Communications Chemistry最新文献_第9页

Toward decoding spatiotemporal signaling activities of reactive immunometabolites with precision immuno-chemical biology tools 利用精准免疫化学生物学工具解码反应性免疫代谢物的时空信号活动

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-02 DOI: 10.1038/s42004-024-01282-4

Kuan-Ting Huang, Yimon Aye

{"title":"Toward decoding spatiotemporal signaling activities of reactive immunometabolites with precision immuno-chemical biology tools","authors":"Kuan-Ting Huang, Yimon Aye","doi":"10.1038/s42004-024-01282-4","DOIUrl":"10.1038/s42004-024-01282-4","url":null,"abstract":"Immune-cell reprogramming driven by mitochondria-derived reactive electrophilic immunometabolites (mt-REMs—e.g., fumarate, itaconate) is an emerging phenomenon of major biomedical importance. Despite their localized production, mt-REMs elicit significantly large local and global footprints within and across cells, through mechanisms involving electrophile signaling. Burgeoning efforts are being put into profiling mt-REMs’ potential protein-targets and phenotypic mapping of their multifaceted inflammatory behaviors. Yet, precision indexing of mt-REMs’ first-responders with spatiotemporal intelligence and locale-specific function assignments remain elusive. Highlighting the latest advances and overarching challenges, this perspective aims to stimulate thoughts and spur interdisciplinary innovations to address these unmet chemical-biotechnological needs at therapeutic immuno-signaling frontiers. Immune-cell reprogramming driven by mitochondria-derived reactive electrophilic immunometabolites (mt-REMs) is an emerging phenomenon of major biomedical importance. Here, the authors highlight the latest advances and overarching challenges in precision indexing of mt-REMs’ cellular responses with spatiotemporal intelligence and locale-specific function assignments.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-16"},"PeriodicalIF":5.9,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01282-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142117971","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

Molecular geometry specific Monte Carlo simulation of the efficacy of diamond crystal formation from diamondoids 针对金刚石晶体形成效率的分子几何蒙特卡洛模拟

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-01 DOI: 10.1038/s42004-024-01261-9

Ta Tang, Sulgiye Park, Thomas Peter Devereaux, Yu Lin, Chunjing Jia

{"title":"Molecular geometry specific Monte Carlo simulation of the efficacy of diamond crystal formation from diamondoids","authors":"Ta Tang, Sulgiye Park, Thomas Peter Devereaux, Yu Lin, Chunjing Jia","doi":"10.1038/s42004-024-01261-9","DOIUrl":"10.1038/s42004-024-01261-9","url":null,"abstract":"Diamondoids are a class of organic molecules with the carbon skeletons isostructural to nano-diamond, and have been shown to be promising precursors for diamond formation. In this work, the formation of diamond crystals from various diamondoid molecule building blocks was studied using our developed molecular geometry specific Monte Carlo method. We maintained the internal carbon skeletons of the diamondoid molecules, and investigated how the carbon-carbon bonds form between diamondoid molecules and how efficient the process is to form diamond crystals. The simulations show that higher diamondoid molecules can produce structures closer to a diamond crystal compared with lower diamondoid molecules. Specifically, using higher diamondoid molecules, larger bulk diamond crystals are formed with fewer vacancies. The higher propensity of certain diamondoids to form diamond crystals reveals insights into the microscopic processes of diamond formation under high-pressure high-temperature conditions. Diamondoids are a series of hydrogen-terminated nanometer-sized hydrocarbons that can be used to synthesize high-quality diamond crystals. Here, the authors use Monte Carlo simulations to study the potentials of different diamondoids in constructing diamond crystals with the assumption that the carbon skeletons keep intact, and find that higher diamondoid molecules are most suitable.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-5"},"PeriodicalIF":5.9,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01261-9.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142100550","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

Deposition temperature-mediated growth of helically shaped polymers and chevron-type graphene nanoribbons from a fluorinated precursor 沉积温度介导的氟化前驱体螺旋形聚合物和雪佛龙型石墨烯纳米带的生长

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-31 DOI: 10.1038/s42004-024-01253-9

Jacob D. Teeter, Mamun Sarker, Wenchang Lu, Chenggang Tao, Arthur P. Baddorf, Jingsong Huang, Kunlun Hong, Jerry Bernholc, Alexander Sinitskii, An-Ping Li

{"title":"Deposition temperature-mediated growth of helically shaped polymers and chevron-type graphene nanoribbons from a fluorinated precursor","authors":"Jacob D. Teeter, Mamun Sarker, Wenchang Lu, Chenggang Tao, Arthur P. Baddorf, Jingsong Huang, Kunlun Hong, Jerry Bernholc, Alexander Sinitskii, An-Ping Li","doi":"10.1038/s42004-024-01253-9","DOIUrl":"10.1038/s42004-024-01253-9","url":null,"abstract":"Graphene nanoribbons (GNRs) of precise size and shape, critical for controlling electronic properties and future device applications, can be realized via precision synthesis on surfaces using rationally designed molecular precursors. Fluorine-bearing precursors have the potential to form GNRs on nonmetallic substrates suitable for device fabrication. Here, we investigate the deposition temperature-mediated growth of a new fluorine-bearing precursor, 6,11-diiodo-1,4-bis(2-fluorophenyl)-2,3-diphenyltriphenylene (C42H24F2I2), into helically shaped polymer intermediates and chevron-type GNRs on Au(111) by combining scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory simulations. The fluorinated precursors do not adsorb on the Au(111) surface at lower temperatures, necessitating an optimum substrate temperature to achieve maximum polymer and GNR lengths. We compare the adsorption behavior with that of pristine chevron precursors and discuss the effects of C-H and C-F bonds. The results elucidate the growth mechanism of GNRs with fluorine-bearing precursors and establish a foundation for future synthesis of GNRs on nonmetallic substrates. Fluorine-bearing precursors offer new opportunities for the on-surface synthesis of graphene nanoribbons, but the growth conditions are critical for achieving optimal results. Here, the authors investigate the deposition temperature-mediated growth of helically shaped polymers and graphene nanoribbons on Au(111) from an internally fluorinated precursor.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01253-9.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142100539","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

Absence of a link between stabilized charge-separated state and structural changes proposed from crystal structures of a photosynthetic reaction center 根据光合作用反应中心晶体结构提出的稳定电荷分离状态与结构变化之间缺乏联系

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-30 DOI: 10.1038/s42004-024-01281-5

Tomoyasu Noji, Keisuke Saito, Hiroshi Ishikita

{"title":"Absence of a link between stabilized charge-separated state and structural changes proposed from crystal structures of a photosynthetic reaction center","authors":"Tomoyasu Noji, Keisuke Saito, Hiroshi Ishikita","doi":"10.1038/s42004-024-01281-5","DOIUrl":"10.1038/s42004-024-01281-5","url":null,"abstract":"Structural differences between illuminated and unilluminated crystal structures led to the proposal that the charge-separated state was stabilized by structural changes in its membrane extrinsic protein subunit H in a bacterial photosynthetic reaction center [Katona, G. et al. Nat. Struct. Mol. Biol. 2005, 12, 630–631]. Here, we explored the proposal by titrating all titratable sites and calculating the redox potential (Em) values in these crystal structures. Contrary to the expected charge-separated states, Em for quinone, Em(QA/QA•–), is even lower in the proposed charge-separated structure than in the ground-state structure. The subunit-H residues, which were proposed to exhibit electron-density changes in the two crystal structures, contribute to an Em(QA/QA•–) difference of only <0.5 mV. Furthermore, the protonation states of the titratable residues in the entire reaction center are practically identical in the two structures. These findings indicate that the proposed structural differences are irrelevant to explaining the significant prolongation of the charge-separated-state lifetime. In bacterial photosynthetic reactions, charge-separated states are thought to be stabilized by structural changes in the membrane extrinsic protein subunit H. Here, the authors probe all titratable sites and calculate values of cofactors, and find that the redox potential for quinone is lower in the proposed charge-separated than in the ground-state structure and that the subunit-H residues contribute to a redox potential difference below 0.5 mV.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01281-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142100538","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

Hydrogen bonding patterns and cooperativity in polyproline II helical bundles 多脯氨酸 II 螺旋束中的氢键模式和合作性

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-30 DOI: 10.1038/s42004-024-01268-2

Rubén López-Sánchez, Douglas V. Laurents, Miguel Mompeán

{"title":"Hydrogen bonding patterns and cooperativity in polyproline II helical bundles","authors":"Rubén López-Sánchez, Douglas V. Laurents, Miguel Mompeán","doi":"10.1038/s42004-024-01268-2","DOIUrl":"10.1038/s42004-024-01268-2","url":null,"abstract":"Hydrogen bond cooperativity (HBC) plays an important role in stabilizing protein assemblies built by α-helices and β-sheets, the most common secondary structures. However, whether HBC exists in other types of protein secondary structures such as polyproline II (PPII) helices remains unexplored. This is intriguing, since PPII systems as assembling blocks are continuously emerging across multiple fields. Here, using a combination of computational chemistry tools and molecular modeling corroborated by experimental observables, we characterize the distinct H-bonding patterns present in PPII helical bundles and establish that HBC stabilizes intermolecular PPII helices as seen in other protein assemblies such as amyloid fibrils. In addition to cooperative interactions in canonical CO···HN H-bonds, we show that analogous interactions in non-canonical CO···HαCα H-bonds are relevant in Gly-rich PPII bundles, thus compensating for the inability of glycine residues to create hydrophobic cores. Our results provide a mechanistic explanation for the assembly of these bundles. Hydrogen bond cooperativity (HBC) plays an important role in the stability of protein assemblies built by α-helices and β-sheets, however, it remains unknown whether HBC also exists in polyproline II (PPII) helices. Here, the authors show that HBC stabilizes intermolecular PPII helices using computational chemistry tools and molecular modeling corroborated by experimental observations.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01268-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142100549","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

A dual growth mode unique for organic crystals relies on mesoscopic liquid precursors 有机晶体特有的双重生长模式依赖于介观液体前驱体。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-28 DOI: 10.1038/s42004-024-01275-3

Manasa Yerragunta, Akash Tiwari, Rajshree Chakrabarti, Jeffrey D. Rimer, Bart Kahr, Peter G. Vekilov

{"title":"A dual growth mode unique for organic crystals relies on mesoscopic liquid precursors","authors":"Manasa Yerragunta, Akash Tiwari, Rajshree Chakrabarti, Jeffrey D. Rimer, Bart Kahr, Peter G. Vekilov","doi":"10.1038/s42004-024-01275-3","DOIUrl":"10.1038/s42004-024-01275-3","url":null,"abstract":"Organic solvents host the synthesis of high-value crystals used as pharmaceuticals and optical devices, among other applications. A knowledge gap persists on how replacing the hydrogen bonds and polar attraction that dominate aqueous environments with the weaker van der Waals forces affects the growth mechanism, including its defining feature, whether crystals grow classically or nonclassically. Here we demonstrate a rare dual growth mode of etioporphyrin I crystals, enabled by liquid precursors that associate with crystal surfaces to generate stacks of layers, which then grow laterally by incorporating solute molecules. Our findings reveal the precursors as mesoscopic solute-rich clusters, a unique phase favored by weak bonds such as those between organic solutes. The lateral spreading of the precursor-initiated stacks of layers crucially relies on abundant solute supply directly from the solution, bypassing diffusion along the crystal surface; the direct incorporation pathway may, again, be unique to organic solvents. Clusters that evolve to amorphous particles do not seamlessly integrate into crystal lattices. Crystals growing fast and mostly nonclassically at high supersaturations are not excessively strained. Our findings demonstrate that the weak interactions typical of organic systems promote nonclassical growth modes by supporting liquid precursors and enabling the spreading of multilayer stacks. Organic solvents are used to produce high-value crystals such as pharmaceuticals, organic semiconductors, and optical devices, but our understanding of the fundamental processes of crystal growth from organic solutions is limited. Here, the authors use time-resolved in situ atomic force microscopy to show a nonclassical, dual growth mode of etioporphyrin I crystals from mesoscopic solute-rich clusters.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-12"},"PeriodicalIF":5.9,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01275-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142092495","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

Post-spinel-type AB2O4 high-pressure phases in geochemistry and materials science 地球化学和材料科学中的后尖晶石型 AB2O4 高压相。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-27 DOI: 10.1038/s42004-024-01278-0

Masaki Akaogi, Takayuki Ishii, Kazunari Yamaura

引用次数: 0

Plasmon-driven chemical transformation of a secondary amide probed by surface enhanced Raman scattering 通过表面增强拉曼散射探测仲酰胺的等离子体驱动化学变化。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-27 DOI: 10.1038/s42004-024-01276-2

Anushree Dutta, Milan Ončák, Farhad Izadi, Eugene Arthur-Baidoo, João Ameixa, Stephan Denifl, Ilko Bald

{"title":"Plasmon-driven chemical transformation of a secondary amide probed by surface enhanced Raman scattering","authors":"Anushree Dutta, Milan Ončák, Farhad Izadi, Eugene Arthur-Baidoo, João Ameixa, Stephan Denifl, Ilko Bald","doi":"10.1038/s42004-024-01276-2","DOIUrl":"10.1038/s42004-024-01276-2","url":null,"abstract":"Plasmon-driven chemical conversion is gaining burgeoning interest in the field of heterogeneous catalysis. Herein, we study the reactivity of N-methyl-4-sulfanylbenzamide (NMSB) at nanocavities of gold and silver nanoparticle aggregates under plasmonic excitation to gain understanding of the respective reaction mechanism. NMSB is a secondary amide, which is a frequent binding motive found in peptides and a common coupling product of organic molecules and biomolecules. Surface-enhanced Raman scattering (SERS) is used as a two-in-one in-situ spectroscopic tool to initiate the molecular transformation process and simultaneously monitor and analyze the reaction products. Supported by dissociative electron attachment (DEA) studies with the gas phase molecule, a hot electron-mediated conversion of NMSB to p-mercaptobenzamide and p-mercaptobenzonitrile is proposed at the plasmonic nanocavities. The reaction rate showed negligible dependence on the external temperature, ruling out the dominant role of heat in the chemical transformation at the plasmonic interface. This is reflected in the absence of a superlinear relationship between the reaction rate constant and the laser power density, and DEA and SERS studies indicate a hot-electron mediated pathway. We conclude that the overall reaction rate is limited by the availability of energetic hot electrons to the NMSB molecule. Photocatalysis driven by surface plasmons is a promising approach for light-driven chemical conversions of molecules under mild conditions. Here, the authors study the reactivity of N-methyl-4-sulfanylbenzamide (NMSB) at the nanocavities of gold and silver nanoparticle aggregates under plasmonic excitation and propose a hot electron-mediated conversion of NMSB to p-mercaptobenzamide and p-mercaptobenzonitrile.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-9"},"PeriodicalIF":5.9,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01276-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142072231","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

The malonyl/acetyl-transferase from murine fatty acid synthase is a promiscuous engineering tool for editing polyketide scaffolds 小鼠脂肪酸合成酶中的丙二酰/乙酰转移酶是一种编辑多酮支架的杂交工程工具。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-24 DOI: 10.1038/s42004-024-01269-1

Lynn Buyachuihan, Simon Reiners, Yue Zhao, Martin Grininger

{"title":"The malonyl/acetyl-transferase from murine fatty acid synthase is a promiscuous engineering tool for editing polyketide scaffolds","authors":"Lynn Buyachuihan, Simon Reiners, Yue Zhao, Martin Grininger","doi":"10.1038/s42004-024-01269-1","DOIUrl":"10.1038/s42004-024-01269-1","url":null,"abstract":"Modular polyketide synthases (PKSs) play a vital role in the biosynthesis of complex natural products with pharmaceutically relevant properties. Their modular architecture makes them an attractive target for engineering to produce platform chemicals and drugs. In this study, we demonstrate that the promiscuous malonyl/acetyl-transferase domain (MAT) from murine fatty acid synthase serves as a highly versatile tool for the production of polyketide analogs. We evaluate the relevance of the MAT domain using three modular PKSs; the short trimodular venemycin synthase (VEMS), as well as modules of the PKSs deoxyerythronolide B synthase (DEBS) and pikromycin synthase (PIKS) responsible for the production of the antibiotic precursors erythromycin and pikromycin. To assess the performance of the MAT-swapped PKSs, we analyze the protein quality and run engineered polyketide syntheses in vitro. Our experiments include the chemoenzymatic synthesis of fluorinated macrolactones. Our study showcases MAT-based reprogramming of polyketide biosynthesis as a facile option for the regioselective editing of substituents decorating the polyketide scaffold. Modular polyketide synthases (PKSs) play a vital role in the biosynthesis of complex natural products with pharmaceutically relevant properties, and their modular architecture makes them an attractive target for engineering to produce platform chemicals and drugs. In this study, the authors demonstrate that the promiscuous malonyl/acetyl-transferase domain (MAT) from murine fatty acid synthase serves as a highly versatile tool for the production of polyketide analogs.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-15"},"PeriodicalIF":5.9,"publicationDate":"2024-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01269-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142055159","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

Modulation between capacitor and conductor for a redox-active 2D bis(terpyridine)cobalt(II) nanosheet via anion-exchange 通过阴离子交换在具有氧化还原活性的二维双（特吡啶）钴（II）纳米片的电容器和导体之间进行调节。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-22 DOI: 10.1038/s42004-024-01274-4

Kenji Takada, Miyu Ito, Naoya Fukui, Hiroshi Nishihara

{"title":"Modulation between capacitor and conductor for a redox-active 2D bis(terpyridine)cobalt(II) nanosheet via anion-exchange","authors":"Kenji Takada, Miyu Ito, Naoya Fukui, Hiroshi Nishihara","doi":"10.1038/s42004-024-01274-4","DOIUrl":"10.1038/s42004-024-01274-4","url":null,"abstract":"Ionic polymers are intriguing materials whose functionality arises from the synergy between ionic polymer backbones and counterions. A key method for enhancing their functionality is the post-synthetic ion-exchange reaction, which is instrumental in improving the chemical and physical properties of polymer backbones and introducing of the functionalities of the counterions. Electronic interaction between host polymer backbone and guest ions plays pivotal roles in property modulation. The current study highlights the modulation of responses to external electric field in cationic bis(terpyridine)cobalt(II) polymer nanofilms through anion-exchange reactions. Initially, as-prepared chloride-containing polymers exhibited supercapacitor behaviour. Introducing anionic metalladithiolenes into the polymers altered the behaviour to either conductive or insulative, depending on the valence of the metalladithiolenes. This modulation was accomplished by fine tuning of charge-transfer interactions between the bis(terpyridine)cobalt(II) complex moieties and redox-active anions. Our findings open up new avenue for ionic polymers, showcasing their potential as versatile platform in materials science. Post-synthetic ion-exchange is a key method for tuning the chemical and physical properties of ionic polymers, but achieving control over functionality through ion-exchange remains challenging. Here, anion-exchange within a redox-active bis(terpyridine)cobalt(II) polymer enables modulation between capacitor and conductor behaviours in response to an external electric field.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-8"},"PeriodicalIF":5.9,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01274-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142035384","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