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Multifunctional ionic liquid to extend the expiration date of precursor solution for perovskite photovoltaics 延长过氧化物光伏前驱体溶液有效期的多功能离子液体
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-23 DOI: 10.1007/s40843-024-3071-8
Yazhou Xu  (, ), Kaiqin Xu  (, ), Shuqin Xiao  (, ), Zhi Xing  (, ), Dengxue Li  (, ), Zongcai Li  (, ), Xiaotian Hu  (, ), Yiwang Chen  (, ), Ting Hu  (, )

At present, the development of perovskite solar cells (PSCs) is progressing rapidly, but the issue of poor stability remains a significant challenge. Achieving a stable precursor solution is crucial for the large-scale production of high-quality PSC films. In this study, we successfully developed a strategy to improve the long-term stability of the precursor solution and improve device performance by employing 1-n-butyl-3-methylimidazolium di-n-butyl phosphate (BMIMBP) as an anti-aging additive. The BP component inhibits the reactivity of I and formamidinium ion through multiple chemical bonds, thereby stabilizing the precursor solution. In addition, the BMIM+ component, which contains an amino group, can form two-dimensional perovskite internally, further enhancing the device stability. This strategy provides valuable guidance for achieving long-term stability in solar cells.

目前,过氧化物太阳能电池(PSCs)的开发进展迅速,但稳定性差的问题仍然是一个重大挑战。获得稳定的前驱体溶液对于大规模生产高质量的 PSC 薄膜至关重要。在这项研究中,我们成功地开发出一种策略,通过使用 1-正丁基-3-甲基咪唑鎓磷酸二正丁酯(BMIMBP)作为抗老化添加剂,提高了前驱体溶液的长期稳定性,并改善了设备性能。BP- 成分可通过多个化学键抑制 I- 和甲脒离子的反应,从而稳定前驱体溶液。此外,含有氨基的 BMIM+ 成分可在内部形成二维包晶,从而进一步提高器件的稳定性。这一策略为实现太阳能电池的长期稳定性提供了宝贵的指导。
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引用次数: 0
Intracellular carbon monoxide release unveils selective antibacterial effects 细胞内一氧化碳释放揭示了选择性抗菌效果
IF 8.1 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-23 DOI: 10.1007/s40843-024-2989-0
Tengfei Ma, Shaoqiu Zheng, Jian Cheng, Guoying Zhang, Jinming Hu

Carbon monoxide (CO) is recognized as a diffusible and biologically membrane-permeable gasotransmitter. However, the question of whether extracellular and intracellular CO delivery would yield similar or distinct biological functions remains unresolved. In this study, utilizing nonmetallic CO-releasing micelles as a platform for localized CO delivery, we present evidence suggesting that selective antibacterial effects against Staphylococcus aureus (S. aureus) are exclusively evident upon intracellular CO release, even in cases of extracellular release with higher CO concentrations showing no comparable effect. To substantiate this assertion, we systematically design micellar nanoparticles with varying sizes, monomer sequences, and shell compositions. Among these variants, only the micelles taken up by S. aureus and capable of intracellular CO release exhibit efficient bacteria-killing properties. We further demonstrate that the selective bactericidal effect is closely linked to the production of hydroxyl radicals after intracellular CO release. Additionally, intracellular CO release proves to be an efficient treatment for S. aureus-induced skin abscesses without the need for additional antibiotics, showcasing synergistic antibacterial and anti-inflammatory effects. These findings underscore the pivotal role of the spatial location of CO release, significantly enhancing our understanding of the pathophysiological functions of gasotransmitters.

一氧化碳(CO)被认为是一种可扩散且具有生物膜渗透性的气体递质。然而,细胞外和细胞内一氧化碳递送是否会产生相似或不同的生物功能这一问题仍未解决。在本研究中,我们利用非金属一氧化碳释放胶束作为一氧化碳局部递送的平台,提出证据表明,对金黄色葡萄球菌(S. aureus)的选择性抗菌作用只在细胞内释放一氧化碳时才明显,即使在细胞外释放较高浓度一氧化碳时也没有类似效果。为了证实这一论断,我们系统地设计了具有不同大小、单体序列和外壳成分的胶束纳米粒子。在这些变体中,只有被金黄色葡萄球菌吸收并能在细胞内释放二氧化碳的胶束才具有高效的杀菌特性。我们进一步证明,选择性杀菌效果与细胞内 CO 释放后产生的羟基自由基密切相关。此外,细胞内 CO 释放被证明是治疗金黄色葡萄球菌诱发的皮肤脓肿的有效方法,无需额外使用抗生素,具有协同抗菌和消炎作用。这些发现强调了一氧化碳释放空间位置的关键作用,极大地促进了我们对气体递质病理生理功能的了解。
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引用次数: 0
Efficient oxygen reduction through metal-free 3D covalent organic frameworks: a novel approach 通过无金属三维共价有机框架实现高效氧还原:一种新方法
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-23 DOI: 10.1007/s40843-024-3039-8
Shanyue Wei  (, ), Xiaowei Wu  (, ), Shufei Zhu  (, ), Zhiyang Wang  (, ), Jiangli Wang  (, ), Can-Zhong Lu  (, ), Yiming Xie  (, )

Covalent organic framework (COF) materials have gained significant applications in electrocatalytic systems due to their structural diversity and tunable functionalities. Moreover, three-dimensional (3D) COFs exhibit multistage pore structures, exposing numerous open sites, which facilitate the oxygen reduction reaction (ORR) process. However, the advancement of 3D COFs for ORR has been hindered by challenges, including limited topologies, the scarcity of building blocks with the required reactivity and symmetries, and difficulties in determining crystalline structures. In this work, we utilized an 8-connectivity building unit and successfully constructed two isoreticular 3D COF materials, which exhibited exceptionally high catalytic activity for 2e oxygen reduction reaction without the addition of any metal or conductive support materials, nor the pyrolyzed process. The electrochemically active surface areas (ECSAs) of the two 3D COFs were found to be 17.19 and 12.18 mF/cm2, respectively, which were significantly higher than those reported from other framework materials.

共价有机框架(COF)材料因其结构的多样性和可调整的功能性,在电催化系统中获得了重要的应用。此外,三维(3D)COF 显示出多级孔隙结构,暴露出大量开放位点,促进了氧还原反应(ORR)过程。然而,用于 ORR 的三维 COF 的发展一直受到各种挑战的阻碍,包括拓扑结构有限、具有所需反应活性和对称性的构建模块稀缺,以及晶体结构难以确定等。在这项工作中,我们利用 8 连接构建单元,成功构建了两种等轴三维 COF 材料,它们在 2e 氧还原反应中表现出极高的催化活性,无需添加任何金属或导电支撑材料,也无需热解过程。两种三维 COF 的电化学活性表面积(ECSA)分别为 17.19 和 12.18 mF/cm2,明显高于其他框架材料。
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引用次数: 0
Providing insight into exchange coupling within nanomagnetism: mechanism, micromagnetic simulation, synthesis and biomedical application 深入了解纳米磁性中的交换耦合:机制、微磁模拟、合成和生物医学应用
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1007/s40843-024-2978-8
Yuting Tang  (, ), Feng Feng  (, ), Guanhua Xu  (, ), Shijie Qin  (, ), Xiaoping Ouyang  (, ), Li Yao  (, ), Xiuyu Wang  (, )

Exchange coupling within nanomagnetism is a rapidly evolving field with significant implications for that plays a crucial role in the development of magnetic nanomaterials. Manipulating exchange coupling interaction enables the magnetic systems to overcome limitations associated with size-dependent magnetic behavior within nano scale, thereby improving their magnetic properties and providing for superior performance in biomedical applications compared with single-phase magnetic materials. Understanding the underlying mechanism of exchange coupling and its impact on macroscopic magnetic properties is crucial for the design and application of such magnetic materials. This review provides an overview of recent advances in interfacial exchange coupling among different magnetic modalities—ferromagnetism, ferrimagnetism, and antiferromagnetism—based on core-shell magnetic nanoparticles (MNPs). Additionally, this review discusses micromagnetic simulations to gain insights into the relationship between the microscopic magnetic structure (size, shape, composition, and exchange coupling) and the resulting macroscopic properties. The controlled synthesis of MNPs is summarized, including one-step method and two-step method. The precise manipulation of interfacial characteristics is of great importance, albeit challenging, as it allows for the fine-tuning of magnetic properties tailored for specific applications. The review also explores potential applications of core-shell MNPs in magnetic resonance imaging, hyperthermia therapy, targeted drug delivery, and advanced neuromodulation.

纳米磁学中的交换耦合是一个快速发展的领域,对磁性纳米材料的发展具有重要影响,并发挥着至关重要的作用。操纵交换耦合相互作用可使磁性系统克服纳米尺度内与尺寸相关的磁性行为限制,从而改善其磁性能,并在生物医学应用中提供优于单相磁性材料的性能。了解交换耦合的基本机制及其对宏观磁性能的影响对于此类磁性材料的设计和应用至关重要。本综述概述了基于核壳磁性纳米粒子(MNPs)的不同磁性模式(铁磁性、铁磁性和反铁磁性)之间的界面交换耦合的最新进展。此外,本综述还讨论了微磁模拟,以深入了解微观磁结构(尺寸、形状、成分和交换耦合)与由此产生的宏观特性之间的关系。综述了 MNPs 的可控合成,包括一步法和两步法。尽管具有挑战性,但对界面特性的精确控制非常重要,因为它可以针对特定应用对磁性能进行微调。综述还探讨了核壳 MNPs 在磁共振成像、热疗、靶向给药和高级神经调控中的潜在应用。
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引用次数: 0
Balancing sensitivity and resolution by feedback regulation of free radicals from Sn-C bonds in tin-oxygen clusters EBL photoresist 通过对锡氧簇 EBL 光刻胶中 Sn-C 键自由基的反馈调节平衡灵敏度和分辨率
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1007/s40843-024-3062-y
Hao Chen  (, ), Xinyan Huang  (, ), Yingdong Zhao  (, ), Jun Zhao  (, ), Pengzhong Chen  (, ), Xiaojun Peng  (, )

Notably, the cleavage of Sn–C bonds in extreme-ultraviolet photoresists containing Sn-oxygen (oxo) clusters and the generation of free radicals upon exposure lead to the chemical linking of Sn-oxo cores and subsequent solubility shifts. The reactivities and migration patterns of the generated radicals substantially influence patterning outcomes, including sensitivity and resolution. Herein, two Snoxo clusters, Sn4-Me-C10 (with Sn–methyl) and Sn4-Bu-C10 (with Sn–butyl), were combined to balance the sensitivity and resolution of photoresists, leveraging the feedback regulation between methyl and butyl free radicals generated from Sn–C bond cleavage. During electron beam lithography exposure, sensitive butyl radicals produced by Sn4-Bu-C10 initiated reactions within Sn4-Me-C10, improving sensitivity. Subsequently, the unstable methyl and bulky adamantyl radicals generated by Sn4-Me-C10 quenched the excess butyl radicals, thus improving the resolution and exposure latitude. Thus, this method leveraging the feedback regulation of free radicals offers new insights into the design of sensitive metal oxide resists with enhanced resolution.

值得注意的是,含有锡氧(oxo)簇的极紫外线光刻胶中锡-C 键的裂解以及曝光后自由基的产生导致了锡氧核的化学连接以及随后的溶解度变化。所产生自由基的反应活性和迁移模式会对图案化结果(包括灵敏度和分辨率)产生重大影响。在此,我们将 Sn4-Me-C10(含 Sn-甲基)和 Sn4-Bu-C10(含 Sn-丁基)这两种 Snoxo 簇结合起来,利用 Sn-C 键裂解产生的甲基和丁基自由基之间的反馈调节,平衡光刻胶的灵敏度和分辨率。在电子束光刻曝光过程中,Sn4-Bu-C10 产生的敏感丁基自由基会在 Sn4-Me-C10 内引发反应,从而提高灵敏度。随后,Sn4-Me-C10 产生的不稳定甲基和笨重金刚烷基自由基淬灭了多余的丁基自由基,从而提高了分辨率和曝光宽容度。因此,这种利用自由基反馈调节的方法为设计具有更高分辨率的灵敏金属氧化物抗蚀剂提供了新的思路。
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引用次数: 0
Quantitative evaluation of various NIR-to-red upconversion mechanisms in NaYF4:20%Yb3+,2%Er3+ nanoparticles 对 NaYF4:20%Yb3+,2%Er3+ 纳米粒子中各种近红外-红外上转换机制的定量评估
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1007/s40843-024-3022-y
Hao Wu  (, ), Lin Yang  (, ), Liangliang Zhang  (, ), Huajun Wu  (, ), Guohui Pan  (, ), Yongshi Luo  (, ), Ligong Zhang  (, ), Feng Liu  (, ), Jiahua Zhang  (, )

In the most popular NaYF4:Yb/Er upconversion nanoparticles (UCNPs), the red emission is attributed to four potential excitation routes encompassing two- and three-photon excitation processes. Consequently, this red emission typically exhibits a super-quadratic dependency on near-infrared (NIR) excitation intensity, with the nonlinear order n being dependent on the individual contributions (Cis) of these four excitation routes. Notably, the Cis values are not constant but significantly impacted by the surface quenching of the UCNPs, leading to a decrease in the n value. However, a quantitative assessment of these variable Cis has not been undertaken, hindering a comprehensive understanding of the quenching effect on the UC mechanisms. In this work, we prepare four NaYF4:Yb/Er nanocrystal samples with varying degrees of surface quenching, achieving through the modulation of particle size and core-shell structure. We quantitatively evaluate the Cis values and identify the primary excitation route responsible for the red emission. Our results reveal that the contribution of three-photon excitation increases from 7% in the 30 nm bare core to 74% in 90 nm core with shell at an excitation intensity of 200 mW cm−2. This observation high-lights the impact of surface quenching suppression. Furthermore, we discover that the quenching effect operates by reducing the lifetimes of the Yb3+2F5/2 and Er3+4S3/2 levels, while enhancing the NIR emission intensity ratio of the Er3+4I13/24I15/2 transition to the Yb3+2F5/22F7/2 transition. Our findings provide physical insights into the excitation mechanisms underlying the red UC emission in NaYF4:Yb/Er UCNPs.

在最流行的 NaYF4:Yb/Er 上转换纳米粒子(UCNPs)中,红色发射归因于四种潜在的激发途径,包括双光子和三光子激发过程。因此,这种红色发射通常与近红外(NIR)激发强度呈超二次函数关系,非线性阶数 n 取决于这四种激发途径的各自贡献(Cis)。值得注意的是,Cis 值并非恒定不变,而是受到 UCNPs 表面淬火的显著影响,从而导致 n 值下降。然而,目前还没有对这些可变的 Cis 值进行定量评估,这阻碍了对 UC 机制的淬火效应的全面了解。在这项工作中,我们制备了四种具有不同表面淬火程度的 NaYF4:Yb/Er 纳米晶体样品,通过调节粒度和核壳结构来实现。我们对 Cis 值进行了定量评估,并确定了红色发射的主要激发途径。我们的研究结果表明,在 200 mW cm-2 的激发强度下,三光子激发的贡献率从 30 nm 裸核的 7% 增加到 90 nm 带壳核的 74%。这一观察结果凸显了表面淬火抑制的影响。此外,我们还发现淬火效应是通过降低 Yb3+2F5/2 和 Er3+4S3/2 水平的寿命来实现的,同时增强了 Er3+4I13/2 → 4I15/2 转变与 Yb3+2F5/2 → 2F7/2 转变的近红外发射强度比。我们的发现为 NaYF4:Yb/Er UCNPs 中红色 UC 发射的激发机制提供了物理见解。
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引用次数: 0
Thermoregulatory molecular sieving in crystals 晶体中的热调节分子筛
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1007/s40843-024-3065-4
Guozhen Liu, Wanqin Jin, Gongping Liu
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引用次数: 0
Aggregation-caused quenching to crystallization-induced emission transformation: hydration-induced luminescence in crystal curcumin with tunable thermochromism for in vivo tracking 聚合引起的淬火到结晶诱导的发射转变:具有可调热致变色的姜黄素晶体中的水合诱导发光,用于体内追踪
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1007/s40843-024-3049-1
Huan Shen  (, ), Peng Shi  (, ), Ergang Liu  (, ), Yuefei Fang  (, ), Shijie Xu  (, ), Junbo Gong  (, ), Yongzhuo Huang  (, )

The development of solid-state materials with switchable luminescence in response to stimuli remains a challenge, especially for organic materials. While crystal water significantly impacts the absorption spectra of organic crystals, it is unclear whether the emission spectra of organic luminescent materials can be systematically manipulated by water. In this study, we successfully obtained curcumin monohydrate (Form X), a channel-type hydrate exhibiting crystallization-induced emission (CIE) at 608 nm (orange fluorescence), which contrasted with the conventional forms of aggregation-caused quenching (ACQ). Thermal treatment induced the release of hydration water, resulting in a new anhydrate (Form IV) that emitted yellow-green fluorescence with the emission peak at 575 nm. Additionally, this approach can be used to track the absorption of curcumin crystals following subcutaneous or intramuscular delivery. The hydratemediated single-crystal-to-single-crystal transition (SCSC) and its associated luminescence transition were reversible and responsive to temperature, offering a green approach for synthesizing and designing aggregation-induced-emission (AIE)-based intelligent luminescent devices for detecting air humidity or drug absorption.

开发可随刺激而切换发光的固态材料仍然是一项挑战,尤其是对有机材料而言。虽然结晶水会对有机晶体的吸收光谱产生重大影响,但有机发光材料的发射光谱是否能被水系统地操纵,目前尚不清楚。在这项研究中,我们成功获得了姜黄素一水合物(形式 X),它是一种通道型水合物,在 608 纳米波长处表现出结晶诱导发射(CIE)(橙色荧光),这与传统形式的聚集诱导淬灭(ACQ)形成了鲜明对比。热处理可诱导水合水的释放,产生新的水合物(形式 IV),发出黄绿色荧光,发射峰在 575 纳米处。此外,这种方法还可用于跟踪姜黄素晶体在皮下或肌肉注射后的吸收情况。水合介导的单晶到单晶转变(SCSC)及其相关的发光转变是可逆的,并对温度有反应,这为合成和设计基于聚集诱导发射(AIE)的智能发光装置提供了一种绿色方法,该装置可用于检测空气湿度或药物吸收。
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引用次数: 0
Enhanced thermal constant B of diamond films for ultrahigh sensitivity negative temperature coefficient thermistors 用于超高灵敏度负温度系数热敏电阻的增强型金刚石薄膜热常数 B
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1007/s40843-024-3053-4
Qiao Chen  (, ), Yimeng Zhao  (, ), Jiawei Li  (, ), Xiyuan Liu  (, ), Xinyue Wang  (, ), Wenxi Zhang  (, ), Hongwei Zhu  (, )

Negative temperature coefficient (NTC) thermistor plays a crucial role in science research and engineering applications for precise temperature monitoring. Although great progress has been achieved in NTC materials, enhancing sensitivity and maintaining this high sensitivity along with linearity across extensive temperature ranges remain a significant challenge. In this study, we introduce a diamond-based thermistor (DT) characterized by its outstanding sensitivity, swift response time, and broad temperature monitoring capabilities. The temperature constant B for this DT, measured from 30 to 300°C (B30/300), achieves an exceptional value of 8012 K, which notably exceeds the temperature sensing capabilities of previously reported NTC thermistors within this extensive range. Moreover, diamond’s unique thermal conductivity and stability significantly boost the response speed and durability of the DT, offering substantial advantages over traditional ceramic thermistors. The enhanced temperature-sensitive properties of the DT are attributed to the presence of impurity elements in polycrystalline diamond. Impedance analysis indicates a hopping conduction mechanism, likely involving C-H or C-N dipoles at the diamond grain boundaries. This study marks a significant leap forward in diamond thermistor technology and sheds light on the mechanisms of thermal active conduction in diamond materials.

负温度系数(NTC)热敏电阻在科学研究和工程应用中的精确温度监测方面发挥着至关重要的作用。虽然负温度系数材料取得了巨大进步,但提高灵敏度并在广泛的温度范围内保持高灵敏度和线性度仍然是一项重大挑战。在本研究中,我们介绍了一种基于金刚石的热敏电阻(DT),它具有出色的灵敏度、快速的响应时间和广泛的温度监测能力。该热敏电阻的温度常数 B 在 30 至 300°C (B30/300) 范围内测量,达到了 8012 K 的优异值,明显超过了之前报道的 NTC 热敏电阻在这一广泛温度范围内的感温能力。此外,金刚石独特的热传导性和稳定性大大提高了 DT 的响应速度和耐用性,与传统陶瓷热敏电阻相比具有显著优势。多晶金刚石中杂质元素的存在增强了 DT 的温度敏感特性。阻抗分析表明了跳变传导机制,可能涉及金刚石晶界的 C-H 或 C-N 偶极子。这项研究标志着金刚石热敏电阻技术的重大飞跃,并揭示了金刚石材料的热活性传导机制。
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引用次数: 0
High performance in Zintl thermoelectrics via reduction in crystal field splitting energy 通过降低晶体场分裂能实现 Zintl 热电半导体的高性能
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-20 DOI: 10.1007/s40843-024-3030-2
Anustoop Das, Kanishka Biswas
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引用次数: 0
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Science China Materials
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