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Borinic Acid-Based Fluorogenic Probes as an Alternative to the Amplex Red Assay for Real-Time H2O2 Monitoring in Live Cells. 基于硼酸的荧光探针作为一种替代Amplex Red法实时监测活细胞中H2O2的方法。
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-25 DOI: 10.1021/acschembio.5c00156
Mathilde Pucher, Kirrthana Makenthirathasan, Hadrien Jalaber, Thomas LeSaux, Oliver Nüsse, Gilles Doisneau, Yann Bourdreux, Blaise Gatin-Fraudet, Ludovic Jullien, Boris Vauzeilles, Dominique Guianvarc'h, Marie Erard, Dominique Urban
{"title":"Borinic Acid-Based Fluorogenic Probes as an Alternative to the Amplex Red Assay for Real-Time H<sub>2</sub>O<sub>2</sub> Monitoring in Live Cells.","authors":"Mathilde Pucher, Kirrthana Makenthirathasan, Hadrien Jalaber, Thomas LeSaux, Oliver Nüsse, Gilles Doisneau, Yann Bourdreux, Blaise Gatin-Fraudet, Ludovic Jullien, Boris Vauzeilles, Dominique Guianvarc'h, Marie Erard, Dominique Urban","doi":"10.1021/acschembio.5c00156","DOIUrl":"https://doi.org/10.1021/acschembio.5c00156","url":null,"abstract":"<p><p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a crucial reactive oxygen species (ROS) involved in regulating both physiological and pathological processes. Excessive H<sub>2</sub>O<sub>2</sub> production can lead to oxidative stress, contributing to aging, cancer, and neurodegenerative diseases. In contrast to other ROS exhibiting short lifespans, H<sub>2</sub>O<sub>2</sub> is relatively stable, and its spatial and temporal dynamics are central to understanding its pathophysiological role. Therefore, the development of fluorescent probes that are highly selective, sensitive, and capable of a rapid response is still required. To date, numerous fluorescent probes have been developed. Among them, boronic acid triggers have attracted considerable attention but often suffer from limited reactivity, preventing real-time H<sub>2</sub>O<sub>2</sub> monitoring. To overcome this lack of reactivity, we report the design and synthesis of new borinic acid-based fluorogenic probes for H<sub>2</sub>O<sub>2</sub> detection in cellular environments. These probes are based on a hemicyanine scaffold functionalized with the borinic acid trigger, which demonstrated superior kinetics compared to its boronic counterpart. These probes enable efficient real-time monitoring of H<sub>2</sub>O<sub>2</sub> in cellular models, both extracellularly and intracellularly. The kinetics of these enzyme-free chemical probes matched that of the gold standard Amplex UltraRed/horseradish peroxidase (HRP) assay, representing a significant advancement in the field and offering a versatile and sensitive tool for studying H<sub>2</sub>O<sub>2</sub>-mediated cell signaling.</p>","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":" ","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144493131","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Solution NMR Analysis Reveals Synergistic β-Arrestin1 Activation by Chemically Synthesized Phosphopeptides of a C-Terminal Tail and ICL3 of NTSR1. 溶液核磁共振分析表明,化学合成的c端尾部磷酸肽和NTSR1的ICL3可协同活化β-Arrestin1。
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-23 DOI: 10.1021/acschembio.5c00257
Zelin Li, Yi Zhang, Jun Liang, Fengyu Jia, Jiacai Song, Demeng Sun, Chaowei Shi, Changlin Tian, Pan Shi
{"title":"Solution NMR Analysis Reveals Synergistic β-Arrestin1 Activation by Chemically Synthesized Phosphopeptides of a C-Terminal Tail and ICL3 of NTSR1.","authors":"Zelin Li, Yi Zhang, Jun Liang, Fengyu Jia, Jiacai Song, Demeng Sun, Chaowei Shi, Changlin Tian, Pan Shi","doi":"10.1021/acschembio.5c00257","DOIUrl":"https://doi.org/10.1021/acschembio.5c00257","url":null,"abstract":"<p><p>β-Arrestins are critical regulators of G-protein-coupled receptors (GPCRs), mediating desensitization, internalization, and activation of alternative downstream signal transduction pathways through selective binding to phosphorylated GPCRs. Although phosphorylation of C-terminal tails (C-tail) and intracellular loop 3 (ICL3) of GPCRs is essential for β-arrestin binding to GPCRs, cooperative interactions of the phosphorylated C-tail or ICL3 of GPCRs for β-arrestin recruitment remain elusive. Here, we chemically synthesized phosphorylated C-tail and ICL3 peptides of neurotensin receptor 1 (NTSR1) and investigated the conformational dynamics of β-arrestin1 during its interaction with the phosphopeptides. Two-dimensional <sup>1</sup>H-<sup>13</sup>C nuclear magnetic resonance (NMR) spectroscopy of <sup>13</sup>C<sup>ε</sup>H3-methionine labeled β-arrestin1 revealed that the phosphorylated C-tail (C-tail-NC 6P), N-cluster of C-tail (C-tail-N 3P), or ICL3 4P triggered conformational changes of β-arrestin1, whereas the C-cluster of the C-tail (C-tail-C 3P) exhibited negligible influence. Additionally, analysis of successive binding of C-tail-NC 6P and ICL3 4P of NTSR1 to β-arrestin1 implied noncompetitive binding of the two segments and displayed allosteric modulation of C-tail or ICL3 in β-arrestin1. These 2D <sup>13</sup>C-methyl-Met NMR data provide direct evidence for interactions between β-arrestin1 and phosphorylated segments of GPCRs, offering a framework to decode the details of β-arrestin signaling.</p>","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":" ","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144473282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Design of an Orally Bioavailable Small Molecule That Modulates the Microtubule-Associated Protein Tau's Pre-mRNA Splicing. 调节微管相关蛋白Tau Pre-mRNA剪接的口服生物可利用小分子的设计。
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-22 DOI: 10.1021/acschembio.5c00260
Peiyuan Zhang, Amirhossein Taghavi, Masahito Abe, Haruo Aikawa, Yoshihiro Akahori, Jonathan L Chen, Yuquan Tong, Jared T Baisden, Michael D Cameron, Jessica L Childs-Disney, Matthew D Disney
{"title":"Design of an Orally Bioavailable Small Molecule That Modulates the Microtubule-Associated Protein Tau's Pre-mRNA Splicing.","authors":"Peiyuan Zhang, Amirhossein Taghavi, Masahito Abe, Haruo Aikawa, Yoshihiro Akahori, Jonathan L Chen, Yuquan Tong, Jared T Baisden, Michael D Cameron, Jessica L Childs-Disney, Matthew D Disney","doi":"10.1021/acschembio.5c00260","DOIUrl":"10.1021/acschembio.5c00260","url":null,"abstract":"<p><p>Frontotemporal dementia with parkinsonism linked to chromosome 17 (FTDP-17) is caused by the aberrant alternative pre-mRNA splicing of microtubule-associated protein tau (<i>MAPT</i>) exon 10, the inclusion of which encodes a toxic tau protein harboring four microtubule domains (4R tau). Here, we describe the design of an RNA-targeted small molecule that thermodynamically stabilizes the structure of a pre-mRNA splicing regulator element in the <i>MAPT</i> pre-mRNA exon 10-intron 10 junction to reduce the inclusion of exon 10 and hence 4R tau abundance. Structure-guided drug design was used to obtain compounds that form a network of specific interactions to the RNA, including multiple interactions between a single nucleotide (nt) A-bulge and the Hoogsteen face of a closing GC base pair, the latter of which was enabled by the design of base triple interactions. A battery of assays revealed that the compound binds the target <i>in vitro</i> and in cells and affects pre-mRNA splicing in various cellular models, including primary neurons from a human tau (htau) knock-in mouse model. The orally bioavailable compound was administered <i>per os</i> (<i>p.o.</i>), where treatment diminished exon 10 inclusion and reduced the 4R tau protein isoform. Further, the molecule mitigated cellular pathologies and behavioral phenotypes observed in the htau transgenic mouse model. This study provides a potentially general pipeline to design compounds that target RNAs, affect disease pathways, and deliver compounds that have oral bioavailability and blood-brain barrier penetrance.</p>","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":" ","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144367623","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Feature-Based Molecular Networking Guided Characterization of Clonocoprogen Siderophores with Anti-Pseudomonas aeruginosa Activity in Nematodes through Immune Up-Regulating Effects. 基于特征的分子网络引导下,通过免疫上调作用表征线虫抗铜绿假单胞菌活性的克隆原铁载体。
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-22 DOI: 10.1021/acschembio.5c00178
Guoliang Zhu, Weize Yuan, Kun Wang, Huimin Wu, Kangjie Lv, Xinye Wang, Alex Tuffour, Biao Ren, Jingyu Zhang, Chenglin Jiang, Yi Jiang, Tom Hsiang, Peter Shen Yu, Frederick M Ausubel, Lixin Zhang, Huanqin Dai, Xueting Liu
{"title":"Feature-Based Molecular Networking Guided Characterization of Clonocoprogen Siderophores with Anti-<i>Pseudomonas aeruginosa</i> Activity in Nematodes through Immune Up-Regulating Effects.","authors":"Guoliang Zhu, Weize Yuan, Kun Wang, Huimin Wu, Kangjie Lv, Xinye Wang, Alex Tuffour, Biao Ren, Jingyu Zhang, Chenglin Jiang, Yi Jiang, Tom Hsiang, Peter Shen Yu, Frederick M Ausubel, Lixin Zhang, Huanqin Dai, Xueting Liu","doi":"10.1021/acschembio.5c00178","DOIUrl":"10.1021/acschembio.5c00178","url":null,"abstract":"<p><p>Antibiotic resistance poses a severe threat to human health, necessitating research into antibiotics with unique mechanisms to combat drug resistance. Natural siderophores and their synthetic derivatives have become a promising resource for the development of anti-infectious agents. In this study, we introduce a new anti-infective agent with a mode of action that enhances host immunity without exerting direct antibacterial activity. We identified immune-activating clonocoprogen siderophores from the fungus <i>Clonostachys rosea</i> isolate CR15020 using an integrated approach, including genome mining, feature-based molecular networking (FBMN) and a nematode screening model. Although these siderophores displayed no inherent antibacterial properties, they significantly improved survival of <i>Caenorhabditis elegans</i> exposed to <i>Pseudomonas aeruginosa</i>, with EC<sub>50</sub> values ranging from 1.85 to 10.86 μM. This protection was achieved through up-regulation of the nematode's p38-MAPK and DAF/IGF immune pathways, as well as reducing the excretion of pyoverdine by <i>P. aeruginosa</i>. By leveraging immune modulation rather than direct bacterial inhibition, this approach offers a promising alternative to conventional antibiotics, addressing the urgent challenge of antibiotic resistance.</p>","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":" ","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144367624","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Human PTGR2 Inactivation Alters Eicosanoid Metabolism and Cytokine Response of Inflammatory Macrophages. 人PTGR2失活改变炎性巨噬细胞的类二十烷代谢和细胞因子反应。
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-20 Epub Date: 2025-05-19 DOI: 10.1021/acschembio.5c00231
Michael W Founds, Olivia L Murtagh, R Justin Grams, Zhihong Li, Anthony M Ciancone, Robert J Seal, Ku-Lung Hsu
{"title":"Human PTGR2 Inactivation Alters Eicosanoid Metabolism and Cytokine Response of Inflammatory Macrophages.","authors":"Michael W Founds, Olivia L Murtagh, R Justin Grams, Zhihong Li, Anthony M Ciancone, Robert J Seal, Ku-Lung Hsu","doi":"10.1021/acschembio.5c00231","DOIUrl":"10.1021/acschembio.5c00231","url":null,"abstract":"<p><p>Prostaglandin reductase 2 (PTGR2) regulates inflammatory lipid signaling through the metabolism of the PGE2 metabolite 15-keto-PGE<sub>2</sub>. PTGR2 inhibitors have been reported but whether small molecule inactivation can recapitulate the anti-inflammatory phenotype observed in PTGR2 knockout systems has not been explored. Here, we disclose an optimized sulfonyl triazole (SuTEx) inhibitor of human PTGR2 that blocks biochemical activity by liganding the noncatalytic tyrosines Y100 and Y265 in the active site. Quantitative and multiplexed chemoproteomics verified covalent engagement of endogenous PTGR2 in THP1 macrophages with moderate proteome-wide selectivity. PTGR2 inactivation with the SuTEx inhibitor resulted in suppression of secreted inflammatory lipids and TNF-α in lipopolysaccharide (LPS)-stimulated macrophages. Collectively, our findings identify a potent covalent inhibitor of human PTGR2 that can serve as a tool compound for exploring lipid metabolism and signaling in macrophages.</p>","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":" ","pages":"1426-1434"},"PeriodicalIF":3.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144100960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-20
Severin Lechner*, Shuyao Sha, Jigar Paras Sethiya, Patrycja Szczupak, Rafal Dolot, Santosh Lomada, Amirhossein Sakhteman, Johanna Tushaus, Polina Prokofeva, Michael Krauss, Ferdinand Breu, Katharina Vögerl, Martin Morgenstern, Martin Hraběde Angelis, Volker Haucke, Thomas Wieland, Carston Wagner, Guillaume Médard, Franz Bracher and Bernhard Kuster*, 
{"title":"","authors":"Severin Lechner*,&nbsp;Shuyao Sha,&nbsp;Jigar Paras Sethiya,&nbsp;Patrycja Szczupak,&nbsp;Rafal Dolot,&nbsp;Santosh Lomada,&nbsp;Amirhossein Sakhteman,&nbsp;Johanna Tushaus,&nbsp;Polina Prokofeva,&nbsp;Michael Krauss,&nbsp;Ferdinand Breu,&nbsp;Katharina Vögerl,&nbsp;Martin Morgenstern,&nbsp;Martin Hraběde Angelis,&nbsp;Volker Haucke,&nbsp;Thomas Wieland,&nbsp;Carston Wagner,&nbsp;Guillaume Médard,&nbsp;Franz Bracher and Bernhard Kuster*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"20 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acschembio.5c00108","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144343652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-20
Xu-Dong Kong*, Meng-Jie Zhang and Christian Heinis*, 
{"title":"","authors":"Xu-Dong Kong*,&nbsp;Meng-Jie Zhang and Christian Heinis*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"20 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acschembio.5c00121","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144343656","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-20
Ines Burkhart, Vivien Rose McKenney, Julia Wirmer-Bartoschek, J. Tassilo Grün, Alexander Heckel and Harald Schwalbe*, 
{"title":"","authors":"Ines Burkhart,&nbsp;Vivien Rose McKenney,&nbsp;Julia Wirmer-Bartoschek,&nbsp;J. Tassilo Grün,&nbsp;Alexander Heckel and Harald Schwalbe*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"20 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acschembio.5c00226","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469157","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-20
Jen Wagner, 
{"title":"","authors":"Jen Wagner,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"20 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acschembio.5c00354","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469159","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 3.5 2区 生物学
ACS Chemical Biology Pub Date : 2025-06-20
Mercedes B. Fisk, Jocelyn Barrera Ramirez, Collin E. Merrick, Timothy A. Wencewicz and Andrew M. Gulick*, 
{"title":"","authors":"Mercedes B. Fisk,&nbsp;Jocelyn Barrera Ramirez,&nbsp;Collin E. Merrick,&nbsp;Timothy A. Wencewicz and Andrew M. Gulick*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"20 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acschembio.5c00286","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144469167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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