Nature chemistry最新文献_第2页

Switchable skeletal editing of quinolines enabled by cyclizative sequential rearrangements. 通过循环顺序重排实现喹啉类的可切换骨架编辑。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-04-07 DOI: 10.1038/s41557-025-01793-0

Di Tian, Yu-Ping He, Lu-Sen Yang, Zhuo-Chen Li, Hua Wu

{"title":"Switchable skeletal editing of quinolines enabled by cyclizative sequential rearrangements.","authors":"Di Tian, Yu-Ping He, Lu-Sen Yang, Zhuo-Chen Li, Hua Wu","doi":"10.1038/s41557-025-01793-0","DOIUrl":"https://doi.org/10.1038/s41557-025-01793-0","url":null,"abstract":"The rapid diversification of core ring structures in complex molecules through switchable skeletal editing is valuable in the drug discovery process. However, controllable methods for chemically divergent modifications of azaarene frameworks using common substrates are challenging, despite the potential to maximize structural diversity and complexity. Here we report the tunable skeletal editing of quinolines through Brønsted acid-catalysed multicomponent reactions of quinoline N-oxides, dialkyl acetylenedicarboxylates and water to generate nitrogen-containing heteroaromatic compounds together with linear compounds in a modular fashion. Specifically, in a one-pot procedure, after cyclization and sequential rearrangement processes, the quinoline N-oxides are easily converted into unique 2-substituted indolines. These then undergo acid-promoted fragmentation to give indoles, base-facilitated ring-opening to afford 2-alkenylanilines and oxidative cyclization to yield isoquinolinones. Catalytic asymmetric skeletal editing of quinolines is also realized, providing enantioenriched benzazepines bearing quaternary stereocentres, and late-stage skeletal modification of quinoline cores in several drugs is demonstrated.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143803894","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

Hyperfine-to-rotational energy transfer in ultracold atom–molecule collisions of Rb and KRb Rb和KRb超冷原子-分子碰撞中的超精细到旋转的能量传递

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-07 DOI: 10.1038/s41557-025-01778-z

Yi-Xiang Liu, Lingbang Zhu, Jeshurun Luke, Mark C. Babin, Marcin Gronowski, Hela Ladjimi, Michał Tomza, John L. Bohn, Timur V. Tscherbul, Kang-Kuen Ni

{"title":"Hyperfine-to-rotational energy transfer in ultracold atom–molecule collisions of Rb and KRb","authors":"Yi-Xiang Liu, Lingbang Zhu, Jeshurun Luke, Mark C. Babin, Marcin Gronowski, Hela Ladjimi, Michał Tomza, John L. Bohn, Timur V. Tscherbul, Kang-Kuen Ni","doi":"10.1038/s41557-025-01778-z","DOIUrl":"https://doi.org/10.1038/s41557-025-01778-z","url":null,"abstract":"Energy transfer between different mechanical degrees of freedom in atom–molecule collisions has been studied and largely understood. However, systems involving spins remain less explored. In this study, we directly observed energy transfer from atomic hyperfine to molecular rotation in the 87Rb ((| {F}_{a},{M}_{{F}_{a}}rangle =| 2,2rangle)) + 40K87Rb (X1Σ+, rotational state N = 0) ⟶ Rb ((| 1,1rangle)) + KRb (N = 0, 1, 2) collision with state-to-state precision. We also performed quantum scattering calculations that rigorously included the coupling between spin and rotational degrees of freedom at short range under the assumption of rigid-rotor KRb monomers moving along a single potential energy surface. The calculated product rotational state distribution deviates from the observations even after extensive tuning of the atom–molecule potential energy surface. In addition, our ab initio calculations indicate that spin–rotation coupling is enhanced close to a conical intersection that is energetically accessible at short range. This, together with the deviation, suggests that vibrational degrees of freedom and conical intersections play an important part in the coupling. Our observations confirm that spin is coupled to mechanical rotation at short range and establish a benchmark for future theoretical studies.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"13 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798277","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

Praseodymium in the formal +5 oxidation state. 正态+5氧化态的镨。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-04-07 DOI: 10.1038/s41557-025-01797-w

Andrew C Boggiano, Chad M Studvick, Sabyasachi Roy Chowdhury, Julie E Niklas, Haruko Tateyama, Hongwei Wu, Johannes E Leisen, Florian Kleemiss, Bess Vlaisavljevich, Ivan A Popov, Henry S La Pierre

{"title":"Praseodymium in the formal +5 oxidation state.","authors":"Andrew C Boggiano, Chad M Studvick, Sabyasachi Roy Chowdhury, Julie E Niklas, Haruko Tateyama, Hongwei Wu, Johannes E Leisen, Florian Kleemiss, Bess Vlaisavljevich, Ivan A Popov, Henry S La Pierre","doi":"10.1038/s41557-025-01797-w","DOIUrl":"https://doi.org/10.1038/s41557-025-01797-w","url":null,"abstract":"Praseodymium in the +5 oxidation state is a long-sought connection between lanthanide, early-transition and actinide metal redox chemistries. Unique among the lanthanide series, evidence for molecular pentavalent praseodymium species has been observed in the gas phase and noble gas matrix isolation conditions. Here we report the low-temperature synthesis and characterization of a molecular praseodymium complex in the formal +5 oxidation state, [Pr5+(NPtBu3)4][X-] (where tBu = tert-butyl and X- = tetrakis(pentafluorophenyl)borate or hexafluorophosphate). Single-crystal X-ray diffraction, solution-state spectroscopic, solution magnetometric, density functional theory and multireference wavefunction-based methods indicate a highly multiconfigurational singlet ground state. An inverted ligand field drives this unique electronic structure, which establishes a critical link in understanding the bonding of high-valent metal complexes across the periodic table.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143803886","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 : 2025-04-07 DOI: 10.1038/s41557-025-01773-4

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

引用次数: 0

Author Correction: Monitoring the formation of infinite-layer transition metal oxides through in situ atomic-resolution electron microscopy 作者更正：通过原位原子分辨率电子显微镜监测无限层过渡金属氧化物的形成

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-07 DOI: 10.1038/s41557-025-01816-w

Yaolong Xing, Inhwan Kim, Kyeong Tae Kang, Jinho Byun, Woo Seok Choi, Jaekwang Lee, Sang Ho Oh

引用次数: 0

A glycan that performs catalysis 具有催化作用的聚糖

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-04 DOI: 10.1038/s41557-025-01794-z

引用次数: 0

Milking riboflavin for all it’s worth 榨取核黄素的全部价值

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-04-03 DOI: 10.1038/s41557-025-01781-4

Zoe A. Hoffpauir, Audrey L. Lamb

引用次数: 0

Optical control of gene expression using a DNA G-quadruplex targeting reversible photoswitch 利用DNA g -四重体靶向可逆光开关的基因表达光学控制

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-03 DOI: 10.1038/s41557-025-01792-1

Xiaoyun Zhang, Somdutta Dhir, Larry Melidis, Yuqi Chen, Zutao Yu, Angela Simeone, Jochen Spiegel, Santosh Adhikari, Shankar Balasubramanian

{"title":"Optical control of gene expression using a DNA G-quadruplex targeting reversible photoswitch","authors":"Xiaoyun Zhang, Somdutta Dhir, Larry Melidis, Yuqi Chen, Zutao Yu, Angela Simeone, Jochen Spiegel, Santosh Adhikari, Shankar Balasubramanian","doi":"10.1038/s41557-025-01792-1","DOIUrl":"https://doi.org/10.1038/s41557-025-01792-1","url":null,"abstract":"Transcriptional regulation is a dynamic process that coordinates diverse cellular activities, and the use of small molecules to perturb gene expression has propelled our understanding of the fundamental regulatory mechanisms. However, small molecules typically lack the spatiotemporal precision required in highly non-invasive, controlled settings. Here we present the development of a cell-permeable small-molecule DNA G-quadruplex (G4) binder, termed G4switch, that can be reversibly toggled on and off by visible light. We have biophysically characterized the light-mediated control of G4 binding in vitro, followed by cellular, genomic mapping of G4switch to G4 targets in chromatin to confirm G4-selective, light-dependent binding in a cellular context. By deploying G4switch in living cells, we show spatiotemporal control over the expression of a set of G4-containing genes and G4-associated cell proliferation. Our studies demonstrate a chemical tool and approach to interrogate the dynamics of key biological processes directly at the molecular level in cells.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"58 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766721","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

Activity of GPCR-targeted drugs influenced by human gut microbiota metabolism 人肠道菌群代谢对gpcr靶向药物活性的影响

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-03 DOI: 10.1038/s41557-025-01789-w

Qihao Wu, Deguang Song, Yanyu Zhao, Andrew A. Verdegaal, Tayah Turocy, Brianna Duncan-Lowey, Andrew L. Goodman, Noah W. Palm, Jason M. Crawford

{"title":"Activity of GPCR-targeted drugs influenced by human gut microbiota metabolism","authors":"Qihao Wu, Deguang Song, Yanyu Zhao, Andrew A. Verdegaal, Tayah Turocy, Brianna Duncan-Lowey, Andrew L. Goodman, Noah W. Palm, Jason M. Crawford","doi":"10.1038/s41557-025-01789-w","DOIUrl":"https://doi.org/10.1038/s41557-025-01789-w","url":null,"abstract":"Microbiota-mediated drug metabolism can affect pharmacological efficacy. Here we conducted a systematic comparative metabolomics investigation of drug metabolism modes by evaluating the impacts of human gut commensal bacteria on 127 G-protein-coupled receptor (GPCR)-targeted drugs. For the most extensively metabolized drugs in our screen, we elucidated both conventional and unconventional drug transformations and the corresponding activities of generated metabolites. Comparisons of drug metabolism by a gut microbial community versus individual species revealed both taxon intrinsic and collaborative processes that influenced the activity of the metabolized drugs against target GPCRs. We also observed iloperidone inactivation by generating unconventional metabolites. The human gut commensal bacteria mixture incorporated sulfur in the form of a thiophene motif, whereas Morganella morganii used a cascade reaction to incorporate amino-acid-derived tricyclic systems into the drug metabolites. Our results reveal a broad impact of human gut commensal bacteria on GPCR-targeted drug structures and activities through diverse microbiota-mediated biotransformations.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"112 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766720","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

Aliens among us 我们中间的外星人

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-04-03 DOI: 10.1038/s41557-025-01780-5

Michelle Francl

引用次数: 0