Nature synthesis最新文献

Modular assembly of bioisosteric bridged aza-frameworks via ring strain release 通过环应变释放的生物等构桥aza框架的模块化组装

Nature synthesis Pub Date : 2026-09-02 DOI: 10.1038/s44160-026-01149-7

Haotian Jiang,Yuxia Dai,Kai Tang,Bo Pan,Hongming Jin,Xiangyang Chen,Yangyang Yang

引用次数: 0

Author Correction: Accelerating synthesis at scale requires a coordinated ecosystem 作者更正：加速大规模合成需要一个协调的生态系统

Nature synthesis Pub Date : 2026-09-02 DOI: 10.1038/s44160-026-01165-7

Brandon R. Sutherland,Varinia Bernales,Alán Aspuru-Guzik

引用次数: 0

Conductive three-dimensional molecular-cluster networks via rare-earth-directed assembly 通过稀土定向组装的导电三维分子簇网络

Nature synthesis Pub Date : 2026-08-26 DOI: 10.1038/s44160-026-01138-w

Zhihao Lu, Qingshun Fan, Song Lin, Cuiming Ren, Changdong Liu, Mingbu Luo, Lehua Zhang, Li Xu, Wei-Hui Fang

{"title":"Conductive three-dimensional molecular-cluster networks via rare-earth-directed assembly","authors":"Zhihao Lu, Qingshun Fan, Song Lin, Cuiming Ren, Changdong Liu, Mingbu Luo, Lehua Zhang, Li Xu, Wei-Hui Fang","doi":"10.1038/s44160-026-01138-w","DOIUrl":"https://doi.org/10.1038/s44160-026-01138-w","url":null,"abstract":"Molecular-based crystalline conductors provide well-defined structural platforms for probing how molecular arrangements govern electronic properties, yet conventional zero-dimensional cluster materials generally exhibit low conductivity owing to the difficulty of establishing efficient conductive networks within isolated systems. Here we show that electron-rich dimeric molecular conductors are constructed by introducing the quasi-aromatic metal-cluster building blocks {MoIV3-py3} (where py represents pyridine) as stereogenic units and encapsulating rare-earth ions. This design enables the formation of d–π···π–d conjugated conductive pathways between isolated clusters. Among the systems studied, hexagonal phases incorporating Sm and Eu exhibit the shortest π···π distance (3.66 Å) and the highest in-plane conductivity (approximately 3 × 10−5 S m−1), over 105× higher than conventional polyoxometalates. Rare-earth incorporation promotes the formation of a semiconducting hexagonal phase and a metallic-like tetragonal phase, while also enabling the modulation of anisotropic charge transport in single crystals. This work not only extends the application of rare-earth elements beyond their conventional roles in magnetism, luminescence and catalysis but also provides a rational design strategy for the tailored construction of cluster-based crystalline materials with targeted electronic properties.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"489 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148853555","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

Access to all stereoisomers of chiral alcohols with multiple stereocentres enabled by machine learning-empowered protein engineering 通过机器学习的蛋白质工程，获得具有多个立体中心的手性醇的所有立体异构体

Nature synthesis Pub Date : 2026-08-21 DOI: 10.1038/s44160-026-01144-y

Zhenyu Lu, Jiahui Zhou, Tao Han, Zhaoyuan Zhang, Weihua Xu, Yixin Cen, Cheng Jiang, Jingxin Zhang, Yue Guo, Chunyang Cao, Meilan Huang, Qi Wu

{"title":"Access to all stereoisomers of chiral alcohols with multiple stereocentres enabled by machine learning-empowered protein engineering","authors":"Zhenyu Lu, Jiahui Zhou, Tao Han, Zhaoyuan Zhang, Weihua Xu, Yixin Cen, Cheng Jiang, Jingxin Zhang, Yue Guo, Chunyang Cao, Meilan Huang, Qi Wu","doi":"10.1038/s44160-026-01144-y","DOIUrl":"https://doi.org/10.1038/s44160-026-01144-y","url":null,"abstract":"Stereodivergent evolution of a single enzyme into a complete set of stereocomplementary variants capable of accessing all stereoisomers of products bearing three or more newly formed stereocentres remains a major challenge in biosynthesis and protein engineering. Achieving this goal requires precise modification of the enzyme’s active site to impart the subtle differences that govern different stereoselectivities. In addition, screening the vast number of variants in such a complicated evolution task represents another substantial bottleneck. Here we present a stereodivergent evolution of alcohol dehydrogenase from Lactobacillus brevis into a set of stereocomplementary variants that allow access to all eight possible alcohol product isomers bearing multiple stereocentres from the asymmetric reduction of 2,2-disubstituted cyclodiketones. A hybrid rational design–machine learning framework (BioStrucTag) was used, which captures the structural features of the pre-organized catalytic pockets specific for certain chiral products via three-dimensional voxel grid representation of ligand–enzyme complexes. In addition, this framework integrates the enzyme’s sequence features obtained from a transformer-based language model, therefore enabling systematic exploration of sequence space with minimal screening. These variants exhibited outstanding stereoselectivity (up to 99:1 enantiomeric ratio, 99:1 diastereomeric ratio) for most of the tested substrates. Furthermore, crystal structures and molecular dynamics studies revealed the molecular basis of enhanced stereoselectivity switching.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"27 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148769216","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

Traceless sortase ligation for chemical protein synthesis 用于化学蛋白合成的无痕分选酶结扎

Nature synthesis Pub Date : 2026-08-20 DOI: 10.1038/s44160-026-01143-z

Yong-Kang Zhou (周永康), Dong-Liang Huang (黄栋梁), Weichen Wang (王玮辰), Shi-Jun Zou (邹世军), Guo-Xia Yu (俞国霞), Long-Jie Wang (王龙杰), Leilei Shi (时磊磊), Shan Tang (唐姗), Ji-Shen Zheng (郑基深)

{"title":"Traceless sortase ligation for chemical protein synthesis","authors":"Yong-Kang Zhou \u0000 (周永康), Dong-Liang Huang \u0000 (黄栋梁), Weichen Wang \u0000 (王玮辰), Shi-Jun Zou \u0000 (邹世军), Guo-Xia Yu \u0000 (俞国霞), Long-Jie Wang \u0000 (王龙杰), Leilei Shi \u0000 (时磊磊), Shan Tang \u0000 (唐姗), Ji-Shen Zheng \u0000 (郑基深)","doi":"10.1038/s44160-026-01143-z","DOIUrl":"https://doi.org/10.1038/s44160-026-01143-z","url":null,"abstract":"Sortase-mediated ligation has emerged as a prominent method for chemical protein synthesis, yet its application is hindered by several inherent constraints, including strict sequence and chirality specificity, reaction reversibility and ligation scars left on the product. Here we report a traceless sortase ligation (TSL) method to overcome these limitations. Our method uniquely features the temporary installation of L-sortase’s natural recognition motifs (LPXTG/GGG) on the reacting partners (one peptide thioester and another N-terminal Cys peptide)—thereby avoiding permanent modifications to the target protein backbone. This approach facilitates efficient intermolecular peptide conjugation via readily available L-sortase, and a subsequent intramolecular native chemical ligation irreversibly traps the ligation intermediate, followed by a quantitative removal of the sortase tags. Consequently, TSL produces homogeneous, ligation-scar-free proteins from a wide range of substrates. The practicality and robustness of TSL were demonstrated by the total synthesis of mirror-image protein CD33-IgC and the semi-synthesis of α-synuclein, showcasing its potential for generating diverse protein targets such as mirror-image proteins and post-translationally modified proteins.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"22 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148769146","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

Chlorine-mediated electrosynthesis of hydrazine from urea 氯介导尿素电合成联氨的研究

Nature synthesis Pub Date : 2026-08-17 DOI: 10.1038/s44160-026-01139-9

Pengtang Wang, Xiaowan Bai, Zhong-Shuai Zhu, Xintong Gao, Yao Zheng, Shi-Zhang Qiao

引用次数: 0

An enthalpy–entropy competition strategy enables moisture-stable and scalable perovskite photovoltaics 焓熵竞争策略使湿稳定性和可扩展的钙钛矿光伏发电成为可能

Nature synthesis Pub Date : 2026-08-17 DOI: 10.1038/s44160-026-01142-0

Zhaoyang Chu, Junliang Li, Jiaju Gao, Sihao Li, Baojin Fan, Zongyi Gu, Yihuan Xie, Yaling Luo, Zhi Xing, Xiangchuan Meng, Hongxiang Li, Xiaotian Hu, Yiwang Chen

{"title":"An enthalpy–entropy competition strategy enables moisture-stable and scalable perovskite photovoltaics","authors":"Zhaoyang Chu, Junliang Li, Jiaju Gao, Sihao Li, Baojin Fan, Zongyi Gu, Yihuan Xie, Yaling Luo, Zhi Xing, Xiangchuan Meng, Hongxiang Li, Xiaotian Hu, Yiwang Chen","doi":"10.1038/s44160-026-01142-0","DOIUrl":"https://doi.org/10.1038/s44160-026-01142-0","url":null,"abstract":"Scalable fabrication of perovskite solar modules is hindered by processing inconsistencies and moisture-induced degradation. Although classic coordination solvents form thermodynamically stable intermediate phases with lead iodide (PbI2) under inert gas atmospheres, they are highly hygroscopic in ambient conditions. Moreover, due to minimal entropy change, this phase is difficult to remove during annealing, leading to micropores and unwanted phases. Here we introduce an enthalpy–entropy competition strategy for scalable, humidity-tolerant perovskite printing, in which dimethyl sulfoxide/N-methylpyrrolidone is replaced by N-butylpyrrolidone. N-butylpyrrolidone forms strong carbonyl–PbI2 coordination at ambient temperatures (enthalpy-driven), yet readily dissociates on heating (entropy-driven), facilitating easier formamidinium iodide embedding and intermediate-phase protection. The strategy yields perovskite solar modules with certified power conversion efficiencies of 23.97% in a 100-cm2 rigid module and 19.71% in a flexible counterpart. Encapsulated devices retain 80% of initial performance after 1,440 hours under the double 85 condition (85 °C, 85% relative humidity), demonstrating outstanding operational durability.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"9 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148769147","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

Asymmetric α-arylation and alkenylation of amines and ethers by a sequential metalation and enantioselective cross-coupling strategy 序贯金属化和对映选择性交叉偶联策略对胺和醚的不对称α-芳基化和烯基化

Nature synthesis Pub Date : 2026-08-12 DOI: 10.1038/s44160-026-01134-0

Sheng Liu, Shiwei Jian, Bobo Wang, Jia-Ming Liu, Zhenyu Gou, Youjun Xu, Xiaofeng Wei, Zi-Chao Wang, Shi-Liang Shi

{"title":"Asymmetric α-arylation and alkenylation of amines and ethers by a sequential metalation and enantioselective cross-coupling strategy","authors":"Sheng Liu, Shiwei Jian, Bobo Wang, Jia-Ming Liu, Zhenyu Gou, Youjun Xu, Xiaofeng Wei, Zi-Chao Wang, Shi-Liang Shi","doi":"10.1038/s44160-026-01134-0","DOIUrl":"https://doi.org/10.1038/s44160-026-01134-0","url":null,"abstract":"Enantioselective C–H metalation coupled with stereospecific cross-coupling is an essential method for forming C(sp2)–C(sp3) bonds; however, current protocols typically rely on stoichiometric chiral auxiliaries such as (–)-sparteine, limiting the development of catalyst-controlled strategies. Here we report a sequential C(sp3)–H bond metalation/enantioselective C(sp2)–C(sp3) cross-coupling strategy that enables Pd-catalysed asymmetric α-arylation and alkenylation of amines and ethers without the need for stoichiometric chiral sources. This approach features readily available reagents and broad substrate compatibility, and delivers both cyclic and acyclic products in high yields and enantioselectivities. Its utility is demonstrated through late-stage functionalization of pharmaceuticals and concise synthesis of chiral ligands and bioactive molecules. Mechanistic studies reveal that the α-arylation of ethers proceeds via dynamic kinetic resolution, whereas that of amines follows a kinetic resolution pathway. Beyond the immediate synthetic utility, we anticipate that this metalation/enantioselective coupling strategy will find application in the functionalization of diverse C–H bonds.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"33 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148728863","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

Orthogonal hydrogenation of alkenes enabled by multifunctional phosphine 多功能膦催化烯烃正交加氢

Nature synthesis Pub Date : 2026-08-11 DOI: 10.1038/s44160-026-01140-2

Dong Wang, Zijiang Yang, Zihao Hu, Huiyuan Wang, Fancong Meng, Shanya Lu, Tao XU

引用次数: 0

Aziridination of inert alkanes via photo-mediated double hydrogen atom transfer 光介导双氢原子转移的惰性烷烃叠氮化反应

Nature synthesis Pub Date : 2026-07-30 DOI: 10.1038/s44160-026-01127-z

Ming-Shang Liu, Hwee Ting Ang, Qing-Yang Zhou, Chu Wang, Xiao-Ye Yu, Jun-Li Ao, Gan Wang, Zi-Hao Jiao, Kendall N. Houk, Jie Wu

{"title":"Aziridination of inert alkanes via photo-mediated double hydrogen atom transfer","authors":"Ming-Shang Liu, Hwee Ting Ang, Qing-Yang Zhou, Chu Wang, Xiao-Ye Yu, Jun-Li Ao, Gan Wang, Zi-Hao Jiao, Kendall N. Houk, Jie Wu","doi":"10.1038/s44160-026-01127-z","DOIUrl":"https://doi.org/10.1038/s44160-026-01127-z","url":null,"abstract":"The direct functionalization of inert alkanes is a long-standing challenge in synthetic chemistry owing to the high bond dissociation energy of C(sp3)–H bonds. Hydrogen atom transfer (HAT) has emerged as a powerful strategy for monofunctionalization, while the development of methods enabling vicinal double functionalization of alkanes remains limited and typically relies on a monofunctionalization–β-elimination–difunctionalization cascade. Here we report the development of a double-HAT process, leveraging the distinctive reactivity of photo-generated triplet sulfonyl nitrenes under visible-light irradiation, to directly transform inert alkanes into aziridines. This approach streamlines the synthesis of diverse aziridines from readily available alkanes, with large-scale synthesis assisted by a high-speed circulation flow platform. Mechanistic insights, supported by both experimental and computational investigations, reveal the formation of an olefin intermediate through a double-HAT process, with the in situ-generated triplet sulfonyl nitrenes and iodosobenzene playing critical roles in the reaction pathway.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"40 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148612631","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