrating VPI with existing photopatterning techniques to achieve top-down hybridization and property modification of polymer structures of different complexity. For this, VPI of diethylzinc (DEZ) is studied for four highly crosslinked acrylate networks that can be patterned by photolithography and two-photon polymerization (2PP): pentaerythritol triacrylate (PETA), pentaerythritol tetraacrylate (PETeA), trimethylolpropane triacrylate (TMPTA) and ethoxylated trimethylolpropane triacrylate (ETPTA). The findings show that for highly crosslinked polymer networks, VPI can be limited by slow precursor diffusion. However, by introducing flexible segments (e.g., ethoxylated chains), the polymer's free volume can be increased, and infiltration is accelerated, leading to faster infiltration times and higher and more uniform inorganic loading. Finally, selective infiltration of ZnO into photolithographically patterned copolymer networks of TMPTA and ETPTA on non-infiltrating poly(methyl methacrylate) (PMMA) is demonstrated illustrating the potential of VPI for advanced maskless patterning strategies.

通过对聚合物进行光图案化处理,可以对许多微电子、微机械和微化学系统进行微加工。在图案化聚合物材料中加入无机物可产生许多有趣的新特性,如增强稳定性、光学性能或电学特性。气相渗透(VPI)技术可通过将气态金属有机前驱体渗透到聚合物中来制造有机-无机混合材料。本研究旨在探索将 VPI 与现有光刻技术相结合的潜力,以实现自上而下的杂化,并对不同复杂程度的聚合物结构进行性能改性。为此,针对四种可通过光刻和双光子聚合(2PP)技术图案化的高交联丙烯酸酯网络,研究了二乙基锌(DEZ)的 VPI:季戊四醇三丙烯酸酯(PETA)、季戊四醇四丙烯酸酯(PETeA)、三羟甲基丙烷三丙烯酸酯(TMPTA)和乙氧基化三羟甲基丙烷三丙烯酸酯(ETPTA)。研究结果表明,对于高度交联的聚合物网络,VPI 可能会受到缓慢的前体扩散的限制。然而,通过引入柔性段(如乙氧基链),聚合物的自由体积可以增加,浸润速度也会加快,从而加快浸润时间,提高无机负载的均匀性。最后,在非浸润性聚甲基丙烯酸甲酯(PMMA)上的 TMPTA 和 ETPTA 的光刻图案化共聚物网络中选择性地浸润氧化锌,说明了 VPI 在先进的无掩模图案化策略方面的潜力。
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引用次数: 0
Thiourea-based rotaxanes: anion transport across synthetic lipid bilayers and antibacterial activity against Staphylococcus aureus† 基于硫脲的轮烷:阴离子在合成脂质双分子层上的转运以及对金黄色葡萄球菌的抗菌活性。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1039/D4MA00794H
Nasim Akhtar, Udyogi N. K. Conthagamage, Sara P. Bucher, Zuliah A. Abdulsalam, Macallister L. Davis, William N. Beavers and Víctor García-López

We report the synthesis of two rotaxanes (1 and 2) whose rings have appended thiourea units for the selective recognition of Cl anions. Rotaxane 1 transports Cl across synthetic lipid bilayers more efficiently than 2, exhibiting EC50 values of 0.243 mol% versus 0.736 mol%, respectively. A control rotaxane (3) without the thiourea units and the individual axle (4) also showed Cl transport, although with much lower efficiency (EC50 values of 4.044 mol% and 4.986 mol%). The unthreaded ring (5) showed the lowest transport activity. This trend highlights the advantage of the interlocked system with a ring containing thiourea units. We also investigated how the membrane composition of liposomes influences the transport activity of 1 and 2, observing higher Cl transport in membranes with higher fluidity. Additionally, we demonstrated that rotaxane 1 can kill drug-resistant and osmotolerant Staphylococcus aureus when used in combination with NaCl or arachidonic acid. The latter is known to increase the fluidity of the membrane in S. aureus, highlighting cooperative behavior. This work provides new insights into how various structural features and the membrane environment influence the anion transport activity of rotaxanes, offering important design principles for optimizing future rotaxanes for biomedical and other applications.

我们报告了两种轮烷(1 和 2)的合成情况,这两种轮烷的环上都附有选择性识别 Cl- 阴离子的硫脲单元。轮烷 1 在合成脂质双分子层中转运 Cl- 的效率高于轮烷 2,其 EC50 值分别为 0.243 mol% 和 0.736 mol%。不含硫脲单元的对照组轮烷(3)和单个轴(4)也显示出 Cl- 的转运,但效率要低得多(EC50 值分别为 4.044 摩尔%和 4.986 摩尔%)。无螺纹环(5)的运输活性最低。这一趋势凸显了含有硫脲单元的环状互锁系统的优势。我们还研究了脂质体的膜组成如何影响 1 和 2 的运输活性,观察到流动性较高的膜具有较高的 Cl- 运输能力。此外,我们还证明了轮烷 1 与氯化钠或花生四烯酸结合使用时,可以杀死耐药和耐渗透的金黄色葡萄球菌。众所周知,花生四烯酸能增加金黄色葡萄球菌膜的流动性,从而突显合作行为。这项研究为了解各种结构特征和膜环境如何影响轮烷的阴离子转运活性提供了新的视角,为优化未来轮烷的生物医学和其他应用提供了重要的设计原则。
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引用次数: 0
The effect of aliovalent dopants on the structural and transport properties of Li6La2BaTa2O12 garnet Li-ion solid electrolytes† 别价掺杂剂对 Li6La2BaTa2O12 石榴石锂离子固体电解质结构和传输特性的影响†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1039/D4MA00679H
Marco Amores, Peter J. Baker, Edmund J. Cussen and Serena A. Cussen

Li-rich garnet solid electrolytes are promising candidates for all-solid-state batteries, allowing for increased energy densities, compatibility with Li-metal anodes and improved safety by replacing flammable organic-based liquid electrolytes. Li-stuffed garnets typically require aliovalent doping to stabilise the highly ionic conductive Iad cubic phase. The role of dopants and their location within the garnet framework can greatly affect the conduction properties of these garnets, yet their impact on the structure and resulting ion transport is not fully understood. Here, we evaluate the effect of aliovalent doping with Al3+, Ga3+ and Zn2+ in the Li6BaLa2Ta2O12 (LBLTO) garnet material. A combination of PXRD and XAS reveals a linear cell parameter contraction with an increase in doping and the preference of the 24d Li+ sites for Al3+ and Zn2+ dopants, with Ga3+ occupying both the 24d and 48g Li+ sites. Macroscopic ionic conductivity analyses by EIS demonstrate an enhancement of the transport properties where addition of small amounts of Al3+ decreases the activation energy to Li+ diffusion to 0.35(4) eV. A detrimental effect on ionic conductivities is observed when dopants were introduced in Li+ pathways and upon decreasing the Li+ concentration. Insights into this behaviour are gleaned from microscopic diffusion studies by muon spin relaxation (μ+SR) spectroscopy, which reveals a low activation energy barrier for Li+ diffusion of 0.16(1) eV and a diffusion coefficient comparable to those of Li7La3Zr2O12 (LLZO) benchmark garnet materials.

富锂石榴石固体电解质是全固态电池的理想候选材料,可提高能量密度,与锂金属阳极兼容,并通过取代易燃的有机液态电解质提高安全性。锂填充石榴石通常需要异价掺杂,以稳定高离子导电性的 Iad 立方相。掺杂剂的作用及其在石榴石框架中的位置会极大地影响这些石榴石的传导性能,但它们对结构和由此产生的离子传输的影响尚未完全明了。在这里,我们评估了在 Li6BaLa2Ta2O12(LBLTO)石榴石材料中掺入 Al3+、Ga3+ 和 Zn2+ 等价物的效果。结合 PXRD 和 XAS 可以发现,随着掺杂量的增加,电池参数呈线性收缩,Al3+ 和 Zn2+掺杂剂偏好 24d Li+ 位点,而 Ga3+ 则同时占据 24d 和 48g Li+ 位点。通过 EIS 进行的宏观离子传导性分析表明,加入少量 Al3+ 后,Li+扩散的活化能降低到 0.35(4) eV,从而增强了传输特性。在 Li+ 通路中引入掺杂剂以及降低 Li+ 浓度时,离子传导性会受到不利影响。通过μ子自旋弛豫(μ+SR)光谱进行的微观扩散研究揭示了这一行为,该研究显示 Li+ 扩散的低活化能势垒为 0.16(1) eV,扩散系数与 Li7La3Zr2O12 (LLZO) 基准石榴石材料相当。
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引用次数: 0
Fast preparation of adhesive, anti-freezing hydrogels with strain- and magnetic-responsive conductivities† 快速制备具有应变和磁响应导电性能的粘合型抗冻水凝胶†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1039/D4MA00642A
Xinyu He, Xinyi Huang, Shuai He, Wei Zhang, Xinhua Li, Yong You and Fang Zuo

Incorporation of magnetic components enables flexible conductive hydrogels to exhibit strain-response properties in the presence of a magnetic field. However, the utilization of flexible conductive hydrogels is constrained under low-temperature conditions, and the mechanical properties of most magnetic hydrogels are poor. In this work, a conductive sensor was developed through Ca2+-initiated radical polymerization, utilizing the synergistic effects of sodium lignosulfonate (SL), calcium chloride (CaCl2), and Fe3O4@laponites (XLG). Fe3O4@XLG not only served as a physical crosslinking agent but also functioned as a magnetic component. Due to the presence of both physical and chemical crosslinking, the Ca2+-Fe3O4@XLG/SL/polyacrylamide (PAM) hydrogel had good mechanical properties. After being placed at −20 °C for 24 h, the Ca2+-Fe3O4@XLG/SL/PAM hydrogel remained intact, soft, and tough, and it still exhibited good stretchability (1029%) and strength (69.7 kPa). In addition, the hydrogel also exhibited good adhesion with various substrates. Strain sensors assembled from the nanocomposite hydrogels achieved a gauge factor of 5.14, a response time of 166 ms, and good stability. The Ca2+-Fe3O4@XLG/SL/PAM hydrogels had magnetic response properties, and they could respond quickly to magnetic field changes in the form of resistance changes. Thus, they have potential applications in magnetic field signal monitoring and soft actuators.

加入磁性成分可使柔性导电水凝胶在磁场作用下表现出应变响应特性。然而,在低温条件下,柔性导电水凝胶的使用受到限制,而且大多数磁性水凝胶的机械性能较差。在这项工作中,利用木质素磺酸钠(SL)、氯化钙(CaCl2)和 Fe3O4@皂石(XLG)的协同作用,通过 Ca2+ 引发的自由基聚合,开发了一种导电传感器。Fe3O4@XLG不仅是一种物理交联剂,也是一种磁性成分。由于同时存在物理和化学交联,Ca2+-Fe3O4@XLG/SL/聚丙烯酰胺(PAM)水凝胶具有良好的机械性能。将 Ca2+-Fe3O4@XLG/SL/PAM 水凝胶在 -20 °C 下放置 24 小时后,它仍然保持完整、柔软和坚韧,并表现出良好的伸展性(1029%)和强度(69.7 kPa)。此外,该水凝胶还与各种基底具有良好的粘附性。用纳米复合水凝胶组装的应变传感器的测量系数为 5.14,响应时间为 166 毫秒,并且具有良好的稳定性。Ca2+-Fe3O4@XLG/SL/PAM 水凝胶具有磁响应特性,能以电阻变化的形式快速响应磁场变化。因此,它们在磁场信号监测和软致动器方面具有潜在的应用前景。
{"title":"Fast preparation of adhesive, anti-freezing hydrogels with strain- and magnetic-responsive conductivities†","authors":"Xinyu He, Xinyi Huang, Shuai He, Wei Zhang, Xinhua Li, Yong You and Fang Zuo","doi":"10.1039/D4MA00642A","DOIUrl":"https://doi.org/10.1039/D4MA00642A","url":null,"abstract":"<p >Incorporation of magnetic components enables flexible conductive hydrogels to exhibit strain-response properties in the presence of a magnetic field. However, the utilization of flexible conductive hydrogels is constrained under low-temperature conditions, and the mechanical properties of most magnetic hydrogels are poor. In this work, a conductive sensor was developed through Ca<small><sup>2+</sup></small>-initiated radical polymerization, utilizing the synergistic effects of sodium lignosulfonate (SL), calcium chloride (CaCl<small><sub>2</sub></small>), and Fe<small><sub>3</sub></small>O<small><sub>4</sub></small>@laponites (XLG). Fe<small><sub>3</sub></small>O<small><sub>4</sub></small>@XLG not only served as a physical crosslinking agent but also functioned as a magnetic component. Due to the presence of both physical and chemical crosslinking, the Ca<small><sup>2+</sup></small>-Fe<small><sub>3</sub></small>O<small><sub>4</sub></small>@XLG/SL/polyacrylamide (PAM) hydrogel had good mechanical properties. After being placed at −20 °C for 24 h, the Ca<small><sup>2+</sup></small>-Fe<small><sub>3</sub></small>O<small><sub>4</sub></small>@XLG/SL/PAM hydrogel remained intact, soft, and tough, and it still exhibited good stretchability (1029%) and strength (69.7 kPa). In addition, the hydrogel also exhibited good adhesion with various substrates. Strain sensors assembled from the nanocomposite hydrogels achieved a gauge factor of 5.14, a response time of 166 ms, and good stability. The Ca<small><sup>2+</sup></small>-Fe<small><sub>3</sub></small>O<small><sub>4</sub></small>@XLG/SL/PAM hydrogels had magnetic response properties, and they could respond quickly to magnetic field changes in the form of resistance changes. Thus, they have potential applications in magnetic field signal monitoring and soft actuators.</p>","PeriodicalId":18242,"journal":{"name":"Materials Advances","volume":" 21","pages":" 8629-8637"},"PeriodicalIF":5.2,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ma/d4ma00642a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142524265","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A dual functional Cu(ii)-coordination polymer and its rGO composite for selective solvent detection and high performance energy storage† 用于选择性溶剂检测和高性能能量储存的双功能铜(ii)配位聚合物及其 rGO 复合材料†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1039/D4MA00762J
Basree, Waris, Arif Ali, Nishat Khan, Mohammad Zain Khan, Ganesh Chandra Nayak, Kafeel Ahmad Siddiqui and Musheer Ahmad

Herein, the fabrication of a new Cu(II)-based coordination polymer {[Cu2(DPP)2(H2O)2]·DPP·2NO3}n (CP-1) (DPP = 1,3-di(4-pyridyl)propane) and its composite (rGO@CP-1) has been done using solvothermal and mechanochemical methods. The crystal structure of the synthesized CP-1 was confirmed utilizing single-crystal X-ray diffraction (SC-XRD). Furthermore, the structural features of the as-synthesized CP-1 and rGO@CP-1 were examined using PXRD, FTIR, TGA, SEM, and HR-TEM analysis. The topological framework of CP-1 shows a 1,3M4-1 underlying net for two fragments and the hydrogen-bonded network shows a 2C1 underlying net topology. The fluorescence detection of transition metal ions and solvents using CP-1 showed promising results of 97.4% DMF and 96.8% Zn2+. Electrochemical study of CP-1 and rGO@CP-1 was performed in an acidic medium (1 M H2SO4) electrolyte utilizing cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD) techniques with a specific capacity of 244.17 F g−1 and 899.54 F g−1 for CP-1 and rGO@CP-1, respectively at 1 A g−1 (current density). Moreover, 98.6% columbic efficiency with 94.62% capacity retention of rGO@CP-1 was obtained at 8 A g−1 up to 2000 cycles.

本文采用溶热法和机械化学法制备了一种新的铜(II)基配位聚合物{[Cu2(DPP)2(H2O)2]-DPP-2NO3}n(CP-1)(DPP = 1,3-二(4-吡啶基)丙烷)及其复合材料(rGO@CP-1)。利用单晶 X 射线衍射 (SC-XRD) 确认了合成的 CP-1 的晶体结构。此外,还利用 PXRD、FTIR、TGA、SEM 和 HR-TEM 分析法研究了合成的 CP-1 和 rGO@CP-1 的结构特征。CP-1 的拓扑框架显示出两个片段的 1,3M4-1 底网,氢键网络显示出 2C1 底网拓扑。使用 CP-1 对过渡金属离子和溶剂进行荧光检测,结果表明,DMF 和 Zn2+ 的荧光检测结果分别为 97.4% 和 96.8%。在酸性介质(1 M H2SO4)电解液中,利用循环伏安法(CV)和电静态充放电(GCD)技术对 CP-1 和 rGO@CP-1 进行了电化学研究,在 1 A g-1 (电流密度)条件下,CP-1 和 rGO@CP-1 的比容量分别为 244.17 F g-1 和 899.54 F g-1。此外,在 8 A g-1 下,rGO@CP-1 的荷电效率为 98.6%,容量保持率为 94.62%,循环次数达 2000 次。
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引用次数: 0
Re-engineering lysozyme solubility and activity through surfactant complexation† 通过表面活性剂复合重新设计溶菌酶的溶解性和活性†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1039/D4MA00720D
Jiaming Mu, Leran Mao, Gavin P. Andrews and Sheiliza Carmali

Hydrophobic ion-pairing is an established solubility engineering technique that uses amphiphilic surfactants to modulate drug lipophilicity and facilitate encapsulation in polymeric and lipid-based drug delivery systems. For proteins, surfactant complexation can also lead to unfolding processes and loss in bioactivity. In this study, we investigated the impact of two surfactants, sodium dodecyl sulphate (SDS) and dioctyl sulfosuccinate (DOSS) on lysozyme's solubility, activity, and structure. SDS and DOSS were combined with lysozyme at increasing charge ratios (4 : 1, 2 : 1, 1 : 1, 1 : 2 and 1 : 4) via hydrophobic ion pairing at pH 4.5. Maximum complexation efficiency at the 1 : 1 charge ratio was confirmed by protein quantitation assays and zeta potential measurements, showing a near neutral surface charge. Lysozyme lipophilicity was successfully increased, with log D n-octanol/PBS values up to 2.5 with SDS and 1.8 with DOSS. Bioactivity assays assessing lysis of M. lysodeikticus cell walls showed up to a 2-fold increase in lysozyme's catalytic ability upon complexation with SDS at ratios less than stoichiometric, suggesting favourable mechanisms of stabilisation. Secondary structural analysis using Fourier-transform infrared spectroscopy indicated that lysozyme underwent a partial unfolding process upon complexation with low SDS concentrations. Molecular dynamic simulations further confirmed that at these low concentrations, a positive conformation was obtained with the active site residue Glu 35 more solvent-exposed. Combined, this suggested that sub-stoichiometric SDS altered the active site's secondary structure through increased backbone flexibility, leading to higher substrate accessibility. For DOSS, low surfactant concentrations retained lysozyme's native function and structure while still increasing the protein's lipophilic character. Our research findings demonstrate that modulation of protein activity can be related to surfactant chemistry and that controlled ion-pairing can lead to re-engineering of lysozyme solubility, activity, and structure. This has significant implications for advanced protein applications in healthcare, particularly towards the development of formulation strategies for oral biotherapeutics.

疏水离子配对是一种成熟的溶解度工程技术,它使用两亲性表面活性剂来调节药物的亲油性,并促进聚合物和脂质给药系统的封装。对于蛋白质来说,表面活性剂复合物也会导致蛋白质的折叠过程和生物活性的丧失。在本研究中,我们研究了十二烷基硫酸钠(SDS)和磺基琥珀酸二辛酯(DOSS)这两种表面活性剂对溶菌酶的溶解度、活性和结构的影响。在 pH 值为 4.5 的条件下,通过疏水离子配对,溶菌酶与 SDS 和 DOSS 的电荷比(4:1、2:1、1:1、1:2 和 1:4)依次增加。电荷比为 1 :蛋白质定量检测和 zeta 电位测量证实了 1 : 1 电荷比时的最高复合效率,显示出接近中性的表面电荷。溶菌酶的亲脂性成功得到了提高,SDS 和 DOSS 的正辛醇/PBS 对数值分别达到了 2.5 和 1.8。评估溶菌酶细胞壁裂解情况的生物活性测定显示,溶菌酶与 SDS 复配后,其催化能力最多可提高 2 倍,而复配比例却小于化学计量比,这表明溶菌酶具有有利的稳定机制。利用傅立叶变换红外光谱进行的二级结构分析表明,溶菌酶在与低浓度 SDS 复配时经历了部分解折过程。分子动力学模拟进一步证实,在这些低浓度条件下,活性位点残基 Glu 35 的溶剂暴露程度较高,从而获得了正构象。综合来看,这表明亚计量 SDS 通过增加骨架的灵活性改变了活性位点的二级结构,从而提高了底物的可及性。就 DOSS 而言,低浓度表面活性剂保留了溶菌酶的原生功能和结构,同时仍增加了蛋白质的亲脂性。我们的研究结果表明,蛋白质活性的调节与表面活性剂的化学性质有关,受控的离子配对可以重新设计溶菌酶的溶解性、活性和结构。这对高级蛋白质在医疗保健领域的应用,尤其是口服生物治疗剂配方策略的开发具有重要意义。
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引用次数: 0
From non-aqueous liquid to solid-state Li–S batteries: design protocols, challenges and solutions 从非水液态锂电池到固态锂电池:设计规程、挑战和解决方案
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-30 DOI: 10.1039/D4MA00666F
Yuxuan Zhang, Fei Qin, Jinwook Baek, Dong Hun Lee, Minyoung Kim, Han-Wook Song and Sunghwan Lee

Traditional Lithium-ion batteries may not satisfy the requirements of advanced batteries, demanding higher energy and power density, broader operating temperature ranges, and faster charging speeds. Solid-state Li–S batteries (SSLSBs) offer significant advantages, including higher theoretical specific capacity, cost-effectiveness, and environmental benefits. This mini-review exclusively introduces design protocols with emphasis on key governing parameters of SSLSBs towards achieving a specific energy of more than 500 W h kg−1. In addition, the distinct fading mechanisms of SSLSBs compared to non-aqueous electrolyte systems and other ASSB systems are summarized and compared. Then, we outline the state-of-the-art strategies to enhance the electrochemical performance of SSLSBs and suggest insightful directions for future research. This review may be of significance to the design of advanced SSLSBs, by mitigating technical challenges, and hence facilitating their practical implementation in energy storage technologies.

传统的锂离子电池可能无法满足先进电池的要求,它们需要更高的能量和功率密度、更宽的工作温度范围和更快的充电速度。固态锂离子电池(SSLSB)具有显著的优势,包括更高的理论比容量、成本效益和环境效益。这篇微型综述专门介绍了固态锂电池的设计协议,重点是固态锂电池实现比能量超过 500 W h kg-1 的关键管理参数。此外,还总结并比较了 SSLSB 与非水电解质系统和其他 ASSB 系统的不同衰减机制。然后,我们概述了提高 SSLSB 电化学性能的最新策略,并为未来的研究提出了富有洞察力的方向。这篇综述可能对设计先进的 SSLSBs 具有重要意义,因为它可以减轻技术挑战,从而促进其在储能技术中的实际应用。
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引用次数: 0
Bio-inspired 3D printing of layered structures utilizing stabilized amorphous calcium carbonate within biodegradable matrices† 利用生物可降解基质中的稳定无定形碳酸钙进行分层结构的生物启发 3D 打印†。
IF 5.2 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-30 DOI: 10.1039/D4MA00580E
Hadar Shaked, Daniela Dobrynin, Iryna Polishchuk, Alexander Katsman and Boaz Pokroy

Many composites in nature are formed in the course of biomineralization. These biocomposites are often produced via an amorphous precursor such as amorphous calcium carbonate (ACC), demonstrating a layered structure. In the current study, robocasting, a 3D-printing technique, was used to print layered structures inspired by the mineralized tissues of Ophiomastix wendtii and Odontodactylus scyllarus, which exhibit a layered organization. Various biodegradable organic matrices with a high percentage (>94%) of ACC reinforcements were compared, and their mechanical properties were studied. With the organic matrix protection, ACC was stabilized for long periods, exceeding even three years, when stored at ambient conditions. The layered structures were printed and fractured using the three-point bending method to evaluate their strength. The fracture interface was examined to weigh the benefits an amorphous precursor may offer in the 3D printing processes of ceramic materials. The fracture interface presented bulk behavior with no distinct layering, resembling the formation of mineral single crystalline tissue in nature and overcoming one of the most critical challenges in 3D printing, namely the inter-layer interfaces. Herein, a bio-inspired, low-temperature route to form layered structures is presented. By fusing the layers together following low-temperature sintering, a composite structure composed of stabilized ACC integrated with biodegradable, environmentally friendly matrices can be obtained.

自然界中的许多复合材料都是在生物矿化过程中形成的。这些生物复合材料通常是通过无定形前体(如无定形碳酸钙(ACC))产生的,并呈现出分层结构。在当前的研究中,受 Ophiomastix wendtii 和 Odontodactylus scyllarus 矿化组织的启发,使用了机器人铸造这种三维打印技术来打印分层结构。我们比较了含有高比例(94%)ACC 增强材料的各种可生物降解有机基质,并研究了它们的机械性能。在有机基质的保护下,ACC 在环境条件下可长期稳定保存,甚至超过三年。对分层结构进行了打印,并使用三点弯曲法对其进行断裂,以评估其强度。对断裂界面进行了检查,以权衡无定形前驱体在陶瓷材料 3D 打印过程中可能带来的益处。断裂界面呈现出没有明显分层的块状行为,类似于自然界中矿物单晶组织的形成,克服了三维打印中最关键的挑战之一,即层间界面。本文介绍了一种受生物启发的低温形成分层结构的方法。通过在低温烧结后将各层融合在一起,可获得由稳定的 ACC 与可生物降解的环保基质组成的复合结构。
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