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Aqueous polycavity hosts composed of porous aromatic polymers within aromatic micelles 由芳香胶束内的多孔芳香聚合物组成的水性多腔宿主

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102616

Shinji Aoyama , Lorenzo Catti , Michito Yoshizawa

Porous aromatic/polyaromatic polymers (PAPs) have been widely investigated as polycavity materials, featuring infinite grid frameworks with high stability. However, in contrast to host-guest functions in mono/oligocavities, the applications of these polycavities remained largely limited, owing to the complete insolubility, ill-defined structures, and inseparability. Here, we report a general strategy for the facile preparation of aqueous polycavity hosts through uptake of insoluble PAPs within aromatic micelles in water. The obtained aqueous host-guest composites, e.g., including a pyrene-benzene-based PAP, are analyzed via solution/solid-state techniques, revealing roughly spherical ∼100 nm-sized particles. The giant composites can be easily size fractionated in a highly monodisperse fashion using a centrifugation-filtration protocol. Importantly, the water-soluble polycavities of the PAPs within the micelle provide cavity-dependent incorporation abilities toward hydrocarbons, accompanying large emission enhancement (up to ∼9-fold) of the semi-rigid polycavities. Medium-sized dyes and hydrocarbons are furthermore co-incorporated into the polycavities, yielding unusual quaternary host-guest composites with enhanced dye-based emission.

多孔芳香族/聚芳香族聚合物（PAPs）作为一种具有高稳定性的无限网格结构的多腔材料得到了广泛的研究。然而，与单/少空腔中的主客体函数相比，由于完全不溶性、结构不明确和不可分离性，这些多空腔的应用仍然很大程度上受到限制。在这里，我们报告了一种通过在水中的芳香胶束中吸收不溶性pap来制备水性多腔寄主的一般策略。通过溶液/固态技术分析获得的水性主客体复合材料，例如，包括芘基PAP，揭示了大约球形~ 100纳米大小的颗粒。这种巨大的复合材料可以很容易地以高度单分散的方式使用离心过滤方案进行尺寸分馏。重要的是，胶束内聚丙烯酰胺的水溶性多腔提供了对碳氢化合物的空腔依赖的结合能力，伴随着半刚性多腔的大发射增强（高达9倍）。中等染料和碳氢化合物进一步结合到多腔中，产生不同寻常的第四季主客体复合材料，增强了染料基发射。

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引用次数: 0

Robust light-harvesting properties upon low-light acclimation in purple bacteria 紫色细菌在弱光驯化过程中强健的光收集特性

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102597

Dihao Wang , Dvir Harris , Chern Chuang , Graham P. Schmidt , Olivia C. Fiebig , Gabriela S. Schlau-Cohen

Purple bacteria convert solar energy into biochemical energy with high quantum efficiency across diverse environments. Under low light, many species increase the number of antenna complexes and replace their primary light-harvesting complex 2 (LH2) with a blue-shifted variant, LH3. The structural basis of the blue shift and its influence on the dynamics of solar energy conversion have remained unclear. Here, we integrated cryogenic electron microscopy, ultrafast spectroscopy, and quantum dynamics simulations to compare LH2 and LH3 from Rhodoblastus acidophilus strain 7750. Our analyses revealed that hydrogen bonding dynamically tunes the transition energy, introducing a previously unreported excitation energy equilibrium between bacteriochlorophyll rings in LH3. This energy redistribution opened new inter-complex pathways, enabling 68% faster energy transport to maintain high conversion efficiency even with the larger antenna. Collectively, these results establish structural modifications as a tunable knob to optimize both absorption and transport for robust light harvesting under fluctuating conditions.

紫色细菌在不同环境下以高量子效率将太阳能转化为生物化学能。在弱光条件下，许多物种增加天线复合物的数量，并用蓝移变体LH3取代其主要的光收集复合物2 （LH2）。蓝移的结构基础及其对太阳能转换动力学的影响尚不清楚。本文采用低温电镜、超快光谱、量子动力学模拟等方法对嗜酸Rhodoblastus acidophilus菌株7750的LH2和LH3进行了比较。我们的分析表明，氢键动态地调节了跃迁能量，在LH3中引入了以前未报道的细菌叶绿素环之间的激发能平衡。这种能量再分配开辟了新的复杂通道，使能量传输速度提高68%，即使使用更大的天线也能保持较高的转换效率。总的来说，这些结果建立了结构修改作为一个可调旋钮，以优化吸收和传输，在波动条件下实现强大的光收集。

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引用次数: 0

Anisotropic node distortions in amorphous MOFs: Low-valent Zr sites as catalytic hotspots 非晶mof的各向异性节点畸变：低价Zr位点作为催化热点

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102619

Till Schertenleib , Mehrdad Asgari , Beatriz Mouriño , Vikram V. Karve , Timo M.O. Felder , Dragos Stoian , Volodymyr Bon , Jian Hao , Andres Ortega-Guerrero , Emad Oveisi , Kumar Varoon Agrawal , Berend Smit , Stefan Kaskel , Simon J.L. Billinge , Wendy L. Queen

We introduce a new approach to defect engineering in Zr-based metal-organic frameworks (Zr-MOFs), aiming to reduce Zr site valency while preserving high node connectivity. Using a rapid heat treatment (RHT) in humid air, oxygen vacancies (O-vacancies) were created in Dresden University of Technology (DUT)-67 through cluster dehydration. Unlike conventional defect engineering, aimed at creating missing-linker defects, this method breaks intra-cluster Zr-

μ_{3}

O–Zr bonds, generating coordinatively unsaturated Zr (Zr_cus) sites. Pair distribution function (PDF) analysis, X-ray absorption spectroscopy (XAS), and density functional theory (DFT) calculations reveal that the O-vacancies lead to symmetry breaking, irreversible node distortions, and framework amorphization. This treatment converts 50% of metal sites to Zr_cus sites, nearly doubling the catalytic activity of DUT-67 in glyoxal conversion to glycolic acid. DFT modeling and in situ PDF analysis highlight the dynamic behavior of Zr clusters under reaction conditions, suggesting a new avenue for defect engineering in Zr-MOFs to enhance catalytic performance.

我们介绍了一种新的Zr基金属有机框架（Zr- mofs）缺陷工程方法，旨在降低Zr位点价的同时保持高节点连通性。在德累斯顿工业大学(DUT)-67中，使用潮湿空气中的快速热处理（RHT），通过簇脱水产生氧空位（o -空位）。与传统缺陷工程不同的是，该方法破坏了簇内Zr-μ3μ 30 - Zr键，生成了协调不饱和Zr （Zrcus）位点。对分布函数（PDF）分析、x射线吸收光谱（XAS）和密度泛函理论（DFT）计算表明，o空位导致对称破缺、不可逆节点畸变和框架非晶化。该处理将50%的金属位点转化为Zrcus位点，将DUT-67在乙二醛转化为乙醇酸的催化活性提高了近一倍。DFT建模和原位PDF分析突出了Zr簇在反应条件下的动态行为，为Zr- mof缺陷工程提高催化性能提供了新的途径。

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引用次数: 0

Manipulation of intramolecular charge transfer in NIR-II emissive organic diradicaloids via a symmetry-breaking design 通过对称破缺设计操纵NIR-II发射有机二根碱分子内电荷转移

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102659

Tingting Huang, Kun Yang, Wei Hu, Lina Feng, Zipeng Wu, Hui Chen, Jianguo Wang, Zebing Zeng

引用次数: 0

Untapped defect-engineering strategy: Cluster dehydroxylation of zirconium-based MOFs 未开发缺陷工程策略：锆基mof的簇脱羟基化

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102823

Bayu I.Z. Ahmad , Phillip J. Milner

In this issue of Chem, Queen and co-workers introduce cluster dehydroxylation by using rapid heat treatment as a new defect-engineering strategy in zirconium-based frameworks. They thoroughly characterize the oxygen-vacancy nature of the defect, primarily by pair distribution function (PDF) analysis. Dehydrated DUT-67 exhibited double the catalytic activity for glyoxal hydration of the pristine material.

在这一期的Chem中，Queen及其同事介绍了通过快速热处理将簇脱羟基化作为锆基框架中新的缺陷工程策略。他们主要通过对分布函数（PDF）分析彻底地表征了缺陷的氧空位性质。脱水后的DUT-67对乙二醛水化的催化活性是原始材料的两倍。

引用次数: 0

Intelligent column chromatography prediction model based on automation and machine learning 基于自动化和机器学习的智能色谱柱预测模型

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102598

Wenchao Wu , Hao Xu , Yang Xu , Peijie Luo , Qingrui Zeng , Yuntian Chen , Yan Xu , Dongxiao Zhang , Fanyang Mo

Efficient compound separation remains a persistent challenge in synthetic chemistry, with column chromatography serving as a critical purification tool. Traditional methods require extensive expertise and repetitive labor—areas where AI offers significant advantages. This study introduces an AI-driven platform to automate data collection and optimize separation processes. By leveraging deep learning, the system predicts key separation parameters, while transfer learning enables adaptation to diverse column specifications. A novel metric, separation probability

(S_{p})

, quantifies the likelihood of successful component isolation and has been experimentally validated. The approach enhances precision, reduces manual intervention, and expands the scope of chromatographic applications, offering a more efficient and scalable solution for chemical purification.

在合成化学中，高效化合物分离一直是一个挑战，柱层析是一种重要的纯化工具。传统的方法需要广泛的专业知识和重复的劳动——在这些领域，人工智能提供了显著的优势。本研究介绍了一个人工智能驱动的平台，用于自动化数据收集和优化分离过程。通过利用深度学习，系统可以预测关键的分离参数，而迁移学习可以适应不同的柱规格。一种新的度量，分离概率SpSp，量化了成功分离组分的可能性，并得到了实验验证。该方法提高了精度，减少了人工干预，扩大了色谱应用范围，为化学净化提供了更有效和可扩展的解决方案。

引用次数: 0

Chemical reactions in lithium-sulfur batteries 锂硫电池中的化学反应

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102629

Yufeng Luo , Zijian Zheng

The sulfur redox pathways in lithium-sulfur (Li-S) batteries involve an intricate 16-electron conversion process featuring multiple polysulfide intermediates. These polysulfides show high solubility and reactivity in ether-based electrolytes, leading to complex electrochemical and chemical reaction branches. Unlike the much-discussed electrochemical reactions, chemical reactions associated with polysulfides have been largely overlooked in the literature. Herein, we comprehensively summarize these polysulfide-associated chemical reactions with different components in Li-S batteries and discuss their crucial impacts on electrochemical performance. We also propose several notable scientific challenges from the perspective of chemical reactions in practical Li-S batteries and outline feasible strategies to address them for future research.

锂硫（li -硫）电池中的硫氧化还原途径涉及一个复杂的16电子转换过程，其中包含多个多硫化物中间体。这些多硫化物在醚基电解质中具有很高的溶解度和反应活性，导致复杂的电化学和化学反应分支。与被广泛讨论的电化学反应不同，与多硫化物相关的化学反应在文献中很大程度上被忽视了。在此，我们全面总结了Li-S电池中不同组分与多硫化物相关的化学反应，并讨论了它们对电化学性能的重要影响。我们还从实际Li-S电池的化学反应角度提出了几个值得注意的科学挑战，并概述了解决这些挑战的可行策略，以供未来的研究。

引用次数: 0

Divergent scaffold redesign of ecteinascidin 743 as a gateway to anticancer macrocycles ecteinascidin 743作为抗癌大周期通道的发散支架重新设计

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102815

Sihyeong Yi , Ji Hyae Lee , Seung Bum Park

Optimizing natural products for drug discovery remains vital yet challenging. In this issue of Chem, Oguri and co-workers apply a divergent synthetic strategy to redesign the scaffold of the anticancer drug ecteinascidin 743, generating 14- to 17-membered macrocycles with shifted bridgehead connectivity. These analogs preserve the core pharmacophore, expand structural space, and fine-tune DNA alkylation and anticancer potency, offering new strategies for natural product-inspired therapeutics.

优化天然产物的药物发现仍然是至关重要的，但具有挑战性。在这一期的《化学》杂志上，Oguri及其同事采用了一种不同的合成策略来重新设计抗癌药物ecteinascidin 743的支架，生成了具有移位桥头堡连接的14到17个成员的大环。这些类似物保留了核心药效团，扩展了结构空间，微调了DNA烷基化和抗癌效力，为天然产物启发的治疗提供了新的策略。

引用次数: 0

Enhancing multi-carbon product formation by increasing water disordering 通过增加水的无序性来促进多碳产物的形成

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102826

Alexis Grimaud

Enhancing the selectivity of carbon monoxide reduction toward multi-carbon products poses a significant challenge. Now, writing in Nature Chemistry, Zhang and colleagues demonstrate that high ionic strength significantly improves C–C coupling by decreasing water ordering on the surface of copper catalysts and thus achieves more than 90% Faradaic efficiency toward multi-carbon products.

提高一氧化碳对多碳产物的还原选择性是一个重大的挑战。现在，在《自然化学》杂志上，Zhang和他的同事们证明，高离子强度通过降低铜催化剂表面的水有序度，显著改善了C-C耦合，从而实现了90%以上的多碳产物的法拉第效率。

引用次数: 0

Abiotic aldol reactions of formaldehyde with ketoses and aldoses—Implications for the prebiotic synthesis of sugars by the formose reaction 甲醛与酮糖和醛糖的非生物醛醇反应——通过甲醛反应合成糖的益生元意义

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-11-13 DOI: 10.1016/j.chempr.2025.102553

Scot M. Sutton , Sunil Pulletikurti , Huacan Lin , Ramanarayanan Krishnamurthy , Charles L. Liotta

The aldol reactions of formaldehyde is the essence of the formose reaction, considered the leading prebiotic pathway for accessing sugars on the early Earth. However, the formose reaction produces an intractable mixture, and efforts to tame the reaction to selectively and efficiently form aldose sugars have been unsuccessful. We have undertaken an NMR-mechanistic study of the aldol reactions of excess formaldehyde with glycolaldehyde, dihydroxyacetone, erythrulose, and erythrose under mild conditions and show that the reaction pathway is dominated by the formation linear ketoses and eventual accumulation of branched ketoses. Formation of C4 and higher aldo-sugars were not observed, implying that neither carbonyl migrations nor retroaldol reactions are occurring. Our results suggest that (1) controlling the aldol reaction of formaldehyde to selectively produce linear aldoses appears unfeasible; and (2) the concept of the formose reaction as a prebiotic source of ribose on early Earth needs serious reconsideration, and other models/options should be explored.

甲醛的醛醇反应是福尔摩斯反应的本质，福尔摩斯反应被认为是早期地球上获取糖的主要益生元途径。然而，福尔摩斯反应产生一种难以处理的混合物，并且努力驯服反应选择性地和有效地形成醛糖糖一直是不成功的。我们在温和条件下对过量甲醛与乙醇醛、二羟基丙酮、赤己糖和红细胞的醛醇反应进行了核磁共振机制研究，结果表明，反应途径主要是线性酮糖的形成和支链酮糖的最终积累。没有观察到C4和高级醛糖的形成，这意味着既没有羰基迁移也没有发生后醛醇反应。我们的研究结果表明：(1)控制甲醛的醛醇反应选择性地产生线性醛糖似乎不可行；(2)福尔摩斯反应作为地球早期核糖的益生元来源的概念需要认真考虑，并应探索其他模型/选择。

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引用次数: 0

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