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‘Living’ anionic polymerization through reversible activation of C–H bonds with a base catalyst 通过碱催化剂对 C-H 键的可逆活化实现 "活 "阴离子聚合反应

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-21 DOI: 10.1038/s41557-024-01611-z

Living anionic polymerization is generally carried out using a metal-based initiator under stringent, and ideally water-free, conditions. Now, proton transfer anionic polymerization is developed using an organic compound with an acidic C–H bond as the initiator in the presence of a base catalyst. This method offers easy access to well-defined polymers under moderate conditions.

活阴离子聚合通常是在严格和理想的无水条件下使用金属引发剂进行的。现在，质子传递阴离子聚合法在碱催化剂的作用下，使用具有酸性 C-H 键的有机化合物作为引发剂。这种方法可在温和的条件下轻松获得定义明确的聚合物。

引用次数: 0

Emerging chiral two-dimensional materials 新兴手性二维材料

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-21 DOI: 10.1038/s41557-024-01595-w

Jinqiao Dong, Yan Liu, Yong Cui

Research into 2D materials has been growing with impressive speed since the discovery of graphene. Such layered materials with ultrathin morphologies and extreme aspect ratios currently display a vast range of properties; however, until recently a conspicuously missing property of 2D materials was global chirality. The situation has changed over the past few years with the implementation of several distinct types of ultrathin chiral 2D crystals. Here we offer a forward-looking perspective on this field to comprehend the fundamentals of global chirality in two dimensions and develop new directions. We specifically discuss the experimental achievements of the emerging chiral 2D materials with a focus on their design strategy, synthesis, structural characterization, fundamental physical properties and possible applications. We will highlight how the molecular-scale local chirality could be significantly transmitted and amplified throughout ultrathin single-crystalline 2D structures, resulting in distinctive global chirality that brings more sophisticated functions. Chirality in extended 2D structures exhibits fundamental differences from molecular-level chirality. This Perspective discusses how local molecular chirality is transmitted and amplified to form distinctive global chirality within ultrathin, single-crystalline 2D materials; it also explores the future challenges and potential of this field.

自发现石墨烯以来，二维材料的研究一直在飞速发展。目前，这种具有超薄形态和极高纵横比的层状材料显示出多种特性；然而，直到最近，二维材料明显缺少的一个特性就是全局手性。过去几年，随着几种不同类型的超薄手性二维晶体的问世，情况发生了变化。在此，我们将以前瞻性的视角来理解二维全局手性的基本原理，并开拓新的研究方向。我们将具体讨论新兴手性二维材料的实验成果，重点关注其设计策略、合成、结构表征、基本物理性质和可能的应用。我们将重点介绍分子尺度的局部手性如何在整个超薄单晶二维结构中得到显著传递和放大，从而产生独特的全局手性，带来更复杂的功能。

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引用次数: 0

Synthesis of model heterojunction interfaces reveals molecular-configuration-dependent photoinduced charge transfer 模型异质结界面的合成揭示了依赖分子构型的光诱导电荷转移

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-20 DOI: 10.1038/s41557-024-01578-x

Jeroen Royakkers, Hanbo Yang, Alexander J. Gillett, Flurin Eisner, Pratyush Ghosh, Daniel G. Congrave, Mohammed Azzouzi, Zahra Andaji-Garmaroudi, Anastasia Leventis, Akshay Rao, Jarvist Moore Frost, Jenny Nelson, Hugo Bronstein

Control of the molecular configuration at the interface of an organic heterojunction is key to the development of efficient optoelectronic devices. Due to the difficulty in characterizing these buried and (probably) disordered heterointerfaces, the interfacial structure in most systems remains a mystery. Here we demonstrate a synthetic strategy to design and control model interfaces, enabling their detailed study in isolation from the bulk material. This is achieved by the synthesis of a polymer in which a non-fullerene acceptor moiety is covalently bonded to a donor polymer backbone using dual alkyl chain links, constraining the acceptor and donor units in a through space co-facial arrangement. The constrained geometry of the acceptor relative to the electron-rich and -poor moieties in the polymer backbone can be tuned to control the kinetics of charge separation and the energy of the resultant charge-transfer state giving insight into factors that govern charge generation at organic heterojunctions. The molecular interactions at an organic heterointerface govern the performance of many optoelectronic devices. Through a combination of synthesis, spectroscopy and modelling, it has now been shown that specific molecular interactions result in improved formation of the charge-transfer state.

控制有机异质结界面的分子构型是开发高效光电设备的关键。由于难以表征这些埋藏的（可能）无序异质界面，大多数系统中的界面结构仍然是一个谜。在这里，我们展示了一种设计和控制模型界面的合成策略，从而能够脱离块体材料对其进行详细研究。这是通过合成一种聚合物来实现的，在这种聚合物中，非富勒烯受体分子通过双烷基链键与供体聚合物骨架共价键合，从而将受体和供体单元限制在通孔空间共面排列中。可以调整受体相对于聚合物主链中富电子和贫电子分子的受限几何形状，以控制电荷分离的动力学和由此产生的电荷转移状态的能量，从而深入了解影响有机异质结电荷产生的各种因素。

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引用次数: 0

Generating synthetic gap junctions using supramolecular amphiphilic giant nanotubes 利用超分子两亲巨型纳米管生成合成缝隙连接

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-20 DOI: 10.1038/s41557-024-01604-y

Ai Kohata, Kazushi Kinbara

The construction of synthetic cells holds great importance for exploring complex biological systems and could potentially provide insights into the origins of life. Now, synthetic gap junctional channels have been developed as a building block to construct synthetic cells that can mediate intercellular transport of ions and bioactive species.

合成细胞的构建对于探索复杂的生物系统具有重要意义，并有可能为生命起源提供启示。现在，合成缝隙连接通道已被开发出来，作为构建合成细胞的基石，它可以介导离子和生物活性物质的细胞间运输。

引用次数: 0

Synthetic model interfaces for the study of intermolecular charge-transfer states 用于研究分子间电荷转移状态的合成模型界面

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-20 DOI: 10.1038/s41557-024-01579-w

The synthesis of model heterojunction interfaces allows for the study of interfacial photoinduced charge-transfer states as a function of molecular structure. This analysis provides molecular-level insight into the factors governing charge generation at organic heterointerfaces and, thus, the efficiency of organic solar cells and other optoelectronic devices.

通过合成模型异质结界面，可以研究作为分子结构函数的界面光诱导电荷转移状态。这种分析能从分子层面深入了解有机异质界面的电荷生成因素，从而了解有机太阳能电池和其他光电设备的效率。

引用次数: 0

Neural-network-based molecular dynamics simulations reveal that proton transport in water is doubly gated by sequential hydrogen-bond exchange 基于神经网络的分子动力学模拟揭示了质子在水中的迁移是由连续的氢键交换双重控制的

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-20 DOI: 10.1038/s41557-024-01593-y

Axel Gomez, Ward H. Thompson, Damien Laage

The transport of excess protons in water is central to acid–base chemistry, biochemistry and energy production. However, elucidating its mechanism has been challenging. Recent nonlinear vibrational spectroscopy experiments could not be explained by existing models. Here we use both vibrational spectroscopy calculations and neural-network-based molecular dynamics simulations that account for nuclear quantum effects for all atoms to determine the proton transport mechanism. Our simulations reveal an equilibrium between two stable proton-localized structures with distinct Eigen-like and Zundel-like hydrogen-bond motifs. Proton transport follows a three-step mechanism gated by two successive hydrogen-bond exchanges: the first reduces the proton-acceptor water coordination, leading to proton transfer, and the second, the rate-limiting step, prevents rapid back-transfer by increasing the proton-donor coordination. This sequential mechanism is consistent with experimental characterizations of proton diffusion, explaining the low activation energy and the prolonged intermediate lifetimes in vibrational spectroscopy. These results are crucial for understanding proton dynamics in biochemical and technological systems.

过量质子在水中的迁移是酸碱化学、生物化学和能源生产的核心。然而，阐明其机理一直是一项挑战。现有模型无法解释最近的非线性振动光谱实验。在这里，我们利用振动光谱计算和基于神经网络的分子动力学模拟（考虑到所有原子的核量子效应）来确定质子传输机制。我们的模拟揭示了两种稳定的质子定位结构之间的平衡，这两种结构具有不同的类 Eigen 和类 Zundel 氢键图案。质子迁移遵循一个由两次连续氢键交换驱动的三步机制：第一步降低质子受体水配位，导致质子转移；第二步，即限制速率的一步，通过增加质子供体配位防止快速反向转移。这种顺序机制与质子扩散的实验特征一致，解释了振动光谱中的低活化能和中间寿命延长的原因。这些结果对于理解生化和技术系统中的质子动力学至关重要。

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引用次数: 0

Machine learning trims the peptide drug design process to a sweet spot 机器学习将多肽药物设计过程缩减至最佳状态

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-16 DOI: 10.1038/s41557-024-01610-0

Chloe E. Markey, Daniel Reker

Drugs that target peptide hormone receptors are of great interest in the treatment of type 2 diabetes. In spite of limited data and vast design spaces, a bespoke computational pipeline has designed peptides that target two receptors with high potency.

靶向肽类激素受体的药物在治疗 2 型糖尿病方面具有重大意义。尽管数据有限，设计空间巨大，但一个定制的计算管道已经设计出了针对两种受体的高效力多肽。

引用次数: 0

Sulfone cross-coupling outcompetes proton transfer 砜交叉偶联取代质子转移

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-15 DOI: 10.1038/s41557-024-01612-y

Chloe D. Wong, Elizabeth R. Jarvo

The development of enantiospecific sulfone reactions has been hindered by the inherent acidity of sulfones, which result in deleterious racemization. Now, the synthesis of enantioenriched diarylalkanes has been reported via sufficiently fast cross-coupling that circumvents racemization of the chiral sulfone.

砜的固有酸性会导致有害的消旋化，这阻碍了对映体特异性砜反应的发展。现在，有报告称，通过足够快的交叉偶联，可以避免手性砜的消旋化，从而合成对映体丰富的二芳基烷烃。

引用次数: 0

A dynamic metal–organic framework photocatalyst 动态金属有机框架光催化剂

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-14 DOI: 10.1038/s41557-024-01607-9

Photocatalytic overall water splitting (OWS) is highly desirable for hydrogen production but challenging owing to rapid charge recombination. We demonstrate a dynamic metal–organic framework (MOF) photocatalyst that achieves OWS via one-step photoexcitation. Upon excitation by light, the MOF undergoes a structural twist that suppresses charge recombination and achieves OWS.

光催化整体水分离（OWS）对于制氢来说非常理想，但由于电荷的快速重组而具有挑战性。我们展示了一种动态金属有机框架（MOF）光催化剂，可通过一步光激发实现 OWS。在光的激发下，MOF 会发生结构扭曲，从而抑制电荷重组并实现 OWS。

引用次数: 0

Discovery of the selenium-containing antioxidant ovoselenol derived from convergent evolution 从聚合进化中发现含硒抗氧化剂卵硒醇

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2024-08-14 DOI: 10.1038/s41557-024-01600-2

Chase M. Kayrouz, Kendra A. Ireland, Vanessa Y. Ying, Katherine M. Davis, Mohammad R. Seyedsayamdost

Selenium is an essential micronutrient, but its presence in biology has been limited to protein and nucleic acid biopolymers. The recent identification of a biosynthetic pathway for selenium-containing small molecules suggests that there is a larger family of selenometabolites that remains to be discovered. Here we identify a recently evolved branch of abundant and uncharacterized metalloenzymes that we predict are involved in selenometabolite biosynthesis using a bioinformatic search strategy that relies on the mapping of composite active site motifs. Biochemical studies confirm this prediction and show that these enzymes form an unusual C–Se bond onto histidine, thus giving rise to a distinct selenometabolite and potent antioxidant that we have termed ovoselenol. Aside from providing insights into the evolution of this enzyme class and the structural basis of C–Se bond formation, our work offers a blueprint for charting the microbial selenometabolome in the future.

硒是人体必需的微量元素，但它在生物学中的存在仅限于蛋白质和核酸生物聚合物。最近发现的含硒小分子生物合成途径表明，还有一个更大的硒代谢物家族有待发现。在这里，我们利用生物信息学搜索策略，通过绘制复合活性位点图案，发现了最近进化的、丰富的、未表征的金属酶分支，并预测它们参与了硒代谢物的生物合成。生化研究证实了这一预测，并表明这些酶在组氨酸上形成了不寻常的 C-Se键，从而产生了一种独特的硒代谢物和强效抗氧化剂，我们称之为卵硒醇。我们的工作不仅为了解这类酶的进化和 C-Se 键形成的结构基础提供了见解，还为未来绘制微生物硒代谢组提供了蓝图。

引用次数: 0

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