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DNA–Iron Oxide Nanoparticles Conjugates: Functional Magnetic Nanoplatforms in Biomedical Applications dna -氧化铁纳米粒子共轭物:生物医学应用中的功能磁性纳米平台
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2020-01-10 DOI: 10.1007/s41061-019-0277-9
José Raúl Sosa-Acosta, Claudia Iriarte-Mesa, Greter A. Ortega, Alicia M. Díaz-García

The use of magnetic nanoparticles (MNPs), such as iron oxide nanoparticles (IONPs), in biomedicine is considered to be a valuable alternative to the more traditional materials due to their chemical stability, cost-effectiveness, surface functionalization, and the possibility to selectively attach and transport targeted species to the desired location under a magnetic field. One of the many main applications of MNPs is DNA separation, which enables genetic material manipulation; consequently, MNPs are used in numerous biotechnological methods, such as gene transfection and molecular recognition systems. In addition, the interaction between the surfaces of MNPs and DNA molecules and the magnetic nature of the resulting composite have facilitated the development of safe and effective gene delivery vectors to treat significant diseases, such as cancer and neurological disorders. Furthermore, the special recognition properties of nucleic acids based on the binding capacity of DNA and the magnetic behavior of the nanoparticles allowing magnetic separation and concentration of analytes have led to the development of biosensors and diagnostic assays; however, both of these applications face important challenges in terms of the improvement of selective nanocarriers and biosensing capacity. In this review, we discuss some aspects of the properties and surface functionalization of MNPs, the interactions between DNA and IONPs, the preparation of DNA nanoplatforms and their biotechnological applications, such as the magnetic separation of DNA, magnetofection, preparation of DNA vaccines, and molecular recognition tools.

磁性纳米颗粒(MNPs),如氧化铁纳米颗粒(IONPs),由于其化学稳定性、成本效益、表面功能化以及在磁场下选择性地附着和运输目标物质到所需位置的可能性,在生物医学中被认为是传统材料的有价值的替代品。MNPs的许多主要应用之一是DNA分离,它使遗传物质操作成为可能;因此,MNPs被用于许多生物技术方法,如基因转染和分子识别系统。此外,MNPs表面与DNA分子之间的相互作用以及所产生的复合材料的磁性,促进了安全有效的基因传递载体的发展,以治疗重大疾病,如癌症和神经系统疾病。此外,基于DNA结合能力的核酸的特殊识别特性和纳米颗粒的磁性行为,允许对分析物进行磁分离和浓缩,导致了生物传感器和诊断分析的发展;然而,在选择性纳米载体和生物传感能力的提高方面,这两种应用都面临着重要的挑战。在这篇综述中,我们讨论了MNPs的性质和表面功能化、DNA和IONPs之间的相互作用、DNA纳米平台的制备及其在生物技术方面的应用,如DNA的磁分离、磁效应、DNA疫苗的制备和分子识别工具。
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引用次数: 23
MOFs-Based Catalysts Supported Chemical Conversion of CO2 基于mofs的催化剂支持CO2化学转化
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2020-01-06 DOI: 10.1007/s41061-019-0269-9
Ying Shi, Shengli Hou, Xiaohang Qiu, Bin Zhao

The dramatic increase in atmospheric carbon dioxide (CO2) concentrations has attracted human attention and many strategies about converting CO2 into high-value chemicals have been put forward. Metal–organic frameworks (MOFs), as a class of versatile materials, have been widely used in CO2 capture and chemical conversion, due to their unique porosity, multiple active centers and good stability and recyclability. Herein, we focused on the processes of chemical conversion of CO2 by MOFs-based catalysts, including the coupling reactions of epoxides, aziridines or alkyne molecules, CO2 hydrogenation, and other CO2 conversion reactions. The synthesized methods and high catalytic activity of MOFs-based materials were also analyzed systematically. Finally, a brief perspective on feasible strategies is presented to improve the catalytic activity of novel MOFs-based materials and explore the new CO2 conversion reactions.

大气中二氧化碳浓度的急剧增加引起了人们的关注,并提出了许多将二氧化碳转化为高价值化学品的策略。金属有机骨架(mof)作为一类多用途材料,由于其独特的多孔性、多个活性中心以及良好的稳定性和可回收性,在CO2捕集和化学转化中得到了广泛的应用。本文重点研究了基于mofs的催化剂对CO2的化学转化过程,包括环氧化物、氮嘧啶或炔分子的偶联反应、CO2加氢反应和其他CO2转化反应。对mofs基材料的合成方法和高催化活性进行了系统分析。最后,对提高新型mofs基材料的催化活性和探索新型CO2转化反应的可行策略进行了简要展望。
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引用次数: 33
DNA Strand Displacement Reaction: A Powerful Tool for Discriminating Single Nucleotide Variants DNA链置换反应:鉴别单核苷酸变异的强大工具
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2020-01-02 DOI: 10.1007/s41061-019-0274-z
Weiyang Tang, Weiye Zhong, Yun Tan, Guan A. Wang, Feng Li, Yizhen Liu

Single-nucleotide variants (SNVs) that are strongly associated with many genetic diseases and tumors are important both biologically and clinically. Detection of SNVs holds great potential for disease diagnosis and prognosis. Recent advances in DNA nanotechnology have offered numerous principles and strategies amenable to the detection and quantification of SNVs with high sensitivity, specificity, and programmability. In this review, we will focus our discussion on emerging techniques making use of DNA strand displacement, a basic building block in dynamic DNA nanotechnology. Based on their operation principles, we classify current SNV detection methods into three main categories, including strategies using toehold-mediated strand displacement reactions, toehold-exchange reactions, and enzyme-mediated strand displacement reactions. These detection methods discriminate SNVs from their wild-type counterparts through subtle differences in thermodynamics, kinetics, or response to enzymatic manipulation. The remarkable programmability of dynamic DNA nanotechnology also allows the predictable design and flexible operation of diverse strand displacement probes and/or primers. Here, we offer a systematic survey of current strategies, with an emphasis on the molecular mechanisms and their applicability to in vitro diagnostics.

单核苷酸变异(snv)与许多遗传疾病和肿瘤密切相关,在生物学和临床上都很重要。snv的检测对疾病的诊断和预后具有很大的潜力。DNA纳米技术的最新进展为snv的检测和定量提供了许多具有高灵敏度、特异性和可编程性的原则和策略。在这篇综述中,我们将重点讨论利用DNA链位移的新兴技术,这是动态DNA纳米技术的基本组成部分。根据其工作原理,我们将目前的SNV检测方法分为三大类,包括使用支点介导的链位移反应、支点交换反应和酶介导的链位移反应的策略。这些检测方法通过热力学、动力学或对酶操作的反应的细微差异来区分snv与野生型。动态DNA纳米技术的显著可编程性也允许各种链位移探针和/或引物的可预测设计和灵活操作。在这里,我们提供了当前策略的系统调查,重点是分子机制及其在体外诊断中的适用性。
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引用次数: 37
Recent Progress in Asymmetric Relay Catalysis of Metal Complex with Chiral Phosphoric Acid 手性磷酸催化金属配合物的不对称催化研究进展
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-12-27 DOI: 10.1007/s41061-019-0263-2
Pu-Sheng Wang, Dian-Feng Chen, Liu-Zhu Gong

Asymmetric metal/organo relay catalysis, utilizing a metal complex and a chiral organocatalyst in a one-pot cascade reaction, is aimed to sequentially impart activation on multiple steps by distinct catalysts. Such a catalysis merges the advantages of both metal catalysis and organocatalysis, providing step-economy, and, more importantly, the potential to achieve inaccessible reactivity by a single catalyst. Chiral phosphoric acids are among the most robust organocatalysts, rendering a broad range of enantioselective bond-forming reactions. The combination of metal complexes and chiral phosphoric acids in a single vessel has been well documented. In particular, the asymmetric relay catalysis of metal complex with chiral phosphoric acid has grown rapidly since 2008. Several excellent reviews have been published to cover almost all examples in this area from 2008 to early 2014; therefore, in this chapter, we will mainly highlight progress from 2014 to mid-2019.

不对称金属/有机接力催化,利用金属配合物和手性有机催化剂在一锅级联反应中,旨在通过不同的催化剂在多个步骤上依次激活。这种催化结合了金属催化和有机催化的优点,提供了阶梯经济,更重要的是,有可能通过单一催化剂实现难以达到的反应性。手性磷酸是最强大的有机催化剂之一,呈现广泛的对映选择性成键反应。金属配合物和手性磷酸在单一容器中的结合已被充分记录。特别是自2008年以来,金属配合物与手性磷酸的不对称接力催化得到了迅速发展。从2008年到2014年初,已经发表了几篇优秀的综述,几乎涵盖了该领域的所有例子;因此,在本章中,我们将重点介绍2014年至2019年中期的进展情况。
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引用次数: 31
Limitations and Prospects for Wastewater Treatment by UV and Visible-Light-Active Heterogeneous Photocatalysis: A Critical Review 紫外光和可见光活性非均相光催化处理废水的局限性与展望
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-12-16 DOI: 10.1007/s41061-019-0272-1
Giuseppina Iervolino, Ian Zammit, Vincenzo Vaiano, Luigi Rizzo

Heterogeneous photocatalysis (HPC) has been widely investigated in recent decades for the removal of a number of contaminants from aqueous matrices, but its application in real wastewater treatment at full scale is still scarce. Indeed, process and technological limitations have made HPC uncompetitive with respect to consolidated processes/technologies so far. In this manuscript, these issues are critically discussed and reviewed with the aim of providing the reader with a realistic picture of the prospective application of HPC in wastewater treatment. Accordingly, consolidated and new photocatalysts (among which the visible active ones are attracting increasing interest among the scientific community), along with preparation methods, are reviewed to understand whether, with increased process efficiency, these methods can be realistically and competitively developed at industrial scale. Precipitation is considered as an attractive method for photocatalyst preparation at the industrial scale; sol–gel and ultrasound may be feasible only if no expensive metal precursor is used, while hydrothermal and solution combustion synthesis are expected to be difficult (expensive) to scale up. The application of HPC in urban and industrial wastewater treatment and possible energy recovery by hydrogen production are discussed in terms of current limitations and future prospects. Despite the fact that HPC has been studied for the removal of pollutants in aqueous matrices for two decades, its use in wastewater treatment is still at a “technological research” stage. In order to accelerate the adoption of HPC at full scale, it is advisable to focus on investigations under real conditions and on developing/improving pilot-scale reactors to better investigate scale-up conditions and the potential to successfully address specific challenges in wastewater treatment through HPC. In realistic terms, the prospective use of HPC is more likely as a tertiary treatment of wastewater, particularly if more stringent regulations come into force, than as pretreatment for industrial wastewater to improve biodegradability.

近几十年来,多相光催化(HPC)在去除水基质中许多污染物方面得到了广泛的研究,但其在实际污水处理中的全面应用仍然很少。事实上,到目前为止,工艺和技术的限制使HPC在整合工艺/技术方面缺乏竞争力。在这份手稿中,这些问题进行了批判性的讨论和审查,目的是为读者提供高性能计算在废水处理中的潜在应用的现实情况。因此,本文综述了复合光催化剂和新型光催化剂(其中可见活性光催化剂正引起科学界越来越多的兴趣)及其制备方法,以了解在提高工艺效率的情况下,这些方法是否能够在工业规模上实现具有竞争力的开发。沉淀法被认为是一种在工业规模上制备光催化剂的有吸引力的方法;溶胶-凝胶法和超声波法只有在不使用昂贵的金属前驱体的情况下才可行,而水热法和溶液燃烧法的合成预计很难(昂贵)扩大规模。讨论了HPC在城市和工业废水处理中的应用,以及可能通过制氢回收能源的方法。尽管HPC用于去除水中污染物的研究已经进行了20年,但它在废水处理中的应用仍处于“技术研究”阶段。为了加速HPC的全面采用,建议将重点放在实际条件下的研究和开发/改进中试规模反应器上,以更好地研究扩大规模的条件和通过HPC成功解决废水处理中特定挑战的潜力。从现实的角度来看,HPC的潜在用途更有可能是作为废水的三级处理,尤其是在更严格的法规生效的情况下,而不是作为工业废水的预处理来提高生物降解性。
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引用次数: 109
Bioconjugated Plasmonic Nanoparticles for Enhanced Skin Penetration 增强皮肤穿透性的生物共轭等离子体纳米颗粒
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-12-16 DOI: 10.1007/s41061-019-0273-0
David Alba-Molina, Juan J. Giner-Casares, Manuel Cano

Plasmonic nanoparticles (NPs) are one of the most promising and studied inorganic nanomaterials for different biomedical applications. Plasmonic NPs have excellent biocompatibility, long-term stability against physical and chemical degradation, relevant optical properties, well-known synthesis methods and tuneable surface functionalities. Herein, we?review recently reported bioconjugated plasmonic NPs using different chemical approaches and loading cargoes (such as drugs, genes, and proteins) for enhancement of transdermal delivery across biological tissues. The main aim is to understand the interaction of the complex skin structure with biomimetic plasmonic NPs. This knowledge is not only important in enhancing transdermal delivery of pharmaceutical formulations but also for controlling undesired skin penetration of industrial products, such as cosmetics, sunscreen formulations and any other mass-usage consumable that contains plasmonic?NPs.

等离子体纳米粒子(NPs)是生物医学领域研究最广泛的无机纳米材料之一。等离子体NPs具有优异的生物相容性、抗物理和化学降解的长期稳定性、相关的光学性质、已知的合成方法和可调的表面功能。在此,我们呢?最近报道了生物共轭等离子体NPs使用不同的化学方法和装载货物(如药物、基因和蛋白质)来增强跨生物组织的透皮递送。主要目的是了解复杂皮肤结构与仿生等离子体NPs的相互作用。这一知识不仅对加强药物配方的透皮递送很重要,而且对控制工业产品(如化妆品、防晒霜配方和任何其他含有等离子体NPs的大量使用消费品)的不希望的皮肤渗透也很重要。
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引用次数: 12
Ferrite Materials for Photoassisted Environmental and Solar Fuels Applications 光辅助环境和太阳能燃料中的铁氧体材料
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-12-16 DOI: 10.1007/s41061-019-0270-3
Patricia Garcia-Muñoz, Fernando Fresno, Víctor A. de la Peña O’Shea, Nicolas Keller

Ferrites are a large class of oxides containing Fe3+ and at least another metal cation that have been investigated for and applied to a wide variety of fields ranging from mature technologies like circuitry, permanent magnets, magnetic recording and microwave devices to the most recent developments in areas like bioimaging, gas sensing and photocatalysis. In the last respect, although ferrites have been less studied than other types of semiconductors, they present interesting properties such as visible light absorption, tuneable optoelectronic properties and high chemical and photochemical stability. The versatility of their chemical composition and of their crystallographic structure opened a playground for developing new catalysts with enhanced efficiency. This article reviews the recent development of the application of ferrites to photoassisted processes for environmental remediation and for the synthesis of solar fuels. Applications in the photocatalytic degradation of pollutants in water and air, photo-Fenton, and solar fuels production, via photocatalytic and photoelectrochemical water splitting and CO2 reduction, are reviewed paying special attention to the relationships between the physico-chemical characteristics of the ferrite materials and their photoactivated performance.

铁氧体是一类含有Fe3+和至少另一种金属阳离子的氧化物,已经被研究并应用于各种领域,从成熟的技术,如电路,永磁体,磁记录和微波器件,到生物成像,气体传感和光催化等领域的最新发展。在最后一个方面,尽管铁氧体的研究比其他类型的半导体少,但它们具有有趣的特性,如可见光吸收,可调谐的光电特性以及高的化学和光化学稳定性。它们的化学成分和晶体结构的多样性为开发效率更高的新型催化剂开辟了广阔的天地。本文综述了铁氧体在光辅助环境修复和太阳能燃料合成中的应用进展。综述了铁氧体材料在光催化降解水和空气中的污染物、光fenton以及通过光催化和光电化学分解水和CO2还原制备太阳能燃料等方面的应用,重点介绍了铁氧体材料的物理化学特性与其光活化性能之间的关系。
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引用次数: 44
Functionalized Dynamic Metal–Organic Frameworks as Smart Switches for Sensing and Adsorption Applications 功能化动态金属有机框架作为传感和吸附应用的智能开关
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-12-11 DOI: 10.1007/s41061-019-0271-2
Binbin Qian, Ze Chang, Xian-He Bu

Over the past two decades, metal–organic frameworks (MOFs) with flexible structures or dynamic behavior have shown great potential as functional materials in many fields. This paper presents a review of these dynamic and functional MOFs, which can undergo controllable and reversible transformation, with regard to their application as smart switches. Trigger conditions, which include physical/chemical stimuli (e.g., guest molecules, light, temperature, pressure), are also discussed. Research methods for investigating the dynamic processes and mechanisms involving experimental characterization and computational modeling are briefly mentioned as well. The emphasis is on the aspects of the design and functionalization of dynamic MOFs. The pre-design of metal nodes, organic linkers, and topology, as well as post-modification of components, increases the possibility of obtaining functionalized dynamic materials. Recent advances with regard to potential applications for dynamic frameworks as smart switches for adsorption and sensing are also reviewed.

在过去的二十年中,具有柔性结构或动态性能的金属有机框架(MOFs)作为功能材料在许多领域显示出巨大的潜力。本文综述了这些动态和功能的MOFs,它们可以进行可控和可逆的转换,并将其应用于智能开关。触发条件,包括物理/化学刺激(例如,客体分子,光,温度,压力),也进行了讨论。简要介绍了研究动态过程和机制的方法,包括实验表征和计算建模。重点是动态MOFs的设计和功能化方面。金属节点、有机连接器和拓扑结构的预先设计,以及组件的后期修改,增加了获得功能化动态材料的可能性。本文还综述了动态框架作为吸附和传感智能开关的潜在应用方面的最新进展。
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引用次数: 13
Regulation of the Degree of Interpenetration in Metal–Organic Frameworks 金属-有机骨架中相互渗透程度的调控
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-12-02 DOI: 10.1007/s41061-019-0268-x
Gaurav Verma, Sydney Butikofer, Sanjay Kumar, Shengqian Ma

Interpenetration in metal–organic frameworks (MOFs) can have significant impacts on the structure, porous nature, and functional applications of MOFs. Considered to be disadvantageous in the initial phases leading to a decrease in surface area, interpenetration has proved to be highly useful for modulation of pore size and selective separation of gases. The importance of interpenetration has been realized over the last decade, and numerous approaches to graft interpenetration and utilize it for improved functions and applications have been achieved. Several factors such astemperature, solvent system, time duration and steric aspects of the ligands have been utilized to regulate the degree of interpenetration (DOI). In this review, we summarize recent advances in regulating the DOI in MOFs and its impact on the resulting properties.

金属-有机骨架(MOFs)的相互渗透对其结构、多孔性和功能应用具有重要影响。在初始阶段,互渗被认为是不利的,导致表面积的减少,但事实证明,互渗对孔径的调节和气体的选择性分离非常有用。在过去的十年中,人们已经认识到相互渗透的重要性,并且已经实现了许多嫁接相互渗透并利用它来改进功能和应用的方法。温度、溶剂体系、时间持续时间和配体的空间等因素都被用来调节相互渗透程度(DOI)。在本文中,我们总结了调控MOFs中DOI的最新进展及其对MOFs性能的影响。
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引用次数: 22
Waste-derived Materials: Opportunities in Photocatalysis 废物衍生材料:光催化的机会
IF 8.6 2区 化学 Q1 Chemistry Pub Date : 2019-11-28 DOI: 10.1007/s41061-019-0264-1
Daily Rodríguez-Padrón, Rafael Luque, Mario J. Muñoz-Batista

Waste-derived materials have been gaining increased attention in recent years due to their great potential and environmentally friendly nature. Several contributions in the literature have covered the advances achieved so far in this area. Nonetheless, to the best of our knowledge, no review has been dedicated specifically to waste-derived or templated photocatalytic materials. Both photocatalysis and (bio)waste-inspired design yield materials of a remarkably green nature. Therefore, the partnership between them may open promising possibilities for both waste valorization and photocatalytic processes, which in turn will lead to sustainable development globally, with the potential for full utilization of renewable energy sources such as biomass and sunlight. Several photocatalytic waste-derived materials, synthetic procedures, and applications will be described throughout this work, including waste-derived/templated TiO2, ZnO, and metal sulfide materials. Special attention will be given to biomass-inspired carbonaceous materials, including carbon quantum dots and graphitic carbon nitride (g-C3N4).

近年来,废物来源的材料由于其巨大的潜力和环境友好性而受到越来越多的关注。文献中的一些贡献涵盖了迄今为止在这一领域取得的进展。尽管如此,据我们所知,还没有专门针对废物衍生或模板化光催化材料的综述。光催化和(生物)废物启发设计产生的材料具有显著的绿色性质。因此,它们之间的伙伴关系可能为废物增值和光催化过程开辟有希望的可能性,这反过来将导致全球可持续发展,并有可能充分利用生物量和阳光等可再生能源。本文将介绍几种光催化废物衍生材料、合成方法和应用,包括废物衍生/模板化TiO2、ZnO和金属硫化物材料。特别关注生物质启发的碳质材料,包括碳量子点和石墨氮化碳(g-C3N4)。
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引用次数: 22
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Topics in Current Chemistry
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