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The Chemist Who Stayed in Gaza 留在加沙的化学家
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-12 DOI: 10.1021/acscentsci.4c01418
Laurel Oldach
Rami Morjan hopes to survive and rebuild.
拉米-莫尔詹希望能够生存下来并重建家园。
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引用次数: 0
Fantastic Frustrated Materials–and Where to Find Them 神奇的受挫材料--从哪里可以找到它们?
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-12 DOI: 10.1021/acscentsci.4c01409
Christopher R. Wiebe
Symmetry and simulations can identify exotic magnetic materials for chemists to target in the laboratory.
通过对称和模拟,化学家们可以在实验室中发现奇特的磁性材料。
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引用次数: 0
Bioinspired, Carbohydrate-Containing Polymers Efficiently and Reversibly Sequester Heavy Metals 受生物启发的含碳水化合物聚合物可高效、可逆地封存重金属
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-11 DOI: 10.1021/acscentsci.4c01010
Sungjin Jeon, Teron Haynie, Samuel Chung, Cassandra E. Callmann
Water scarcity and heavy metal pollution are significant challenges in today’s industrialized world. Conventional heavy metal remediation methods are often inefficient and energy-intensive, and produce chemical sludge. To address these issues, we developed a bioinspired, carbohydrate-containing polymer system for efficient and selective heavy metal removal. Using ring opening metathesis polymerization, we synthesized polymers bearing amphiphilic glucuronate side chains capable of selectively binding heavy metal cations in mixed media. In samples containing high concentrations of heavy metals (>550 ppb), these polymers rapidly form a filterable precipitate upon metal capture, reducing the concentration of cation to <1.5 ppb within 3 min, as measured by inductively coupled plasma mass spectrometry. This system effectively removes cadmium ions from highly contaminated solutions to levels below the Agency for Toxic Substances and Disease Registry limit for Cd2+ in drinking water and selectively removes both Cd2+ and Pb2+ from lake water spiked with trace amounts of metal. Acidification triggers protonation of the glucuronate groups, releasing the heavy metals and resolubilizing the polymer. This capture-and-release process can be repeated over multiple cycles without loss of binding capacity. As such, this study introduces a novel class of recyclable materials with pH-responsive properties, offering potential for applications in water remediation and beyond.
水资源短缺和重金属污染是当今工业化世界面临的重大挑战。传统的重金属修复方法往往效率低下、能耗高,而且会产生化学污泥。为了解决这些问题,我们开发了一种受生物启发的含碳水化合物聚合物系统,用于高效、选择性地去除重金属。通过开环偏聚,我们合成了带有两亲性葡萄糖醛酸侧链的聚合物,这种聚合物能够在混合介质中选择性地结合重金属阳离子。在含有高浓度重金属(550 ppb)的样品中,这些聚合物在捕获金属后会迅速形成可过滤的沉淀,通过电感耦合等离子体质谱法测量,在 3 分钟内将阳离子浓度降至 1.5 ppb。该系统能有效去除高度污染溶液中的镉离子,使其含量低于美国有毒物质和疾病登记署规定的饮用水中 Cd2+ 的限值,并能选择性地去除湖泊水中的 Cd2+ 和 Pb2+。酸化会引发葡萄糖醛酸基团质子化,释放重金属并使聚合物溶解。这种捕获和释放过程可以多次重复,而不会丧失结合能力。因此,这项研究引入了一类具有 pH 响应特性的新型可回收材料,为水修复等领域的应用提供了潜力。
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引用次数: 0
Bioinspired, Carbohydrate-Containing Polymers Efficiently and Reversibly Sequester Heavy Metals 受生物启发的含碳水化合物聚合物可高效、可逆地封存重金属
IF 12.7 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-11 DOI: 10.1021/acscentsci.4c0101010.1021/acscentsci.4c01010
Sungjin Jeon, Teron Haynie, Samuel Chung and Cassandra E. Callmann*, 

Water scarcity and heavy metal pollution are significant challenges in today’s industrialized world. Conventional heavy metal remediation methods are often inefficient and energy-intensive, and produce chemical sludge. To address these issues, we developed a bioinspired, carbohydrate-containing polymer system for efficient and selective heavy metal removal. Using ring opening metathesis polymerization, we synthesized polymers bearing amphiphilic glucuronate side chains capable of selectively binding heavy metal cations in mixed media. In samples containing high concentrations of heavy metals (>550 ppb), these polymers rapidly form a filterable precipitate upon metal capture, reducing the concentration of cation to <1.5 ppb within 3 min, as measured by inductively coupled plasma mass spectrometry. This system effectively removes cadmium ions from highly contaminated solutions to levels below the Agency for Toxic Substances and Disease Registry limit for Cd2+ in drinking water and selectively removes both Cd2+ and Pb2+ from lake water spiked with trace amounts of metal. Acidification triggers protonation of the glucuronate groups, releasing the heavy metals and resolubilizing the polymer. This capture-and-release process can be repeated over multiple cycles without loss of binding capacity. As such, this study introduces a novel class of recyclable materials with pH-responsive properties, offering potential for applications in water remediation and beyond.

A novel carbohydrate-based polymer removes heavy metals from water, forming a recyclable, pH-responsive precipitate. It is highly efficient, needs no carrier matrix, and holds promise for water remediation.

水资源短缺和重金属污染是当今工业化世界面临的重大挑战。传统的重金属修复方法往往效率低下、能耗高,而且会产生化学污泥。为了解决这些问题,我们开发了一种受生物启发的含碳水化合物聚合物系统,用于高效、选择性地去除重金属。通过开环偏聚,我们合成了带有两亲性葡萄糖醛酸侧链的聚合物,能够在混合介质中选择性地结合重金属阳离子。在含有高浓度重金属(550 ppb)的样品中,这些聚合物在捕获金属后会迅速形成可过滤的沉淀,通过电感耦合等离子体质谱法测量,在 3 分钟内将阳离子浓度降至 1.5 ppb。该系统能有效去除高度污染溶液中的镉离子,使其含量低于美国有毒物质和疾病登记署规定的饮用水中 Cd2+ 的限值,并能选择性地去除湖泊水中的 Cd2+ 和 Pb2+。酸化会引发葡萄糖醛酸基团质子化,释放出重金属并使聚合物溶解。这种捕获和释放过程可以多次重复,而不会丧失结合能力。因此,这项研究引入了一类具有 pH 值响应特性的新型可回收材料,为水修复及其他领域的应用提供了潜力。这种新型碳水化合物基聚合物能去除水中的重金属,形成可回收的 pH 响应沉淀物。它效率高,无需载体基质,有望用于水污染治理。
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引用次数: 0
Discovering Classical Spin Liquids by Topological Search of High Symmetry Nets 通过拓扑搜索高对称性网络发现经典自旋液体
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-11 DOI: 10.1021/acscentsci.4c01020
Joseph A. M. Paddison, Matthew J. Cliffe
Spin liquids are a paradigmatic example of a nontrivial state of matter. The search for new spin liquids is a key interdisciplinary challenge. Geometrical frustration─where the geometry of the net that the spins occupy precludes the generation of a simple ordered state─is a particularly fruitful way to generate these intrinsically disordered states. Prior focus has been on a handful of high symmetry nets. There are, however, many three-dimensional nets, each of which has the potential to form unique states. In this paper, we investigate the high symmetry nets─those which are both vertex- and edge-transitive─for the simplest possible interaction sets: nearest-neighbor couplings of antiferromagnetic Heisenberg and Ising spins. While the well-known crs (pyrochlore) net is the only nearest-neighbor Heisenberg antiferromagnet which does not order, we identify two new frustrated nets (lcx and thp) possessing finite temperature Heisenberg spin-liquid states with strongly suppressed magnetic ordering and noncollinear ground states. With Ising spins, we identify three new classical spin liquids that do not order down to T/J = 0.01. We highlight materials that contain these high symmetry nets, and which could, if substituted with appropriate magnetic ions, potentially host these unusual states. Our systematic survey will guide searches for novel magnetic phases.
自旋液体是非微观物质状态的典型例子。寻找新的自旋液体是一项关键的跨学科挑战。几何挫折--即自旋占据的网的几何形状排除了简单有序态的产生--是产生这些内在无序态的一种特别富有成效的方法。之前的研究主要集中在少数几个高对称性网络上。然而,还有许多三维网络,每个网络都有可能形成独特的状态。在本文中,我们针对最简单的相互作用集--反铁磁性海森堡自旋和伊辛自旋的近邻耦合--研究了同时具有顶点和边缘传递性的高对称性网。众所周知的crs(火成岩)网是唯一不存在有序性的近邻海森堡反铁磁体,而我们发现了两个新的受挫网(lcx 和 thp),它们拥有有限温度的海森堡自旋液态,具有强抑制磁有序性和非共线基态。通过伊辛自旋,我们发现了三种新的经典自旋液体,它们在 T/J = 0.01 时不存在有序性。我们重点介绍了含有这些高对称性网的材料,如果用适当的磁离子替代,这些材料就有可能承载这些不寻常的状态。我们的系统调查将为寻找新型磁性相提供指导。
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引用次数: 0
A Conversation with Alba Álvarez-Martín 对话阿尔芭-阿尔瓦雷斯-马丁
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1021/acscentsci.4c01408
Jonathan Feakins
The cultural heritage scientist is adapting a medical imaging technique to analyze paintings in Amsterdam’s Rijksmuseum.
这位文化遗产科学家正在采用一种医学成像技术来分析阿姆斯特丹莱克斯博物馆的绘画作品。
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引用次数: 0
A Conversation with Alba Álvarez-Martín 对话阿尔芭-阿尔瓦雷斯-马丁
IF 12.7 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1021/acscentsci.4c0140810.1021/acscentsci.4c01408
Jonathan Feakins, 

The cultural heritage scientist is adapting a medical imaging technique to analyze paintings in Amsterdam’s Rijksmuseum.

这位文化遗产科学家正在采用一种医学成像技术来分析阿姆斯特丹莱克斯博物馆的绘画作品。
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引用次数: 0
Loss of Diphthamide Increases DNA Replication Stress in Mammalian Cells by Modulating the Translation of RRM1 失去双硫酰胺会通过调节 RRM1 的翻译增加哺乳动物细胞的 DNA 复制压力
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-06 DOI: 10.1021/acscentsci.4c00967
Jiaqi Zhao, Byunghyun Ahn, Hening Lin
Diphthamide (DPH) is a highly conserved post-translational modification exclusively present in eukaryotic translation elongation factor 2 (eEF2), with its loss leading to embryonic lethality in mice and developmental disorders in humans. In this study, we unveil the role of diphthamide in mammalian cell DNA damage stress, with a particular emphasis on DNA replication stress. We developed a systematic strategy to identify human proteins affected by diphthamide with a combination of computational profiling and quantitative proteomics. Through this approach, we determine that the translation of RRM1 is modulated by diphthamide via −1 frameshifting. Importantly, our results reveal that the dysregulation of RRM1 translation in DPH-deficient cells is causally linked to elevated DNA replication stress. These findings provide a potential explanation for how diphthamide deficiency leads to cancer and developmental defects in humans.
双硫酰胺(DPH)是一种高度保守的翻译后修饰,只存在于真核生物翻译伸长因子 2(eEF2)中,其缺失会导致小鼠胚胎死亡和人类发育障碍。在这项研究中,我们揭示了双硫酰胺在哺乳动物细胞 DNA 损伤应激中的作用,尤其是在 DNA 复制应激中的作用。我们开发了一种系统化的策略,结合计算剖析和定量蛋白质组学来识别受双酞胺影响的人类蛋白质。通过这种方法,我们确定 RRM1 的翻译受双硫仑影响的途径是-1 框移位。重要的是,我们的研究结果表明,DPH缺陷细胞中RRM1翻译的失调与DNA复制压力的升高有因果关系。这些发现为双硫仑缺乏症如何导致人类癌症和发育缺陷提供了一个潜在的解释。
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引用次数: 0
Pauli Exclusion by n→π* Interactions: Implications for Paleobiology n→π* 相互作用的保利排斥:对古生物学的影响
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-04 DOI: 10.1021/acscentsci.4c00971
Jinyi Yang, Volga Kojasoy, Gerard J. Porter, Ronald T. Raines
Proteins have evolved to function in an aqueous environment. Collagen, which provides the bodily scaffold for animals, has a special need to retain its integrity. This need was addressed early on, as intact collagen has been detected in dinosaur fossils, even though peptide bonds have a half-life of only ∼500 years in a neutral aqueous solution. We sought to discover the physicochemical basis for this remarkable resistance to hydrolysis. Using experimental and computational methods, we found that a main-chain acyl group can be protected from hydrolysis by an O···C═O n→π* interaction with a neighboring acyl group. These interactions engage virtually every peptide bond in a collagen triple helix. This protection, which arises from the Pauli exclusion principle, could underlie the preservation of ancient collagen.
蛋白质的进化是为了在水环境中发挥作用。为动物提供身体支架的胶原蛋白特别需要保持其完整性。尽管肽键在中性水溶液中的半衰期只有 500 年,但在恐龙化石中发现了完整的胶原蛋白。我们试图发现这种显著的抗水解性的物理化学基础。利用实验和计算方法,我们发现主链酰基可以通过与邻近酰基的 O-C═O n→π* 相互作用来防止水解。这些相互作用几乎涉及胶原蛋白三螺旋中的每一个肽键。这种源于保利排斥原理的保护作用可能是古老胶原蛋白得以保存的原因。
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引用次数: 0
Generative Deep Learning-Based Efficient Design of Organic Molecules with Tailored Properties 基于生成式深度学习的定制特性有机分子高效设计
IF 18.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-30 DOI: 10.1021/acscentsci.4c00656
Minhi Han, Joonyoung F. Joung, Minseok Jeong, Dong Hoon Choi, Sungnam Park
Innovative approaches to design molecules with tailored properties are required in various research areas. Deep learning methods can accelerate the discovery of new materials by leveraging molecular structure–property relationships. In this study, we successfully developed a generative deep learning (Gen-DL) model that was trained on a large experimental database (DBexp) including 71,424 molecule/solvent pairs and was able to design molecules with target properties in various solvents. The Gen-DL model can generate molecules with specified optical properties, such as electronic absorption/emission peak position and bandwidth, extinction coefficient, photoluminescence (PL) quantum yield, and PL lifetime. The Gen-DL model was shown to leverage the essential design principles of conjugation effects, Stokes shifts, and solvent effects when it generated molecules with target optical properties. Additionally, the Gen-DL model was demonstrated to generate practically useful molecules developed for real-world applications. Accordingly, the Gen-DL model can be a promising tool for the discovery and design of novel molecules with tailored properties in various research areas, such as organic photovoltaics (OPVs), organic light-emitting diodes (OLEDs), organic photodiodes (OPDs), bioimaging dyes, and so on.
各个研究领域都需要创新方法来设计具有定制特性的分子。深度学习方法可以利用分子结构-性质关系加速新材料的发现。在本研究中,我们成功开发了一种生成式深度学习(Gen-DL)模型,该模型在包括 71,424 对分子/溶剂的大型实验数据库(DBexp)上进行了训练,能够在各种溶剂中设计出具有目标特性的分子。Gen-DL 模型可以生成具有指定光学特性的分子,如电子吸收/发射峰位置和带宽、消光系数、光致发光量子产率和光致发光寿命。研究表明,Gen-DL 模型在生成具有目标光学特性的分子时,充分利用了共轭效应、斯托克斯位移和溶剂效应等基本设计原理。此外,Gen-DL 模型还被证明可以生成为实际应用而开发的实用分子。因此,Gen-DL 模型有望成为发现和设计具有定制特性的新型分子的工具,应用于有机光伏(OPV)、有机发光二极管(OLED)、有机光电二极管(OPD)、生物成像染料等多个研究领域。
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引用次数: 0
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