Nature chemistry最新文献

英文中文

Rethinking sustainable pathways for PFAS 重新思考PFAS的可持续发展路径。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-07 DOI: 10.1038/s41557-025-02044-y

He Xian, Xuemei Li, Cheng Zhang

引用次数: 0

Quantum quacks 量子的江湖郎中

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-06 DOI: 10.1038/s41557-025-02028-y

Michelle Francl

It is 100 years since the initial development of quantum mechanics, and not only did it bring with it a greater understanding of the world around us, it also introduced a new lexicon. Now, Michelle Francl wonders how the language of quantum mechanics has been flipped to the dark side and appropriated by pseudoscience.

自量子力学最初发展至今已有100年，它不仅使我们对周围的世界有了更深入的了解，而且还引入了一个新的词汇。现在，米歇尔·弗兰（Michelle Francl）想知道量子力学的语言是如何被翻转到黑暗的一面，并被伪科学所盗用的。

引用次数: 0

Two roads to lithium nucleation 锂成核有两条路

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-06 DOI: 10.1038/s41557-025-02023-3

Tao Gao, Yunan Qin

Lithium nucleation at the metal anode surface dictates the morphologies of lithium deposits, which impact battery stability and performances. Now, a physics-based framework decouples substrate- and solid-electrolyte interphase-controlled nucleation pathways by examining the interplay of short-range transport and reaction.

金属阳极表面的锂成核决定了锂沉积的形态，影响电池的稳定性和性能。现在，一个基于物理的框架通过检查短程传输和反应的相互作用来解耦基底和固体电解质间相控制的成核途径。

引用次数: 0

Stereoselective total synthesis of skew-tetramantane 斜四烷的立体选择性全合成

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-06 DOI: 10.1038/s41557-025-02026-0

Xiao-Yu Li, Christof Sparr

引用次数: 0

Sweet molecular containers 甜分子容器

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-06 DOI: 10.1038/s41557-025-02033-1

Sophie R. Beeren

Sophie Beeren discusses the development of cyclodextrins, moving from laboratory curiosities to common ingredients in daily products, active pharmaceutical ingredients and building blocks for supramolecular chemistry.

Sophie Beeren讨论了环糊精的发展，从实验室的好奇心到日常用品中的常见成分，活性药物成分和超分子化学的构建模块。

引用次数: 0

The catalytic enantioselective [1,2]-Wittig rearrangement cascade of allylic ethers 烯丙醚催化对映选择性[1,2]-Wittig重排级联

IF 21.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-06 DOI: 10.1038/s41557-025-02022-4

Tengfei Kang, Justin O’Yang, Kevin Kasten, Samuel S. Allsop, Toby Lewis-Atwell, Elliot H. E. Farrar, Martin Juhl, David B. Cordes, Aidan P. McKay, Matthew N. Grayson, Andrew D. Smith

The catalytic enantioselective [1,2]-Wittig rearrangement of allylic ethers constitutes a recognized synthetic challenge as it is traditionally considered to arise from a non-concerted reaction pathway via formation and recombination of radical pairs. Here we show a catalytic enantioselective solution to this challenge, demonstrating that [1,2]-Wittig products are generated via an alternative reaction cascade to traditional dogma. The developed process employs a chiral bifunctional iminophosphorane catalyst to promote an initial enantioselective [2,3]-sigmatropic rearrangement. A subsequent base-promoted, stereoconvergent, fragmentation–recombination process that proceeds with high enantiospecificity and retention of configuration, formally equivalent to a Woodward–Hoffmann forbidden thermal [1,3]-sigmatropic rearrangement, generates [1,2]-Wittig products in up to 97:3 enantiomeric ratio. Supported by extensive quantum chemistry calculations, this chirality transfer process will have broad implications for fundamental stereocontrol in organic transformations.

烯丙醚的催化对映选择性[1,2]-Wittig重排构成了公认的合成挑战，因为它传统上被认为是通过自由基对的形成和重组的非协调反应途径产生的。在这里，我们展示了一种催化对映选择性解决方案来应对这一挑战，证明[1,2]-Wittig产物是通过与传统的反应级联产生的。所开发的工艺采用手性双功能亚磷烷催化剂来促进初始的对映选择性[2,3]-符号重排。随后的碱基促进、立体收敛、片段-重组过程具有高对映体特异性和构型保留，形式上相当于Woodward-Hoffmann禁忌热[1,3]-符号重排，产生[1,2]-Wittig产物，对映体比例高达97:3。在大量量子化学计算的支持下，这种手性转移过程将对有机转化中的基本立体控制产生广泛的影响。

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引用次数: 0

Molecular systems engineering of synthetic cells 合成细胞的分子系统工程

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-06 DOI: 10.1038/s41557-025-02019-z

Marcus Fletcher, Bradley Diggines, Yuval Elani

Building synthetic versions of biological cells from the bottom up offers an unprecedented opportunity to understand the rules of life and harness cellular capabilities in biotechnology. Whereas substantial progress has been made in recapitulating elementary cell functions, we argue that accelerating the engineering of synthetic cells requires a shift in research practices. The dominant approach—rationally designing and integrating functional modules—becomes restrictive when dealing with the massively complex biochemical pathways associated with life, especially when design principles remain unclear. We advocate moving away from theoretical rational design towards a data-driven model that is centred on library generation. Inspired by a systems chemistry perspective, this strategy prioritizes the systematic creation and distribution of composition–function libraries. To enable this, experimental strategies must integrate high-throughput synthetic cell generation, automation and closed-feedback control of workflows. Broad adoption will also require greater emphasis on quantitative benchmarking, and the de-skilling of techniques, supporting effective laboratory-to-laboratory collaboration. Living cells rely on the choreography of multiple simultaneous functions, without clear boundaries between molecular subsystems. Replicating these capabilities in synthetic cells would represent a major advance in understanding life. This Perspective argues that this challenge requires a shift away from modular design concepts, towards a strategy that integrates the theoretical principles of systems chemistry with data-driven high-throughput experimental methods.

从下至上构建生物细胞的合成版本，为理解生命规律和利用生物技术中的细胞能力提供了前所未有的机会。尽管在概括基本细胞功能方面已经取得了实质性进展，但我们认为加速合成细胞的工程需要研究实践的转变。在处理与生命相关的大规模复杂生化途径时，尤其是在设计原则尚不明确的情况下，理性地设计和整合功能模块这一主流方法变得非常有限。我们提倡从理论上的理性设计转向以图书馆生成为中心的数据驱动模型。受系统化学观点的启发，该策略优先考虑组合函数库的系统创建和分布。为了实现这一点，实验策略必须集成高通量合成细胞生成、自动化和工作流程的封闭反馈控制。广泛采用还需要更加强调定量基准和技术去技能化，支持有效的实验室间合作。活细胞依赖于多种同步功能的编排，分子子系统之间没有明确的界限。在合成细胞中复制这些能力将代表着对生命理解的重大进步。这一观点认为，这一挑战需要从模块化设计概念转向将系统化学的理论原理与数据驱动的高通量实验方法相结合的策略。

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引用次数: 0

Intralayer bidentate diammoniums for stable two-dimensional perovskites 稳定二维钙钛矿的层内双齿金刚石。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-05 DOI: 10.1038/s41557-025-02038-w

Chenjian Lin, Yuanhao Tang, Zhichen Nian, Aidan H. Coffey, Yunfei Wang, Hanjun Yang, Pengfei Wu, Yu-Ting Yang, Syed Joy, Kenneth R. Graham, Wenzhan Xu, Chenhui Zhu, Brett M. Savoie, Letian Dou

Two-dimensional (2D) metal halide perovskites have attracted considerable attention for optoelectronic applications. Conventional 2D perovskites include Ruddlesden–Popper (R-P), Dion–Jacobson (D-J) and alternating cation phases. Here we introduce a class of 2D perovskite incorporating intralayer bidentate ligands, termed B-D phase perovskites, designed to enhance structural diversity and stability. We synthesized bidentate ligands with a rigid core unit and two ipsilateral ammonium-terminated linker groups, and obtained single crystals incorporating these B-D ligands with intralayer bidentate coordination. Molecular dynamics simulations reveal that the B-D ligand exhibits stronger binding energies to the inorganic layer compared with its R-P and D-J phase counterparts. Polycrystalline thin films of B-D phase showed superior thermal resistance, outperforming R-P and D-J phase analogues by 1,600% and 140% respectively, based on absorption stability assessments. Photovoltaic devices incorporating the B-D ligand exhibited higher power conversion efficiency and extended stability. These findings establish B-D phase 2D perovskites as a promising platform for next-generation optoelectronic applications, advancing ligand engineering for metal halide perovskites and other hybrid materials. Two-dimensional metal halide perovskites exhibit diverse structures, but tuning their intralayer structure is challenging. Now, ammonium-terminated bidentate linkers have been used to develop 2D perovskites. These materials exhibit superior thermal resistance and improved photovoltaic performance compared with their Ruddlesden–Popper and Dion–Jacobson counterparts.

二维（2D）金属卤化物钙钛矿在光电应用中引起了广泛的关注。传统的二维钙钛矿包括Ruddlesden-Popper （R-P）、Dion-Jacobson （D-J）和交替阳离子相。本文介绍了一类含有层内双齿配体的二维钙钛矿，称为B-D相钙钛矿，旨在增强结构的多样性和稳定性。我们合成了具有刚性核单元和两个同侧端氨连接基团的双齿配体，并获得了含有这些具有层内双齿配位的B-D配体的单晶。分子动力学模拟表明，与R-P和D-J相相比，B-D配体对无机层具有更强的结合能。根据吸收稳定性评估，B-D相的多晶薄膜表现出优异的耐热性，比R-P和D-J相的类似物分别高出1600%和140%。结合B-D配体的光伏器件表现出更高的功率转换效率和扩展的稳定性。这些发现确立了B-D相2D钙钛矿作为下一代光电应用的有前途的平台，推进了金属卤化物钙钛矿和其他杂化材料的配体工程。

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引用次数: 0

Direct enantioselective C(sp³)-H coupling of N-alkyl anilines via metallaphotoredox catalysis. 金属光氧化还原催化n -烷基苯胺的直接对映选择性C(sp3)-H偶联。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-05 DOI: 10.1038/s41557-025-02018-0

Weisai Zu, Xiang Wan, Haoran Wu, Jingwen Huo, Cankun Zhang, Chengyang Li, Yongliang Huang, Zhen Xu, Yumin Xu, Tao Li, Junliang Cheng, Jian-Liang Ye, Cheng Wang, Haohua Huo

Amine functionalization is crucial in pharmaceutical and agrochemical synthesis yet direct enantioselective α-C(sp³)-H functionalization of N-alkyl anilines remains challenging. Here we show a metallaphotoredox-catalysed radical approach for α-C(sp³)-H arylation of N-alkyl anilines, introducing a simple, sterically hindered aryl ketone photocatalyst. This key innovation slows undesired back-electron transfer, enabling efficient α-anilinoalkyl radical generation. Our strategy uses a sequential single-electron transfer and proton transfer process, thereby overcoming multiple limitations of existing methods. In conjunction with a chiral nickel catalyst, we have achieved site-selective, enantioselective arylation of diverse N-alkyl anilines with various (hetero)aryl halides. The method exhibits exceptional functional group tolerance, enabling modular functionalization of complex molecular structures. This approach provides an effective route to valuable α-aryl amines, offering significant possibilities for drug discovery and streamlining challenging synthetic sequences.

胺的功能化在医药和农化合成中至关重要，但n -烷基苯胺的直接对映选择性α-C(sp3)-H功能化仍然具有挑战性。在这里，我们展示了一种金属光氧化还原催化n -烷基苯胺α-C(sp3)-H芳基化的自由基方法，引入了一种简单的，位阻芳基酮光催化剂。这一关键创新减缓了不希望的反向电子转移，使α-苯胺烷基自由基的高效生成成为可能。我们的策略使用顺序的单电子转移和质子转移过程，从而克服了现有方法的多重局限性。结合手性镍催化剂，我们已经实现了不同n -烷基苯胺与不同（杂）芳基卤化物的位置选择性，对映选择性芳基化。该方法表现出特殊的官能团耐受性，使复杂分子结构的模块化功能化成为可能。这种方法为α-芳基胺提供了有效的途径，为药物发现和简化具有挑战性的合成序列提供了重要的可能性。

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引用次数: 0

Unravelling gas evolution mechanisms in battery electrode materials. 解开电池电极材料中的气体演化机制。

IF 20.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry

Pub Date : 2026-01-05 DOI: 10.1038/s41557-025-02016-2

Wentao Wang, Weihong Li, Fengjiao Yu, Qihao Pu, Jinguo Miao, Shaojie Han, Yuping Wu, Liwei Chen, Yanbin Shen, Yuhui Chen

LiFe_xMn₁_-xPO₄ positive electrode materials show significant potential for enhancing battery safety, power density and cost-effectiveness. However, gas evolution shortens the cyclability and raises additional safety concerns, presenting a major challenge. The gas evolution mechanisms in LiFe_xMn₁_-xPO₄ batteries are poorly understood, impeding the material improvement efforts. Here we examine a LiFe_xMn₁_-xPO₄-graphite full cell, simultaneously quantifying and probing gas evolution from positive and negative electrodes. We found over 90% of the evolved gas was composed of CO₂ and H₂. CO₂ originated from side reactions at LiFe_xMn₁_-xPO₄, with almost equal contributions from electrochemical and chemical pathways. H₂ resulted from chemical side reactions at the graphite's solid-electrolyte interface and was closely associated with the dissolution of Mn/Fe ions from the LiFe_xMn₁_-xPO₄. We developed a LiFe_xMn₁_-xPO₄ with a dense carbon layer coating, which inhibited metal ion dissolution by an order of magnitude and minimized side reactions at both electrodes. A 4.1-Ah pouch cell exhibited stable performance over 540 cycles with over 90% capacity retention.

LiFexMn1-xPO4正极材料在提高电池安全性、功率密度和成本效益方面具有重要的潜力。然而，气体的演化缩短了循环性，并引发了额外的安全问题，这是一个重大挑战。人们对LiFexMn1-xPO4电池中的气体演化机制知之甚少，这阻碍了材料的改进工作。在这里，我们研究了lifexmn1 - xpo4 -石墨全电池，同时定量和探测了正负极的气体演化。我们发现超过90%的气体是由CO2和H2组成的。CO2来源于LiFexMn1-xPO4的副反应，电化学和化学途径的贡献几乎相等。H2由石墨固电解质界面的化学副反应产生，并与LiFexMn1-xPO4中Mn/Fe离子的溶解密切相关。我们开发了一种具有致密碳层涂层的LiFexMn1-xPO4，它可以在两个电极上抑制金属离子的溶解，并最小化副反应。4.1 ah的袋状电池在540次循环中表现出稳定的性能，容量保持率超过90%。

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