Communications Chemistry最新文献_第7页

Synthesis and application of a photocaged-L-lactate for studying the biological roles of L-lactate. 光笼型l -乳酸盐的合成及应用，研究l -乳酸盐的生物学作用。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-05 DOI: 10.1038/s42004-025-01495-1

Ikumi Miyazaki, Kelvin K Tsao, Yuki Kamijo, Yusuke Nasu, Takuya Terai, Robert E Campbell

{"title":"Synthesis and application of a photocaged-L-lactate for studying the biological roles of L-lactate.","authors":"Ikumi Miyazaki, Kelvin K Tsao, Yuki Kamijo, Yusuke Nasu, Takuya Terai, Robert E Campbell","doi":"10.1038/s42004-025-01495-1","DOIUrl":"10.1038/s42004-025-01495-1","url":null,"abstract":"L-Lactate, once considered a metabolic waste product of glycolysis, is now recognized as a vitally important metabolite and signaling molecule in multiple biological pathways. However, exploring L-lactate's emerging intra- and extra-cellular roles is hindered by a lack of tools to perturb L-lactate concentration intracellularly and extracellularly. Photocaged compounds are a powerful way to introduce bioactive molecules with spatiotemporal precision using illumination. Here, we report the development of a photocaged derivative of L-lactate, 4-methoxy-7-nitroindolinyl-L-lactate (MNI-L-lac), that releases L-lactate upon illumination. We validated MNI-L-lac in cell culture by demonstrating that the photorelease of L-lactate elicits a response from genetically encoded extra- and intracellular L-lactate biosensors (eLACCO1, eLACCO2.1, R-iLACCO1.2). To demonstrate the utility of MNI-L-lac, we employed the photorelease of L-lactate to activate G protein-coupled receptor 81 (GPR81), as revealed by the inhibition of adenylyl cyclase activity and concomitant decrease of cAMP. These results indicate that MNI-L-lac may be useful for perturbing the concentration of endogenous L-lactate in order to investigate L-lactate's roles in metabolic and signaling pathways.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"104"},"PeriodicalIF":5.9,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11972357/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143788103","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tuning the electronic states of Pd(II) defect-engineered metal-organic framework catalysts for efficient conversion of isocyanides. 调节钯（II）缺陷工程金属有机框架催化剂的电子态以实现异氰酸酯的高效转化。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-05 DOI: 10.1038/s42004-025-01492-4

Shaoting Su, Yilei Cao, Yanwei Ren, Huanfeng Jiang, Wanqing Wu

{"title":"Tuning the electronic states of Pd(II) defect-engineered metal-organic framework catalysts for efficient conversion of isocyanides.","authors":"Shaoting Su, Yilei Cao, Yanwei Ren, Huanfeng Jiang, Wanqing Wu","doi":"10.1038/s42004-025-01492-4","DOIUrl":"10.1038/s42004-025-01492-4","url":null,"abstract":"Recently, defective sites in MOFs have become an important tool for tuning the catalytic performance of MOFs. Herein, we report a heterogeneous catalyst \"Pd-UiO-67(N)x\" by utilizing the active site of defective MOF to modulate the electronic state of Pd, which demonstrates excellent catalytic performances in the oxidative cyclization reaction of isocyanides with o-aminophenols benefiting from the electron-deficient nature of the Pd species. When the Pd loading in defective Pd-UiO-67(N)x system was decreased to 0.37 mol %, the catalytic efficiency was significantly enhanced and the Pd turnover number (TON) increased to 232, which was 27 and 2.6 times higher than that of homogeneous Pd catalysts and defect-free Pd-UiO-67(N)0, respectively. The open pore structure of d-MOFs supports the adsorption of o-aminophenols. Additionally, the domain-limiting effect of the framework restricts the aggregation of Pd, resulting in good stability of the Pd species, which without significant loss of its activity in five consecutive reaction cycles. This work provides an insight into the improvement of stereoelectronic properties of organometallic catalysts through defect-engineered MOFs.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"105"},"PeriodicalIF":5.9,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11972350/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143788105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Streamlined gram-scale natural N-glycan production using reversible tagging after oxidative release of natural glycans. 流线型克级天然n -聚糖生产使用可逆标记氧化释放后的天然聚糖。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-04 DOI: 10.1038/s42004-025-01499-x

Qing Zhang, Yi Lasanajak, Menxin Yan, Golden Chen, Xuezheng Song

{"title":"Streamlined gram-scale natural N-glycan production using reversible tagging after oxidative release of natural glycans.","authors":"Qing Zhang, Yi Lasanajak, Menxin Yan, Golden Chen, Xuezheng Song","doi":"10.1038/s42004-025-01499-x","DOIUrl":"10.1038/s42004-025-01499-x","url":null,"abstract":"The study of natural glycans is fundamental to modern glycomics; however, the functional analysis of these glycans is limited by their low natural abundance, structural heterogeneity, and the absence of efficient preparative-scale isolation methods. Here, we present a streamlined approach for the gram-scale production of complex natural N-glycans in their reducing form by combining oxidative release of natural glycans (ORNG) using household bleach, an innovative cleavable tag chemistry, and optimized multi-dimensional chromatography. Our ORNG process releases N-glycans from kilogram-scale of natural sources containing various glycoproteins, which can be efficiently attached with a 4-aminobenzoate tag, facilitating the selective separation of these glycans from other biomolecules. The tagged glycans can be purified via dry-load HILIC flash chromatography at gram scale followed by reverse-phase HPLC. Treatment with Oxone quantitatively cleaves the tag, regenerating the free reducing N-glycans in high yield. This method provides an accessible, gram-scale source of complex N-glycans, including complex asymmetric structures that are challenging to synthesize through conventional chemoenzymatic approaches. We believe this approach represents a versatile strategy for acquiring complex natural glycans, opening new avenues for the functional exploration of N-glycans in glycoscience.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"103"},"PeriodicalIF":5.9,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11971423/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143788100","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Impact of a Terahertz electromagnetic field on the ion permeation of potassium and sodium channels. 太赫兹电磁场对钾和钠离子通道渗透的影响。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-03 DOI: 10.1038/s42004-025-01503-4

Zigang Song, Lingfeng Xue, Qi Ouyang, Chen Song

{"title":"Impact of a Terahertz electromagnetic field on the ion permeation of potassium and sodium channels.","authors":"Zigang Song, Lingfeng Xue, Qi Ouyang, Chen Song","doi":"10.1038/s42004-025-01503-4","DOIUrl":"10.1038/s42004-025-01503-4","url":null,"abstract":"Ion channels are essential for various physiological processes, and their defects are associated with many diseases. Previous research has revealed that a Terahertz electromagnetic field can alter the channel conductance by affecting the motion of chemical groups of ion channels, and hence regulate the electric signals of neurons. In this study, we conducted molecular dynamics simulations to systematically investigate the effects of terahertz electromagnetic fields on the ion permeation of voltage-gated potassium and sodium channels, particularly focusing on the bound ions in the selectivity filters that have not been extensively studied previously. Our results identified multiple new characteristic frequencies and showed that 1.4, 2.2, or 2.9 THz field increases the ion permeability of Kv1.2, and 2.5 or 48.6 THz field increases the ion permeability of Nav1.5. Such effects are specific to the frequencies and directions of the electric field, which are determined by the intrinsic oscillation motions of the permeating ions in the selectivity filter or certain chemical groups of the ion channels. The amplitude of the THz field positively correlates with the change in ion permeation. This study demonstrates that THz fields can specifically regulate ion channel conductances by multiple mechanisms, which may carry great potential in biomedical applications.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"101"},"PeriodicalIF":5.9,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11965498/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143771700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Interfacial lithiation of lithium aluminum titanium phosphate explored by ⁷Li NMR. 用7Li核磁共振研究磷酸铝钛锂的界面锂化。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-03 DOI: 10.1038/s42004-025-01505-2

Annika Marko, Thomas Scheiber, Bernhard Gadermaier, H Martin R Wilkening

{"title":"Interfacial lithiation of lithium aluminum titanium phosphate explored by 7Li NMR.","authors":"Annika Marko, Thomas Scheiber, Bernhard Gadermaier, H Martin R Wilkening","doi":"10.1038/s42004-025-01505-2","DOIUrl":"10.1038/s42004-025-01505-2","url":null,"abstract":"Lithium aluminum titanium phosphate (LATP) is well-established as a crystalline electrolyte offering fast Li+ diffusion pathways. However, when in contact with lithium metal, LATP forms a mixed-conducting interphase, potentially impacting the performance of LATP-based batteries. During lithiation, Ti4+ is partially reduced to form Ti3+, and Li+ occupies vacant sites within the NaSICON-type structure. Here, we employed 7Li nuclear magnetic resonance (NMR) to investigate changes in Li+ diffusivity induced by chemical lithiation using n-butyllithium. Chemical lithiation allowed us to mimic the structural and dynamic changes occurring within a lithium metal battery. Our findings reveal that lithiation does not hinder Li+ diffusivity; rather, 7Li NMR relaxation measurements indicate enhanced Li+ ion hopping processes. Despite the formation of a lithiated interfacial layer that propagates inward, the dynamic properties of LATP-characterized by Li-rich and Li-poor domains-remain resilient. These results highlight that electrochemical degradation does not compromise the intrinsic ion dynamics of LATP.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"102"},"PeriodicalIF":5.9,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11968875/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143779345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Topologically-crosslinked hydrogels based on γ-cyclodextrins. 基于γ-环糊精的拓扑交联水凝胶。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-02 DOI: 10.1038/s42004-025-01469-3

Ella Sapsford, Davide Michieletto

{"title":"Topologically-crosslinked hydrogels based on γ-cyclodextrins.","authors":"Ella Sapsford, Davide Michieletto","doi":"10.1038/s42004-025-01469-3","DOIUrl":"10.1038/s42004-025-01469-3","url":null,"abstract":"Biomimetic strategies are increasingly the focus of materials scientists looking to improve or invent new materials. Topology is an important component in nature, but the synthetic incorporation of mechanically interlocked moieties is challenging. Rotaxanes are one of the simplest ways to introduce topological complexity to a polymer gel. As mobile crosslinks, the rotaxane's cyclic host molecules redistributes applied stress typically endowing the material with enhanced toughness and stretchability. Gamma-cyclodextrin (γ-CD) is a larger homologue of alpha-cyclodextrin (α-CD) and it allows uncommon double-threaded topologies to be synthesised without metal templating removing additional synthetic steps and toxicity. γ-CDs are good candidates for a slide-ring crosslinkers that, added to a commodity or novel polymer, could augment the mechanical properties of hydrogels in novel ways with respect to traditional polyrotaxanes and slide-ring gels (SRGs). Despite the rapid uptake of γ-CD as novel mechanical crosslinkers, the body of literature is currently limited. In this paper we thus review recent works on γ-CD functionalised materials, offer a comparison with α-CD materials, and compare the mechanical performance of the papers discussed in plots of material properties. Finally, we discuss potential directions and unique uses of γ-CD uncommon double-threaded topology.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"99"},"PeriodicalIF":5.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11965564/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143771721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Towards precision medicine using biochemically triggered cleavable conjugation. 使用生化触发可切割偶联的精准医学。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-02 DOI: 10.1038/s42004-025-01491-5

Badri Parshad, Smriti Arora, Balram Singh, Yuanwei Pan, Jianbin Tang, Zhigang Hu, Hirak K Patra

{"title":"Towards precision medicine using biochemically triggered cleavable conjugation.","authors":"Badri Parshad, Smriti Arora, Balram Singh, Yuanwei Pan, Jianbin Tang, Zhigang Hu, Hirak K Patra","doi":"10.1038/s42004-025-01491-5","DOIUrl":"10.1038/s42004-025-01491-5","url":null,"abstract":"Personalised and precision medicines are emerging as the future of therapeutic strategies. Biochemically triggered cleavable conjugation is thus crucial and timely due to its potential to response as per the loco-regional environment. It enables targeted release of therapeutic agents in response to specific biochemical signals and thus minimizing off-target effects and improving treatment precision. It holds promise in a range of biomedical applications, including cancer therapy, senolytic therapy, gene therapy, and regenerative medicine. The focus of this review is to offer comprehensive insight into the significance of biochemically cleavable conjugations within intrinsically stimuli-responsive architectures. Pathological conditions and alteration in tissues microenvironment in the body exhibit distinct biochemical settings characterized by change in redox potential, pH level, hypoxia, reactive oxygen species (ROS), and various catalytic protein/enzyme overexpression. Understanding these intrinsic features is crucial for researchers aiming to develop intelligent cleavable bio-engineered systems for biomedicines. By strategically designing cleavable linkage, researchers can leverage the variations in the tumor, infection, inflammation, and senescence microenvironments. Through an extensive examination of relevant literature, we present a comprehensive classification of the intrinsic physicochemical differences found in pathological areas and their applications in drug delivery, prodrug activation, imaging, and theranostics for future personalised medicines. This review will provide comprehensive guidance and critical insights to researchers in both industry and academia who are involved in the design of advanced, functional biochemically cleavable conjugations.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"100"},"PeriodicalIF":5.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11965331/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143771726","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Development of potential immunomodulatory ligands targeting natural killer T cells inspired by gut symbiont-derived glycolipids. 由肠道共生体衍生的糖脂激发的靶向自然杀伤T细胞的潜在免疫调节配体的开发。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-01 DOI: 10.1038/s42004-025-01497-z

Jesang Lee, Sumin Son, Minha Lee, Seung Bum Park

{"title":"Development of potential immunomodulatory ligands targeting natural killer T cells inspired by gut symbiont-derived glycolipids.","authors":"Jesang Lee, Sumin Son, Minha Lee, Seung Bum Park","doi":"10.1038/s42004-025-01497-z","DOIUrl":"10.1038/s42004-025-01497-z","url":null,"abstract":"α-Galactosylceramide (α-GalCer) is a prototypical antigen recognized by natural killer T (NKT) cells, a subset of T cells crucial for immune regulation. Despite its significance, the complex structure-activity relationship of α-GalCer and its analogs remains poorly understood, particularly in defining the structural determinants of NKT cell responses. In this study, we designed and synthesized potential immunomodulatory ligands targeting NKT cells, inspired by glycolipids derived from the gut symbiont Bacteroides fragilis. A series of α-GalCer analogs with terminal iso-branched sphinganine backbones was developed through rational modification of the acyl chain. Our results identified the C3' hydroxyl group as a structural element that impairs glycolipid presentation by CD1d, as evidenced by reduced IL-2 secretion and weak competition with a potent CD1d ligand. Notably, among C3'-deoxy α-GalCer analogs, those containing an α-chloroacetamide group exhibited robust NKT cell activation with Th2 selectivity. Computational docking and mass spectrometry analyses further confirmed the substantial interaction of α-chloroacetamide analogs to CD1d. These findings underscore the potential of leveraging microbiota-derived glycolipid structures to selectively modulate NKT cell functions for therapeutic purposes.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"98"},"PeriodicalIF":5.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11961698/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143763059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ab-initio dynamic study of mechanisms for dust-mediated molecular hydrogen formation in space. 空间尘埃介导的分子氢形成机制的从头算动力学研究。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-01 DOI: 10.1038/s42004-025-01489-z

Yuzhen Guo, David R McKenzie

{"title":"Ab-initio dynamic study of mechanisms for dust-mediated molecular hydrogen formation in space.","authors":"Yuzhen Guo, David R McKenzie","doi":"10.1038/s42004-025-01489-z","DOIUrl":"10.1038/s42004-025-01489-z","url":null,"abstract":"The reason for the abundance of molecular hydrogen (H2) in space remains unresolved. Here we study collision dynamics under spacelike conditions to test H2 formation mechanisms where carbonaceous dust grains may have a catalytic role. Density functional theory molecular dynamics simulates atomic hydrogen capture and H2 formation on the surface of buckminsterfullerene as a carbonaceous cosmic dust model. Maximally localized Wannier functions are applied to examine the electronic bonding during transition states. The fullerene surface is shown to be effective at warm (50K) and low (10K) temperatures in achieving atomic H chemisorption, potentially explaining the observed broad temperature range for efficient H2 formation. We revise the Eley-Rideal mechanism and propose that both it and the Langmuir-Hinshelwood mechanism, induced by thermal hopping, contribute to bursts of H2 formation during energetic events. Additionally, we show how fullerene maintains the abundance of H2 in space by selectively preventing H2 molecules from capture.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"97"},"PeriodicalIF":5.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11961578/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143763052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Impact of stack pressure on coulometric titration time analysis. 堆压对库仑滴定时间分析的影响。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-04-01 DOI: 10.1038/s42004-025-01496-0

Jaka Sivavec, Kostiantyn V Kravchyk, Maksym V Kovalenko

引用次数: 0