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Stabilizing lithium deposition within bimodal porous SiO2-TiO2 microspheres as 3D host structure 在作为三维宿主结构的双峰多孔二氧化硅-二氧化钛微球中稳定锂沉积
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1007/s12274-024-6934-5
Noeul Kim, Jae Hun Choi, Min Kim, Dae Soo Jung, Yun Chan Kang

Three-dimensional (3D) host materials for lithium metal anodes (LMAs) have gained attention because they can mitigate volume expansion and local current density through their large surface area and suppress the dendritic growth of lithium. Recent research on 3D host materials has focused on conductive materials; however, the benefits of 3D host materials cannot be fully utilized because lithium deposition begins at the top of the structure. Herein, we fabricate SiO2-TiO2 composite microspheres with bimodal pore structures (bi-SiTiO) by simple spray pyrolysis. These microspheres effectively store lithium within the structure from the bottom of the electrode while preventing lithium dendrite formation. Focused ion beam-scanning transmission electron microscopy (FIB-STEM) analysis reveals that the lithiophilic properties of composite microspheres enhanced their effectiveness in storing lithium, with small pores acting as “lithium-ion sieves” for a uniform lithium-ion flux and large pores that provide sufficient volume for lithium deposition. The bi-SiTiO composite microspheres exhibit a high Coulombic efficiency of 98.5% over 200 cycles at 2.0 mA·cm−2 when operated in a lithium half-cell. With a high lithium loading of 5.0 mAh·cm−2, the symmetrical cell of the bi-SiTiO electrode sustains more than 900 h. A full cell coupled with an LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode also exhibits enhanced electrochemical properties in terms of cycling stability and rate capability.

用于锂金属阳极(LMAs)的三维(3D)宿主材料因其大表面积可减轻体积膨胀和局部电流密度,并抑制锂的树枝状生长而备受关注。最近关于三维宿主材料的研究主要集中在导电材料上;然而,由于锂沉积始于结构的顶部,三维宿主材料的优势无法得到充分利用。在这里,我们通过简单的喷雾热解方法制造出了具有双峰孔结构的 SiO2-TiO2 复合微球(bi-SiTiO)。这些微球能从电极底部有效地将锂储存在结构中,同时防止锂枝晶的形成。聚焦离子束扫描透射电子显微镜(FIB-STEM)分析表明,复合微球的亲锂特性增强了其存储锂的有效性,小孔可作为 "锂离子筛",实现均匀的锂离子通量,而大孔能为锂沉积提供足够的体积。当在锂半电池中以 2.0 mA-cm-2 的电流运行 200 次时,双硅钛氧化物复合微球表现出高达 98.5% 的库仑效率。在 5.0 mAh-cm-2 的高锂负载条件下,双 SiTiO 电极的对称电池可维持 900 小时以上。与 LiNi0.8Co0.1Mn0.1O2 (NCM811) 阴极耦合的全电池在循环稳定性和速率能力方面也表现出更强的电化学特性。
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引用次数: 0
Construction of ternary Sn/SnO2/nitrogen-doped carbon superstructures as anodes for advanced lithium-ion batteries 构建作为先进锂离子电池阳极的三元锡/二氧化锰/掺氮碳上层结构
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-28 DOI: 10.1007/s12274-024-6931-8
Zizhou Shen, Xiaotian Guo, Hongye Ding, Dianheng Yu, Yihao Chen, Nana Li, Huijie Zhou, Songtao Zhang, Jun Wu, Huan Pang

Pristine tin (Sn) and tin dioxide (SnO2) have sparked wide interest owing to their abundant resources and superior theoretical capacity. Nevertheless, the obvious volume expansion effect upon cycling and undesirable conductivity of Sn-based materials lead to undesirable specific capacity. In this work, a nanostructured Sn/SnO2/nitrogen-doped carbon (NC) superstructure was prepared through a facile electrospray-carbonization strategy. The Sn/SnO2 nanoparticles (NPs) were uniformly dispersed in a spherical NC matrix, which prevented the volume expansion and aggregation of NPs and facilitated the ion diffusion and charge transfer kinetics. When the optimized Sn/SnO2/NC superstructures were employed as lithium-ion battery anodes, a remarkable specific capacity of 747.9 mAh·g−1 over 200 cycles at 0.5 A·g−1 and a superior cyclability of 644.1 mAh·g−1 over 1000 cycles at 2 A·g−1 were obtained. This effective synthetic strategy for synthesizing superstructures provides valuable insights for the advancement of lithium-ion batteries.

原始锡(Sn)和二氧化锡(SnO2)因其丰富的资源和卓越的理论容量而引发了广泛的兴趣。然而,锡基材料在循环过程中明显的体积膨胀效应和不理想的导电性导致了不理想的比容量。在这项工作中,通过一种简便的电喷雾碳化策略制备了一种纳米结构的 Sn/SnO2/ 掺氮碳(NC)上层结构。Sn/SnO2纳米颗粒(NPs)均匀地分散在球形的NC基体中,防止了NPs的体积膨胀和聚集,促进了离子扩散和电荷转移动力学。将优化后的 Sn/SnO2/NC 超结构用作锂离子电池阳极时,在 0.5 A-g-1 条件下循环 200 次可获得 747.9 mAh-g-1 的显著比容量,在 2 A-g-1 条件下循环 1000 次可获得 644.1 mAh-g-1 的卓越循环性。这种合成超结构的有效合成策略为锂离子电池的发展提供了宝贵的启示。
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引用次数: 0
Unipolar p-type monolayer WSe2 field-effect transistors with high current density and low contact resistance enabled by van der Waals contacts 利用范德华接触实现高电流密度和低接触电阻的单极 p 型单层 WSe2 场效应晶体管
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1007/s12274-024-6942-5
Miaomiao Li, Xinyu Zhang, Zimei Zhang, Gang Peng, Zhihong Zhu, Jia Li, Shiqiao Qin, Mengjian Zhu

High-performance field-effect transistors (FETs) based on atomically thin two-dimensional (2D) semiconductors have demonstrated great promise in post-Moore integrated circuits. However, unipolar p-type 2D semiconductor transistors yet remain challenging and suffer from low saturation current density (less than 10 µA·µm−1) and high contact resistance (larger than 100 kΩ·µm), mainly limited by the Schottky barrier induced by the mismatch of the work-functions and the Fermi level pinning at the metal contact interfaces. Here, we overcome these two obstacles through van der Waals (vdW) integration of high work-function metal palladium (Pd) as the contacts onto monolayer WSe2 grown by chemical vapor deposition (CVD) method. We demonstrate unipolar p-type monolayer WSe2 FETs with superior device performance: room temperature on-state current density exceeding 100 µA·µm−1, contact resistance of 12 kΩ·µm, on/off ratio over 107, and field-effect hole mobility of ~ 103 cm2·V−1·s−1. Electrical transport measurements reveal that the Fermi level pinning effect is completely effectively eliminated in monolayer WSe2 with vdW Pd contacts, leading to a Schottky barrier-free Ohmic contact at the metal-semiconductor junctions. Combining the advantages of large-scale vdW contact strategy and CVD growth, our results pave the way for wafer-scale fabrication of complementary-metal-oxide-semiconductor (CMOS) logic circuits based on atomically thin 2D semiconductors.

基于原子薄二维(2D)半导体的高性能场效应晶体管(FET)在后摩尔集成电路中大有可为。然而,单极对型二维半导体晶体管仍面临挑战,饱和电流密度低(小于 10 µA-µm-1),接触电阻大(大于 100 kΩ-µm),主要受限于工作函数不匹配和金属接触界面费米级针销所引起的肖特基势垒。在这里,我们通过范德华(vdW)集成高功函数金属钯(Pd),将其作为触点,通过化学气相沉积(CVD)方法生长到单层 WSe2 上,从而克服了这两个障碍。我们展示了具有卓越器件性能的单极 p 型单层 WSe2 FET:室温导通电流密度超过 100 µA-µm-1,接触电阻为 12 kΩ-µm,导通/关断比超过 107,场效应空穴迁移率约为 103 cm2-V-1-s-1。电传输测量结果表明,在具有 vdW Pd 触点的单层 WSe2 中,费米级钉扎效应被完全有效地消除,从而在金属-半导体结点上形成了肖特基无势垒欧姆接触。结合大规模 vdW 接触策略和 CVD 生长的优势,我们的研究成果为在晶圆级制造基于原子薄二维半导体的互补金属氧化物半导体 (CMOS) 逻辑电路铺平了道路。
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引用次数: 0
Integrated in-memory sensor and computing of artificial vision system based on reversible bonding transition-induced nitrogen-doped carbon quantum dots (N-CQDs) 基于可逆键合转变诱导的氮掺杂碳量子点(N-CQDs)的人工视觉系统的集成式内存传感器和计算器
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1007/s12274-024-6966-x
Tianqi Yu, Jie Li, Wei Lei, Suhaidi Shafe, Mohd Nazim Mohtar, Nattha Jindapetch, Paphavee van Dommelen, Zhiwei Zhao

Carbon quantum dots (CQDs) have been used in memristors due to their attractive optical and electronic properties, which are considered candidates for brain-inspired computing devices. In this work, the performance of CQDs-based memristors is improved by utilizing nitrogen-doping. In contrast, nitrogen-doped CQDs (N-CQDs)-based optoelectronic memristors can be driven with smaller programming voltages (−0.6 to 0.7 V) and exhibit lower powers (78 nW/0.29 µW). The physical mechanism can be attributed to the reversible transition between C–N and C=N with lower binding energy induced by the electric field and the generation of photogenerated carriers by ultraviolet light irradiation, which adjusts the conductivity of the initial N-CQDs to implement resistance switching. Importantly, the convolutional image processing based on various cross kernels is efficiently demonstrated by stable multi-level storage properties. An N-CQDs-based optoelectronic reservoir computing implements impressively high accuracy in both no noise and various noise modes when recognizing the Modified National Institute of Standards and Technology (MNIST) dataset. It illustrates that N-CQDs-based memristors provide a novel strategy for developing artificial vision system with integrated in-memory sensor and computing.

碳量子点(CQDs)因其极具吸引力的光学和电子特性而被用于忆阻器,并被认为是脑启发计算设备的候选器件。在这项研究中,利用氮掺杂技术提高了基于碳量子点的忆阻器的性能。相比之下,氮掺杂的 CQDs(N-CQDs)光电忆阻器可以用较小的编程电压(-0.6 至 0.7 V)驱动,并表现出较低的功率(78 nW/0.29 µW)。其物理机制可归因于电场诱导的具有较低结合能的 C-N 和 C=N 之间的可逆转变,以及紫外线照射产生的光生载流子,从而调整初始 N-CQD 的电导率,实现电阻开关。重要的是,基于各种交叉核的卷积图像处理通过稳定的多级存储特性得到了有效展示。在识别美国国家标准与技术研究院(MNIST)的修正数据集时,基于 N-CQDs 的光电存储计算在无噪声和各种噪声模式下都实现了令人印象深刻的高精度。这说明基于 N-CQDs 的忆阻器为开发集成内存传感器和计算的人工视觉系统提供了一种新策略。
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引用次数: 0
Effect of heat and bubble mass transfer on the efficiency of alkaline electrolysis hydrogen production 热量和气泡传质对碱性电解制氢效率的影响
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1007/s12274-024-6922-9
Nian Xu, Bingbing Qiu, Zucun Rui, Tianxiang Ji, Zilong Liu, Huaqiang Chu

This review highlights the critical effects of heat transfer and bubble mass transfer in alkaline water electrolysis on hydrogen generation efficiency. To improve heat transfer performance, the study focuses on reducing electrical resistance and controlling the electrolysis system’s temperature. It proposes innovative strategies such as using metal matrix composites and catalysts to optimize electrode structure, precise temperature and pressure regulation and enhanced electrolyte concentration. Additionally, the study examines the dynamics of bubble mass transfer, proposing effective strategies to reduce bubble coverage, including hydrophilic electrodes, mechanically circulating the electrolyte and voltage smoothing with pressure swinging. This study contributes to the advancement of hydrogen energy technology with practical strategies. By adjusting the electrolysis system to optimize the combined effect of these factors, we can improve the efficiency, economy and environmental friendliness of hydrogen production. This will contribute to the transformation of the global energy mix and the implementation of sustainable development strategies.

本综述强调了碱性水电解过程中传热和气泡传质对制氢效率的关键影响。为提高传热性能,研究重点是降低电阻和控制电解系统的温度。研究提出了创新策略,如使用金属基复合材料和催化剂优化电极结构、精确调节温度和压力以及提高电解液浓度。此外,该研究还探讨了气泡传质的动力学,提出了减少气泡覆盖的有效策略,包括亲水性电极、电解液机械循环以及利用压力摆动平滑电压。这项研究为氢能技术的发展提供了实用的策略。通过调整电解系统以优化这些因素的综合效应,我们可以提高制氢的效率、经济性和环保性。这将有助于全球能源结构的转型和可持续发展战略的实施。
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引用次数: 0
Interfacial activation of alkaline phosphatase induced by hydrophilic metal—organic frameworks 亲水性金属有机框架诱导碱性磷酸酶的界面活化
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1007/s12274-024-6929-2
Dongyan Chen, Yi Xu, Jie Wei, Munetaka Oyama, Quansheng Chen, Xiaomei Chen

Encapsulating natural enzymes in metal—organic frameworks (MOFs) can maintain the original biological functions of enzymes in harsh environments. However, the nature of interfacial interactions between a MOF and enzyme is currently unclear, rendering effective regulation of the biocatalytic activity of the enzyme@MOF composite difficult. Differences in the hydrophilicity of MOF carriers are closely related to the conformational changes and catalytic properties of the enzyme. In this study, the catalytic activity, stability, and conformational changes of alkaline phosphatase (ALP) encapsulated in hydrophilic zeolite imidazolate framework-90 (ZIF-90) and hydrophobic ZIF-8 were systematically investigated using experimental methods and molecular dynamics simulations. The results demonstrated that hydrophilic ZIF-90-encapsulated ALP exhibited superior stability and was 2.22-fold more retained catalytically active than hydrophobic ALP@ZIF-8 after 20 cycles of utilization. Moreover, the hydrophilic interface provided by ZIF-90 effectively regulated the structure of ALP to maintain the optimal catalytic conformation of its active center. The practical application of highly bioactive ALP@ZIF-90 was demonstrated by employing it in a self-calibrated colorimetric/fluorescence dual-mode sensing method for the efficient, reliable, and accurate detection of methyl paraoxon. This study provides new insights for improving enzyme immobilization strategies and promoting the rapid development of enzyme@MOF composites for catalytic and sensing applications.

将天然酶封装在金属有机框架(MOFs)中,可以在恶劣环境中保持酶原有的生物功能。然而,目前尚不清楚 MOF 与酶之间界面相互作用的性质,因此难以有效调节酶@MOF 复合材料的生物催化活性。MOF 载体亲水性的差异与酶的构象变化和催化特性密切相关。本研究利用实验方法和分子动力学模拟系统研究了亲水性沸石咪唑酸盐框架-90(ZIF-90)和疏水性 ZIF-8 封装的碱性磷酸酶(ALP)的催化活性、稳定性和构象变化。结果表明,亲水性 ZIF-90 包封的 ALP 具有更高的稳定性,在使用 20 个周期后,其催化活性的保持率是疏水性 ALP@ZIF-8 的 2.22 倍。此外,ZIF-90 提供的亲水界面有效调节了 ALP 的结构,使其活性中心保持最佳催化构象。通过将高生物活性 ALP@ZIF-90 应用于自校准比色/荧光双模式传感方法,对甲基对硫磷进行高效、可靠和准确的检测,证明了它的实际应用价值。这项研究为改进酶固定化策略和促进酶@MOF 复合材料在催化和传感应用领域的快速发展提供了新的见解。
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引用次数: 0
Drawing highly ordered MXene fibers from dynamically aggregated hydrogels 从动态聚合的水凝胶中提取高度有序的 MXene 纤维
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1007/s12274-024-6930-9
Shengyang Zhou, Xuan Li, Yilin Zhang, Joseph Halim, Chao Xu, Johanna Rosen, Maria Strømme

Assembly of two-dimensional (2D) nanomaterials into well-organized architectures is pivotal for controlling their function and enhancing performance. As a promising class of 2D nanomaterials, MXenes have attracted significant interest for use in wearable electronics due to their unique electrical and mechanical properties. However, facile approaches for fabricating MXenes into macroscopic fibers with controllable structures are limited. In this study, we present a strategy for easily spinning MXene fibers by incorporating polyanions. The introduction of poly(acrylic acid) (PAA) into MXene colloids has been found to alter MXene aggregation behavior, resulting in a reduced concentration threshold for lyotropic liquid crystal phase. This modification also enhances the viscosity and shear sensitivity of MXene colloids. Consequently, we were able to draw continuous fibers directly from the gel of MXene aggregated with PAA. These fibers exhibit homogeneous diameter and high alignment of MXene nanosheets, attributed to the shear-induced long-range order of the liquid crystal phase. Furthermore, we demonstrate proof-of-concept applications of the ordered MXene fibers, including textile-based supercapacitor, sensor and electrical thermal management, highlighting their great potential applied in wearable electronics. This work provides a guideline for processing 2D materials into controllable hierarchical structures by regulating aggregation behavior through the addition of ionic polymers.

将二维(2D)纳米材料组装成组织良好的结构对于控制其功能和提高性能至关重要。作为一类前景广阔的二维纳米材料,MXenes 因其独特的电气和机械特性在可穿戴电子设备中的应用引起了极大的兴趣。然而,将 MXenes 制成具有可控结构的宏观纤维的简便方法非常有限。在本研究中,我们提出了一种通过加入聚阴离子轻松纺制 MX 烯纤维的策略。研究发现,将聚(丙烯酸)(PAA)引入 MXene 胶体可改变 MXene 的聚集行为,从而降低各向同性液晶相的浓度阈值。这种改性还提高了 MXene 胶体的粘度和剪切敏感性。因此,我们能够直接从与 PAA 聚合的 MXene 凝胶中提取连续纤维。这些纤维显示出均匀的直径和 MXene 纳米片的高度排列,这归功于液晶相的剪切诱导长程有序性。此外,我们还展示了有序 MXene 纤维的概念验证应用,包括基于纺织品的超级电容器、传感器和电热管理,凸显了其在可穿戴电子产品中的巨大应用潜力。这项工作为通过添加离子聚合物调节聚集行为,将二维材料加工成可控的分层结构提供了指导。
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引用次数: 0
Development of aqueous-phase CdSeS magic-size clusters at room temperature and quantum dots at elevated temperatures 在室温下开发水相硒化镉神奇尺寸团簇,在高温下开发量子点
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-24 DOI: 10.1007/s12274-024-6884-y
Yao Jiang, Zhe Wang, Shasha Wang, Chunchun Zhang, Chaoran Luan, Xiaoqin Chen, Kui Yu

Little is known about the synthesis of colloidal ternary semiconductor magic-size clusters (MSCs) and quantum dots (QDs) in an aqueous environment. We report here the first synthesis of aqueous-phase CdSeS MSC-380 (displaying sharp optical absorption peaking at ∼ 380 nm) at room temperature and QDs at elevated temperatures. The reaction contains CdCl2·2.5H2O, 3-mercaptopropionic acid (MPA, HS–(CH2)2–COOH), selenourea (SeU, NH2–C(Se)–NH2), and thioacetamide (TAA, CH3–C(S)–NH2). Prior to the nucleation and growth (N/G) of QDs, there are clusters formed at 25 °C. The prenucleation-stage clusters are the precursor compound of CdSeS MSC-380 (PC-380). The PC is relatively transparent in optical absorption; in the presence of a primary amine butylamine (BTA, CH3–(CH2)3–NH2), the PC transforms to absorbing CdSeS MSC-380. At 80 °C, the PC decreases and the N/G of CdSeS QDs appears. The present study paves the way to the aqueous-phase synthesis of ternary CdSeS MSCs and QDs, providing an in-depth understanding of the cluster formation in the prenucleation stage of CdSeS QDs.

人们对在水环境中合成胶体三元半导体魔法尺寸团簇(MSCs)和量子点(QDs)知之甚少。我们在此报告了首次在室温下合成水相 CdSeS MSC-380(在 ∼ 380 nm 处显示尖锐的光吸收峰值)和在高温下合成 QDs 的过程。反应物包括 CdCl2-2.5H2O、3-巯基丙酸(MPA,HS-(CH2)2-COOH)、硒脲(SeU,NH2-C(Se)-NH2)和硫代乙酰胺(TAA,CH3-C(S)-NH2)。在 QDs 成核和生长(N/G)之前,25 ℃ 下会形成团簇。成核前阶段的团簇是 CdSeS MSC-380 (PC-380)的前体化合物。PC 的光吸收相对透明;在伯胺丁胺(BTA,CH3-(CH2)3-NH2)的存在下,PC 转变为可吸收的 CdSeS MSC-380。80 °C 时,PC 下降,出现 CdSeS QD 的 N/G。本研究为三元 CdSeS MSCs 和 QDs 的水相合成铺平了道路,深入了解了 CdSeS QDs 成核前阶段的团簇形成。
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引用次数: 0
Protein-nucleic acid hybrid nanostructures for molecular diagnostic applications 用于分子诊断的蛋白质-核酸杂交纳米结构
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-24 DOI: 10.1007/s12274-024-6925-6
Noah R. Sundah, Yuxuan Seah, Auginia Natalia, Xiaoyan Chen, Panida Cen, Yu Liu, Huilin Shao

Molecular diagnostic technologies empower new clinical opportunities in precision medicine. However, existing approaches face limitations with respect to performance, operation and cost. Biological molecules including proteins and nucleic acids are being increasingly adopted as tools in the development of new molecular diagnostic technologies. In particular, leveraging their complementary properties—the functional diversity of proteins and the precision programmability of nucleic acids—a wide range of protein-nucleic acid hybrid nanostructures have been developed. These hybrid structures take diverse forms, ranging from one-dimensional to three-dimensional hybrids, as static assemblies to dynamic machines, and possess myriad functions to recognize target biomarkers, encode vast information and execute catalytic activities. Motivated by recent advances in this area of molecular nanotechnology, we review the state-of-art design and application of various types of protein-nucleic acid hybrid nanostructures for molecular diagnostics, and present an outlook on the challenges and opportunities for emerging pre-clinical and clinical applications, highlighting the promise for earlier detection, more refined diagnosis and highly tailored treatment decision that ultimately lead to improved patient outcomes.

分子诊断技术为精准医疗带来了新的临床机遇。然而,现有的方法在性能、操作和成本方面存在局限性。包括蛋白质和核酸在内的生物分子正越来越多地被用作开发新型分子诊断技术的工具。特别是,利用它们的互补特性--蛋白质的功能多样性和核酸的精确可编程性--已经开发出了多种蛋白质-核酸混合纳米结构。这些杂交结构形式多样,从一维到三维杂交,从静态组装到动态机器,具有识别目标生物标记物、编码大量信息和执行催化活性等多种功能。在分子纳米技术这一领域最新进展的推动下,我们回顾了用于分子诊断的各种类型蛋白质-核酸杂交纳米结构的最新设计和应用,并展望了新出现的临床前和临床应用所面临的挑战和机遇,强调了更早检测、更精细诊断和高度定制化治疗决策的前景,这些最终将改善患者的预后。
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引用次数: 0
Synthesis of palladium-rare earth alloy as a high-performance bifunctional catalyst for direct ethanol fuel cells 合成用于直接乙醇燃料电池的高性能双功能钯稀土合金催化剂
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-24 DOI: 10.1007/s12274-024-6933-6
Qingqing Li, Chang Sun, Xiaolei Sun, Zijun Yin, Yaping Du, Jin-Cheng Liu, Feng Luo

Direct ethanol fuel cells (DEFCs) have drawn attention for their simplicity, rapid start-up, high power density and environmental friendliness. Despite these advantages, the widespread application of DEFCs faces challenges, primarily due to the inadequate performance of anode and cathode catalysts. Pd-based materials have shown exceptional catalytic activity for both the ethanol oxidation reaction (EOR) and the oxygen reduction reaction (ORR). Alloying noble metals with rare earth elements has emerged as an effective strategy to further enhance the catalytic activity by modulating the electronic structure. In this study, we synthesized a series of palladium-rare earth (Pd3RE) alloys supported on carbon to serve as bifunctional catalysts that efficiently promote both ORR and EOR. Compared to Pd/C, the Pd3Tb/C catalyst exhibits 3.1-fold and 1.8-fold enhancement in activity for ORR and EOR, respectively. The charge transfer in the Pd3Tb/C results in an electron-rich Pd component, thereby weakening the binding energy with oxygen species and facilitating the two reactions.

直接乙醇燃料电池(DEFC)因其操作简单、启动迅速、功率密度高和环境友好而备受关注。尽管具有这些优点,但直接乙醇燃料电池的广泛应用仍面临挑战,主要原因是阳极和阴极催化剂的性能不足。钯基材料在乙醇氧化反应(EOR)和氧还原反应(ORR)中都表现出了卓越的催化活性。贵金属与稀土元素的合金化已成为通过调节电子结构进一步提高催化活性的有效策略。在本研究中,我们合成了一系列以碳为载体的钯稀土(Pd3RE)合金,作为双功能催化剂,可有效促进 ORR 和 EOR。与 Pd/C 相比,Pd3Tb/C 催化剂的 ORR 和 EOR 活性分别提高了 3.1 倍和 1.8 倍。Pd3Tb/C 中的电荷转移产生了富电子钯成分,从而削弱了与氧物种的结合能,促进了这两种反应。
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引用次数: 0
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