Communications Chemistry最新文献_第3页

Multiphase detection of crucial biological amines using a 2,4,6-tristyrylpyrylium dye.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-15 DOI: 10.1038/s42004-025-01459-5

Shivani Tripathi, Banchhanidhi Prusti, Manab Chakravarty

{"title":"Multiphase detection of crucial biological amines using a 2,4,6-tristyrylpyrylium dye.","authors":"Shivani Tripathi, Banchhanidhi Prusti, Manab Chakravarty","doi":"10.1038/s42004-025-01459-5","DOIUrl":"10.1038/s42004-025-01459-5","url":null,"abstract":"The strong electrophilicity of arylpyrylium salts was recognized for the colorimetric detection of vital amine analytes, limited to ammonia or methylamines and putrescine as biogenic amine. This report presents conformationally twisted, electrophilic triphenylamine-linked 2,4,6-tristyrylpyrylium salt PyTPA as a single dye to sense various aliphatic/aromatic biogenic amines, nicotine, and guanidine rapidly in nanomolar concentrations. This unexplored styrylpyrylium design offers specific electronic conjugations, steric/geometric constraints with hydrophobicity, and decent thermal/photostability, facilitating precise diverse amines detection in unique fashions. The deep-violet solution/solid dye responded remarkably at 298 K with quick decoloration against putrescine, cadaverine, spermidine, spermine, histamines, serotonin, and 2-phenylethylamine. Further, this dye could detect nicotine at 313 K and guanidine at 298 K distinctively with diminished absorption and unexpected red-shifted emission enhancement. Variation in mechanistic path is recognized in detecting amines holding mono/di-NH2 groups and short/ long alkane chains, elucidated by mass, 1H-NMR, FT-IR, SEM, PXRD, and XPS studies. The notable detection of these biogenic amines in different phases is employed for onsite applications to detect fresh chicken and tuna. Nicotine in natural tobacco leaves was identified. Such pyrylium salt provides promising advancements in this class of molecules in detecting diverse biologically significant amines.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"81"},"PeriodicalIF":5.9,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11910641/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143633735","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

Orthogonally conjugated phthalocyanine-porphyrin oligomer for NIR photothermal-photodynamic antibacterial treatment.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-14 DOI: 10.1038/s42004-025-01470-w

Guixue Lian, Wanru Zhao, Gaoqiang Ma, Sen Zhang, Ailin Wu, Lin Wang, Dongjiao Zhang, Wei Liu, Jianzhuang Jiang

{"title":"Orthogonally conjugated phthalocyanine-porphyrin oligomer for NIR photothermal-photodynamic antibacterial treatment.","authors":"Guixue Lian, Wanru Zhao, Gaoqiang Ma, Sen Zhang, Ailin Wu, Lin Wang, Dongjiao Zhang, Wei Liu, Jianzhuang Jiang","doi":"10.1038/s42004-025-01470-w","DOIUrl":"10.1038/s42004-025-01470-w","url":null,"abstract":"With the increase of antibiotic resistance worldwide, there is an urgent demand to develop new fungicides and approaches to address the threat to human health posed by the ineffectiveness of traditional antibiotics. In this work, an orthogonal conjugated uniform oligomer bactericide of SiPc-ddCPP was constructed between silicon phthalocyanine and porphyrin, which can effectively treat infection through photodynamic-photothermal combined therapy without considering drug resistance. Compared with organic photothermal agents induced by unstable H-aggregation with blue-shifted absorption and fluorescence/ROS quenching, this orthogonal-structured uniform SiPc-ddCPP nanoparticle shows remarkably stability and NIR photothermal effect (η = 31.15%) along with fluorescence and ROS generation. Antibacterial studies have shown that both Gram-positive and Gram-negative bacteria could be efficiently annihilated in a few minutes through synergistic PDT-PTT along with satisfactory bacterial targeting. These results suggest SiPc-ddCPP is a multifunctional NIR bactericide, which afford a new approach of synergistic PDT-PTT sterilization to conquer the crisis of antibiotic resistance.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"80"},"PeriodicalIF":5.9,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11909192/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143633746","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

Opportunities and challenges in modelling ligand adsorption on semiconductor nanocrystals.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-13 DOI: 10.1038/s42004-025-01471-9

Xin Qi

引用次数: 0

Chemoenzymatic synthesis.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-13 DOI: 10.1038/s42004-025-01451-z

Paweł Borowiecki, Sandy Schmidt

引用次数: 0

Rational engineering of a thermostable α-oxoamine synthase biocatalyst expands the substrate scope and synthetic applicability.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-13 DOI: 10.1038/s42004-025-01448-8

Ben Ashley, Sam Mathew, Mariyah Sajjad, Yaoyi Zhu, Nikita Novikovs, Arnaud Baslé, Jon Marles-Wright, Dominic J Campopiano

{"title":"Rational engineering of a thermostable α-oxoamine synthase biocatalyst expands the substrate scope and synthetic applicability.","authors":"Ben Ashley, Sam Mathew, Mariyah Sajjad, Yaoyi Zhu, Nikita Novikovs, Arnaud Baslé, Jon Marles-Wright, Dominic J Campopiano","doi":"10.1038/s42004-025-01448-8","DOIUrl":"10.1038/s42004-025-01448-8","url":null,"abstract":"Carbon-carbon bond formation is one of the key pillars of organic synthesis. Green, selective and efficient biocatalytic methods for such are therefore highly desirable. The α-oxoamine synthases (AOSs) are a class of pyridoxal 5'-phosphate (PLP)-dependent, irreversible, carbon-carbon bond-forming enzymes, which have been limited previously by their narrow substrate specificity and requirement of acyl-CoA thioester substrates. We recently characterized a thermophilic enzyme from Thermus thermophilus (ThAOS) with a much broader substrate scope and described its use in a chemo-biocatalytic cascade process to generate pyrroles in good yields and timescales. Herein, we report the structure-guided engineering of ThAOS to arrive at variants able to use a greatly expanded range of amino acid and simplified N-acetylcysteamine (SNAc) acyl-thioester substrates. The crystal structure of the improved ThAOS V79A variant with a bound PLP:L-penicillamine external aldimine ligand, provides insight into the properties of the engineered biocatalyst.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"78"},"PeriodicalIF":5.9,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11906848/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143623960","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

Stabilization of a miniprotein fold by an unpuckered proline surrogate.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-12 DOI: 10.1038/s42004-025-01474-6

Madison M Wright, Benjamin H Rajewski, Taylor A Gerrein, Zhiyi Xu, Lorna J Smith, W Seth Horne, Juan R Del Valle

{"title":"Stabilization of a miniprotein fold by an unpuckered proline surrogate.","authors":"Madison M Wright, Benjamin H Rajewski, Taylor A Gerrein, Zhiyi Xu, Lorna J Smith, W Seth Horne, Juan R Del Valle","doi":"10.1038/s42004-025-01474-6","DOIUrl":"10.1038/s42004-025-01474-6","url":null,"abstract":"The unique role of proline in modulating protein folding and recognition makes it an attractive target for substitution to generate new proteomimetics. The design, synthesis, and conformational analysis of non-canonical surrogates can also aid in parsing the role of prolyl stereoelectronic effects on structure. We recently described the synthesis and conformational analysis of dehydro-δ-azaproline (ΔaPro), a novel unsaturated analogue of proline featuring a planar dehydropyrazine ring. When incorporated into host sequences, this backbone N-aminated proline surrogate forms an acylhydrazone bond with an unusually high trans rotamer bias and low isomerization barrier. Here, we used CD, NMR spectroscopy, and MD simulations to evaluate the impact of ΔaPro substitution within the polyproline II (PPII) and loop regions of the avian pancreatic polypeptide (aPP). The ΔaPro residue strongly favors PPII conformation and stabilizes the aPP tertiary fold when incorporated at select positions within the miniprotein. A variant featuring three ΔaPro substitutions was found to significantly enhance the thermal stability of wild-type aPP despite compromising protein dimerization. Our results suggest that the stability of proline-rich folds relies more on backbone torsional preferences than ring puckering and informs strategies for the incorporation of ΔaPro into thermally stable and functional proteomimetics.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"76"},"PeriodicalIF":5.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11904010/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143613793","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

XFEL crystallography reveals catalytic cycle dynamics during non-native substrate oxidation by cytochrome P450BM3.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-12 DOI: 10.1038/s42004-025-01440-2

Satoshi Nagao, Wako Kuwano, Takehiko Tosha, Keitaro Yamashita, Joshua Kyle Stanfield, Chie Kasai, Shinya Ariyasu, Kunio Hirata, Go Ueno, Hironori Murakami, Hideo Ago, Masaki Yamamoto, Osami Shoji, Hiroshi Sugimoto, Minoru Kubo

{"title":"XFEL crystallography reveals catalytic cycle dynamics during non-native substrate oxidation by cytochrome P450BM3.","authors":"Satoshi Nagao, Wako Kuwano, Takehiko Tosha, Keitaro Yamashita, Joshua Kyle Stanfield, Chie Kasai, Shinya Ariyasu, Kunio Hirata, Go Ueno, Hironori Murakami, Hideo Ago, Masaki Yamamoto, Osami Shoji, Hiroshi Sugimoto, Minoru Kubo","doi":"10.1038/s42004-025-01440-2","DOIUrl":"10.1038/s42004-025-01440-2","url":null,"abstract":"Cytochrome P450s are haem-containing enzymes, catalysing the regio- and stereospecific oxidation of non-activated hydrocarbons. Among these, the bacterial P450BM3 is a promising biocatalyst due to its high enzymatic activity. Given the significant conformational flexibility of this enzyme, understanding protein-substrate interactions and associated structural dynamics are crucial for designing P450BM3-based biocatalysts. Herein, employing an X-ray free electron laser in combination with freeze-trap crystallography and spectroscopy techniques, we captured the intact structures of engineered P450BM3s in the initial stages of catalysis during styrene epoxidation, in the presence of a decoy molecule. We found that the iron reduction significantly altered the active-site orientation of styrene, driven by structural changes in surrounding helices and hydrogen-bonding networks. Oxygen binding to iron further stabilised its productive orientation, providing a molecular basis for the experimentally observed enzyme kinetics and enantioselectivities. This study reveals the substrate dynamics of a P450 enzyme, showcasing how changes in haem chemistry affect enzyme structure and substrate orientation.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"63"},"PeriodicalIF":5.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11903658/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143613795","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

Ca²⁺-triggered allosteric catalysts crosstalk with cellular redox systems through their foldase- and reductase-like activities.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-11 DOI: 10.1038/s42004-025-01466-6

Rumi Mikami, Yuhei Sato, Shingo Kanemura, Takahiro Muraoka, Masaki Okumura, Kenta Arai

{"title":"Ca2+-triggered allosteric catalysts crosstalk with cellular redox systems through their foldase- and reductase-like activities.","authors":"Rumi Mikami, Yuhei Sato, Shingo Kanemura, Takahiro Muraoka, Masaki Okumura, Kenta Arai","doi":"10.1038/s42004-025-01466-6","DOIUrl":"10.1038/s42004-025-01466-6","url":null,"abstract":"Effective chemical catalysts can artificially control intracellular metabolism. However, in conventional catalytic chemistry, activity and cytotoxicity have a trade-off relationship; thus, driving catalysts in living cells remains challenging. To overcome this critical issue at the interface between catalytic chemistry and biology, we developed cell-driven allosteric catalysts that exert catalytic activity at specific times. The synthesized allosteric redox catalysts up- and downregulated their foldase- and antioxidase-like activities in response to varying Ca2+ concentrations, which is a key factor for maintenance of the redox status in cells. In the absence of Ca2+ or at low Ca2+ concentrations, the compounds were mostly inactive and hence did not affect cell viability. In contrast, under specific conditions with elevated cytosolic Ca2+ concentrations, the activated compounds resisted the redox imbalance induced by the reactive oxygen species generated by Ca2+-stimulated mitochondria. Smart catalysts that crosstalk with biological phenomena may provide a platform for new prodrug development guidelines.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"74"},"PeriodicalIF":5.9,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11897157/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143604028","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

Bile acid derivatives as novel co-adsorbents for enhanced performance of blue dye-sensitized solar cells. 胆汁酸衍生物作为新型共吸附剂用于提高蓝色染料敏化太阳能电池的性能。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-10 DOI: 10.1038/s42004-025-01433-1

Kezia Sasitharan, Allan J Mora Abarca, Fabio Cucinotta, Leslie W Pineda, Victor Hugo Soto Tellini, Marina Freitag

{"title":"Bile acid derivatives as novel co-adsorbents for enhanced performance of blue dye-sensitized solar cells.","authors":"Kezia Sasitharan, Allan J Mora Abarca, Fabio Cucinotta, Leslie W Pineda, Victor Hugo Soto Tellini, Marina Freitag","doi":"10.1038/s42004-025-01433-1","DOIUrl":"10.1038/s42004-025-01433-1","url":null,"abstract":"Diketopyrrolopyrrole-based blue dyes in dye-sensitized solar cells (DSCs) exhibit promise for building-integrated photovoltaics, but their efficiency is compromised by dye aggregation-induced charge recombination. Novel bile acid derivative co-adsorbents featuring bulky hydrophobic substituents at the 3-β position were synthesized to address this challenge. These molecules, designed to modulate intermolecular electronic interactions, effectively altered the TiO2 surface coverage dynamics, as evidenced by UV-Vis spectroscopy and dye-loading kinetics. Systematic variation of hydrophilic substituents revealed structure-function relationships in dye separation efficacy. Devices incorporating these co-adsorbers achieved power conversion efficiencies (PCE) of 7.6%, surpassing reference devices (5.2%) and those using conventional chenodeoxycholic acid co-adsorbers (6.4%). The optimized devices exhibited a 30% increase in short-circuit current density, 30 mV enhancement in open-circuit voltage, and 60% peak external quantum efficiency at 550 nm. Time-resolved photoluminescence spectroscopy confirmed suppressed non-radiative recombination, while transient absorption spectroscopy revealed accelerated electron injection rates from 6.4 ps to 4.6 ps. Electrochemical impedance spectroscopy elucidated the mechanism of reduced interfacial recombination. These findings present a molecular engineering strategy for mitigating lateral charge transfer in planar dye systems, advancing semi-transparent hybrid photovoltaics.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"75"},"PeriodicalIF":5.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11894181/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143596412","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

Isoaspartate-containing galanin in rat hypothalamus.

IF 5.9 2区化学

Communications Chemistry Pub Date : 2025-03-08 DOI: 10.1038/s42004-025-01475-5

Samuel Okyem, David H Mast, Elena V Romanova, Stanislav S Rubakhin, Jonathan V Sweedler

{"title":"Isoaspartate-containing galanin in rat hypothalamus.","authors":"Samuel Okyem, David H Mast, Elena V Romanova, Stanislav S Rubakhin, Jonathan V Sweedler","doi":"10.1038/s42004-025-01475-5","DOIUrl":"10.1038/s42004-025-01475-5","url":null,"abstract":"The isoaspartate residue is a spontaneous, time-dependent post-translational modification (PTM) of proteins and peptides, associated with in vivo protein aggregation and changes in molecule lifetime. While this is considered a slow modification impacting long lived proteins, surprisingly, we observed this PTM at high levels within the relatively short-lived neuropeptide galanin (Gal). The combination of liquid chromatography-trapped ion mobility mass spectrometry and protein Isoaspartyl methyltransferase assays demonstrated that 20 ± 2% of the mature Gal contain L-Isoaspartate residue in the hypothalamus of Rattus norvegicus. Aspartate in Gal isomerizes spontaneously under mildly acidic conditions within 48 h in vitro, much faster than previously assumed. Gal with the L-isoaspartate PTM significantly enhanced fibril formation. Transmission electron microscopy revealed differences in morphology of fibrils formed by D17Isoasparte Gal compared to the unmodified peptide. Observed characteristics of D17Isoasparte Gal suggest a potential mechanism for the development of in vivo Gal fibril deposits previously reported in the brain.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"72"},"PeriodicalIF":5.9,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11890773/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143585022","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