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Correction to Depolymerization within a Circular Plastics System. 纠正循环塑料系统中的解聚现象。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acs.chemrev.4c00473
Robbie A Clark, Michael P Shaver
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引用次数: 0
Emerging Atomistic Modeling Methods for Heterogeneous Electrocatalysis. 用于异相电催化的新兴原子模型方法。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acs.chemrev.3c00735
Zachary Levell, Jiabo Le, Saerom Yu, Ruoyu Wang, Sudheesh Ethirajan, Rachita Rana, Ambarish Kulkarni, Joaquin Resasco, Deyu Lu, Jun Cheng, Yuanyue Liu

Heterogeneous electrocatalysis lies at the center of various technologies that could help enable a sustainable future. However, its complexity makes it challenging to accurately and efficiently model at an atomic level. Here, we review emerging atomistic methods to simulate the electrocatalytic interface with special attention devoted to the components/effects that have been challenging to model, such as solvation, electrolyte ions, electrode potential, reaction kinetics, and pH. Additionally, we review relevant computational spectroscopy methods. Then, we showcase several examples of applying these methods to understand and design catalysts relevant to green hydrogen. We also offer experimental views on how to bridge the gap between theory and experiments. Finally, we provide some perspectives on opportunities to advance the field.

异相电催化是有助于实现可持续未来的各种技术的核心。然而,由于其复杂性,要在原子层面准确有效地建模具有挑战性。在此,我们回顾了模拟电催化界面的新兴原子方法,并特别关注具有建模挑战性的成分/效应,如溶解、电解质离子、电极电位、反应动力学和 pH 值。此外,我们还回顾了相关的计算光谱学方法。然后,我们展示了应用这些方法了解和设计绿色氢气相关催化剂的几个实例。我们还就如何弥合理论与实验之间的差距提出了实验观点。最后,我们对推动该领域发展的机遇提出了一些看法。
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引用次数: 0
Introduction: Operando and In Situ Studies in Catalysis and Electrocatalysis 简介:催化和电催化的操作和原位研究。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1021/acs.chemrev.4c00184
Beatriz Roldán Cuenya*,  and , Miguel A. Bañares*, 
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引用次数: 0
How to Propose a Great Chemical Reviews Article 如何撰写精彩的化学品评论文章。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1021/acs.chemrev.4c00414
David S. Ginger*, 
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引用次数: 0
Single Atom Catalysts Based on Earth-Abundant Metals for Energy-Related Applications. 基于地球富集金属的单原子催化剂在能源相关领域的应用。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1021/acs.chemrev.4c00155
Štĕpán Kment, Aristides Bakandritsos, Iosif Tantis, Hana Kmentová, Yunpeng Zuo, Olivier Henrotte, Alberto Naldoni, Michal Otyepka, Rajender S Varma, Radek Zbořil

Anthropogenic activities related to population growth, economic development, technological advances, and changes in lifestyle and climate patterns result in a continuous increase in energy consumption. At the same time, the rare metal elements frequently deployed as catalysts in energy related processes are not only costly in view of their low natural abundance, but their availability is often further limited due to geopolitical reasons. Thus, electrochemical energy storage and conversion with earth-abundant metals, mainly in the form of single-atom catalysts (SACs), are highly relevant and timely technologies. In this review the application of earth-abundant SACs in electrochemical energy storage and electrocatalytic conversion of chemicals to fuels or products with high energy content is discussed. The oxygen reduction reaction is also appraised, which is primarily harnessed in fuel cell technologies and metal-air batteries. The coordination, active sites, and mechanistic aspects of transition metal SACs are analyzed for two-electron and four-electron reaction pathways. Further, the electrochemical water splitting with SACs toward green hydrogen fuel is discussed in terms of not only hydrogen evolution reaction but also oxygen evolution reaction. Similarly, the production of ammonia as a clean fuel via electrocatalytic nitrogen reduction reaction is portrayed, highlighting the potential of earth-abundant single metal species.

与人口增长、经济发展、技术进步以及生活方式和气候模式变化相关的人类活动导致能源消耗持续增长。与此同时,在能源相关过程中经常用作催化剂的稀有金属元素不仅因其天然储量低而成本高昂,而且由于地缘政治原因,其可用性往往受到进一步限制。因此,以单原子催化剂(SACs)为主要形式的富土金属电化学能量存储和转换技术是高度相关且适时的技术。在本综述中,讨论了富集地球的单原子催化剂在电化学储能和电催化将化学品转化为燃料或高能量产品中的应用。此外,还评估了氧还原反应,该反应主要用于燃料电池技术和金属空气电池。针对双电子和四电子反应途径,分析了过渡金属 SAC 的配位、活性位点和机理。此外,还从氢进化反应和氧进化反应两个方面讨论了利用 SACs 进行电化学水分离以获得绿色氢燃料的问题。同样,还描绘了通过电催化氮还原反应生产氨作为清洁燃料的过程,凸显了富土单金属物种的潜力。
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引用次数: 0
Light from Afield: Fast, High-Resolution, and Layer-Free Deep Vat 3D Printing. 来自远方的光:快速、高分辨率和无层深槽三维打印。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1021/acs.chemrev.4c00134
Parth Chansoria, Riccardo Rizzo, Dominic Rütsche, Hao Liu, Paul Delrot, Marcy Zenobi-Wong

Harnessing light for cross-linking of photoresponsive materials has revolutionized the field of 3D printing. A wide variety of techniques leveraging broad-spectrum light shaping have been introduced as a way to achieve fast and high-resolution printing, with applications ranging from simple prototypes to biomimetic engineered tissues for regenerative medicine. Conventional light-based printing techniques use cross-linking of material in a layer-by-layer fashion to produce complex parts. Only recently, new techniques have emerged which deploy multidirection, tomographic, light-sheet or filamented light-based image projections deep into the volume of resin-filled vat for photoinitiation and cross-linking. These Deep Vat printing (DVP) approaches alleviate the need for layer-wise printing and enable unprecedented fabrication speeds (within a few seconds) with high resolution (>10 μm). Here, we elucidate the physics and chemistry of these processes, their commonalities and differences, as well as their emerging applications in biomedical and non-biomedical fields. Importantly, we highlight their limitations, and future scope of research that will improve the scalability and applicability of these DVP techniques in a wide variety of engineering and regenerative medicine applications.

利用光来交联光致发光材料已经彻底改变了三维打印领域。各种利用宽光谱光成型的技术已经问世,作为实现快速和高分辨率打印的一种方法,其应用范围从简单的原型到再生医学的生物仿生工程组织。传统的光基打印技术采用逐层交联材料的方式生产复杂部件。直到最近,才出现了一些新技术,这些技术采用多向、层析、光片或丝状光基图像投射到树脂填充槽的深处,进行光引发和交联。这些深槽打印(DVP)方法减轻了分层打印的需要,实现了前所未有的制造速度(几秒钟内)和高分辨率(>10 μm)。在此,我们将阐明这些工艺的物理和化学原理、共性和差异,以及它们在生物医学和非生物医学领域的新兴应用。重要的是,我们强调了它们的局限性以及未来的研究范围,这将提高这些 DVP 技术在各种工程和再生医学应用中的可扩展性和适用性。
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引用次数: 0
Noncanonical Amino Acids in Biocatalysis. 生物催化中的非典型氨基酸
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-03 DOI: 10.1021/acs.chemrev.4c00120
Zachary Birch-Price, Florence J Hardy, Thomas M Lister, Anna R Kohn, Anthony P Green

In recent years, powerful genetic code reprogramming methods have emerged that allow new functional components to be embedded into proteins as noncanonical amino acid (ncAA) side chains. In this review, we will illustrate how the availability of an expanded set of amino acid building blocks has opened a wealth of new opportunities in enzymology and biocatalysis research. Genetic code reprogramming has provided new insights into enzyme mechanisms by allowing introduction of new spectroscopic probes and the targeted replacement of individual atoms or functional groups. NcAAs have also been used to develop engineered biocatalysts with improved activity, selectivity, and stability, as well as enzymes with artificial regulatory elements that are responsive to external stimuli. Perhaps most ambitiously, the combination of genetic code reprogramming and laboratory evolution has given rise to new classes of enzymes that use ncAAs as key catalytic elements. With the framework for developing ncAA-containing biocatalysts now firmly established, we are optimistic that genetic code reprogramming will become a progressively more powerful tool in the armory of enzyme designers and engineers in the coming years.

近年来,出现了强大的遗传密码重编程方法,可将新的功能成分作为非典型氨基酸(ncAA)侧链嵌入蛋白质中。在这篇综述中,我们将说明氨基酸构件集的扩大如何为酶学和生物催化研究带来了大量新机遇。通过引入新的光谱探针和有针对性地替换单个原子或功能基团,基因代码重编程为酶机制的研究提供了新的视角。NcAAs 还被用于开发具有更高活性、选择性和稳定性的工程生物催化剂,以及具有人工调控元件、能对外部刺激做出反应的酶。也许最雄心勃勃的是,遗传密码重编程和实验室进化相结合,产生了使用 ncAAs 作为关键催化元件的新型酶。随着含 ncAA 生物催化剂开发框架的牢固确立,我们乐观地认为,在未来几年里,遗传密码重编程将逐渐成为酶设计师和工程师的有力工具。
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引用次数: 0
Evolution of Pyrrolysyl-tRNA Synthetase: From Methanogenesis to Genetic Code Expansion 吡咯糖基-tRNA 合成酶的进化:从甲烷生成到遗传密码扩展
IF 62.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-02 DOI: 10.1021/acs.chemrev.4c00031
Nikolaj G. Koch, Nediljko Budisa
Over 20 years ago, the pyrrolysine encoding translation system was discovered in specific archaea. Our Review provides an overview of how the once obscure pyrrolysyl-tRNA synthetase (PylRS) tRNA pair, originally responsible for accurately translating enzymes crucial in methanogenic metabolic pathways, laid the foundation for the burgeoning field of genetic code expansion. Our primary focus is the discussion of how to successfully engineer the PylRS to recognize new substrates and exhibit higher in vivo activity. We have compiled a comprehensive list of ncAAs incorporable with the PylRS system. Additionally, we also summarize recent successful applications of the PylRS system in creating innovative therapeutic solutions, such as new antibody–drug conjugates, advancements in vaccine modalities, and the potential production of new antimicrobials.
20 多年前,人们在特定的古细菌中发现了吡咯赖氨酸编码翻译系统。我们的综述概述了曾经默默无闻的吡咯赖氨酸-tRNA 合成酶(PylRS)tRNA 对如何为新兴的遗传密码扩展领域奠定了基础。我们的主要重点是讨论如何成功改造 PylRS,使其识别新底物并表现出更高的体内活性。我们汇编了一份可与 PylRS 系统结合的 ncAAs 综合清单。此外,我们还总结了 PylRS 系统最近在创造创新治疗方案方面的成功应用,如新型抗体-药物共轭物、疫苗模式的进步以及新型抗菌药的潜在生产。
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引用次数: 0
P-Stereogenic Phosphorus Ligands in Asymmetric Catalysis. 不对称催化中的 P-Stereogenic 磷配体。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-02 DOI: 10.1021/acs.chemrev.3c00875
Tsuneo Imamoto

Chiral phosphorus ligands play a crucial role in asymmetric catalysis for the efficient synthesis of useful optically active compounds. They are largely categorized into two classes: backbone chirality ligands and P-stereogenic phosphorus ligands. Most of the reported ligands belong to the former class. Privileged ones such as BINAP and DuPhos are frequently employed in a wide range of catalytic asymmetric transformations. In contrast, the latter class of P-stereogenic phosphorus ligands has remained a small family for many years mainly because of their synthetic difficulty. The late 1990s saw the emergence of novel P-stereogenic phosphorus ligands with their superior enantioinduction ability in Rh-catalyzed asymmetric hydrogenation reactions. Since then, numerous P-stereogenic phosphorus ligands have been synthesized and used in catalytic asymmetric reactions. This Review summarizes P-stereogenic phosphorus ligands reported thus far, including their stereochemical and electronic properties that afford high to excellent enantioselectivities. Examples of reactions that use this class of ligands are described together with their applications in the construction of key intermediates for the synthesis of optically active natural products and therapeutic agents. The literature covered dates back to 1968 up until December 2023, centering on studies published in the late 1990s and later years.

手性磷配体在不对称催化高效合成有用的光学活性化合物方面发挥着至关重要的作用。它们主要分为两类:骨架手性配体和 P-stereogenic 磷配体。大多数已报道的配体都属于前一类。BINAP 和 DuPhos 等优势配体经常用于各种催化不对称转化。相比之下,后一类 P-stereogenic 磷配体多年来一直是一个小家族,主要原因是其合成困难。20 世纪 90 年代末,新型 P-stereogenic 磷配体出现,它们在 Rh 催化的不对称氢化反应中具有卓越的对映诱导能力。从那时起,许多 P-stereogenic 磷配体被合成并用于催化不对称反应。本综述总结了迄今为止报道的 P-stereogenic 磷配体,包括它们的立体化学和电子特性,这些配体可提供高至卓越的对映选择性。文中还介绍了使用这类配体进行反应的实例,以及它们在合成具有光学活性的天然产物和治疗药物的关键中间体中的应用。所涉及的文献可追溯到 1968 年,直至 2023 年 12 月,主要集中在 20 世纪 90 年代后期及以后发表的研究。
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引用次数: 0
Proline Analogues 脯氨酸类似物。
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1021/acs.chemrev.4c00007
Vladimir Kubyshkin,  and , Marina Rubini, 

Within the canonical repertoire of the amino acid involved in protein biogenesis, proline plays a unique role as an amino acid presenting a modified backbone rather than a side-chain. Chemical structures that mimic proline but introduce changes into its specific molecular features are defined as proline analogues. This review article summarizes the existing chemical, physicochemical, and biochemical knowledge about this peculiar family of structures. We group proline analogues from the following compounds: substituted prolines, unsaturated and fused structures, ring size homologues, heterocyclic, e.g., pseudoproline, and bridged proline-resembling structures. We overview (1) the occurrence of proline analogues in nature and their chemical synthesis, (2) physicochemical properties including ring conformation and cis/trans amide isomerization, (3) use in commercial drugs such as nirmatrelvir recently approved against COVID-19, (4) peptide and protein synthesis involving proline analogues, (5) specific opportunities created in peptide engineering, and (6) cases of protein engineering with the analogues. The review aims to provide a summary to anyone interested in using proline analogues in systems ranging from specific biochemical setups to complex biological systems.

在参与蛋白质生物生成的氨基酸的典型种类中,脯氨酸作为一种氨基酸扮演着独特的角色,它呈现的是一种改良的骨架而不是侧链。模仿脯氨酸但改变其特定分子特征的化学结构被定义为脯氨酸类似物。这篇综述文章总结了有关这一特殊结构家族的现有化学、物理化学和生物化学知识。我们将脯氨酸类似物分为以下几类:取代脯氨酸、不饱和和融合结构、环尺寸同源物、杂环(如假脯氨酸)和桥接脯氨酸相似结构。我们概述了(1)脯氨酸类似物在自然界中的出现及其化学合成,(2)理化性质,包括环构象和顺/反酰胺异构化,(3)在商业药物中的应用,如最近获准用于治疗 COVID-19 的 nirmatrelvir,(4)涉及脯氨酸类似物的肽和蛋白质合成,(5)在肽工程中创造的特定机会,以及(6)使用类似物进行蛋白质工程的案例。本综述旨在为任何有兴趣在从特定生化装置到复杂生物系统中使用脯氨酸类似物的人提供一个总结。
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引用次数: 0
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