Nature synthesis最新文献_第10页

Electrophotocatalytic decarboxylative vicinal dichlorination of aliphatic carboxylic acids 脂肪族羧酸的光电催化脱羧邻近二氯化

IF 22.6

Nature synthesis Pub Date : 2026-05-26 DOI: 10.1038/s44160-026-01088-3

Kun Cui, Yajuan Li, Shu-Fan He, Guoying Zhang, Daixi Li, Tao Shen

{"title":"Electrophotocatalytic decarboxylative vicinal dichlorination of aliphatic carboxylic acids","authors":"Kun Cui, Yajuan Li, Shu-Fan He, Guoying Zhang, Daixi Li, Tao Shen","doi":"10.1038/s44160-026-01088-3","DOIUrl":"10.1038/s44160-026-01088-3","url":null,"abstract":"Decarboxylative functionalization of aliphatic carboxylic acids is a powerful strategy in organic synthesis, yet most methods focus on decarboxylative monofunctionalization. Merging decarboxylation with selective activation of an adjacent C–H bond to deliver vicinal difunctionalization has remained elusive. Here we report an electrophotocatalytic decarboxylative vicinal dichlorination of aliphatic carboxylic acids using 1,2-dichloroethane as both the solvent and the chlorine source. Mechanistic studies indicate the formation of an alkene intermediate via photocatalytic dehydrogenative decarboxyolefination, followed by electrochemical vicinal chlorination. The protocol operates under mild conditions, tolerates diverse functionality and enables late-stage vicinal dichlorination of bioactive molecules and natural products, underscoring its practicality and potential for streamlined synthesis. Decarboxylative functionalization of aliphatic carboxylic acids is a powerful strategy in organic synthesis, yet most methods focus on decarboxylative monofunctionalization. Now, an electrophotocatalytic decarboxylative vicinal dichlorination of aliphatic carboxylic acids has been developed to enable late-stage decarboxylative difunctionalization of bioactive molecules and natural products.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 9","pages":"1349-1359"},"PeriodicalIF":22.6,"publicationDate":"2026-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148904491","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

Photoenzymatic catalysis through computation 通过计算光酶催化

IF 2

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01080-x

Thomas West

引用次数: 0

Challenges and opportunities in integrating biocatalysis with photo- and electrocatalysis for scalable synthesis 将生物催化与光催化和电催化相结合以实现可扩展合成的挑战和机遇

IF 2

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01087-4

Monica Brachi, Vamshi Krishna Kamaja, Shelley D. Minteer

引用次数: 0

Bridging interfacial electron transfer for efficient electrocatalytic coupling reactions 高效电催化偶联反应的桥接界面电子转移

IF 22.6

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01081-w

Chengdong Yang, Yun Gao, Wenshuo Shang, Wenwen Cai, Yueqing Wang, Jizhen Ma, Yi Wang, Jintao Zhang

{"title":"Bridging interfacial electron transfer for efficient electrocatalytic coupling reactions","authors":"Chengdong Yang, Yun Gao, Wenshuo Shang, Wenwen Cai, Yueqing Wang, Jizhen Ma, Yi Wang, Jintao Zhang","doi":"10.1038/s44160-026-01081-w","DOIUrl":"10.1038/s44160-026-01081-w","url":null,"abstract":"Heterogeneous molecular catalysts have emerged as promising platforms for electroreduction reactions, yet their performance is limited by inefficient interfacial electron transfer across poorly coupled molecule–electrode interfaces. Here we report an interfacial engineering strategy using oxygen-functionalized ketjenblack as an electronic bridge to mitigate this interfacial barrier between spatially distorted copper phthalocyanine and the carbon matrix, enabling efficient electrochemical C–C coupling of benzaldehyde to achieve a hydrobenzoin production rate of 0.62 mmol h−1 cm−2. Experimental and theoretical analyses elucidate that the reinforced conjugation promotes *ketyl intermediate formation and drives subsequent C–C coupling through nucleophilic attack on benzaldehyde. The nucleophilicity index (f+) of aldehyde groups is identified as a key descriptor governing both reaction kinetics and stereoselectivity, where higher f+ values correlate with accelerated reduction rates and improved stereochemical outcomes. This interfacial modulation strategy is validated through enhanced performance in N=N coupling of nitrobenzene, CO2 electroreduction and nitrite reduction. This work provides a general approach to regulate efficient molecular–electrode interfaces, addressing a key bottleneck in heterogeneous electrocatalysis. Upgrading biomass-derived carbon-oxygenates into value-added chemicals has emerged as a promising strategy to reduce reliance on crude oil as a carbon source. Here a bioinspired design of molecular catalysts is reported to promote interfacial electron transfer, enabling efficient electrochemical C–C coupling of different aldehydes.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1589-1600"},"PeriodicalIF":22.6,"publicationDate":"2026-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149125916","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

Self-driving labs for research and development in industry 用于工业研发的自动驾驶实验室

IF 22.6

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01084-7

Jet-Sing Lee

引用次数: 0

Topological anionic confinement enables synthesis of 2D high-entropy molybdates under mild conditions 拓扑阴离子约束可以在温和条件下合成二维高熵钼酸盐

IF 22.6

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01085-6

Bin Chen, Qicheng Zhang, Honglin Du, Pengwei Zhao, Weipeng Zhao, Mingjun Cen, Zhuo Chen, Shuya Zhang, Linjie Guan, Yizhe Hu, Tianhao Niu, Lin Gu, Danyun Xu, Wenchao Peng, Yang Li, Junliang Sun, Xiaobin Fan

{"title":"Topological anionic confinement enables synthesis of 2D high-entropy molybdates under mild conditions","authors":"Bin Chen, Qicheng Zhang, Honglin Du, Pengwei Zhao, Weipeng Zhao, Mingjun Cen, Zhuo Chen, Shuya Zhang, Linjie Guan, Yizhe Hu, Tianhao Niu, Lin Gu, Danyun Xu, Wenchao Peng, Yang Li, Junliang Sun, Xiaobin Fan","doi":"10.1038/s44160-026-01085-6","DOIUrl":"10.1038/s44160-026-01085-6","url":null,"abstract":"Two-dimensional high-entropy materials offer vast opportunities, yet their low-temperature synthesis with compositional homogeneity and anisotropic morphology remains challenging, due to thermodynamic competition between entropy-driven mixing and strain-induced phase segregation. Here we report a topological anionic confinement strategy that uses MoO42− tetrahedra as spatially defined scaffolds to suppress cation segregation. This strategy enables the single-step, template-free synthesis of a series of two-dimensional high-entropy molybdate assemblies (M3(MoO4)4·4H2O, M = Mn, Fe, Co, Ni, Cu or Zn) at 120 °C. In situ liquid-phase transmission electron microscopy unveils a non-classical crystallization pathway, where metastable clusters undergo a dissolution–regrowth process for compositional homogenization before coalescing via oriented attachment into well-defined nanoplates, a process critically modulated by interfacial energy. This work not only provides a solution to a long-standing synthetic bottleneck but also establishes topological anionic confinement as a versatile method for entropy-stabilized anisotropic nanomaterial design under mild conditions, opening new avenues for diverse functional applications. Two-dimensional high-entropy materials are of interest for diverse applications, but low-temperature synthesis remains challenging. Now a topological anionic confinement strategy is reported in which MoO42⁻ tetrahedral scaffolds template two-dimensional high-entropy molybdates at 120 °C. Metastable clusters homogenize via a dissolution–regrowth process and then coalesce into well-defined nanoplates.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1542-1551"},"PeriodicalIF":22.6,"publicationDate":"2026-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149126007","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

One-pot synthesis of hierarchically integrated covalent organic framework heterojunctions for photocatalysis 光催化层次化共价有机框架异质结的一锅合成

IF 22.6

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01077-6

Wen-Zhuang Wang, Ya Lu, Chao Liu, Yubin Fu, Xin Zhao, Hong-Xin Xu, Fei Song, Jing-Yuan Ma, Yi-Xue Xu, Shun-Feng Li, Qiao-Yan Qi, Shun-Qi Xu, Xin Zhao

{"title":"One-pot synthesis of hierarchically integrated covalent organic framework heterojunctions for photocatalysis","authors":"Wen-Zhuang Wang, Ya Lu, Chao Liu, Yubin Fu, Xin Zhao, Hong-Xin Xu, Fei Song, Jing-Yuan Ma, Yi-Xue Xu, Shun-Feng Li, Qiao-Yan Qi, Shun-Qi Xu, Xin Zhao","doi":"10.1038/s44160-026-01077-6","DOIUrl":"10.1038/s44160-026-01077-6","url":null,"abstract":"Covalent organic frameworks (COFs) with crystalline networks and large surface areas provide an ideal platform to mimic natural structures for photosynthesis. However, it remains challenging to construct complex, multistate architectures using single-component COFs. Herein, inspired by leaf morphology, we demonstrate a one-pot synthesis for constructing a one-dimensional (1D) COF and a three-dimensional (3D) COF from identical binary monomers, yielding a hierarchically integrated COF heterostructure (1D@3DCOF-2). The 1D chains and 3D porous frameworks form in situ and are spatially integrated, forming a homogeneous S-scheme heterojunction that yields a built-in electric field for enhanced charge carrier dynamics. The hydrophilic 1D COF possesses excellent light-harvesting and Pt anchoring capacities, and the porous 3D COF ensures efficient mass transfer. With Pt as a cocatalyst, 1D@3DCOF-2 achieved an excellent hydrogen evolution rate (HER) of 45.7 mmol g−1 h−1 under visible light irradiation, surpassing that of the individual 3D COF (31.1 mmol g−1 h−1) and inactive 1D COF. Additionally, a higher rate up to 50.8 mmol g−1 h−1 was achieved in seawater. This work establishes a one-pot synthetic strategy for constructing multistage COFs towards nature-inspired high-performance heterostructures. A hierarchically integrated 1D@3D covalent organic framework heterostructure is constructed via a one-pot synthesis, leading to the formation of an S-scheme heterojunction with a built-in electric field. The heterostructure has a photocatalytic H2 evolution rate of 45.7 mmol g−1 h−1, outperforming both of the constituent single-component COFs.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1565-1574"},"PeriodicalIF":22.6,"publicationDate":"2026-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149125918","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

Enantioselective synthesis of sulfur-stereogenic alkyl sulfilimines with C(sp3)–H-derived alkyl radicals using copper catalysis 用铜催化以C(sp3) - h衍生烷基自由基对映选择性合成硫立体基烷基亚胺

IF 22.6

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01091-8

Li-Wen Fan, Li Qin, Chen-Yu Xiao, Jun-Bin Tang, Hang Lv, Qiao Song, Fu Liu, Jia-Peng Wang, Yu-Shuai Zhang, Dai-Lei Yuan, Jun-Qian Bian, Qiang-Shuai Gu, Xin-Yuan Liu

{"title":"Enantioselective synthesis of sulfur-stereogenic alkyl sulfilimines with C(sp3)–H-derived alkyl radicals using copper catalysis","authors":"Li-Wen Fan, Li Qin, Chen-Yu Xiao, Jun-Bin Tang, Hang Lv, Qiao Song, Fu Liu, Jia-Peng Wang, Yu-Shuai Zhang, Dai-Lei Yuan, Jun-Qian Bian, Qiang-Shuai Gu, Xin-Yuan Liu","doi":"10.1038/s44160-026-01091-8","DOIUrl":"10.1038/s44160-026-01091-8","url":null,"abstract":"Sulfur-stereogenic motifs are important in natural products, pharmaceuticals, agrochemicals and chiral ligands and catalysts, and are increasingly explored in functional materials. Direct enantioselective S-alkylation using non-prochiral C(sp3)–H bonds, particularly unactivated ones, offers an ideal atom-economical route to sulfur-stereogenic centres, yet remains highly challenging as their activation typically requires strong oxidants, and chemo- and enantiocontrol in the ensuing radical processes are inherently difficult. Here we report an enantioselective radical S–C cross-coupling between C(sp3)–H substrates and N-acyl sulfenamides, combining hydrogen atom transfer with sequential stereodiscrimination and chirality transfer. Two complementary protocols under photoinduced and thermal conditions were developed to convert primary and secondary unactivated alkanes, as well as diverse α-functionalized alkanes, into alkyl radicals that engage N-acyl sulfenamides, delivering sulfur-stereogenic alkyl sulfilimines with high enantioselectivity. The utility of this method is demonstrated by gram-scale reactions, downstream transformations into other sulfur-based chiral architectures and late-stage functionalization of pharmaceuticals and related compounds. Unactivated alkanes are difficult to use in enantioselective synthesis. Now a copper-catalysed radical S–C cross-coupling strategy enables their direct conversion into sulfur-stereogenic alkyl sulfilimines with high enantioselectivity. Two complementary methods using photo- and thermal chemistry combine hydrogen atom transfer with enantioselective copper-mediated S-stereocentre formation and chirality-transferring radical substitution.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1623-1633"},"PeriodicalIF":22.6,"publicationDate":"2026-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149126009","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

Constructing artificial methylotrophic S. cerevisiae for chondroitin sulfate production using a multidimensional combinatorial strategy 利用多维组合策略构建人工甲基化酿酒酵母生产硫酸软骨素

IF 22.6

Nature synthesis Pub Date : 2026-05-22 DOI: 10.1038/s44160-026-01079-4

Lei Li, Yixun Jiang, Wenjie Ma, Chenying Li, Ruirui Shi, Guangyao Tang, Yaxin He, Jiaqi Li, Zepin Guo, Yuxin Zhang, Shuhong Mao, Mingdong Yao, Zhengqiang Jiang, Fuping Lu, Hui-Min Qin

{"title":"Constructing artificial methylotrophic S. cerevisiae for chondroitin sulfate production using a multidimensional combinatorial strategy","authors":"Lei Li, Yixun Jiang, Wenjie Ma, Chenying Li, Ruirui Shi, Guangyao Tang, Yaxin He, Jiaqi Li, Zepin Guo, Yuxin Zhang, Shuhong Mao, Mingdong Yao, Zhengqiang Jiang, Fuping Lu, Hui-Min Qin","doi":"10.1038/s44160-026-01079-4","DOIUrl":"10.1038/s44160-026-01079-4","url":null,"abstract":"The concept of a methanol-based circular bioeconomy envisions the conversion of greenhouse gases into one-carbon compounds, which are subsequently utilized to produce high-value-added products. However, the toxicity of intermediates limits the metabolic efficiency within chassis strains. Here a carbon metabolism reconfiguration strategy combined with adaptive laboratory evolution was applied to engineer an artificial methylotrophic yeast by accelerating the flux of toxic intermediates into the central carbon metabolism. After modifying the key gene Sfa1 identified by adaptive laboratory evolution and introducing a light-responsive switch to dynamically redirect the carbon flux, the engineered strain not only restored its growth in minimal medium with 2% methanol, but also synthesized chondroitin sulfate A driven by the dark reaction. Furthermore, we designed a 3′-phosphoadenosine-5′-phosphosulfate supply strategy and energy adapter to increase the sulfonation level. This study illustrates the exciting potential of methylotrophic Saccharomyces cerevisiae as a platform for biosynthesis. A methanol-based circular bioeconomy envisions the conversion of greenhouse gases into one-carbon compounds, which are subsequently utilized to enable sustainable biomanufacturing. Here a carbon metabolism reconfiguration strategy combined with adaptive laboratory evolution is adopted to obtain methylotrophic Saccharomyces cerevisiae capable of producing chondroitin sulfate A.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1575-1588"},"PeriodicalIF":22.6,"publicationDate":"2026-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149125917","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

Shining light on all-carbon quaternary stereocentre synthesis 照亮全碳四元立体中心的合成

IF 2

Nature synthesis Pub Date : 2026-05-20 DOI: 10.1038/s44160-026-01090-9

Francesca Paradisi

引用次数: 0