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α-Ketoglutarate-Dependent Dioxygenase-Catalyzed Macrocyclization in RiPPs. α-酮戊二酸依赖双加氧酶催化的RiPPs大环化。
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30 Epub Date: 2025-07-16 DOI: 10.1021/jacs.5c07332
Yinzheng Xia, Ying Shi, Zhixi Xiao, Xiangqian Xie, Boning Wang, Hongwei Yao, Huan Wang
{"title":"α-Ketoglutarate-Dependent Dioxygenase-Catalyzed Macrocyclization in RiPPs.","authors":"Yinzheng Xia, Ying Shi, Zhixi Xiao, Xiangqian Xie, Boning Wang, Hongwei Yao, Huan Wang","doi":"10.1021/jacs.5c07332","DOIUrl":"10.1021/jacs.5c07332","url":null,"abstract":"<p><p>α-Ketoglutarate-dependent dioxygenases (αKGDs) are versatile biocatalysts for oxidative reactions, yet their role in ribosomally synthesized and post-translationally modified peptide (RiPP) macrocyclization remains unexplored. In this study, we uncover the widespread co-occurrence of JmjC domain-containing αKGDs (JMJDs) with diverse RiPP subfamilies in biosynthetic gene clusters (BGCs) through bioinformatic analysis. Specifically, we identify a conserved group of class II lanthipeptide BGCs encoding a two-component JMJD pair. As a representative example, heterologous reconstitution of the <i>cor</i> BGC from <i>Streptomyces corchorusii</i>, encoding a class II lanthipeptide synthetase CorM and the αKGD pair CorB-CorD, yields the metal-binding lanthipeptide corsin, which features a methyllanthionine (MeLan) ring and a unique Cys(S)-Tyr(Cβ) cross-link. Functional studies reveal that CorM installs a MeLan ring in the precursor peptide CorA, while the CorB-CorD pair catalyzes oxidative Cys(S)-Tyr(Cβ) cross-linking. Mechanistic investigations demonstrate that CorD, a canonical JMJD, catalyzes the Tyr7 Cβ-H abstraction and generates a <i>para</i>-quinone methide (<i>p</i>QM) intermediate, which undergoes Michael addition with Cys3. CorB, an inactive JMJD homologue, is essential for catalysis, unveiling a unique two-component αKGD system. This work expands the RiPP enzymatic toolkit by introducing αKGDs as radical catalysts for macrocyclization and advances our understanding of the diverse enzymatic strategies driving RiPP structural diversification.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"26693-26703"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144647916","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
An Anaerobic Biomimetic Metal-Free AIE Polymersome Nanozyme as NADH Oxidase Mimic for Photocatalytic Tumor Suppression by Impairing Cancer Cell Energy Metabolism under Hypoxia. 厌氧仿生无金属AIE聚合体纳米酶作为NADH氧化酶模拟物在缺氧条件下通过损害癌细胞能量代谢光催化抑瘤
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30 Epub Date: 2025-07-17 DOI: 10.1021/jacs.5c06533
Yandong Ma, Yakui Deng, Wei Xue, Xin Ji, Min-Hui Li
{"title":"An Anaerobic Biomimetic Metal-Free AIE Polymersome Nanozyme as NADH Oxidase Mimic for Photocatalytic Tumor Suppression by Impairing Cancer Cell Energy Metabolism under Hypoxia.","authors":"Yandong Ma, Yakui Deng, Wei Xue, Xin Ji, Min-Hui Li","doi":"10.1021/jacs.5c06533","DOIUrl":"10.1021/jacs.5c06533","url":null,"abstract":"<p><p>The intracellular balance between nicotinamide adenine dinucleotide and its reduced form (NAD<sup>+</sup>/NADH) is essential for cell metabolism. The NAD<sup>+</sup>/NADH redox imbalance strategy using NADH-oxidase-mimic nanozymes has emerged as an attractive antitumor strategy. Here, we develop a photocatalytic metal-free nanozyme that is a polymer vesicle (polymersome) self-assembled from PEG-block-poly(amino acid) functionalized by photocatalytic moieties with aggregation-induced emission (AIE). To enhance biocompatibility and tumor-targetability, the vesicle is coated with a folate-modified red-blood-cell membrane (FA-RBC) to get biomimetic AIE polymersome nanozyme (BV). Unlike conventional photocatalysts, BV can achieve the cyclical photocatalytic process for NADH-NAD<sup>+</sup> conversion without O<sub>2</sub> or additional electron acceptors. A new mechanism is proposed in which adjacent excited triplet molecules in the AIE assembly play the role of electron acceptors for complete NADH-NAD<sup>+</sup> conversion and catalyst turnover. This O<sub>2</sub>-independent photocatalysis is appealing in anticancer treatment since the tumor has a hypoxic microenvironment. <i>In vitro</i> and <i>in vivo</i> investigations demonstrate BV induces a severe NAD<sup>+</sup>/NADH imbalance under hypoxia to lead to inhibition of oxidative phosphorylation and glycolysis, which triggers the energy crisis in 4T1 cancer cells and in the 4T1 tumor of a subcutaneous xenograft model. This work presents a novel approach of cancer therapy through the photocatalytic impairment of tumor energy metabolism by metal-free nanozyme.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"26557-26572"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144657883","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
Low-Electromotive Force-Driven Sodium Compensation for Optimizing Na Deposition in Rechargeable Sodium Batteries. 低电动势驱动钠补偿优化可充电钠电池钠沉积。
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30 Epub Date: 2025-07-17 DOI: 10.1021/jacs.5c06704
Yu-Ying Zhang, Chao-Hui Zhang, Yu-Jie Guo, Xu-Sheng Zhang, Min Fan, Xin-Hai Meng, Xing Zhang, Yao Zhao, Fuyi Wang, Sen Xin, Yu-Guo Guo, Li-Jun Wan
{"title":"Low-Electromotive Force-Driven Sodium Compensation for Optimizing Na Deposition in Rechargeable Sodium Batteries.","authors":"Yu-Ying Zhang, Chao-Hui Zhang, Yu-Jie Guo, Xu-Sheng Zhang, Min Fan, Xin-Hai Meng, Xing Zhang, Yao Zhao, Fuyi Wang, Sen Xin, Yu-Guo Guo, Li-Jun Wan","doi":"10.1021/jacs.5c06704","DOIUrl":"10.1021/jacs.5c06704","url":null,"abstract":"<p><p>Sufficient active Na<sup>+</sup> and stable electrode-electrolyte interfaces enable anode-free sodium batteries to achieve high energy densities and long operational lifespan. Here, we establish the critical role of low electromotive force (EMF) in promoting uniform Na deposition and stable interfacial chemistry by minimizing overpotential and mitigating steep concentration gradients. We accordingly designed a versatile cathode, Na-replenished P2-type oxides (NRP2), with reversible overstoichiometric Na-ion insertion that incorporates sodium compensation and promotes Na leveling deposition. By releasing the prestored Na-ions at a low voltage, the NRP2 cathode supplements the loss of active Na<sup>+</sup> during the initial formation of the solid electrolyte interphase (SEI). Simultaneously, it creates a low EMF to facilitate uniform and dense metal deposition at the anode surface. The deposited Na metal shows a regular two-dimensional polygonal morphology, in contrast to the dendritic morphology with the high EMF condition. As a result, the rechargeable Na-metal batteries that employ the NRP2-50 demonstrate a capacity retention of 90.1% after 500 cycles and capacity retention of 97.4% over 50 cycles in an anode-free geometry.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"26573-26583"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144657890","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
Asymmetric Access to δ-Hydroxy α-Amino Acids Bearing Two Adjacent Stereocenters from Inert Allylic Alcohols Via Cu/Ru Relay Catalysis. 通过Cu/Ru接力催化从惰性烯丙醇中不对称获得带两个相邻立体中心的δ-羟基α-氨基酸。
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30 Epub Date: 2025-07-21 DOI: 10.1021/jacs.5c07896
Qi Xiong, Bo-Bin Chen, Xiu-Qin Dong, Chun-Jiang Wang
{"title":"Asymmetric Access to δ-Hydroxy α-Amino Acids Bearing Two Adjacent Stereocenters from Inert Allylic Alcohols Via Cu/Ru Relay Catalysis.","authors":"Qi Xiong, Bo-Bin Chen, Xiu-Qin Dong, Chun-Jiang Wang","doi":"10.1021/jacs.5c07896","DOIUrl":"10.1021/jacs.5c07896","url":null,"abstract":"<p><p>Herein, we developed an efficient Cu/Ru relay catalytic system to achieve an asymmetric cascade reaction through merging hydrogen-borrowing and asymmetric Michael addition between inert allylic alcohols and ketoimine ester, enabling the efficient synthesis of biologically relevant chiral α-amino δ-hydroxy acid derivatives bearing two vicinal tertiary stereocenters in good yields with high diastereoselectivity and excellent enantioselectivity. This operationally simple and scalable protocol features excellent atom- and step-economy, broad substrate tolerance, and redox-neutral conditions. The synthetic utility was further exemplified through gram-scale synthesis, diverse downstream derivatizations, and a streamlined formal synthesis of l-pyrrolysine. Mechanistic investigations identified the Michael addition as both the stereodetermining and rate-limiting step in the cascade sequence.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"26102-26108"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144681673","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
Regiodivergent Interrupted Ni-Catalyzed Chain-Walking of Unsaturated Alcohol Side-Chains via Traceless Activating Groups. 不饱和醇侧链通过无迹激活基团的区域发散中断镍催化链行走。
IF 15 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30 DOI: 10.1021/jacs.5c09426
Hao Wang,Huihui Zhang,Marta Martínez-Belmonte,Jordi Benet-Buchholz,Ruben Martin
{"title":"Regiodivergent Interrupted Ni-Catalyzed Chain-Walking of Unsaturated Alcohol Side-Chains via Traceless Activating Groups.","authors":"Hao Wang,Huihui Zhang,Marta Martínez-Belmonte,Jordi Benet-Buchholz,Ruben Martin","doi":"10.1021/jacs.5c09426","DOIUrl":"https://doi.org/10.1021/jacs.5c09426","url":null,"abstract":"Herein, we describe a regiodivergent interrupted chain-walking of unsaturated aliphatic alcohols. The method leverages the potential of traceless groups to forge C(sp3)-C(sp3) and C(sp3)-nitrogen bonds at distal methylene sp3 C-H sites, with site selectivity dictated by a judicious choice of the ligand. The protocol is distinguished by its broad applicability, offering unconventional disconnections to access β/γ-substituted aliphatic alcohols that are difficult to reach otherwise.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"13 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737296","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
Reversible C-H Bond Activation of Unactivated Arenes by a Nickel-Silylene Complex. 镍-硅烯配合物活化未活化芳烃的可逆碳氢键。
IF 15 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30 DOI: 10.1021/jacs.5c10922
Leon Gomm,Hui Zhu,Gregor Schnakenburg,Senada Nozinovic,Stefan Grimme,Connie C Lu
{"title":"Reversible C-H Bond Activation of Unactivated Arenes by a Nickel-Silylene Complex.","authors":"Leon Gomm,Hui Zhu,Gregor Schnakenburg,Senada Nozinovic,Stefan Grimme,Connie C Lu","doi":"10.1021/jacs.5c10922","DOIUrl":"https://doi.org/10.1021/jacs.5c10922","url":null,"abstract":"A nickel-silylene complex is shown to reversibly activate benzene via C-H bond activation at ambient temperature. The benzene C-H bond formally adds across the Ni-Si core to form a nickel-silyl complex with an H-Si-Ni-Ph linkage bearing a highly covalent Ni-Si bond (2.2363(6) Å). Dissolution of this product in neat arene solvent, e.g., toluene, trifluorotoluene, or anisole, resulted in the complete conversion to the aryl C-H activated product of the solvent and, thereby, demonstrates the facile reversibility of C-H bond activation across the Ni-Si core. The various arene C-H bond activations by the reactive Ni(0)-silylene species were investigated using density functional theory calculations. In all cases, the arene initially forms an η2-adduct to Ni(0), and then C-H activation proceeds via a concerted oxidative addition at only the Ni center. The Si center assists C-H bond activation by sharing the redox burden with Ni while stabilizing the resultant hydride.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"25 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737323","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
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30
Qi Xiong, Bo-Bin Chen, Xiu-Qin Dong* and Chun-Jiang Wang*, 
{"title":"","authors":"Qi Xiong,&nbsp;Bo-Bin Chen,&nbsp;Xiu-Qin Dong* and Chun-Jiang Wang*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"147 30","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacs.5c07896","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30
Xiang Wang, Xiaowan Han, Xiaoyuan Tian, Hosoowi Lee, Caihong Xiang, Chaorui Wang, Liang Luo, Hai-Yu Hu*, Guangle Niu* and Juyoung Yoon*, 
{"title":"","authors":"Xiang Wang,&nbsp;Xiaowan Han,&nbsp;Xiaoyuan Tian,&nbsp;Hosoowi Lee,&nbsp;Caihong Xiang,&nbsp;Chaorui Wang,&nbsp;Liang Luo,&nbsp;Hai-Yu Hu*,&nbsp;Guangle Niu* and Juyoung Yoon*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"147 30","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacs.5c10005","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30
{"title":"","authors":"","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"147 30","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jav147i030_1965527","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
IF 15.6 1区 化学
Journal of the American Chemical Society Pub Date : 2025-07-30
Chenchen Zhao, Yuanwei Pan, Lei Cao, Yuji Tang, Xiaoyuan Chen, Xingzhong Zhao and Lang Rao*, 
{"title":"","authors":"Chenchen Zhao,&nbsp;Yuanwei Pan,&nbsp;Lei Cao,&nbsp;Yuji Tang,&nbsp;Xiaoyuan Chen,&nbsp;Xingzhong Zhao and Lang Rao*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"147 30","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":15.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacs.5c02774","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
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