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Opposed Aromatic Surfaces Behave as Independent Binding Sites for Carbohydrate Stacking: Analysis of Sandwich-like CH/π/CH Complexes 相对的芳香族表面是碳水化合物堆叠的独立结合点:三明治状 CH/π/CH 复合物分析
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-14 DOI: 10.1021/jacsau.4c0079510.1021/jacsau.4c00795
Laura Díaz-Casado, Enrique Mann, Ester Jiménez-Moreno, Alejandro Villacampa, Laura Montalvillo-Jiménez, Claudia Sánchez-García, Francisco Corzana, Jesús Jiménez-Barbero, Ana María Gómez, Andrés G. Santana and Juan Luis Asensio*, 

CH/π bonds are versatile elements for the construction of complex molecular architectures, thus playing key roles in many biomolecular recognition processes. Although seldom acknowledged, aromatic units are inherently bivalent and can participate in CH/π bonds through either face simultaneously, leading to the formation of ternary stacking complexes. This sandwich-like arrangement is by far the most common in natural complexes and could potentially lead to negative cooperativity due to unfavorable polarization or electrostatic effects, especially when polarized CH fragments are involved. To evaluate the energetics of such interaction modes, we selected a biologically relevant model, carbohydrate/aromatic stacking, and conducted an experimental analysis comparing binary CH/π interactions to ternary CH/π/CH stacking. Our approach utilized a dynamic combinatorial strategy, which is well-suited to reveal minor stability differences among aromatic complexes. Our results showed that carbohydrate/aromatic stacking is relatively insensitive to molecular recognition events occurring on the opposite side of the aromatic platform, whether exposed to water or involved in additional CH/π contacts, with free energy fluctuations lower than 10%. Based on these data, for all practical purposes, the two opposing aromatic surfaces can be considered independent, noninteracting binding sites, making aromatic platforms optimal connecting elements for supramolecular cross-linking.

CH/π 键是构建复杂分子结构的多功能元素,因此在许多生物分子识别过程中发挥着关键作用。尽管人们很少认识到,芳香族单元本质上是二价的,可以同时通过任一面参与 CH/π 键,从而形成三元堆积复合物。这种类似三明治的排列方式是迄今为止天然复合物中最常见的,由于不利的极化或静电效应,特别是涉及极化的 CH 片段时,有可能导致负合作性。为了评估这种相互作用模式的能效,我们选择了一个与生物相关的模型--碳水化合物/芳香族堆积,并进行了实验分析,将二元 CH/π 相互作用与三元 CH/π/CH 堆积进行了比较。我们的方法采用了动态组合策略,这种策略非常适合揭示芳香族复合物之间的微小稳定性差异。我们的研究结果表明,碳水化合物/芳香族堆叠对发生在芳香族平台另一侧的分子识别事件相对不敏感,无论是暴露在水中还是参与额外的 CH/π 接触,其自由能波动都低于 10%。基于这些数据,就所有实际目的而言,两个相对的芳香表面可被视为独立的、非相互作用的结合位点,从而使芳香平台成为超分子交联的最佳连接元素。
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引用次数: 0
Divergent Synthesis of Chiroptical Molecular Switches Based on 1,2-Diaxial Atropisomers 基于 1,2-二轴异构体的光电分子开关的异构合成
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-14 DOI: 10.1021/jacsau.4c0077710.1021/jacsau.4c00777
Tian-Jiao Han, Qiu-Le Yang, Jiaen Hu, Min-Can Wang and Guang-Jian Mei*, 

The development of chiroptical molecular switches for chiral sensing, data communication, optical displays, chiral logic gates, and asymmetric catalysis is currently a vibrant frontier of science and technology. Herein, we report a practical artificial dynamic system based on a 1,2-diaxial atropisomer. Organocatalytic parallel kinetic resolution allows the divergent synthesis of two sets of stereoisomers with vicinal C–C and N–N axes from the same racemic single-axis substrates. By simply varying the configuration of the single catalyst, all four stereoisomers are accessible. The successive conduction of covalent unlocking/locking and thermal-isomerization processes enables sequential switching between all four atropisomeric states with electronic circular dichroism signal reversal, providing an example of multistate chiroptical molecular switches.

开发用于手性传感、数据通信、光学显示、手性逻辑门和不对称催化的气光分子开关是当前充满活力的科技前沿。在此,我们报告了一种基于 1,2-二轴异构体的实用人工动态系统。通过有机催化平行动力学解析,可以从相同的外消旋单轴底物中合成两组具有邻接 C-C 轴和 N-N 轴的立体异构体。只需改变单一催化剂的构型,就能获得所有四种立体异构体。通过共价解锁/锁定和热异构化过程的连续进行,可以在所有四种异构体状态之间进行顺序切换,同时实现电子圆二色性信号反转,从而提供了一个多态气旋分子开关的实例。
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引用次数: 0
Selective [3 + 2] C–H/C–H Alkyne Annulation via Dual (Distal) C(β, δ)–H Bond Activation Relay: A Novel Therapeutic Quinazolone-Tethered Benzofulvenes for Oral Cancer 通过双(远端)C(β, δ)-H键活化中继实现选择性[3 + 2] C-H/C-H炔烃环化:治疗口腔癌的新型喹唑啉酮系苯并呋喃类药物
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-11 DOI: 10.1021/jacsau.4c0080210.1021/jacsau.4c00802
Dinesh Parshuram Satpute, Garvita Narang, Harshal Rohit, Jagdish Manjhi, Divita Kumar, Sangita Dattatray Shinde, Shyam Kumar Lokhande, Priyanka Patel Vatsa, Vinal Upadhyay, Shivkanya Madhavrao Bhujbal, Amit Mandoli* and Dinesh Kumar*, 

In contrast to proximal C–H bond activations, distal C–H bond activation is fundamentally more challenging and requires distinctly specialized directing partners or techniques. In this context, we report an unprecedented dual (distal) β-C(benzylic)–H and δ-C(aryl)–H bond activation relay protocol for the chemo-, regio-, and stereoselective construction of heterocycle-tethered benzofulvenes via [3 + 2] CH/CH-alkyne annulation under palladium catalysis. The protocol overrides the more favorable [4 + 2] CH/NH annulation and does not follow the vinylic C–H bond activation pathway. Mechanistic studies provide insight into the favored cyclopalladation of key intermediates (resulting from β-C(benzylic)–H bond cleavage) through relay δ-C(aryl)–H cleavage (vs N–H cleavage) prior to reductive elimination, which is the key to desired annulation. The synthesized new chemical entities (NCEs) constitute a novel scaffold with favorable anticancer activity against oral squamous cell carcinoma (OSCC). Detailed biomolecular studies, including RNA-sequencing and analysis, indicate that these compounds (4e and 4w) arrest the cell cycle at the S-phase and target multiple cancer hallmarks, such as the activation of apoptotic pathways and impairment of mitochondrial activity simultaneously, suggesting their chemotherapeutic potential for oral cancer by addressing the complexity and adaptability of cancer cells in chorus.

与近端 C-H 键活化相比,远端 C-H 键活化从根本上说更具挑战性,需要独特的专业指导伙伴或技术。在此背景下,我们报告了一种前所未有的双(远端)β-C(苄基)-H 和 δ-C(芳基)-H 键活化中继方案,用于在钯催化下通过 [3 + 2] CH/CH-alkyne 环化反应,化合、区域和立体选择性地构建杂环系苯并呋喃。该方案取代了更有利的 [4 + 2] CH/NH 环化,并且不遵循乙烯基 C-H 键活化途径。机理研究深入揭示了关键中间体(由 β-C(苄基)-H 键裂解产生)在还原消除之前通过中继 δ-C(芳基)-H 裂解(相对于 N-H 裂解)进行环钯化的有利条件,而还原消除是实现理想环化的关键。合成的新化学实体(NCE)构成了一种新型支架,对口腔鳞状细胞癌(OSCC)具有良好的抗癌活性。详细的生物分子研究(包括 RNA 序列测定和分析)表明,这些化合物(4e 和 4w)能使细胞周期停滞在 S 期,并同时针对多种癌症标志,如激活凋亡通路和损害线粒体活性,这表明它们具有针对口腔癌的化疗潜力,能解决癌细胞在合唱中的复杂性和适应性问题。
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引用次数: 0
Catalytic Hydrodeoxygenation of Mixed Plastic Wastes into Sustainable Naphthenes 催化加氢脱氧将混合塑料废料转化为可持续环烷烃
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-11 DOI: 10.1021/jacsau.4c0070110.1021/jacsau.4c00701
Jieyi Liu, Nan Wang, Sibao Liu* and Guozhu Liu*, 

The chemical upcycling of plastic wastes by converting them into valuable fuels and chemicals represents a sustainable approach as opposed to landfilling and incineration. However, it encounters challenges in dealing with mixed plastic wastes due to their complex composition and sorting/cleaning costs. Here, we present a one-pot hydrodeoxygenation (HDO) method for converting mixed plastic wastes containing poly(ethylene terephthalate) (PET), polycarbonate (PC), and poly(phenylene oxide) (PPO) into sustainable naphthenes under mild reaction conditions. To facilitate this process, we developed a cost-effective, contaminant-tolerant, and reusable Ni/HZSM-5 bifunctional catalyst through an ethylene glycol-assisted impregnation method. The metallic Ni site plays a pivotal role in catalyzing C–O and C–C cleavages as well as hydrogenation reactions, while the acidic site of HZSM-5 facilitates dehydration and isomerization reactions. The collaboration between metal and acid dual sites on Ni/HZSM-5 enabled efficient HDO of a wide range of substrates, including bottles, textile fibers, pellets, sheets, CDs/DVDs, and plastics without cleaning or pigments removal and even their various mixtures, into naphthenes with a high yield up to 99% at 250 °C and 4 MPa H2 within 4–6 h. Furthermore, the metal-acid balance of the Ni/HZSM-5 catalyst is crucial for determining both HDO activity and product distribution. This proposed one-pot HDO process utilizing earth-abundant metal catalysts provides a promising avenue toward practical valorization of mixed plastic wastes.

通过将塑料废物转化为有价值的燃料和化学品,对其进行化学升级再循环,是一种有别于填埋和焚烧的可持续方法。然而,由于混合塑料废物的复杂成分和分类/清洁成本,这种方法在处理混合塑料废物时遇到了挑战。在此,我们介绍了一种单锅加氢脱氧(HDO)方法,可在温和的反应条件下将含有聚对苯二甲酸乙二酯(PET)、聚碳酸酯(PC)和聚环氧苯丙酯(PPO)的混合塑料废物转化为可持续环烷。为了促进这一过程,我们通过乙二醇辅助浸渍法,开发出了一种具有成本效益、耐污染且可重复使用的 Ni/HZSM-5 双功能催化剂。金属镍位点在催化 C-O 和 C-C 裂解以及氢化反应中发挥了关键作用,而 HZSM-5 的酸性位点则促进了脱水和异构化反应。通过 Ni/HZSM-5 上金属和酸性双位点的协同作用,可以在 250 °C 和 4 MPa H2 条件下,在 4-6 小时内将多种基质(包括瓶子、纺织纤维、颗粒、片材、CD/DVD 和未清洗或未去除颜料的塑料,甚至它们的各种混合物)高效地 HDO 成环烷,收率高达 99%。这种利用富土金属催化剂的一锅式 HDO 工艺为混合塑料废物的实用化提供了一条前景广阔的途径。
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引用次数: 0
Metal-Free Aziridination of Unactivated Olefins via Transient N-Pyridinium Iminoiodinanes 通过瞬时 N-吡啶鎓亚氨基碘烷对未活化烯烃进行无金属叠氮反应
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-10 DOI: 10.1021/jacsau.4c0055610.1021/jacsau.4c00556
Hao Tan, Phong Thai, Uddalak Sengupta, Isaac R. Deavenport, Cali M. Kucifer and David C. Powers*, 

We describe a metal-free aziridination of unactivated olefins to generate N-pyridinium aziridines. Subsequent cross-coupling affords N-aryl aziridines, and reductive depyridylation affords N–H aziridines. Kinetics experiments, based on a variable time normalization analysis (VTNA), indicate that aziridination proceeds via a highly electrophilic N-pyridinium iminoiodinane intermediate. These studies expand build-and-couple aziridine synthesis to unactivated olefins and introduce charge-enhanced electrophilicity into the chemistry of iminoiodinanes.

我们描述了一种对未活化烯烃进行无金属氮丙啶化反应生成 N-吡啶氮丙啶的方法。随后的交叉偶联反应生成 N-芳基氮丙啶,还原脱吡啶反应生成 N-H 氮丙啶。基于可变时间归一化分析(VTNA)的动力学实验表明,氮丙啶化作用是通过一个高亲电性的 N-吡啶亚氨基碘烷中间体进行的。这些研究将内置偶联氮丙啶合成扩展到未活化的烯烃,并将电荷增强亲电性引入亚氨基碘烷的化学反应中。
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引用次数: 0
Effect of Thermal Stress on Morphology in High-Performance Organic Photovoltaic Blends 热应力对高性能有机光伏混合物形态的影响
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-10 DOI: 10.1021/jacsau.4c0063110.1021/jacsau.4c00631
Haoyu Zhao, Nathaniel Prine, Soumya Kundu, Guorong Ma and Xiaodan Gu*, 

Thermal stress is a critical factor causing long-term instability in bulk heterojunction (BHJ) layers of organic photovoltaic (OPV) devices. This study provides direct insights into the thermal properties of Y6, PM6, and their binary blends by employing fast differential scanning calorimetry (flash DSC) to analyze their chain dynamics. The glass transition temperatures (Tg) of Y6 and PM6 were measured, with Y6 exhibiting a Tg of 175.2 °C and PM6 showing two Tgs at 39.7 and 107.6 °C. Our findings indicate that average OPVs’ operational temperatures are lower than the blend’s primary Tg of 138.2 °C. Thus, the mobility of PM6 and Y6 is not the critical factor that results in drastic drifts in the device morphology. Instead, we discovered that the crystallization of small molecules Y6 in the BHJ film at elevated operation temperatures significantly contributes to the morphological instability of the BHJ layer, based on a flash DSC isotherm crystallization study. The crystallization of the acceptor leads to severe phase separation between donors and acceptors and results in device failure. The acceptor Y6’s crystallization rate also increased when blended with donor PM6, compared to that of pure Y6 molecules. Furthermore, AFM–IR analysis of the morphology of the BHJ layer after high thermal stress of 200 °C revealed an apparent demixing of donor PM6 and acceptor Y6, revealing Y6 globules about 200 nm in diameter, with PM6 domains surrounding the Y6 regions. This crystallization-induced morphology change was later confirmed to correlate well with the device performance drop. This study offers valuable insights into the origin of BHJ layer instability in OPV devices containing nonfullerene small molecule acceptors and polymer donors. Additionally, it emphasizes the importance of addressing thermal stress to enhance the performance and durability of such devices and informs strategies for developing more stable organic solar cells.

热应力是导致有机光伏(OPV)器件的体异质结(BHJ)层长期不稳定的关键因素。本研究采用快速差示扫描量热法(flash DSC)分析 Y6、PM6 及其二元共混物的链动力学,从而直接了解它们的热特性。测量了 Y6 和 PM6 的玻璃化转变温度 (Tg),Y6 的 Tg 为 175.2 ℃,PM6 的两个 Tg 分别为 39.7 ℃ 和 107.6 ℃。我们的研究结果表明,OPV 的平均工作温度低于混合物的主要 Tg(138.2 °C)。因此,PM6 和 Y6 的迁移率并不是导致器件形态急剧变化的关键因素。相反,根据闪速 DSC 等温线结晶研究,我们发现小分子 Y6 在 BHJ 膜中的结晶在较高的工作温度下极大地加剧了 BHJ 层的形态不稳定性。受体的结晶会导致供体和受体之间出现严重的相分离,从而导致器件失效。与纯 Y6 分子相比,受体 Y6 与供体 PM6 混合后的结晶速率也有所增加。此外,在 200 °C 的高热应力下对 BHJ 层的形貌进行原子力显微镜-红外分析后发现,供体 PM6 和受体 Y6 发生了明显的脱混,显示出直径约 200 nm 的 Y6 球状,Y6 区域周围是 PM6 域。这种结晶引起的形态变化后来被证实与器件性能下降密切相关。这项研究为了解含有非富勒烯小分子受体和聚合物供体的 OPV 器件中 BHJ 层不稳定性的起源提供了宝贵的见解。此外,它还强调了解决热应力问题以提高此类器件的性能和耐用性的重要性,并为开发更稳定的有机太阳能电池提供了参考策略。
{"title":"Effect of Thermal Stress on Morphology in High-Performance Organic Photovoltaic Blends","authors":"Haoyu Zhao,&nbsp;Nathaniel Prine,&nbsp;Soumya Kundu,&nbsp;Guorong Ma and Xiaodan Gu*,&nbsp;","doi":"10.1021/jacsau.4c0063110.1021/jacsau.4c00631","DOIUrl":"https://doi.org/10.1021/jacsau.4c00631https://doi.org/10.1021/jacsau.4c00631","url":null,"abstract":"<p >Thermal stress is a critical factor causing long-term instability in bulk heterojunction (BHJ) layers of organic photovoltaic (OPV) devices. This study provides direct insights into the thermal properties of Y6, PM6, and their binary blends by employing fast differential scanning calorimetry (flash DSC) to analyze their chain dynamics. The glass transition temperatures (<i>T</i><sub>g</sub>) of Y6 and PM6 were measured, with Y6 exhibiting a <i>T</i><sub>g</sub> of 175.2 °C and PM6 showing two <i>T</i><sub>g</sub>s at 39.7 and 107.6 °C. Our findings indicate that average OPVs’ operational temperatures are lower than the blend’s primary <i>T</i><sub>g</sub> of 138.2 °C. Thus, the mobility of PM6 and Y6 is not the critical factor that results in drastic drifts in the device morphology. Instead, we discovered that the crystallization of small molecules Y6 in the BHJ film at elevated operation temperatures <i>significantly contributes</i> to the morphological instability of the BHJ layer, based on a flash DSC isotherm crystallization study. The crystallization of the acceptor leads to severe phase separation between donors and acceptors and results in device failure. The acceptor Y6’s crystallization rate also increased when blended with donor PM6, compared to that of pure Y6 molecules. Furthermore, AFM–IR analysis of the morphology of the BHJ layer after high thermal stress of 200 °C revealed an apparent demixing of donor PM6 and acceptor Y6, revealing Y6 globules about 200 nm in diameter, with PM6 domains surrounding the Y6 regions. This crystallization-induced morphology change was later confirmed to correlate well with the device performance drop. This study offers valuable insights into the origin of BHJ layer instability in OPV devices containing nonfullerene small molecule acceptors and polymer donors. Additionally, it emphasizes the importance of addressing thermal stress to enhance the performance and durability of such devices and informs strategies for developing more stable organic solar cells.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4334–4344 4334–4344"},"PeriodicalIF":8.5,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00631","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Integrated Materials Design and Process Engineering for n-Type Polymer Thermoelectrics n 型聚合物热电的集成材料设计和工艺工程
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-09 DOI: 10.1021/jacsau.4c0063810.1021/jacsau.4c00638
Xin-Yu Deng, Zhi Zhang and Ting Lei*, 

Polymer thermoelectrics (TEs) have attracted increasing interest in recent years, owing to their great potential in intimate integration with wearable electronics for powering small electronics/sensors and personal temperature regulation. Over the past few decades, substantial progress has been made in enhancing polymer TE performance. However, the electrical conductivity and power factor of most n-doped polymers are about an order of magnitude lower than those of their p-type counterparts, impeding the development of highly efficient polymer TE devices. In addition, unlike well-studied inorganic materials, the complex charge transport mechanism and polymer–dopant interactions in polymer TE materials have hindered a comprehensive understanding of the structure–property relationships. This Perspective aims to survey recent achievements in understanding the charge transport mechanism and selectively provide some critical insights into molecular design and process engineering for n-type polymer TEs. We also highlight the great potential of polymer TEs in wearable electronics and offer an outlook for future development.

近年来,聚合物热电(TE)在与可穿戴电子设备紧密结合,为小型电子设备/传感器供电以及调节个人体温方面具有巨大潜力,因此吸引了越来越多的关注。过去几十年来,在提高聚合物热电半导体性能方面取得了长足的进步。然而,大多数 n 型掺杂聚合物的导电性和功率因数比 p 型聚合物低大约一个数量级,阻碍了高效聚合物 TE 器件的开发。此外,与研究透彻的无机材料不同,聚合物 TE 材料中复杂的电荷传输机制和聚合物-掺杂剂相互作用阻碍了对其结构-性能关系的全面了解。本视角旨在考察近年来在理解电荷传输机制方面取得的成就,并有选择性地为 n 型聚合物 TE 的分子设计和工艺工程提供一些重要见解。我们还强调了聚合物 TE 在可穿戴电子设备中的巨大潜力,并对未来发展进行了展望。
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引用次数: 0
Total Synthesis of (−)-Bipolarolide D (-)-联苯内酯 D 的全合成
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-09 DOI: 10.1021/jacsau.4c0068010.1021/jacsau.4c00680
Gleb A. Chesnokov, Julia Friedli, Francis J. Carta and Karl Gademann*, 

(−)-Bipolarolide D is an ophiobolin-derived sesteterpenoid with a unique tetraquinane (5/5/5/5) tetracyclic skeleton decorated with a diverse set of functionalities. Herein we report a robust, scalable, and efficient total synthesis of this natural product in 1.8% overall yield. The developed approach features a diastereoselective Pauson–Khand reaction, a highly efficient Rautenstrauch cycloisomerization, and radical cyclization to forge the carbon backbone and the installation of the side chain via crotylation with 1-methyl-2-propenylmagnesium chloride followed by Suzuki cross-coupling.

(-)-Bipolarolide D 是一种源自蛇床子素的雌甾烷类化合物,具有独特的四喹啉(5/5/5/5)四环骨架,并饰有多种功能。在此,我们报告了一种稳健、可扩展且高效的天然产物全合成方法,总产率为 1.8%。所开发的方法包括非对映选择性保森-汉德反应、高效的劳滕斯特劳赫环异构化、自由基环化以形成碳骨架,以及通过 1-甲基-2-丙烯基氯化镁的巴豆酰化作用安装侧链,然后进行铃木交叉偶联。
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引用次数: 0
Enzymatic Routes to Designer Hemicelluloses for Use in Biobased Materials 设计用于生物基材料的半纤维素的酶法途径
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-08 DOI: 10.1021/jacsau.4c0046910.1021/jacsau.4c00469
Thu V. Vuong, Mohammad Aghajohari, Xuebin Feng, Amanda K. Woodstock, Deepti M. Nambiar, Zeina C. Sleiman, Breeanna R. Urbanowicz* and Emma R. Master*, 

Various enzymes can be used to modify the structure of hemicelluloses directly in vivo or following extraction from biomass sources, such as wood and agricultural residues. Generally, these enzymes can contribute to designer hemicelluloses through four main strategies: (1) enzymatic hydrolysis such as selective removal of side groups by glycoside hydrolases (GH) and carbohydrate esterases (CE), (2) enzymatic cross-linking, for instance, the selective addition of side groups by glycosyltransferases (GT) with activated sugars, (3) enzymatic polymerization by glycosynthases (GS) with activated glycosyl donors or transglycosylation, and (4) enzymatic functionalization, particularly via oxidation by carbohydrate oxidoreductases and via amination by amine transaminases. Thus, this Perspective will first highlight enzymes that play a role in regulating the degree of polymerization and side group composition of hemicelluloses, and subsequently, it will explore enzymes that enhance cross-linking capabilities and incorporate novel chemical functionalities into saccharide structures. These enzymatic routes offer a precise way to tailor the properties of hemicelluloses for specific applications in biobased materials, contributing to the development of renewable alternatives to conventional materials derived from fossil fuels.

各种酶可直接在体内或从木材和农业残留物等生物质来源提取后用于改变半纤维素的结构。一般来说,这些酶可通过以下四种主要策略促进半纤维素的设计:(1) 酶水解,例如糖苷水解酶(GH)和碳水化合物酯酶(CE)选择性去除侧基;(2) 酶交联,例如糖基转移酶(GT)选择性添加活化糖的侧基、(4) 酶功能化,特别是通过碳水化合物氧化还原酶的氧化作用和胺转氨酶的胺化作用。因此,本视角将首先重点介绍在调节半纤维素聚合度和侧基组成方面发挥作用的酶,随后将探讨可增强交联能力并将新型化学功能结合到糖结构中的酶。这些酶法路线提供了一种精确的方法,可针对生物基材料的特定应用调整半纤维素的特性,从而有助于开发可再生替代品,取代从化石燃料中提取的传统材料。
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引用次数: 0
Pyrimidine Azepine Targets the Plasmodium bc 1 Complex and Displays Multistage Antimalarial Activity. 嘧啶氮杂环庚烷以疟原虫 bc 1 复合物为靶标,发挥多级抗疟活性
IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-07 eCollection Date: 2024-10-28 DOI: 10.1021/jacsau.4c00674
Juliana Calit, Surendra K Prajapati, Ernest D Benavente, Jessica E Araújo, Bingbing Deng, Kazutoyo Miura, Yasmin Annunciato, Igor M R Moura, Miho Usui, Jansen F Medeiros, Carolina H Andrade, Sabrina Silva-Mendonça, Anton Simeonov, Richard T Eastman, Carole A Long, Maisa da Silva Araujo, Kim C Williamson, Anna Caroline C Aguiar, Daniel Y Bargieri

Malaria control and elimination efforts would benefit from the identification and validation of new malaria chemotherapeutics. Recently, a transgenic Plasmodium berghei line was used to perform a series of high-throughput in vitro screens for new antimalarials acting against the parasite sexual stages. The screens identified pyrimidine azepine chemotypes with potent activity. Here, we validate the activity of PyAz90, the most potent pyrimidine azepine chemotype identified, against P. falciparum and P. vivax in the asexual and sexual stages. PyAz90 blocked parasite transmission to the mosquito vector at nanomolar concentrations and inhibited in vitro asexual parasite multiplication with a fast-action profile. Through the generation of P. falciparum PyAz90-resistant parasites and in vitro assays of mitochondrial activity, we identified cytochrome b as a molecular target of PyAz90. This work characterizes a promising chemotype that can be explored for the future development of new antimalarials targeting the Plasmodium cytochrome bc 1 complex.

疟疾控制和消除工作将受益于新疟疾化疗药物的鉴定和验证。最近,我们利用转基因疟原虫品系进行了一系列高通量体外筛选,以寻找针对寄生虫有性阶段的新型抗疟药物。这些筛选确定了具有强效活性的嘧啶氮杂环庚烷化学型。在这里,我们验证了 PyAz90 的活性,它是已发现的最有效的嘧啶氮杂环庚烷化学型,对恶性疟原虫和间日疟原虫的无性阶段和有性阶段均有作用。PyAz90 在纳摩尔浓度下可阻断寄生虫向蚊媒的传播,并能快速抑制体外无性寄生虫的繁殖。通过产生恶性疟原虫 PyAz90 抗性寄生虫和线粒体活性体外检测,我们确定细胞色素 b 是 PyAz90 的分子靶标。这项工作描述了一种很有前景的化学类型,可用于今后开发针对疟原虫细胞色素 bc 1 复合物的新型抗疟药。
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引用次数: 0
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