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Enhancing DNA-based Nanodevices Activation through Cationic Peptide Acceleration of Strand Displacement 通过阳离子肽加速链位移增强 DNA 纳米器件的活化能力
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-13 DOI: 10.1039/d4nh00252k
Xianxue Zhang, Ruikai Du, Shichao Xu, Xinyue Wang, Zhen-Gang Wang
Dynamic DNA-based nanodevices offer versatile molecular-level operations, while a majority of them suffer from the sluggish kinetics, impeding the advancement of device complexity. In this work, we present the self-assembly of a cationic peptide with DNA to expedite toehold-mediated DNA strand displacement (TMSD) reactions, a fundamental mechanism enabling the dynamic control and actuation of DNA nanostructures. The target DNA was modified with a fluorophore and a quencher, so that the TMSD process can be monitored by observing the time-dependent fluorescence changes. The boosting effect of the peptides is found to be dependent on the peptide/DNA N/P ratio, the toehold/invader binding affinity, and the ionic strength with stronger effects observed at lower ionic strength, suggesting electrostatic interactions play a key role. Furthermore, we demonstrate that the cationic peptide enhances the responsiveness and robustness of DNA machinery tweezer or logic circuits (AND and OR) involving multiple strand displacement reactions in parallel and cascade, highlighting its broad utility across DNA-based systems of varying complexity. This work offers a versatile approach to enhance the efficiency of toehold-mediated DNA nanodevices, facilitating flexible design and broader applications.
基于 DNA 的动态纳米器件提供了多功能的分子级操作,但其中大多数器件都存在动力学缓慢的问题,阻碍了器件复杂性的提高。在这项工作中,我们介绍了阳离子肽与DNA的自组装,以加速趾hold介导的DNA链位移(TMSD)反应,这是实现DNA纳米结构动态控制和驱动的基本机制。目标 DNA 经荧光团和淬灭剂修饰后,可通过观察随时间变化的荧光变化来监测 TMSD 过程。研究发现,肽的增效作用取决于肽/DNA N/P比、趾持/入侵者结合亲和力以及离子强度,在离子强度较低时观察到的增效作用更强,这表明静电相互作用发挥了关键作用。此外,我们还证明了阳离子肽能提高 DNA 机械镊子或逻辑电路(AND 和 OR)的响应速度和稳健性,这些电路涉及并行和级联的多链置换反应,突出了它在不同复杂程度的 DNA 系统中的广泛用途。这项工作提供了一种多功能方法来提高趾持介导的 DNA 纳米器件的效率,从而促进灵活的设计和更广泛的应用。
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引用次数: 0
Circular RNA oligonucleotides: Enzymatic synthesis and scaffolding for nanoconstruction 环状 RNA 寡核苷酸:酶法合成和纳米结构支架
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1039/d4nh00236a
Shijie Li, Yanxin Chu, Xin Guo, Chengde Mao, Shou-Jun Xiao
We report the efficient synthesis of monomeric circular RNAs (circRNAs) in the size range of 16−44 nt with a novel DNA dumbbell splinting plus T4 DNA ligation strategy. Such a DNA dumbbell splinting strategy was developed by one group among ours recently for near-quantitative conversion of short linear DNAs into monomeric circular ones. Furthermore, using the 44 nt circRNA as scaffold strands, we constructed hybrid RNA:DNA and pure RNA:RNA double crossover tiles and their assemblies of nucleic acid nanotubes and flat arrays.
我们报告了利用一种新颖的 DNA 哑铃拼接加 T4 DNA 连接策略高效合成大小范围为 16-44 nt 的单体环状 RNA(circRNA)的情况。我们中的一个研究小组最近开发出了这种 DNA 哑铃拼接策略,可将短线性 DNA 近乎定量地转化为单体环状 DNA。此外,我们还以 44 nt circRNA 为支架链,构建了混合 RNA:DNA 和纯 RNA:RNA 双交叉瓦片及其核酸纳米管和扁平阵列组装体。
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引用次数: 0
Electron beam lithography of GeTe through polymorphic phase transformation 通过多晶相变实现 GeTe 的电子束光刻技术
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1039/d4nh00035h
Hu Zhang, Meng Li, Shao-Bo Mi, Shaodong Cheng, Lu Lu, Zhi-Gang Chen
We report two previously undiscovered phases of GeTe including the sphalerite (c-) phase and the hexagonal (h-) phase with interlayer van der Waals gaps. A polymorphic phase transformation from rhombohedral α-GeTe to c- and h-GeTe near room temperature is first realized via electron beam irradiation. Their underlying thermodynamics and kinetics are illustrated by the in-situ heating experiments and molecular dynamics simulation. Density-functional theory calculation indicates that c-GeTe exhibits typical metallic behavior and h-GeTe is a narrow-gap semiconductor with a strong spin-orbital coupling effect. Our findings shed light on a strategy for designing GeTe-based quantum devices compromising nanopillars and heterostructures via an atomic-scale electron beam lithography technique.
我们报告了两种以前未被发现的 GeTe 相,包括闪锌矿(c-)相和具有层间范德华间隙的六方(h-)相。通过电子束辐照,在室温附近首次实现了从斜方体α-GeTe到c-和h-GeTe的多晶相变。原位加热实验和分子动力学模拟说明了它们的基本热力学和动力学。密度泛函理论计算表明,c-GeTe 具有典型的金属特性,而 h-GeTe 则是一种具有强烈自旋轨道耦合效应的窄隙半导体。我们的研究结果为通过原子尺度电子束光刻技术设计基于 GeTe 的量子器件(包括纳米柱和异质结构)提供了策略启示。
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引用次数: 0
Multi-metallic MOF based composites for environmental applications: synergizing metal centers and interactions. 基于多金属 MOF 的环境应用复合材料:金属中心与相互作用的协同作用。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-10 DOI: 10.1039/d4nh00140k
Wei Wang, Bergoi Ibarlucea, Chuanhui Huang, Renhao Dong, Muhannad Al Aiti, Shirong Huang, Gianaurelio Cuniberti

The escalating threat of environmental issues to both nature and humanity over the past two decades underscores the urgency of addressing environmental pollutants. Metal-organic frameworks (MOFs) have emerged as highly promising materials for tackling these challenges. Since their rise in popularity, extensive research has been conducted on MOFs, spanning from design and synthesis to a wide array of applications, such as environmental remediation, gas storage and separation, catalysis, sensors, biomedical and drug delivery systems, energy storage and conversion, and optoelectronic devices, etc. MOFs possess a multitude of advantageous properties such as large specific surface area, tunable porosity, diverse pore structures, multi-channel design, and molecular sieve capabilities, etc., making them particularly attractive for environmental applications. MOF-based composites inherit the excellent properties of MOFs and also exhibit unique physicochemical properties and structures. The tailoring of central coordinated metal ions in MOFs is critical for their adaptability in environmental applications. Although many reviews on monometallic, bimetallic, and polymetallic MOFs have been published, few reviews focusing on MOF-based composites with monometallic, bimetallic, and multi-metallic centers in the context of environmental pollutant treatment have been reported. This review addresses this gap by providing an in-depth overview of the recent progress in MOF-based composites, emphasizing their applications in hazardous gas sensing, electromagnetic wave absorption (EMWA), and pollutant degradation in both aqueous and atmospheric environments and highlighting the importance of the number and type of metal centers present. Additionally, the various categories of MOFs are summarized. MOF-based composites demonstrate significant promise in addressing environmental challenges, and this review provides a clear and valuable perspective on their potential in environmental applications.

过去二十年来,环境问题对自然和人类的威胁不断升级,这凸显了解决环境污染物问题的紧迫性。金属有机框架(MOFs)已成为应对这些挑战的极有前途的材料。自 MOFs 开始流行以来,人们对其进行了广泛的研究,从设计和合成到广泛的应用,如环境修复、气体储存和分离、催化、传感器、生物医学和药物输送系统、能量储存和转换以及光电器件等。MOFs 具有多种优势特性,如比表面积大、孔隙率可调、孔隙结构多样、多通道设计和分子筛功能等,因此在环境应用方面特别具有吸引力。基于 MOF 的复合材料继承了 MOF 的优良特性,同时也表现出独特的物理化学特性和结构。定制 MOF 中的中心配位金属离子对其在环境应用中的适应性至关重要。尽管有关单金属、双金属和多金属 MOFs 的综述已经发表了很多,但很少有综述关注在环境污染物处理中基于 MOFs 的单金属、双金属和多金属中心复合材料。本综述针对这一空白,深入综述了基于 MOF 的复合材料的最新进展,强调了它们在有害气体传感、电磁波吸收 (EMWA) 以及水环境和大气环境中污染物降解方面的应用,并强调了存在的金属中心的数量和类型的重要性。此外,还总结了 MOF 的各种类别。基于 MOF 的复合材料在应对环境挑战方面大有可为,本综述从一个清晰而有价值的角度阐述了它们在环境应用中的潜力。
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引用次数: 0
Oxidative stress modulating nanomaterials and their biochemical roles in nanomedicine 氧化应激调节纳米材料及其在纳米医学中的生化作用
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-10 DOI: 10.1039/d4nh00171k
Kapil Patel, Zalike Keskin Erdogan, Prasad Sawadkar, Nik Syahirah Aliaa, Mark R. Shannon, Madhumita Patel, Lady Barrios Silva, Rajkumar Patel, David Y. S. Chau, Jonathan Campbell Knowles, Adam Periman, Hae-Won Kim
Many pathological conditions are predominantly associated with oxidative stress, arising from reactive oxygen species (ROS); therefore, the modulation of redox activities has been a key strategy to restore normal tissue functions. Current approaches involve establishing a favorable cellular redox environment through the administration of therapeutic drugs and redox-active nanomaterials (RANs). In particular, RANs not only provide a stable and reliable means of therapeutic delivery but also possess the capacity to finely tune various interconnected components, including radicals, enzymes, proteins, transcription factors, and metabolites. Here, we discuss the roles that engineered RANs play in a spectrum of pathological conditions, such as cancer, neurodegenerative diseases, infections, and inflammation. We visualize the dual functions of RANs as both generator and scavenger of ROS, emphasizing their profound impact on diverse cellular functions. The focus of this review is solely on inorganic redox-active nanomaterials (inorganic RANs). Additionally, we deliberate on the challenges associated with current RANs-based approaches and propose potential research directions for their future clinical translation.
许多病理状况主要与活性氧(ROS)引起的氧化应激有关;因此,调节氧化还原活动一直是恢复正常组织功能的关键策略。目前的方法包括通过施用治疗药物和氧化还原活性纳米材料(RANs)来建立有利的细胞氧化还原环境。特别是,氧化还原活性纳米材料不仅能提供稳定可靠的治疗给药方式,还能精细调节各种相互关联的成分,包括自由基、酶、蛋白质、转录因子和代谢物。在这里,我们将讨论工程 RANs 在癌症、神经退行性疾病、感染和炎症等一系列病理情况中发挥的作用。我们直观地展示了 RANs 作为 ROS 生成器和清除器的双重功能,强调了它们对各种细胞功能的深远影响。本综述的重点仅在于无机氧化还原活性纳米材料(无机 RANs)。此外,我们还探讨了当前基于 RANs 的方法所面临的挑战,并为其未来的临床转化提出了潜在的研究方向。
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引用次数: 0
Luminescent carbon dots versus quantum dots and gold nanoclusters as sensors 发光碳点与量子点和纳米金簇作为传感器的比较
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-09 DOI: 10.1039/d4nh00107a
J. S. Anjali Devi, S. Madanan Anju, LEKHA G M, R. S. Aparna, Sony George
The ultra-small nanoparticles, including quantum dots, gold nanoclusters (AuNCs) and carbon dots (CDs), have emerged as a promising class of fluorescent material because of their molecular like properties and widespread applications in sensing and imaging. However, the fluorescence properties of ultra-small gold nanoparticles (i.e., AuNCs) and CDs are more complicated and well distinguished from conventional quantum dots or organic dye molecules. In this frontiers, we highlight the recent development in the fundamental understanding of the fluorescence emission mechanism of these ultra-small nanoparticles. Moreover, this review carefully analyses the underlying principles of ultra-small nanoparticle sensors. We expected that this information on ultra-small nanoparticles can fuel the research aimed to achieve precise control over their fluorescence properties and the broadening of their applications.
包括量子点、金纳米团簇(AuNCs)和碳点(CDs)在内的超小型纳米粒子因其类似分子的特性而成为一类前景广阔的荧光材料,并在传感和成像领域得到广泛应用。然而,超小型金纳米颗粒(即 AuNCs)和碳点的荧光特性更为复杂,与传统量子点或有机染料分子有很大区别。在这篇前沿论文中,我们重点介绍了对这些超小纳米粒子荧光发射机制的基本认识的最新进展。此外,这篇综述还仔细分析了超小纳米粒子传感器的基本原理。我们希望这些关于超小纳米粒子的信息能够推动旨在实现对其荧光特性的精确控制和扩大其应用范围的研究。
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引用次数: 0
Innovations of metallic contacts on semiconducting 2D transition metal dichalcogenides toward advanced 3D-structured field-effect transistors. 半导体二维过渡金属二卤化物金属触点的创新,迈向先进的三维结构场效应晶体管。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-08 DOI: 10.1039/d4nh00030g
Byeongchan Kim, Seojoo Lee, Jin-Hong Park

2D semiconductors, represented by transition metal dichalcogenides (TMDs), have the potential to be alternative channel materials for advanced 3D field-effect transistors, such as gate-all-around field-effect-transistors (GAAFETs) and complementary field-effect-transistors (C-FETs), due to their inherent atomic thinness, moderate mobility, and short scaling lengths. However, 2D semiconductors encounter several technological challenges, especially the high contact resistance issue between 2D semiconductors and metals. This review provides a comprehensive overview of the high contact resistance issue in 2D semiconductors, including its physical background and the efforts to address it, with respect to their applicability to GAAFET structures.

以过渡金属二掺杂物(TMDs)为代表的二维半导体,由于其固有的原子薄度、中等迁移率和短缩放长度,有潜力成为先进三维场效应晶体管(如全栅场效应晶体管(GAAFETs)和互补场效应晶体管(C-FETs))的替代通道材料。然而,二维半导体也遇到了一些技术挑战,尤其是二维半导体与金属之间的高接触电阻问题。本综述全面概述了二维半导体的高接触电阻问题,包括其物理背景和解决该问题的努力,以及它们对 GAAFET 结构的适用性。
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引用次数: 0
Insight into mechanism for remarkable photocatalytic hydrogen evolution of Cu/Pr dual atom co-modified TiO2. 洞察 Cu/Pr 双原子共修饰 TiO2 卓越的光催化氢进化机理。
IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-08 DOI: 10.1039/d4nh00196f
Hongshun Zheng, Baoye Zi, Tong Zhou, Guoyang Qiu, Zhongge Luo, Qingjie Lu, Alain Rafael Puente Santiago, Yumin Zhang, Jianhong Zhao, Jin Zhang, Tianwei He, Qingju Liu

The development of high-activity photocatalysts is crucial for the current large-scale development of photocatalytic hydrogen applications. Herein, we have developed a strategy to significantly enhance the hydrogen photocatalytic activity of Cu/Pr di-atom co-modified TiO2 architectures by selectively anchoring Cu single atoms on the oxygen vacancies of the TiO2 surface and replacing a trace of Ti atoms in the bulk with rare earth Pr atoms. Calculation results demonstrated that the synergistic effect between Cu single atoms and Pr atoms regulates the electronic structure of Cu/Pr-TiO2, thus promoting the separation of photogenerated carriers and their directional migration to Cu single atoms for the photocatalytic reaction. Furthermore, the d-band center of Cu/Pr-TiO2, which is located at -4.70 eV, optimizes the adsorption and desorption behavior of H*. Compared to TiO2, Pr-TiO2, and Cu/TiO2, Cu/Pr-TiO2 displays the best H* adsorption Gibbs free energy (-0.047 eV). Furthermore, experimental results confirmed that the photogenerated carrier lifetime of Cu/Pr-TiO2 is not only the longest (2.45 ns), but its hydrogen production rate (34.90 mmol g-1 h-1) also significantly surpasses those of Cu/TiO2 (13.39 mmol g-1 h-1) and Pr-TiO2 (0.89 mmol g-1 h-1). These findings open up a novel atomic perspective for the development of optimal hydrogen activity in dual-atom-modified TiO2 photocatalysts.

开发高活性光催化剂对于当前大规模开发光催化氢气应用至关重要。在此,我们开发了一种策略,通过选择性地将 Cu 单原子锚定在 TiO2 表面的氧空位上,并用稀土 Pr 原子取代块体中的微量 Ti 原子,从而显著提高了 Cu/Pr 二原子共修饰 TiO2 结构的氢光催化活性。计算结果表明,Cu 单原子和 Pr 原子之间的协同效应调节了 Cu/Pr-TiO2 的电子结构,从而促进了光生载流子的分离及其向 Cu 单原子的定向迁移,以进行光催化反应。此外,Cu/Pr-TiO2 的 d 带中心位于 -4.70 eV,优化了 H* 的吸附和解吸行为。与 TiO2、Pr-TiO2 和 Cu/TiO2 相比,Cu/Pr-TiO2 显示出最佳的 H* 吸附吉布斯自由能(-0.047 eV)。此外,实验结果证实,Cu/Pr-TiO2 的光生载流子寿命不仅最长(2.45 ns),而且其产氢速率(34.90 mmol g-1 h-1)也大大超过了 Cu/TiO2 (13.39 mmol g-1 h-1)和 Pr-TiO2(0.89 mmol g-1 h-1)。这些发现为在双原子修饰的二氧化钛光催化剂中开发最佳氢气活性开辟了新的原子视角。
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引用次数: 0
Mechanical Regulation to Interfacial Thermal Transport in GaN/Diamond Heterostructures for Thermal Switch 用于热交换器的氮化镓/金刚石异质结构中对界面热传输的机械调节
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-08 DOI: 10.1039/d4nh00245h
Xiaotong Yu, Yifan Li, Renjie He, Yanwei Wen, Rong Chen, Baoxing Xu, Yuan Gao
Gallium nitride offers an ideal material platform for the next-generation high-power electronics device. Thermal management against the ever-growing power density has become a major bottleneck to the performance, reliability, and lifetime of the devices. GaN/diamond heterostructures are usually adopted to facilitate heat dissipation, given the extraordinary thermal conduction properties of diamonds. However, the thermal transport is limited by the interfacial conductance at the material interface between GaN and diamond, which is associated with significant mechanical stress at the atomic level. In this work, we investigate the effect of mechanical on the interfacial thermal conductance of heterostructures using full-atom non-equilibrium molecular dynamics simulations. We found that the heterostructure possesses severe mechanical stress at the interface in the absence of loading, which is due to lattice mismatch. Upon tensile/compressive loading, the interfacial stress is more pronounced, and the strain is not identical across the interface owing to the contrasting elastic moduli of GaN and diamond. In addition, the interfacial thermal conductance can be adjusted by 400% due to the applied mechanical loading. More detailed analyses reveal that the change in the interfacial thermal conductance is related to the surface roughness and interfacial bonding strength, described by a generalized relationship. Moreover, phonon analyses suggest that the unequal mechanical deformation under compressive strain in GaN and diamond induces different frequency shifts in the phonon spectra, leading to enhancement in phonon overlapping energy, which promotes phonon transport at the interface and elevates the thermal conductance, and vice versa for tensile strain. The effect of strain on interface thermal conductance preserves for various temperatures. Based on the mechanical tunability of thermal conductance, we propose a conceptual design of a mechanical thermal switch that regulates thermal conductance with excellent sensitivity and high responsiveness. This study offers a fundamental understanding of how mechanical strain can adjust interface thermal conductance in GaN/diamond heterostructures from the aspect of mechanical stress, deformation, and phonon properties. These results and findings lay the theoretical foundation for designing thermal management devices in a strain environment and shed light on developing intelligent thermal devices by leveraging the interplay between mechanics and thermal transport.
氮化镓为下一代大功率电子器件提供了理想的材料平台。面对不断增长的功率密度,热管理已成为设备性能、可靠性和使用寿命的主要瓶颈。由于金刚石具有非凡的热传导特性,因此通常采用氮化镓/金刚石异质结构来促进散热。然而,热传输受限于氮化镓和金刚石之间材料界面的界面传导,而界面传导与原子级的巨大机械应力有关。在这项工作中,我们利用全原子非平衡分子动力学模拟研究了机械对异质结构界面热传导的影响。我们发现,异质结构在无负载的情况下,由于晶格失配,在界面上具有严重的机械应力。在拉伸/压缩载荷作用下,界面应力更加明显,而且由于氮化镓和金刚石的弹性模量不同,整个界面的应变也不尽相同。此外,由于施加了机械负载,界面热导率可调整 400%。更详细的分析表明,界面热导率的变化与表面粗糙度和界面结合强度有关,两者之间存在广义关系。此外,声子分析表明,氮化镓和金刚石在压缩应变下的不等机械变形会引起声子频谱的不同频率偏移,导致声子重叠能增强,从而促进声子在界面上的传输并提高热导率,反之亦然。在不同温度下,应变对界面热导率的影响保持不变。基于热导的机械可调性,我们提出了一种机械热开关的概念设计,它能以出色的灵敏度和高响应性调节热导。这项研究从机械应力、形变和声子特性等方面,从根本上理解了机械应变如何调节氮化镓/金刚石异质结构中的界面热导。这些结果和发现为在应变环境中设计热管理器件奠定了理论基础,并为利用力学和热传输之间的相互作用开发智能热器件提供了启示。
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引用次数: 0
Colloidal TiO2 Nanocrystals with Engineered Defectivity and Optical Properties 具有工程缺陷和光学特性的胶体二氧化钛纳米晶体
IF 9.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-05 DOI: 10.1039/d4nh00143e
Julia J. Chang, Livio Gamba, Bin Yuan, Sandro Mignuzzi, Riccardo Sapienza, Francesco Mezzadri, Ludovico Cademartiri
Partially reduced forms of titanium dioxide (sometimes called “black” titania) have attracted widespread interest as promising photocatalysts of oxidation due to their absorption in the visible. The main approaches to produce it rely on postprocessing at high temperatures (up to 800 °C) and high pressures (up to 40 bar) or on highly reactive precursors (e.g., TiH2), and yield powders with poorly controlled sizes, shapes, defect concentrations and distributions. We describe an approach for the one-step synthesis of TiO2 colloidal nanocrystals at atmospheric pressure and temperatures as low as 280°C. The temperature of reaction allows to control the density of oxygen vacancies by nearly two orders of magnitude independently of their size, shape, or colloidal stability. This synthetic pathway appears to produce vacancies that are homogeneously distributed in the nanocrystals, rather than being concentrated in an amorphous shell. As a result the defects are protected from oxidation and result in stable optical properties in oxidizing environments.
部分还原形式的二氧化钛(有时称为 "黑色 "二氧化钛)因其在可见光下的吸收能力,作为一种有前途的氧化光催化剂引起了广泛的兴趣。生产二氧化钛的主要方法依赖于高温(高达 800 °C)高压(高达 40 巴)或高活性前驱体(如 TiH2)的后处理,产生的粉末尺寸、形状、缺陷浓度和分布控制不佳。我们介绍了一种在大气压力和低至 280°C 的温度下一步合成 TiO2 胶体纳米晶体的方法。反应温度可将氧空位的密度控制在近两个数量级,而与它们的大小、形状或胶体稳定性无关。这种合成途径似乎能产生均匀分布在纳米晶体中的空位,而不是集中在无定形的外壳中。因此,这些缺陷可防止氧化,从而在氧化环境中保持稳定的光学特性。
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引用次数: 0
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Nanoscale Horizons
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