Nature chemistry最新文献

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Biomolecular condensates sustain pH gradients at equilibrium through charge neutralization 生物分子凝聚物通过电荷中和维持pH梯度在平衡状态。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-29 DOI: 10.1038/s41557-025-02039-9

Hannes Ausserwöger, Rob Scrutton, Charlotte M. Fischer, Tomas Sneideris, Daoyuan Qian, Ella de Csilléry, Ieva Baronaite, Kadi L. Saar, Alan Z. Białek, Marc Oeller, Georg Krainer, Titus M. Franzmann, Sina Wittmann, Juan M. Iglesias-Artola, Gaetano Invernizzi, Anthony A. Hyman, Simon Alberti, Nikolai Lorenzen, Tuomas P. J. Knowles

Electrochemical gradients are essential to the functioning of cells and form across membranes using active transporters. Here we show in contrast that condensed biomolecular systems—often termed condensates—sustain pH gradients without any external energy input. By studying individual condensates on the micrometre scale using a microdroplet platform, we reveal dense-phase pH shifts towards conditions of minimal electrostatic repulsion. We demonstrate that protein condensates can drive substantial alkaline and acidic gradients, which are compositionally tunable and can extend to complex architectures sustaining multiple unique pH conditions simultaneously. Through in silico characterization of human proteomic condensate networks, we further highlight potential wide-ranging electrochemical properties emerging from condensation in nature, while correlating intracellular condensate pH gradients with complex biomolecular composition. Together, the emergent nature of condensation shapes distinct pH microenvironments, thereby creating a regulatory mechanism to modulate biochemical activity in living and artificial systems. pH is a critical regulator of (bio)chemical processes and therefore tightly regulated in nature. Now, proteins have been shown to possess the functionality to drive pH gradients without requiring energy input or membrane enclosure but through condensation. Protein condensates can drive unique pH gradients that modulate biochemical activity in both living and artificial systems.

电化学梯度对细胞的功能至关重要，并通过活性转运体形成跨膜。在这里，我们展示了在没有任何外部能量输入的情况下，凝聚的生物分子系统（通常称为凝聚物）维持pH梯度。通过使用微液滴平台在微米尺度上研究单个凝聚体，我们揭示了密相pH值向最小静电排斥条件的变化。我们证明了蛋白质凝聚物可以驱动大量的碱性和酸性梯度，这些梯度在成分上是可调的，并且可以扩展到同时维持多种独特pH条件的复杂结构。通过对人类蛋白质组学冷凝水网络的硅表征，我们进一步强调了自然界冷凝水产生的潜在广泛的电化学特性，同时将细胞内冷凝水pH梯度与复杂的生物分子组成联系起来。总之，缩合的涌现性塑造了不同的pH微环境，从而创造了一种调节生物和人工系统中生化活性的调节机制。

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引用次数: 0

Small alkali cations direct CO electroreduction to hydrocarbons rather than oxygenates. 小的碱离子将CO电还原成碳氢化合物而不是氧合物。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-29 DOI: 10.1038/s41557-025-02061-x

Weiyan Ni, Yongxiang Liang, Yufei Cao, Zhu Chen, Rui Kai Miao, Bosi Peng, Zeyan Liu, Yanjiang Liu, Huajie Ze, Xiao Wang, Dongha Kim, Sungjin Park, Jiaqi Yu, Panos Papangelakis, Victor Boureau, Muhammad Imran, Qiyou Wang, Pengfei Ou, Xiao-Yan Li, Ke Xie, Roham Dorakhan, Erfan Shirzadi, George C Schatz, David Sinton, Jun Ge, Jie Zeng, Edward H Sargent

Electrochemical CO reduction has the potential to enable low-carbon-intensity chemicals and fuels, but the reaction yields a mixture of multi-carbon products, and the underlying selectivity-driving mechanisms are unclear. Here we explore trends in alkali cations and find, in contradistinction to carbon dioxide electroreduction, that lithium promotes ethylene production. We study the electrolyte-catalyst interface using operando Raman spectroscopy and simulations and find that hydrated Li⁺ on the electrode surface has the greatest hydrogen bonding and the least cation-dipole interaction with the oxygen site on intermediates. These interactions suppress hydrogenation on carbon and promote the competing hydrodeoxygenation reaction that leads to hydrocarbons. We leverage this understanding and reduce the oxygen affinity of copper via antimony doping, suppressing the formation of the O-tethered CHCHO* intermediate on the surface that would otherwise lead to oxygenates. Combining these strategies, we achieve an ethylene faradaic efficiency of 79% at 150 mA cm^-2 and an energy efficiency of 39% in a membrane electrode assembly electrolyser.

电化学CO还原有可能实现低碳强度的化学品和燃料，但该反应产生多碳产物的混合物，潜在的选择性驱动机制尚不清楚。在这里，我们探索碱阳离子的趋势，并发现，与二氧化碳电还原相比，锂促进乙烯生产。我们使用operando拉曼光谱和模拟研究了电解质-催化剂界面，发现电极表面的水合Li+具有最大的氢键和最小的阳离子-偶极子相互作用。这些相互作用抑制碳上的氢化反应，并促进产生碳氢化合物的竞争性加氢脱氧反应。我们利用这一认识，通过掺杂锑来降低铜的氧亲和性，抑制表面o系链CHCHO*中间体的形成，否则会导致氧合物的形成。结合这些策略，我们在150 mA cm-2下实现了79%的乙烯法拉第效率，在膜电极组装电解槽中实现了39%的能量效率。

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引用次数: 0

Bridged bicycloalkanes through thermal [2+2] cycloaddition 热[2+2]环加成桥联环烷烃

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-28 DOI: 10.1038/s41557-025-02054-w

Meiyun Gao, Xiao Shen

The [2+2] cycloaddition of two alkenes is the most efficient route to four-membered carbocycles, but it is thermally forbidden. Now, installing fluorine atoms at the alkene terminus enables intramolecular thermally crossed [2+2] cycloaddition, providing a strategy for constructing gem-difluoro heterobicyclo[n.1.1]alkanes.

两个烯烃的[2+2]环加成是生成四元碳环最有效的途径，但它是热禁止的。现在，在烯烃末端安装氟原子可以实现分子内热交叉[2+2]环加成，为构建宝石-二氟杂双环[n.1.1]烷烃提供了一种策略。

引用次数: 0

Current-assisted dual-atom catalyst sequentially boosts low-temperature propane combustion through atomic relay 电流辅助双原子催化剂通过原子接力先后促进低温丙烷燃烧

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-26 DOI: 10.1038/s41557-025-02062-w

Yangfei Fang, Xinyu Han, Kaijie Liu, Zhaoxu Yuan, Yannan Li, Songyun Tao, Zeshu Zhang, Cheng Rao, Qi Fu, Guan Peng, Xiangguang Yang, Dingsheng Wang, Yibo Zhang, Wuping Liao

引用次数: 0

Electrochemical reduction of PFAS PFAS的电化学还原

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-26 DOI: 10.1038/s41557-026-02069-x

引用次数: 0

Collective asymmetric synthesis of the Strychnos alkaloids via thiophene S,S-dioxide cycloadditions. 噻吩S，S-二氧化环加成法合成马钱子生物碱的集体不对称反应。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-23 DOI: 10.1038/s41557-025-02041-1

Kun Ho 'Kenny' Park, Jisook Park, Nils Frank, Hanwen Zhang, Peilin Tian, Yasmine Biddick, Fernanda Duarte, Edward A Anderson

The Strychnos alkaloids have long been regarded as landmark targets for chemical synthesis due to their captivating architectures and notorious biological properties. However, the design of approaches that access multiple family members in an asymmetric, concise and atom-economical fashion remains an important challenge. Here we show that thiophene S,S-dioxides (TDOs) offer a modular, rapid entry to Strychnos natural products via inverse electron demand Diels-Alder cascades. We demonstrate that exceptional levels of stereocontrol can be achieved in asymmetric TDO cycloadditions, affording tricyclic indolines of utility in medicinal chemistry research and enabling the stereoselective synthesis of eight Strychnos alkaloids by the shortest routes described so far, including a synthesis of the iconic family member brucine. Using a machine-learning approach, computational studies provide insight into the source of stereoinduction and reveal an intriguing and unexpected spontaneous cheletropic extrusion of SO₂.

马钱子生物碱由于其迷人的结构和臭名昭著的生物学特性，长期以来一直被认为是化学合成的标志性目标。然而，以不对称、简洁和原子经济的方式访问多个家庭成员的方法设计仍然是一个重要的挑战。在这里，我们展示了噻吩S，S-二氧化物（TDOs）通过逆电子需求Diels-Alder级联提供了一个模块化的，快速进入马钱子属天然产物的途径。我们证明了在不对称TDO环加成中可以实现特殊水平的立体控制，为药物化学研究提供了三环吲哚类药物，并通过迄今为止描述的最短路线实现了8种马钱子生物碱的立体选择性合成，包括合成了标志性的家族成员马钱子碱。利用机器学习方法，计算研究提供了对立体感应来源的深入了解，并揭示了一个有趣的、意想不到的SO2自发电变挤压。

引用次数: 0

Engineering the electronic properties of DNA. 设计DNA的电子特性。

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-23 DOI: 10.1038/s41557-026-02066-0

引用次数: 0

Hyperpyramidalized alkenes with bond orders near 1.5 as synthetic building blocks 键阶接近1.5的超锥体化烯烃作为合成构件

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-21 DOI: 10.1038/s41557-025-02055-9

Jiaming Ding, Sarah A. French, Christina A. Rivera, Arismel Tena Meza, Dominick C. Witkowski, K. N. Houk, Neil K. Garg

Alkenes typically have trigonal planar geometries at each terminus, with favourable σ- and π-bonding leading to a bond order of ~2. Here we consider unusual alkenes that possess an extreme form of geometric distortion, termed hyperpyramidalization. In a hyperpyramidalized alkene, geometries deviate remarkably from the typical trigonal planar alkene geometry, leading to weak π-bonding and abnormal alkene bond orders approaching 1.5. Cubene and 1,7-quadricyclene, first validated in 1988 and 1979, respectively, but overlooked for decades since, are the focus of the present study. We leverage their unusually weak π-bonds in cycloadditions, enabling the construction of complex scaffolds and access to previously unrealized chemical space. The origins of the unusually low bond orders were investigated using computational methods. These efforts are expected to prompt future studies of molecules that display hyperpyramidalization or atypical bond orders.

烯烃具有典型的三角平面几何形状，具有良好的σ键和π键，键序为~2。这里我们考虑不寻常的烯烃具有极端形式的几何扭曲，称为超锥体化。在超锥体化的烯烃中，几何结构明显偏离了典型的平面三角形烯烃几何结构，导致弱π键和异常键序接近1.5。三苯和1,7-四环，分别在1988年和1979年首次被证实，但几十年来一直被忽视，是本研究的重点。我们在环加成中利用了它们异常弱的π键，使得构建复杂的支架和进入以前未实现的化学空间成为可能。用计算方法研究了异常低键序的起源。这些努力有望促进未来对显示超锥体化或非典型键序的分子的研究。

引用次数: 0

Towards single-crystalline two-dimensional poly(arylene vinylene) covalent organic frameworks. 单晶二维聚（芳烯-乙烯烯）共价有机框架。

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-20 DOI: 10.1038/s41557-025-02048-8

Shaik Ghouse,Ziang Guo,Sergio Gámez-Valenzuela,David Mücke,Bowen Zhang,Lei Gao,Silvia Paasch,Yubin Fu,Chuanhui Huang,Chandrashekar Naisa,Eike Brunner,Mischa Bonn,M Carmen Ruiz Delgado,Junliang Sun,Ruqiang Zou,Ute Kaiser,Mingchao Wang,Xinliang Feng

Vinylene-linked two-dimensional (2D) conjugated covalent organic frameworks, or 2D poly(arylene vinylene)s (2D PAVs), are promising polymer semiconductors for (opto-)electronics, photocatalysis and electrochemistry. However, conventional solvothermal synthesis often produces 2D PAVs that are poorly crystalline or difficult to access. Here we introduce a Mannich-elimination strategy that converts 8 2D imine-covalent organic frameworks into 11 highly crystalline 2D PAVs though a reversible C=C bond formation mechanism enabling precise crystallization control. This versatile approach affords robust 2D PAVs with honeycomb, square or kagome lattices, specific surface area up to ∼2,000 m2 g-1 and lattice-mismatch tolerance up to 3.5%. High-resolution transmission electron microscopy and continuous rotation electron diffraction reveal molecular-level ordering in a 2-µm-sized triphenylbenzene-based single-crystalline 2D PAV. We demonstrate that crystallinity profoundly influences charge transport, with benzotrithiophene-based 2D PAVs exhibiting charge mobilities tenfold higher than their amorphous analogues or 2D polyimine precursors. This work establishes a general route to highly crystalline 2D conjugated polymer materials for robust applications.

乙烯连接的二维（2D）共轭共价有机框架，或2D聚（芳烯-乙烯）s (2D pav)，是很有前途的（光电）电子、光催化和电化学聚合物半导体。然而，传统的溶剂热合成通常会产生结晶性差或难以接近的2D pav。在这里，我们介绍了一种曼尼奇消除策略，通过可逆的C=C键形成机制将8个二维亚胺共价有机框架转化为11个高结晶的二维pav，从而实现精确的结晶控制。这种通用的方法提供了坚固的二维pav，具有蜂窝，方形或kagome晶格，比表面积高达~ 2,000 m2 g-1，晶格错配容忍度高达3.5%。高分辨率透射电子显微镜和连续旋转电子衍射揭示了2微米大小的三苯苯基单晶二维PAV的分子水平有序。我们证明了结晶度深刻地影响电荷传输，苯并三噻吩基二维pav的电荷迁移率比它们的无定形类似物或二维聚酰亚胺前体高十倍。这项工作为高结晶二维共轭聚合物材料的稳健应用建立了一条通用途径。

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引用次数: 0

Magnetism adds a dimension to ammonia oxidation electrocatalysts 磁性为氨氧化电催化剂增加了一个维度。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-20 DOI: 10.1038/s41557-025-02058-6

Simon K. Beaumont

Solid catalysts are typically optimized by changing their structure to control the strength of the adsorption bond. Now, magnetic spin-ordering offers an orthogonal energetic lever with which to enhance the otherwise sluggish kinetics of the ammonia oxidation reaction.

固体催化剂通常通过改变其结构来控制吸附键的强度来优化。现在，磁自旋排序提供了一个正交的能量杠杆，以提高其他缓慢的氨氧化反应动力学。

引用次数: 0

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