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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, MULTIDISCIPLINARY 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
Asymmetric Reactions Enabled by Cooperative Enantioselective Amino- and Lewis Acid Catalysis 协同对映选择性氨基酸和路易斯酸催化实现的不对称反应
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-11-25 DOI: 10.1007/s41061-019-0261-4
Pier Giorgio Cozzi, Andrea Gualandi, Simone Potenti, Francesco Calogero, Giacomo Rodeghiero

Organocatalysis—the branch of catalysis featuring small organic molecules as the catalysts—has, in the last decade, become of central importance in the field of asymmetric catalysis, so much that it is now comparable to metal catalysis and biocatalysis. Organocatalysis is rationalized and classified by a number of so-called activation modes, based on the formation of a covalent or not-covalent intermediate between the organocatalyst and the organic substrate. Among all the organocatalytic activation modes, enamine and iminium catalysis are widely used for the practical preparation of valuable products and intermediates, both in academic and industrial contexts. In both cases, chiral amines are employed as catalysts. Enamine activation mode is generally employed in the reaction with electrophiles, while nucleophiles require the iminium activation mode. Commonly, in both modes, the reaction occurs through well-organized transitions states. A large variety of partners can react with enamines and iminium ions, due to their sufficient nucleophilicity and electrophilicity, respectively. However, despite the success, organocatalysis still suffers from narrow scopes and applications. Multicatalysis is a possible solution for these drawbacks because the two different catalysts can synergistically activate the substrates, with a simultaneous activation of the two different reaction partners. In particular, in this review we will summarize the reported processes featuring Lewis acid catalysis and organocatalytic activation modes synergically acting and not interfering with each other. We will focus our attention on the description of processes in which good results cannot be achieved independently by organocatalysis or Lewis acid catalysis. In these examples of cooperative dual catalysis, a number of new organic transformations have been developed. The review will focus on the possible strategies, the choice of the Lewis acid and the catalytic cycles involved in the effective reported combination. Additionally, some important key points regarding the rationale for the effective combinations will be also included. π-Activation of organic substrates by Lewis acids, via formation of electrophilic intermediates, and their reaction with enamines will be also discussed in this review.

有机催化是催化的一个分支,以小有机分子为催化剂,在过去十年中,它在不对称催化领域中变得至关重要,以至于现在可以与金属催化和生物催化相媲美。基于在有机催化剂和有机底物之间形成共价或非共价中间体,有机催化被合理化和分类为许多所谓的激活模式。在所有的有机催化活化方式中,无论是在学术上还是在工业上,烯胺和胺催化都被广泛用于实际制备有价值的产品和中间体。在这两种情况下,手性胺被用作催化剂。与亲电试剂的反应一般采用烯胺活化方式,而亲核试剂则需要最小活化方式。通常,在这两种模式中,反应都是通过组织良好的过渡态发生的。由于胺类和胺类离子具有足够的亲核性和亲电性,大量的络合物可以分别与它们发生反应。然而,尽管取得了成功,有机催化仍然受到范围和应用范围的限制。多催化是一种可能的解决方案,因为两种不同的催化剂可以协同激活底物,同时激活两种不同的反应伙伴。特别是,在这篇综述中,我们将总结Lewis酸催化和有机催化活化模式协同作用而互不干扰的报道过程。我们将把注意力集中在不能通过有机催化或路易斯酸催化独立获得良好结果的过程的描述上。在这些协同双重催化的例子中,已经发展出一些新的有机转化。本文将重点讨论Lewis酸的选择和催化循环等可能的策略。此外,关于有效组合的基本原理的一些重要关键点也将包括在内。本文还将讨论路易斯酸通过形成亲电中间体对有机底物的π活化及其与胺的反应。
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引用次数: 53
Mechanochemical Forces as a Synthetic Tool for Zero- and One-Dimensional Titanium Oxide-Based Nano-photocatalysts 机械化学力作为零和一维氧化钛基纳米光催化剂的合成工具
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-11-25 DOI: 10.1007/s41061-019-0262-3
Dimitrios A. Giannakoudakis, Gregory Chatel, Juan Carlos Colmenares
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引用次数: 30
Enamine/Transition Metal Combined Catalysis: Catalytic Transformations Involving Organometallic Electrophilic Intermediates 烯胺/过渡金属组合催化:涉及有机金属亲电中间体的催化转化
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-11-16 DOI: 10.1007/s41061-019-0267-y
Samson Afewerki, Armando Córdova

The concept of merging enamine activation catalysis with transition metal catalysis is an important strategy, which allows for selective chemical transformations not accessible without this combination. The amine catalyst activates the carbonyl compounds through the formation of a reactive nucleophilic enamine intermediate and, in parallel, the transition metal activates a wide range of functionalities such as allylic substrates through the formation of reactive electrophilic π-allyl-metal complex. Since the first report of this strategy in 2006, considerable effort has been devoted to the successful advancement of this technology. In this chapter, these findings are highlighted and discussed.

将烯胺活化催化与过渡金属催化合并的概念是一种重要的策略,它允许没有这种组合就无法实现选择性化学转化。胺催化剂通过形成反应性亲核烯胺中间体激活羰基化合物,同时,过渡金属通过形成反应性亲电π-烯丙基金属配合物激活广泛的功能,如烯丙基底物。自2006年这一战略的第一份报告发布以来,为成功地推进这一技术作出了相当大的努力。在本章中,这些发现被强调和讨论。
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引用次数: 12
Organocatalysis Combined with Photocatalysis 有机催化与光催化相结合
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-11-15 DOI: 10.1007/s41061-019-0265-0
Yi-Yin Liu, Jing Liu, Liang-Qiu Lu, Wen-Jing Xiao

Over the past decade, the combination of visible light photocatalysis and organocatalysis has made remarkable progress in modern chemical synthesis. In these dual catalysis system, photocatalysts or photosensitizers absorb visible light to induce their photoexcited states which can activate unreactive substrates via electron or energy transfer mechanisms, and organocatalysts are usually employed to regulate the chemical reactivity of the other substrates. By doing so, two reactive species react with each in a selective—especially enantioselective—way, to provide the final products. This article summarizes the recent development of cooperative catalysis by the combination of organocatalysis and photocatalysis in asymmetric organic synthesis. These reactions are classified according to the manner of activation of the organocatalysts. Enamine/iminium catalysts are used to activate unreactive carbonyl molecules. Nucleophilic catalysts including nitrogen heterocycle carbene catalysts and tertiary amine catalysts are employed to reverse the reactivity of electrodeficient substrates including aldehydes and enals. Chiral Br?nsted acid catalysts are used to activate substrates by forming key H-bonding complexes between substrates and catalysts.

近十年来,可见光光催化与有机催化的结合在现代化学合成中取得了令人瞩目的进展。在这些双重催化体系中,光催化剂或光敏剂吸收可见光诱导其光激发态,通过电子或能量转移机制激活未反应的底物,而有机催化剂通常用于调节其他底物的化学反应性。通过这样做,两种活性物质以选择性(尤其是对映体选择性)的方式相互反应,从而产生最终产物。本文综述了不对称有机合成中有机催化与光催化相结合的协同催化的最新进展。这些反应根据有机催化剂的活化方式进行分类。烯胺/铝催化剂用于激活不活泼的羰基分子。亲核催化剂包括氮杂环碳催化剂和叔胺催化剂被用来逆转包括醛和烯醛在内的缺电底物的反应性。手性Br吗?嵌套酸催化剂通过在底物和催化剂之间形成键氢键配合物来激活底物。
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引用次数: 15
Heterogeneous Catalyzed Thermochemical Conversion of Lignin Model Compounds: An Overview 木质素模型化合物的非均相催化热化学转化研究综述
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-11-14 DOI: 10.1007/s41061-019-0260-5
Mikel Oregui-Bengoechea, Ion Agirre, Aitziber Iriondo, Alexander Lopez-Urionabarrenechea, Jesus M. Requies, Iker Agirrezabal-Telleria, Kepa Bizkarra, V. Laura Barrio, Jose F. Cambra

Thermochemical lignin conversion processes can be described as complex reaction networks involving not only de-polymerization and re-polymerization reactions, but also chemical transformations of the depolymerized mono-, di-, and oligomeric compounds. They typically result in a product mixture consisting of a gaseous, liquid (i.e., mono-, di-, and oligomeric products), and solid phase. Consequently, researchers have developed a common strategy to simplify this issue by replacing lignin with simpler, but still representative, lignin model compounds. This strategy is typically applied to the elucidation of reaction mechanisms and the exploration of novel lignin conversion approaches. In this review, we present a general overview of the latest advances in the principal thermochemical processes applied for the conversion of lignin model compounds using heterogeneous catalysts. This review focuses on the most representative lignin conversion methods, i.e., reductive, oxidative, pyrolytic, and hydrolytic processes. An additional subchapter on the reforming of pyrolysis oil model compounds has also been included. Special attention will be given to those research papers using “green” reactants (i.e., H2 or renewable hydrogen donor molecules in reductive processes or air/O2 in oxidative processes) and solvents, although less environmentally friendly chemicals will be also considered. Moreover, the scope of the review is limited to those most representative lignin model compounds and to those reaction products that are typically targeted in lignin valorization.

热化学木质素转化过程可以描述为复杂的反应网络,不仅涉及解聚和再聚合反应,还涉及解聚的单、二、低聚化合物的化学转化。它们通常会产生由气态、液态(即单、双、低聚产物)和固相组成的产品混合物。因此,研究人员已经开发出一种共同的策略,通过用更简单但仍具有代表性的木质素模型化合物代替木质素来简化这一问题。这一策略通常应用于阐明反应机制和探索新的木质素转化途径。本文综述了利用多相催化剂转化木质素模型化合物的主要热化学过程的最新进展。本文综述了木质素最具代表性的转化方法,即还原法、氧化法、热解法和水解法。另外还包括了关于热解油模型化合物重整的分章。将特别注意那些使用“绿色”反应物(即还原过程中的H2或可再生氢供体分子或氧化过程中的空气/O2)和溶剂的研究论文,尽管也将考虑不太环保的化学品。此外,回顾的范围仅限于那些最具代表性的木质素模型化合物和那些通常针对木质素增值的反应产物。
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引用次数: 13
State-of-the-Art and Prospects of Biomolecules: Incorporation in Functional Metal–Organic Frameworks 生物分子的研究现状与展望:在功能金属有机框架中的应用
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-10-30 DOI: 10.1007/s41061-019-0258-z
Wenjie Duan, Zhengfeng Zhao, Hongde An, Zhenjie Zhang, Peng Cheng, Yao Chen, He Huang

Given the unique properties of metal–organic frameworks (MOFs) including adjustable porosity, high surface area, and easy modification, they have attracted great attention as excellent solid supports for the incorporation of biomolecules. The formed biomolecules–MOFs composites show promising prospects in various fields such as biocatalysis, drug delivery, and biosensing. This review focuses on the state-of-the-art of biomolecules-incorporation using MOFs. Moreover, the relationship between properties of MOFs and biomolecules-incorporation is also discussed and highlighted. We hope this work will inspire the innovation in this emerging field for highly efficient synthesis of biomolecules–MOFs composites with various properties and advanced applications.

由于金属有机骨架具有孔隙度可调、比表面积大、易修饰等独特的性能,作为生物分子掺入的良好固体载体受到了广泛的关注。形成的生物分子- mofs复合材料在生物催化、药物传递和生物传感等领域具有广阔的应用前景。本文综述了利用mof结合生物分子的研究进展。此外,还讨论并强调了MOFs的性质与生物分子掺入之间的关系。我们希望这项工作能够激发这一新兴领域的创新,以高效合成具有各种性能和先进应用的生物分子- mofs复合材料。
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引用次数: 20
Current Status of Microporous Metal–Organic Frameworks for Hydrocarbon Separations 用于烃类分离的微孔金属-有机骨架研究现状
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-10-29 DOI: 10.1007/s41061-019-0257-0
Jiyan Pei, Kai Shao, Ling Zhang, Hui-Min Wen, Bin Li, Guodong Qian

Separation of hydrocarbon mixtures into single components is a very important industrial process because all represent very important energy resources/raw chemicals in the petrochemical industry. The well-established industrial separation technology highly relies on the energy-intensive cryogenic distillation processes. The discovery of new materials capable of separating hydrocarbon mixtures by adsorbent-based separation technologies has the potential to provide more energy-efficient industrial processes with remarkable energy savings. Porous metal–organic frameworks (MOFs), also known as porous coordination polymers, represent a new class of porous materials that offer tremendous promise for hydrocarbon separations because of their easy tunability, designability, and functionality. A number of MOFs have been designed and synthesized to show excellent separation performance on various hydrocarbon separations. Here, we summarize and highlight some recent significant advances in the development of microporous MOFs for hydrocarbon separation applications.

将烃类混合物分离成单一组分是一个非常重要的工业过程,因为它们在石化工业中都是非常重要的能源/原料化学品。成熟的工业分离技术高度依赖于高能耗的低温精馏过程。能够通过基于吸附剂的分离技术分离碳氢化合物混合物的新材料的发现,有可能提供更节能的工业过程,并显著节省能源。多孔金属有机框架(mof),也被称为多孔配位聚合物,代表了一类新的多孔材料,由于其易于调节性、可设计性和功能性,为碳氢化合物分离提供了巨大的希望。设计和合成了许多mof,在各种烃类分离中表现出优异的分离性能。在此,我们总结并重点介绍了用于烃类分离的微孔mof的最新进展。
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引用次数: 29
Synthesis and Applications of Porous Organosulfonate-Based Metal–Organic Frameworks 多孔有机磺酸盐基金属-有机骨架的合成与应用
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-10-26 DOI: 10.1007/s41061-019-0259-y
Guiyang Zhang, Honghan Fei
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引用次数: 12
Cationic Organic Catalysts or Ligands in Concert with Metal Catalysts 阳离子有机催化剂或配体与金属催化剂的协同作用
IF 8.6 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2019-10-25 DOI: 10.1007/s41061-019-0256-1
Kohsuke Ohmatsu, Takashi Ooi

Cooperative dual catalysis and bifunctional catalysis have emerged as reliable strategies for the development of hitherto difficult asymmetric transformations because they could deliver new reactivity and selectivity, and allow for the employment of substrates not amenable to reaction systems relying on a single, monofunctional catalysts. Furthermore, these modes of catalysis often improve yields and stereoselectivities via the precise recognition and simultaneous activation of nucleophiles and electrophiles. Efforts towards utilizing chiral cationic organic catalysts for asymmetric cooperative catalysis with metal complexes have provided a unique platform to address the challenging issues associated with reaction development. Chiral onium ions, such as tetraalkylammonium, guanidinium, and azolium ions, are employed mainly to control the reactivity and stereochemistry of anionic intermediates through electrostatic and hydrogen-bonding interactions. Metal complexes complement the synergy of the catalysis by activating the substrates via the formation of electrophilic π-allyl complexes, Lewis acid–base adducts, nucleophilic ate complexes, etc. The electrostatic interactions between cations and anions also offer a means to construct complex molecular assemblies, and, thus, onium ions are useful not only for controlling pairing with anionic species, but also for the design of supramolecular catalysts. The combination of onium ions and metal complexes leads to the introduction of novel concepts and powerful strategies for the development of catalysts and chemical transformations.

协同双催化和双功能催化已经成为发展迄今为止困难的不对称转化的可靠策略,因为它们可以提供新的反应活性和选择性,并允许使用不适合依赖单一,单功能催化剂的反应系统的底物。此外,这些催化模式通常通过精确识别和亲核试剂和亲电试剂的同时激活来提高产率和立体选择性。利用手性阳离子有机催化剂与金属配合物进行不对称协同催化的努力为解决与反应发展相关的挑战性问题提供了一个独特的平台。手性离子,如四烷基铵、胍和唑离子,主要通过静电和氢键相互作用来控制阴离子中间体的反应性和立体化学。金属配合物通过形成亲电性π-烯丙基配合物、路易斯酸碱加合物、亲核酸盐配合物等活化底物来补充催化的协同作用。阳离子和阴离子之间的静电相互作用也为构建复杂的分子组装提供了一种手段,因此,铵离子不仅可用于控制与阴离子的配对,而且可用于超分子催化剂的设计。离子和金属配合物的结合为催化剂和化学转化的发展带来了新的概念和强有力的策略。
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引用次数: 15
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Topics in Current Chemistry
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