Nature synthesis最新文献_第3页

Generating reliable and reproducible data for reusable quantum chemical reaction free-energy profiles 为可重复使用的量子化学反应自由能谱生成可靠和可重复的数据

IF 2

Nature synthesis Pub Date : 2025-07-28 DOI: 10.1038/s44160-025-00838-z

Maren Podewitz

{"title":"Generating reliable and reproducible data for reusable quantum chemical reaction free-energy profiles","authors":"Maren Podewitz","doi":"10.1038/s44160-025-00838-z","DOIUrl":"10.1038/s44160-025-00838-z","url":null,"abstract":"Computational exploration of reaction mechanisms to support and guide experimental efforts has become a key tool in organic and inorganic chemistry. Here, key challenges and best practices for generating reliable, reproducible and reusable data for quantum chemical calculations of reaction free-energy profiles are addressed. By examining critical factors, such as the choice of computational and chemical model, and addressing common sources of errors due to shortcomings of the employed (standard) methodology, the author provides guidance for increasing the reliability of reported computational results. Best practices for data reporting and data accessibility are discussed, and emphasis is placed on supporting researchers who use computational methods to interpret experimental results and guide synthetic efforts. This Perspective also highlights practical recommendations and technical solutions to improve data reuse and foster advancements in organic and inorganic molecular chemistry. The guidance of experimental studies with computational exploration of reaction mechanisms has become a key tool in chemistry. This Perspective highlights challenges and best practices for generating reliable, reproducible and reusable data for quantum chemical calculations of reaction free-energy profiles.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 8","pages":"913-921"},"PeriodicalIF":20.0,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pushing the bounds for metal alloys 推动金属合金的发展

IF 2

Nature synthesis Pub Date : 2025-07-28 DOI: 10.1038/s44160-025-00862-z

Yanfei Zhu

引用次数: 0

Pyrroles to pyridines 吡咯变成吡啶

IF 2

Nature synthesis Pub Date : 2025-07-28 DOI: 10.1038/s44160-025-00856-x

Peter W. Seavill

引用次数: 0

Base-promoted azaarene and polyazaarene synthesis through C–C bond cleavage and alkyl transfer 通过C-C键裂解和烷基转移，碱促进氮扎芳烃和聚氮扎芳烃的合成

IF 2

Nature synthesis Pub Date : 2025-07-17 DOI: 10.1038/s44160-025-00833-4

Yong-Ze Chen, Xiang-Huan Shan, Bo Yang, Lin Tie, Yu Liu, Jia-Le Fu, Jian-Ping Qu, Yan-Biao Kang

{"title":"Base-promoted azaarene and polyazaarene synthesis through C–C bond cleavage and alkyl transfer","authors":"Yong-Ze Chen, Xiang-Huan Shan, Bo Yang, Lin Tie, Yu Liu, Jia-Le Fu, Jian-Ping Qu, Yan-Biao Kang","doi":"10.1038/s44160-025-00833-4","DOIUrl":"10.1038/s44160-025-00833-4","url":null,"abstract":"Multisubstituted azaarenes and conjugated polyazaarenes are important heterocycles in chemistry and materials science. Here we report the discovery of a carbon–carbon bond cleavage and alkyl transfer approach for the synthesis of azaarenes or conjugated polyazaarenes, which is promoted by potassium tert-butoxide. Neither precious-metal catalysts nor directing groups are required. This strategy is enabled by an alkyl transfer, releasing aryl methanes, such as toluene, as the only by-product. This general and versatile method enables the divergent synthesis of a variety of highly functionalized azaarenes and polyazaarenes. In addition, several azaarenes were found to have visible-light photocatalytic reactivities. Potassium tert-butoxide is used in a precious-metal-free alkyl transfer strategy for synthesizing azaarenes and polyazaarenes from alkenes and nitriles via carbon–carbon bond cleavage. This method produces aryl methanes as the sole by-product and allows divergent synthesis of functionalized azaarenes, some of which exhibit visible-light photocatalytic reactivity.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 10","pages":"1288-1296"},"PeriodicalIF":20.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145256865","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Strain-dependent enantioselectivity in mechanochemically coupled catalytic hydrogenation 机械化学耦合催化加氢中菌株依赖的对映体选择性

IF 2

Nature synthesis Pub Date : 2025-07-17 DOI: 10.1038/s44160-025-00839-y

Xujun Zheng, Chun-Yu Chiou, Robert T. O’Neill, Chenghao Duan, Yichen Yu, Jack Malek, Nelson A. Rivera Jr, Roman Boulatov, Stephen L. Craig, Ross A. Widenhoefer

{"title":"Strain-dependent enantioselectivity in mechanochemically coupled catalytic hydrogenation","authors":"Xujun Zheng, Chun-Yu Chiou, Robert T. O’Neill, Chenghao Duan, Yichen Yu, Jack Malek, Nelson A. Rivera Jr, Roman Boulatov, Stephen L. Craig, Ross A. Widenhoefer","doi":"10.1038/s44160-025-00839-y","DOIUrl":"10.1038/s44160-025-00839-y","url":null,"abstract":"The ultimate realization of top-down atomic manipulation is to push or pull molecules in a way that changes their function, such as catalysis. The forces in a stretched polymer distort molecular conformation in ways that couple to reactivity, but the use of this type of polymer mechanochemistry to bias the outcome of a reaction has been limited to stoichiometric reactions. Here we demonstrate that the selectivity of a catalytic site can be manipulated by straining a polymer support to which the catalyst is covalently bound. The enantiomeric ratio of the products of the hydrogenation of a series of 2-acetamidoacrylates by a bisphosphine rhodium catalyst increases with macroscopic strain, reaching up to twice its initial value when the support is compressed by 73% in a single dimension. Reactivity reverts upon relaxing support. Control experiments, structure–activity studies using strained macrocycles, and computations support mechanochemical coupling as the dominant cause of the improved selectivity and suggest that larger effects are possible with advances controlling the molecular topology of the supporting network. The selectivity of a catalytic reaction is manipulated by straining a polymer support to which the catalyst is covalently bound. Enantioselective rhodium-catalysed hydrogenation of a series of 2-acetamidoacrylates is shown to increase with macroscopic strain, with enantiomeric ratios reaching twice their initial values.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 10","pages":"1319-1328"},"PeriodicalIF":20.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s44160-025-00839-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145256862","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Building complex biochemicals from one-carbon compounds 从单碳化合物中构建复杂的生物化学物质

IF 2

Nature synthesis Pub Date : 2025-07-08 DOI: 10.1038/s44160-025-00835-2

Blake J. Rasor, Simone Giaveri, Andreas M. Küffner, Tobias J. Erb

{"title":"Building complex biochemicals from one-carbon compounds","authors":"Blake J. Rasor, Simone Giaveri, Andreas M. Küffner, Tobias J. Erb","doi":"10.1038/s44160-025-00835-2","DOIUrl":"10.1038/s44160-025-00835-2","url":null,"abstract":"Life—ranging from cellular processes to the complexities of modern societies—requires a diverse array of chemicals to function. Whereas humans have become adept at synthesizing incredible chemical diversity over the past two centuries, these practices still rely on the use (and breakdown) of fossil resources. However, the challenge of climate change makes it clear that sustainable chemical synthesis requires alternative methods and substrates. The growing abundance of carbonaceous gases in the atmosphere (in particular, carbon dioxide and methane) could serve as feedstocks for such a sustainable synthesis transition, and biological systems are adept at converting one-carbon (C1) compounds into more complex molecules. This Review discusses recent developments and future opportunities for the biosynthesis of chemicals from C1 substrates via cellular and cell-free systems. In addition to the diverse range of products synthesized using natural or designed C1 conversion pathways in vivo or in vitro, we discuss the benefits of spatio-temporal organization and hybrid catalysis to increase the efficiency of enzymatic chemical synthesis from C1 substrates. One-carbon compounds, including carbon dioxide and methane, represent a sustainable resource for chemical conversions. This Review highlights recent advances in the biochemical upgrading of one-carbon substrates to value-added products using a combination of cellular, cell-free and abiotic catalysis strategies.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 7","pages":"787-798"},"PeriodicalIF":20.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123083","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Topochemical exfoliation of metal oxyhydroxides for the electrolytic oxygen evolution reaction 电解析氧反应中金属氢氧化物的拓扑化学剥离

IF 2

Nature synthesis Pub Date : 2025-07-07 DOI: 10.1038/s44160-025-00837-0

Sihong Wang, Qu Jiang, Chuan Hu, Haoyue Zhang, Ruohan Feng, Chaoran Zhang, Chia-Shuo Hsu, Cuiping Guo, Hao Ming Chen, Young Moo Lee, Di Zhang, Fang Song

{"title":"Topochemical exfoliation of metal oxyhydroxides for the electrolytic oxygen evolution reaction","authors":"Sihong Wang, Qu Jiang, Chuan Hu, Haoyue Zhang, Ruohan Feng, Chaoran Zhang, Chia-Shuo Hsu, Cuiping Guo, Hao Ming Chen, Young Moo Lee, Di Zhang, Fang Song","doi":"10.1038/s44160-025-00837-0","DOIUrl":"10.1038/s44160-025-00837-0","url":null,"abstract":"Thin nanosheets of metal oxyhydroxides (MOOHs) are promising for a range of applications, including electronics, optics, electrochemistry and catalysis. However, their synthesis remains challenging. Here we address this by introducing a topochemical oxidizing approach that enables the production of stable aqueous colloids of four different MOOH nanosheets. Chemically implanted active oxygen species are shown to facilitate the exfoliation of bulk MOOHs with an efficiency strongly dependent on their abundance. Spectroscopic analysis combined with theoretical calculations reveals that alkali cations stabilize negatively charged active oxygen species through electrostatic interactions, regulating the repulsive forces between the layers, and thereby facilitating effective exfoliation. As-produced Cs+-CoFeOOH nanosheets have high electrocatalytic performances for the oxygen evolution reaction, achieving 1 A cm−2 at a cell voltage of 1.62 V in an anion-exchange membrane water electrolyser. This work presents an alternative strategy for exfoliating MOOHs and may open new avenues for fabricating two-dimensional materials from delamination-resistant layered compounds. A topochemical oxidation process is developed to exfoliate metal oxyhydroxides, in which active oxygen species and alkali cations modulate interlayer repulsion. The resulting Cs⁺-CoFeOOH nanosheets demonstrate exceptional electrocatalytic performance for the oxygen evolution reaction.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 10","pages":"1308-1318"},"PeriodicalIF":20.0,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145256849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Supramolecular templating for two-dimensional crystalline polymers with mechanical bonds 具有机械键的二维结晶聚合物的超分子模板

IF 2

Nature synthesis Pub Date : 2025-07-04 DOI: 10.1038/s44160-025-00832-5

Dejing Xu, Yuping Wang

引用次数: 0

Gram-per-litre-scale production of lutein by engineered Corynebacterium 利用工程棒状杆菌生产每升克的叶黄素

IF 2

Nature synthesis Pub Date : 2025-07-04 DOI: 10.1038/s44160-025-00826-3

Hyunmin Eun, Cindy Pricilia Surya Prabowo, Sang Yup Lee

{"title":"Gram-per-litre-scale production of lutein by engineered Corynebacterium","authors":"Hyunmin Eun, Cindy Pricilia Surya Prabowo, Sang Yup Lee","doi":"10.1038/s44160-025-00826-3","DOIUrl":"10.1038/s44160-025-00826-3","url":null,"abstract":"Lutein is commonly used as a supplement for ocular health. However, commercial lutein is mainly extracted from marigold flowers, an inefficient process that includes secondary metabolites. Here, building on our previous research on lutein synthesis in engineered Escherichia coli, we report the development of a microbial platform for efficient lutein production using metabolically engineered Corynebacterium glutamicum. We engineered C. glutamicum to produce lycopene and introduced the lutein biosynthesis pathway. Then, we substantially enhanced lutein production by optimizing the haem pathway, engineering the P450 reductase and utilizing an optimal electron-channelling scaffold system to improve electron transfer reactions, addressing the rate-limiting steps in lutein synthesis. This approach achieved a substantial increase in lutein production, reaching a concentration of 1.78 g l−1, with a content of 19.51 mg per gram dry cell weight and a productivity of 32.88 mg l−1 h−1 in fed-batch fermentation. This approach allows gram-per-litre-scale microbial production of lutein. Commercial lutein is mainly extracted from marigold flowers, which is an inefficient process. Now a gram-per-litre-scale process for microbial production of lutein is reported using metabolically engineered Corynebacterium glutamicum. By integrating flux optimization, engineered cytochrome P450 enzymes, electron-channelling scaffolds and fermentation strategies, this approach provides a microbial platform for lutein biosynthesis.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 10","pages":"1200-1211"},"PeriodicalIF":20.0,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145256861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tunable porosity in 3D bioprinting 3D生物打印中的可调孔隙度

IF 2

Nature synthesis Pub Date : 2025-07-03 DOI: 10.1038/s44160-025-00848-x

Johannes Kreutzer

引用次数: 0