Nature synthesis最新文献_第8页

Dynamic anionic sublattice engineering in perovskite heterostructures for perovskite–silicon tandem solar cells 钙钛矿-硅串联太阳能电池异质结构中的动态阴离子亚晶格工程

Nature synthesis Pub Date : 2026-07-09 DOI: 10.1038/s44160-026-01111-7

Qiaoyan Ma, Yousheng Wang, Meng Li, Yuchen Yang, Yong Wang, Chenxu He, Jianzha Zheng, Yinghui Peng, Daxin Xiao, Jing Peng, Huanyong Li, Chong Liu, Zijia Li, Jiandong Fan, Yaohua Mai

引用次数: 0

Hyperspace exploration using robotics for the discovery of mechanistically distinct transformations and complex functional products 利用机器人技术进行超空间探索，以发现机械上不同的转换和复杂的功能产品

IF 22.6

Nature synthesis Pub Date : 2026-07-02 DOI: 10.1038/s44160-026-01096-3

Daniel Matuszczyk, Rafał Frydrych, Wai-Shing Wong, Yankai Jia, Yaroslav I. Sobolev, Jan Hanus, Juhyeong Lee, Bartosz A. Grzybowski

{"title":"Hyperspace exploration using robotics for the discovery of mechanistically distinct transformations and complex functional products","authors":"Daniel Matuszczyk, Rafał Frydrych, Wai-Shing Wong, Yankai Jia, Yaroslav I. Sobolev, Jan Hanus, Juhyeong Lee, Bartosz A. Grzybowski","doi":"10.1038/s44160-026-01096-3","DOIUrl":"10.1038/s44160-026-01096-3","url":null,"abstract":"Chemical reactions are traditionally viewed as linear transformations, yet in reality they unfold as mechanistic networks embedded within multidimensional ‘hyperspaces’ of conditions. Systematic exploration of these spaces can redirect classical reactions into unexpected branches representing new reactivity patterns. Here we report the discovery of a pseudo-seven-component transformation within the hyperspace of the century-old Biginelli reaction, yielding polycyclic products with substantial structural and stereochemical complexity. These products also exhibit rare supramolecular behaviours, from hierarchical assembly to metal-programmed chiral sorting. Together, these findings demonstrate that hyperspace exploration can uncover mechanistically distinct and functionally useful reactions, expanding the boundaries of chemical reactivity. The hyperspace of reaction conditions of the Biginelli reaction is scanned using a robotic platform, revealing a pseudo-seven-component transformation that yields a bicyclic product featuring rare supramolecular behaviour. This work shows that the chemical reaction is a switchable network embedded within a hyperspace of conditions, rather than a linear transformation.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1532-1541"},"PeriodicalIF":22.6,"publicationDate":"2026-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s44160-026-01096-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148385829","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

Electrophotocatalysis for direct vicinal dichlorination of carboxylic acids 羧酸直接邻二氯化的光电催化

IF 22.6

Nature synthesis Pub Date : 2026-07-02 DOI: 10.1038/s44160-026-01103-7

Luca Massaro, Helena Lundberg

引用次数: 0

Automated exploration of the Biginelli reaction hyperspace 比奇内利反应超空间的自动探索

IF 22.6

Nature synthesis Pub Date : 2026-07-02 DOI: 10.1038/s44160-026-01098-1

Theodore Tyrikos-Ergas, Eric T. Sletten

引用次数: 0

Refactoring pikromycin synthase for the modular biosynthesis of macrolide antibiotics in E. coli 重组大环内酯类抗生素在大肠杆菌中的模块化生物合成

Nature synthesis Pub Date : 2026-06-29 DOI: 10.1038/s44160-026-01108-2

Takeshi Miyazawa, Ramesh Bista, Adrian T. Keatinge-Clay

{"title":"Refactoring pikromycin synthase for the modular biosynthesis of macrolide antibiotics in E. coli","authors":"Takeshi Miyazawa, Ramesh Bista, Adrian T. Keatinge-Clay","doi":"10.1038/s44160-026-01108-2","DOIUrl":"https://doi.org/10.1038/s44160-026-01108-2","url":null,"abstract":"While engineering modular polyketide synthases (PKSs) using the recently updated module boundary has yielded libraries of triketide–pentaketides, this strategy has not yet been applied to the combinatorial biosynthesis of macrolactones or macrolide antibiotics. Here we developed a two-plasmid system for the construction and expression of PKSs and used it to obtain a refactored pikromycin PKS in Escherichia coli that produces 49 mg of narbonolide per litre of culture. The replacement, insertion, deletion and mutagenesis of modules enabled access to hexaketide, heptaketide and octaketide derivatives. Supplying enzymes for desosamine biosynthesis and transfer enabled production of narbomycin, pikromycin, YC-17, methymycin and five derivatives thereof. By using native docking domains, knocking out pathways competing with desosamine biosynthesis and supplying the editing thioesterase PikAV, the titre of narbomycin was boosted 58-fold to 37 mg l−1. The second and third modules of the refactored pikromycin synthase were swapped with others to yield three new narbomycin analogues, investigate structure–activity relationships and demonstrate how libraries of macrolide antibiotics can be readily accessed.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"55 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148385807","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

Electrified direct epoxidation of light hydrocarbons using alkene-binding atomic sites 利用烯烃结合原子位的轻烃电直接环氧化反应

Nature synthesis Pub Date : 2026-06-25 DOI: 10.1038/s44160-026-01104-6

Yongxiang Liang, Yiqing Chen, Yu Yang, Rong Xia, Jianan Erick Huang, Zedong Zhang, Bosi Peng, Zeyan Liu, Huajie Ze, Aamir Hassan Shah, Yali Ji, Fengwang Li, Ke Xie, Edward H. Sargent

{"title":"Electrified direct epoxidation of light hydrocarbons using alkene-binding atomic sites","authors":"Yongxiang Liang, Yiqing Chen, Yu Yang, Rong Xia, Jianan Erick Huang, Zedong Zhang, Bosi Peng, Zeyan Liu, Huajie Ze, Aamir Hassan Shah, Yali Ji, Fengwang Li, Ke Xie, Edward H. Sargent","doi":"10.1038/s44160-026-01104-6","DOIUrl":"https://doi.org/10.1038/s44160-026-01104-6","url":null,"abstract":"Direct electrochemical epoxidation of alkenes could reduce the carbon intensity of epoxidation processes. However, highly selective electrified epoxidation is hindered by the competing oxygen evolution reaction. Analysis of the best-performing electrocatalysts reported to date reveals that propylene binds weakly to their surfaces while oxygen evolution intermediates predominate. Here we attempted to find catalysts on which surface-adsorbed propylene resides in proximity to reactive oxygen species. Screening a series of dopants revealed a volcano-type relationship between epoxidation activity and propylene adsorption, with indium-doped platinum–palladium oxide (In-PtPdOx) achieving the highest performance. The propylene oxide Faradaic efficiency reached 66% at 70 mA cm−2 and 58% at 100 mA cm−2, with a high productivity of 1,080 μmol cm−2 h−1. Integration into a membrane electrode assembly enabled a 46 wt% propylene oxide stream. Mechanistic characterization indicated that indium incorporation elevates the valence of platinum, strengthening metal–π C–C interactions with propylene and balancing propylene co-adsorption with reactive oxygen intermediates, thereby suppressing the oxygen evolution reaction and enabling highly selective epoxidation.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"71 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336506","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

Membrane remodelling for increased methanol tolerance in Komagataella phaffii 法菲Komagataella phaffii膜重塑对甲醇耐受性的提高

IF 22.6

Nature synthesis Pub Date : 2026-06-25 DOI: 10.1038/s44160-026-01092-7

Shuai Wang, Liu Yang, Zhixuan Li, Hui Ye, Fei Teng, Jun Yang, Chunting Ye, Dexun Fan, Shuangyan Han

{"title":"Membrane remodelling for increased methanol tolerance in Komagataella phaffii","authors":"Shuai Wang, Liu Yang, Zhixuan Li, Hui Ye, Fei Teng, Jun Yang, Chunting Ye, Dexun Fan, Shuangyan Han","doi":"10.1038/s44160-026-01092-7","DOIUrl":"10.1038/s44160-026-01092-7","url":null,"abstract":"Methanol is a promising C1 feedstock for bioproduction but its cytotoxicity limits applications. Here we enhanced Komagataella phaffii GS115 methanol tolerance to 10–13% (v/v) by overexpressing four genes (phosphatidylethanolamine methyltransferase (PET2), phosphatidylserine synthase (PSA), PAS_chr1-4_0178 (0178) and PAS_chr2-2_0267 (0267)) (S33 strain). Our results show that, under high methanol stress, S33 undergoes membrane lipid remodelling-driven metabolic reprogramming, with central carbon flux being redistributed from the pentose phosphate pathway and citric acid cycle towards glycolysis. Within this framework, 0178 encodes a vacuolar transporter of sulfur-containing amino acids, which we propose supports phospholipid methylation and redox balance. Meanwhile, 0267 encodes a peroxisomal thiolase-degrading long‑chain fatty acyl‑CoAs, limiting toxic long-chain sphingolipid accumulation, maintaining membrane stability. These genes enable S33 to achieve lipid titre of approximately 40 g l−1 under non-sterile fed‑batch fermentation conditions. This work positions S33 as a methanol-tolerant K. phaffii chassis for further strain and process development. Bioproduction from methanol is often challenging owing to the cytotoxicity of methanol. Here a methanol-tolerant Komagataella phaffii chassis is engineered by overexpressing four membrane genes, increasing tolerance to 10–13% methanol and enabling non-sterile lipid production (>40 g l−1) via membrane lipid remodelling and metabolic rewiring.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1514-1531"},"PeriodicalIF":22.6,"publicationDate":"2026-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336505","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

Metal-free hydrogenation of viologens to piperidine derivatives for bacterial inhibition 无金属氢化viologens合成哌啶衍生物的抑菌作用

IF 22.6

Nature synthesis Pub Date : 2026-06-23 DOI: 10.1038/s44160-026-01099-0

Bai-Tong Liu, Timothy Y.-Z. Li, Nathan C. Incandela, Isaac Conway, Xianhui Tang, Guangcheng Wu, Han Han, Enxu Liu, Sheng-Nan Lei, Bohan Tang, Haomiao Xie, Cheng Li, Yanli Zhao, K. N. Houk, J. Fraser Stoddart

{"title":"Metal-free hydrogenation of viologens to piperidine derivatives for bacterial inhibition","authors":"Bai-Tong Liu, Timothy Y.-Z. Li, Nathan C. Incandela, Isaac Conway, Xianhui Tang, Guangcheng Wu, Han Han, Enxu Liu, Sheng-Nan Lei, Bohan Tang, Haomiao Xie, Cheng Li, Yanli Zhao, K. N. Houk, J. Fraser Stoddart","doi":"10.1038/s44160-026-01099-0","DOIUrl":"10.1038/s44160-026-01099-0","url":null,"abstract":"The hydrogenation of aromatic viologens to their non-aromatic derivatives holds promise for biomedical and materials science applications. Conventional hydrogenation methods, however, rely on harsh reductants and high-cost metal catalysts. Here we report a safe, metal-free hydrogenation strategy that uses formic acid as a sustainable reductant, facilitated by an azeotropic mixture with N,N-dimethylformamide. This method enables the efficient conversion of diverse viologen derivatives into their reduced 4-(piperidin-4-yl)-3-piperideine counterparts. A key advantage of this process is the tendency of the products to undergo spontaneous crystallization, streamlining purification and enabling direct structural characterization. We demonstrate the broad applicability of this transformation across a range of architectures, including viologen-based small molecules, macrocyclic compounds and porous organic frameworks. Mechanistic investigations integrating mass spectrometry, single-crystal X-ray diffraction and density functional theory calculations reveal a reduction pathway analogous to the Eschweiler–Clarke and Lukeš reactions. In addition, several reduced scaffolds demonstrate antimicrobial activity. A metal-free hydrogenation method converts rigid aromatic viologen units into flexible piperidine-based structures using formic acid. The transformation induces pronounced conformational changes in macrocycles and extends across diverse architectures, providing access to functional piperidine materials with potential antimicrobial activity.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1506-1513"},"PeriodicalIF":22.6,"publicationDate":"2026-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148305267","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

Interface-regulated vapour crystallization for ultrapure perovskite LEDs 超纯钙钛矿led的界面调节蒸汽结晶

Nature synthesis Pub Date : 2026-06-22 DOI: 10.1038/s44160-026-01100-w

Jian Mao, Qichun Gu, Yunzhou Deng, Milos Dubajic, Thomas A. Selby, Yorrick Boeije, Xinjuan Li, Yang Lu, Zhengkang Qu, Sebastiaan Hoek, Linfeng Pan, Weidong Xu, Tianjun Liu, Yuqi Sun, Yu Zhang, Benedetta Gaggio, Zimu Wei, Zher Ying Ooi, Yutong Han, Alessandro J. Mirabelli, Eunyoung Choi, Shenyu Nie, Yi Shen, Hayley Gilbert, Yuanle Tian, Xian Wei Chua, Joo Sung Kim, Xiaoliang Mo, Fengxian Xie, Jianlu Wang, Judith L. MacManus-Driscoll, Meikang Han, Junhao Chu, Neil C. Greenham, Henning Sirringhaus, Caterina Ducati, Tiarnan A. S. Doherty, Paul A. Midgley, Miguel Anaya, Samuel D. Stranks

{"title":"Interface-regulated vapour crystallization for ultrapure perovskite LEDs","authors":"Jian Mao, Qichun Gu, Yunzhou Deng, Milos Dubajic, Thomas A. Selby, Yorrick Boeije, Xinjuan Li, Yang Lu, Zhengkang Qu, Sebastiaan Hoek, Linfeng Pan, Weidong Xu, Tianjun Liu, Yuqi Sun, Yu Zhang, Benedetta Gaggio, Zimu Wei, Zher Ying Ooi, Yutong Han, Alessandro J. Mirabelli, Eunyoung Choi, Shenyu Nie, Yi Shen, Hayley Gilbert, Yuanle Tian, Xian Wei Chua, Joo Sung Kim, Xiaoliang Mo, Fengxian Xie, Jianlu Wang, Judith L. MacManus-Driscoll, Meikang Han, Junhao Chu, Neil C. Greenham, Henning Sirringhaus, Caterina Ducati, Tiarnan A. S. Doherty, Paul A. Midgley, Miguel Anaya, Samuel D. Stranks","doi":"10.1038/s44160-026-01100-w","DOIUrl":"https://doi.org/10.1038/s44160-026-01100-w","url":null,"abstract":"Achieving ultranarrow spectral linewidth and broad spectral tunability in light-emitting diodes (LEDs) remains challenging due to linewidth broadening from compositional and size heterogeneities. Here we report an interface-regulated vapour crystallization strategy that enables precise control over the spectral linewidth of solution-processed halide perovskite thin films. Underlying materials that exhibit minimal molecular interactions with perovskite precursors, exemplified by poly(9-vinylcarbazole), facilitate smooth ion diffusion and crystallization assisted by dimethylformamide vapour. This mechanism leads to perovskite films with both horizontal and vertical homogeneity and low inhomogeneous broadening comparable to that of perovskite single crystals. We demonstrate perovskite films with ultranarrow photoluminescence linewidths of 13.6 nm, 13.7 nm, 13.8 nm and 14.4 nm for emissions at 464 nm, 474 nm, 483 nm and 522 nm, respectively. This enables us to achieve sky-blue perovskite LEDs with narrow electroluminescence linewidths of 14.7 nm and a peak external quantum efficiency of 24.6%, with comparable linewidths and performance in LEDs spanning the pure blue to pure green. This work offers a practical and scalable strategy to realize narrow spectral linewidth, broad spectral tunability and high performance in thin film LEDs.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"339 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148291440","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

The importance of nano-edges in atomic stencilling and chiroptically active assembly of patchy gold tetrahedra 纳米边缘在贴片金四面体原子刻版和共色活性组装中的重要性

IF 22.6

Nature synthesis Pub Date : 2026-06-18 DOI: 10.1038/s44160-026-01095-4

Xiaoying Lin, Chansong Kim, Thi Vo, Tommy Waltmann, Haihua Liu, Jun Lu, Jiahui Li, Yu-Shen Liu, Suraj Kannur, Junseo Lee, Chu-Yun Hwang, Falon C. Kalutantirige, Lehan Yao, Nicholas A. Kotov, Sharon C. Glotzer, Qian Chen

{"title":"The importance of nano-edges in atomic stencilling and chiroptically active assembly of patchy gold tetrahedra","authors":"Xiaoying Lin, Chansong Kim, Thi Vo, Tommy Waltmann, Haihua Liu, Jun Lu, Jiahui Li, Yu-Shen Liu, Suraj Kannur, Junseo Lee, Chu-Yun Hwang, Falon C. Kalutantirige, Lehan Yao, Nicholas A. Kotov, Sharon C. Glotzer, Qian Chen","doi":"10.1038/s44160-026-01095-4","DOIUrl":"10.1038/s44160-026-01095-4","url":null,"abstract":"Molecular patterning of proteins with atomic precision encodes folding and recognition. Emulating this patterning on synthetic surfaces can integrate multifunctionality with directional interactions for catalysis, biomedicine, nanomanufacturing and agriculture. Here we extend recently reported atomic stencilling, where iodides mask Au{111} facets to direct polymer grafting, to gold nanotetrahedra. Despite all faces being {111}, unexpected patch patterns emerge due to nanoparticle edges. Tuning edge exposure, solvent polarity and polymer–polymer interactions leads to seven distinct patch patterns on a single tetrahedron shape. Polymer scaling theory and simulations that explicitly consider edge accessibility chart a phase diagram spanning more than 30 conditions and quantitatively matching experiments. The patchy nanotetrahedra self-assemble via corner-, edge- or face-sharing motifs analogous to molecular complexes, which exhibit plasmonic chiroptical activity confirmed by ultrafast electron microscopy and finite-difference time-domain calculations. These results show that atomic stencilling precision makes nanoscopic edge features critically important, offering scalable, multiplexed and site-selective functionalization. Patchy tetrahedra with seven distinct patterns are synthesized using atomic stencilling. The experimentally mapped phase diagram of more than 30 conditions is rationalized by polymer scaling theory and molecular dynamics simulations that account for the critical importance of nano-edges. It is found that polyelectrolyte complexation drives patch-to-patch assembly with emergent chiroptical properties.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"5 10","pages":"1634-1647"},"PeriodicalIF":22.6,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148291102","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