Nature chemistry最新文献_第5页

Leveraging relaxation-optimized 1H–13CF correlations in 4-19F-phenylalanine as atomic beacons for probing structure and dynamics of large proteins 利用弛豫优化的4- 19f -苯丙氨酸中的1H-13CF相关性作为探测大蛋白质结构和动力学的原子信标

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-05-05 DOI: 10.1038/s41557-025-01818-8

Andras Boeszoermenyi, Denitsa L. Radeva, Sebastian Schindler, Veronica Valadares, Krishna M. Padmanabha Das, Abhinav Dubey, Thibault Viennet, Max Schmitt, Peter Kast, Vladimir M. Gelev, Nikolay Stoyanov, Nikola Burdzhiev, Ognyan Petrov, Scott Ficarro, Jarred Marto, Ezekiel A. Geffken, Sirano Dhe-Paganon, Hyuk-Soo Seo, Nathan D. Alexander, Richard B. Cooley, Ryan A. Mehl, Helena Kovacs, Clemens Anklin, Wolfgang Bermel, Ilya Kuprov, Koh Takeuchi, Haribabu Arthanari

{"title":"Leveraging relaxation-optimized 1H–13CF correlations in 4-19F-phenylalanine as atomic beacons for probing structure and dynamics of large proteins","authors":"Andras Boeszoermenyi, Denitsa L. Radeva, Sebastian Schindler, Veronica Valadares, Krishna M. Padmanabha Das, Abhinav Dubey, Thibault Viennet, Max Schmitt, Peter Kast, Vladimir M. Gelev, Nikolay Stoyanov, Nikola Burdzhiev, Ognyan Petrov, Scott Ficarro, Jarred Marto, Ezekiel A. Geffken, Sirano Dhe-Paganon, Hyuk-Soo Seo, Nathan D. Alexander, Richard B. Cooley, Ryan A. Mehl, Helena Kovacs, Clemens Anklin, Wolfgang Bermel, Ilya Kuprov, Koh Takeuchi, Haribabu Arthanari","doi":"10.1038/s41557-025-01818-8","DOIUrl":"https://doi.org/10.1038/s41557-025-01818-8","url":null,"abstract":"NMR spectroscopy of biomolecules provides atomic level information into their structure, dynamics and interactions with their binding partners. However, signal attenuation from line broadening caused by fast relaxation and signal overlap often limits the application of NMR to large macromolecular systems. Here we leverage the slow relaxation properties of 13C nuclei attached to 19F in aromatic 19F–13C spin pairs as well as the spin–spin coupling between the fluorinated 13C nucleus and the hydrogen atom at the meta-position to record two-dimensional 1H–13CF correlation spectra with transverse relaxation-optimized spectroscopy selection on 13CF. To accomplish this, we synthesized [4-19F13Cζ; 3,5-2H2ε] Phe, engineered for optimal relaxation properties, and adapted a residue-specific route to incorporate this residue globally into proteins and a site-specific 4-19F Phe encoding strategy. This approach resulted in narrow linewidths for proteins ranging from 30 kDa to 180 kDa, enabling interaction studies with small-molecule ligands without requiring specialized 19F-compatible probes.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"113 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143905685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Flue gas desulfurization and SO₂ recovery within a flexible hydrogen-bonded organic framework. 柔性氢键有机框架内的烟气脱硫和SO2回收。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-05-01 Epub Date: 2025-02-26 DOI: 10.1038/s41557-025-01744-9

Lin Li, Xuan Zhang, Xin Lian, Laiyu Zhang, Zhiyuan Zhang, Xiongli Liu, Tengfei He, Baiyan Li, Banglin Chen, Xian-He Bu

{"title":"Flue gas desulfurization and SO2 recovery within a flexible hydrogen-bonded organic framework.","authors":"Lin Li, Xuan Zhang, Xin Lian, Laiyu Zhang, Zhiyuan Zhang, Xiongli Liu, Tengfei He, Baiyan Li, Banglin Chen, Xian-He Bu","doi":"10.1038/s41557-025-01744-9","DOIUrl":"10.1038/s41557-025-01744-9","url":null,"abstract":"The removal of SO2 from flue gas remains a challenge. Adsorption-based separation of SO2 using porous materials has been proposed as a more energy-efficient and cost-effective alternative to more traditional methods such as cryogenic distillations. Here we report a flexible hydrogen-bonded organic framework (HOF-NKU-1) that enables the sieving of SO2 through the guest-adaptive response and shape-memory effect of the material. HOF-NKU-1 exhibits a high selectivity of 7,331 for the separation of SO2/CO2 and a high SO2 storage density of 3.27 g cm-3 within the pore space at ambient conditions. The hydrophobic nature of HOF-NKU-1 enables high dynamic SO2 uptake and SO2 recovery, even in conditions of 95% humidity. The SO2/CO2 separation mechanism is studied through combinatorial gas sorption isotherms, breakthrough experiments and single-crystal diffraction studies, paving the way for the development of multifunctional shape-memory porous materials in the future.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":"727-733"},"PeriodicalIF":19.2,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143516252","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Supramolecular coordination cages as crystalline sponges through a symmetry mismatch strategy. 超分子配位笼通过对称失配策略作为结晶海绵。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-05-01 Epub Date: 2025-03-05 DOI: 10.1038/s41557-025-01750-x

Wei He, Yikuan Yu, Kenta Iizuka, Hiroki Takezawa, Makoto Fujita

{"title":"Supramolecular coordination cages as crystalline sponges through a symmetry mismatch strategy.","authors":"Wei He, Yikuan Yu, Kenta Iizuka, Hiroki Takezawa, Makoto Fujita","doi":"10.1038/s41557-025-01750-x","DOIUrl":"10.1038/s41557-025-01750-x","url":null,"abstract":"The crystalline sponge method enables single-crystal X-ray diffraction analysis of guests absorbed within single-crystalline porous materials. However, its application with large or highly polar guests remains challenging. In this study, we addressed some of these limitations using palladium-based octahedron-shaped M6L4 (Td) coordination cages as crystalline sponges. The key to facilitate the crystallization of the cage is the addition of large aromatic polysulfonates ('sticker' anions); the symmetry mismatch between the cage and the sticker (D2h) results in a low-symmetry space group (P <math> <mover><mrow><mn>1</mn></mrow> <mo>¯</mo></mover> </math> ), preventing guest disorder and leading to the formation of guest-accessible channels in the crystal. Guests can be encapsulated either before or after cage crystallization. The size and host-guest properties of the cavity enable analysis of a broad range of compounds, including water-soluble molecules, large amphiphilic molecules (molecular weight of ~1,200) and molecular aggregates. We have demonstrated the versatility of the cage-sticker strategy through its application to a triaugmented triangular-prism-shaped M9L6 cage, extending the guest scope to medium-sized pharmaceutical molecules.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":"653-662"},"PeriodicalIF":19.2,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143567659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Synthesis of strained, air-stable boracycles via boron-carbon-centred diradicals. 通过以硼碳为中心的双自由基合成应变、空气稳定的硼环。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-05-01 Epub Date: 2025-04-23 DOI: 10.1038/s41557-025-01807-x

Xinmou Wang, Peiqi Zhang, Zhiyi Yang, Weixuan Sun, Hairong Lyu, Zhenyang Lin, Yangjian Quan

{"title":"Synthesis of strained, air-stable boracycles via boron-carbon-centred diradicals.","authors":"Xinmou Wang, Peiqi Zhang, Zhiyi Yang, Weixuan Sun, Hairong Lyu, Zhenyang Lin, Yangjian Quan","doi":"10.1038/s41557-025-01807-x","DOIUrl":"https://doi.org/10.1038/s41557-025-01807-x","url":null,"abstract":"Boracycles are important functional scaffolds, often exhibiting superior or unique performance compared with their carbon analogues. Five-membered oxaboracycles are key pharmacophores in Food and Drug Administration-approved boron drugs. Meanwhile, six-membered boron-doped polycyclic aromatic hydrocarbons enhance the diversification and functionality of molecular materials. However, boron-containing four-membered rings are less studied owing to limited preparative approaches. Their inherent ring strain makes their synthesis thermodynamically unfavourable and hinders the exploration of their properties and applications. Here we report a triplet energy transfer catalysis for crafting air-stable benzoboretenes through intramolecular coupling of boron-carbon-centred diradicals. In addition, by modulating substrate π-conjugation structures and excitation energies, boron-carbon-centred diradicals can undergo formal 1,6- and 1,5-cyclization to deliver dihydroborinine and dihydrocyclopropaborole derivatives, respectively. The metal-free neutral reaction conditions ensure a broad reaction scope, resulting in structurally diverse boracycles that are stable enough to be purified via column chromatography. Further modification of the boracycles enables the facile synthesis of oxaborabicycles and dihydroborinine-fused polycyclic aromatic hydrocarbons with unique optoelectronic properties.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"17 5","pages":"663-671"},"PeriodicalIF":19.2,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143972380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Progress and future directions in borophene research. 硼罗芬研究进展及未来发展方向。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-05-01 Epub Date: 2025-04-07 DOI: 10.1038/s41557-025-01773-4

Qiucheng Li, Eden B Aklile, Albert Tsui, Mark C Hersam

引用次数: 0

Synthesis of zwitterionic open-shell bilayer spironanographenes. 两性离子开壳双层螺环石墨烯的合成。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-04-30 DOI: 10.1038/s41557-025-01810-2

Juan Lión-Villar, Jesús M Fernández-García, Samara Medina Rivero, Josefina Perles, Shaofei Wu, Daniel Aranda, Jishan Wu, Shu Seki, Juan Casado, Nazario Martín

{"title":"Synthesis of zwitterionic open-shell bilayer spironanographenes.","authors":"Juan Lión-Villar, Jesús M Fernández-García, Samara Medina Rivero, Josefina Perles, Shaofei Wu, Daniel Aranda, Jishan Wu, Shu Seki, Juan Casado, Nazario Martín","doi":"10.1038/s41557-025-01810-2","DOIUrl":"https://doi.org/10.1038/s41557-025-01810-2","url":null,"abstract":"Molecular nanographenes (NGs) are nanoscale graphene fragments obtained by organic synthetic protocols. Here we report the bottom-up synthesis of two spiro-NGs formed by two substituted hexa-peri-hexabenzocoronenes (HBCs), spiro-NG and F-spiro-NG. The X-ray crystal structure of the deca-tert-butyl-functionalized spiro-NG shows a bilayer disposition of the HBCs in face-to-face contact. By contrast, F-spiro-NG, which features tert-butyl substituents on one HBC unit, and fluorine on the other HBC unit, is an electron donor-acceptor bilayer NG. The structural assembly of the donor and acceptor graphenic layers enables an electron-transfer process that leads to the formation of a zwitterionic open shell, paramagnetic species constituted by a radical cation and a radical anion located in the donor and the acceptor HBCs, respectively. Magnetic and spectroelectrochemical experiments, together with theoretical calculations, support the persistent/dominant charge-separated nature of F-spiro-NG. Furthermore, photoconductivity measurements show a significant increase of the charge carrier mobility in the case of F-spiro-NG (Σμ = 6 cm2 V-1 s-1) compared with spiro-NG.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144025265","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Bench-stable boracyclobutenes Bench-stable boracyclobutenes

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-28 DOI: 10.1038/s41557-025-01814-y

Leo Wessel, René Frank

引用次数: 0

Transition-metal-free ammonia synthesis 无过渡金属氨合成

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-24 DOI: 10.1038/s41557-025-01806-y

Yeqin Guan, Ping Chen

引用次数: 0

Porous metal–organic polyhedra with a gecko’s grip 多孔金属有机多面体和壁虎的抓地力

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-24 DOI: 10.1038/s41557-025-01811-1

Vincent Guillerm

引用次数: 0

Lanthanide-nickel molecular intermetallic complexes featuring a ligand-free Ni^2- anion in endohedral fullerenes. 内嵌富勒烯中具有无配体Ni2阴离子的镧系镍分子金属间配合物。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-04-23 DOI: 10.1038/s41557-025-01802-2

Panfeng Chuai, Ziqi Hu, Yang-Rong Yao, Zhanxin Jiang, Aman Ullah, Ya Zhao, Weiren Cheng, Muqing Chen, Eugenio Coronado, Shangfeng Yang, Zujin Shi

{"title":"Lanthanide-nickel molecular intermetallic complexes featuring a ligand-free Ni2- anion in endohedral fullerenes.","authors":"Panfeng Chuai, Ziqi Hu, Yang-Rong Yao, Zhanxin Jiang, Aman Ullah, Ya Zhao, Weiren Cheng, Muqing Chen, Eugenio Coronado, Shangfeng Yang, Zujin Shi","doi":"10.1038/s41557-025-01802-2","DOIUrl":"https://doi.org/10.1038/s41557-025-01802-2","url":null,"abstract":"Transition metals (TMs) typically exhibit rich redox chemistry and can be found in various oxidation states. In most cases, TMs are positively charged. Strong π-accepting ligands have been shown to stabilize molecular complexes with TMs in formal negative oxidation states. By contrast, organic-ligand-free TM anions remain rare, limited to intermetallic compounds based on third-row TMs such as gold or platinum. Here we report the synthesis of air-stable lanthanide-nickel molecular intermetallic complexes featuring a ligand-free Ni2- confined within fullerenes, namely, Tb2Ni@C82. The charged Tb2Ni lanthanide nickelide cluster forms metal-only Lewis pairs, featuring strongly polarized Tb-Ni covalent bonds with short bond lengths in the range of 2.50-2.57 Å. X-ray absorption spectroscopy supports the -2 oxidation state of Ni with 3d104s2 electron count, in line with the spectroscopic and magnetic measurements, and theoretical study. This finding opens up an efficient way to stabilize intermetallic clusters with elusive nucleophilic TM anions by confining them inside molecular carbon cages.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144014003","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0