IF 8.7

JACS Au Pub Date : 2025-08-07 DOI: 10.1021/jacsau.5c00624

Li-Na Zhang, Yuan-Feng Wei, Xiao-Yun Ran, Lei Shi, Zhou-Yu Wang, Shan-Yong Chen, Cheng Yi, Xiao-Qi Yu* and Kun Li*,

{"title":"Liberating Exciton Transfer as a Pioneering Strategy to Construct Type I Photosensitizers for Hypoxia Deep-Seated Metastases Suppression","authors":"Li-Na Zhang, Yuan-Feng Wei, Xiao-Yun Ran, Lei Shi, Zhou-Yu Wang, Shan-Yong Chen, Cheng Yi, Xiao-Qi Yu* and Kun Li*, ","doi":"10.1021/jacsau.5c00624","DOIUrl":"https://doi.org/10.1021/jacsau.5c00624","url":null,"abstract":"Type I photosensitizers (PSs) have revolutionized traditional photodynamic therapy for hypoxia tumors by eliminating oxygen dependence. Nevertheless, the current development of Type I PSs faces formidable obstacles stemming from the paucity of universal regulatory strategies that steer molecular systems toward efficient reactive oxygen species (ROS) generation through the Type I electron transfer pathway. Herein, we propose the “liberating exciton transfer” strategy to construct a series of Type I PSs (IDMX, X = H, F, Cl, Br) with remarkable generation of superoxide radicals (O2•–) and hydroxyl radicals (•OH). In this strategy, the halogen (F, Cl, and Br) modifications act as the “sharp hook” to release triplet excitons from their “cage”, allowing them to move more freely and interact more effectively with substrates. Among them, IDMBr demonstrates superior photodynamic efficacy, enabling effective tumor cell ablation under hypoxic conditions and suppression of deep-seated pulmonary metastatic lesions and exhibiting significant clinical potential. This work establishes a novel strategy for developing Type I PSs, substantially advancing photodynamic therapy for hypoxic tumors.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3982–3993"},"PeriodicalIF":8.7,"publicationDate":"2025-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00624","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892650","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Function Provision to Fe–Porphyrin Complexes for CO2 Reduction 铁-卟啉配合物对CO2还原的作用

IF 8.7

JACS Au Pub Date : 2025-08-06 DOI: 10.1021/jacsau.5c00564

Maho Imai, Shigeyuki Masaoka* and Mio Kondo*,

引用次数: 0

Organocatalytic Kinetic Resolution of Ferroceno[c]isoquinolines through Asymmetric Transfer Hydrogenation 二茂铁[c]异喹啉类化合物不对称转移加氢的有机催化动力学拆分

IF 8.7

JACS Au Pub Date : 2025-08-05 DOI: 10.1021/jacsau.5c00698

Yan-Jiang Yu, Zheng Liu, Yi-Qian Yang, Mu-Wang Chen*, Rong-Zhen Liao and Yong-Gui Zhou*,

引用次数: 0

Correction to “A Cocatalytic System for Electrooxidation of Primary, Secondary, and Benzyl Alcohols Based on a Triruthenium Oxo-Centered Cluster and NHPI” 更正“基于三钌氧中心簇和NHPI的伯、仲、苄醇电氧化共催化体系”

IF 8.7

JACS Au Pub Date : 2025-08-05 DOI: 10.1021/jacsau.5c00916

Mollie C. Morrow, and , Charles W. Machan*,

引用次数: 0

Magnetic Field-Driven Interface Hydroxylation via the Vibrational Stark Effect Boosts Alkaline Hydrogen Evolution Reaction 磁场驱动界面羟基化作用下的振动Stark效应促进碱氢析出反应

IF 8.7

JACS Au Pub Date : 2025-08-05 DOI: 10.1021/jacsau.5c00585

Xiayan Yao, Jianwei Guo, Zhi Wang*, Guoyu Qian, XiangYu Wang, Dong Wang* and Xuzhong Gong*,

{"title":"Magnetic Field-Driven Interface Hydroxylation via the Vibrational Stark Effect Boosts Alkaline Hydrogen Evolution Reaction","authors":"Xiayan Yao, Jianwei Guo, Zhi Wang*, Guoyu Qian, XiangYu Wang, Dong Wang* and Xuzhong Gong*, ","doi":"10.1021/jacsau.5c00585","DOIUrl":"https://doi.org/10.1021/jacsau.5c00585","url":null,"abstract":"Tuning interfacial water structures is a fundamental yet underexplored strategy for advancing the hydrogen evolution reaction (HER) and broader electrocatalytic processes. Here, we demonstrate a universal and scalable catalytic optimization strategy via the magnetic field-driven reconfiguration of interfacial water at the molecular level. Unlike conventional magnetohydrodynamic (MHD) strategies focusing on mass transport, this work pioneers a molecular-level interfacial water structure modulation via the vibrational Stark effect (VSE), achieving intrinsic catalytic enhancement for HER. In situ Raman spectroscopy and molecular dynamics (MD) simulations reveal that the permanent magnetic field-induced amplification of the DDAA configuration population is governed by the VSE, leading to a restructured interfacial weak hydrogen bond (HB) network and enhanced charge transfer kinetics. As a result, under a 1 T permanent magnetic field and a controlled flow rate of 100 mL/min, the HER overpotential is reduced by 50 mV at 10 mA·cm–2, with stable performance sustained for over 10 h, a level of enhancement far exceeding previous magnetic field-assisted HER studies. Beyond HER, this strategy offers a generalizable approach for tuning interfacial water structures, which could be extended to other electrocatalytic reactions, where HB networks and interfacial water structuring play a critical role. As a result, the overpotential was reduced by 50 mV at 10 mA·cm–2, and a 15.40% increase in current density was achieved under industrial alkaline electrolysis conditions, demonstrating clear advantages over existing magnetic field-assisted HER strategies. This study provided a scalable, molecular-level catalytic interface engineering approach, offering valuable insights into advanced electrocatalytic processes and significant potential for industrial hydrogen production technologies.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3926–3943"},"PeriodicalIF":8.7,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00585","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Planarization of Twisted Push–Pull Probes by Stretching Rather than by Compression: Core-Substituted Fluorescent Flippers as Materials Mechanosensors 通过拉伸而不是压缩使扭曲推拉探针平面化：核取代荧光鳍作为材料机械传感器

IF 8.7

JACS Au Pub Date : 2025-08-05 DOI: 10.1021/jacsau.5c00579

Khurnia Krisna Puji Pamungkas, Riku Yamamoto, Maxime Vonesch, Naomi Sakai, Yoshimitsu Sagara* and Stefan Matile*,

{"title":"Planarization of Twisted Push–Pull Probes by Stretching Rather than by Compression: Core-Substituted Fluorescent Flippers as Materials Mechanosensors","authors":"Khurnia Krisna Puji Pamungkas, Riku Yamamoto, Maxime Vonesch, Naomi Sakai, Yoshimitsu Sagara* and Stefan Matile*, ","doi":"10.1021/jacsau.5c00579","DOIUrl":"https://doi.org/10.1021/jacsau.5c00579","url":null,"abstract":"Fluorescent flippers are twisted push–pull mechanophores that report planarization with red-shifted absorption and an increase in fluorescence intensity and lifetime. Until today, their planarization by physical forces has focused on compression to visualize physical forces in biology. Here, we show that planarization can also be achieved by stretching of flipper probes that are equipped with tethers in their core and to visualize mechanical stress in polymeric materials. The synthesis of dithieno[3,2-b:2’,3′-d]thiophene dimers with alcohols extending from their twisted core is accomplished in 17 steps. Covalently integrated into polyurethanes, these core-substituted flippers exhibit an excitation-wavelength-dependent fluorescence enhancement upon polymer stretching, validating their mode of action. Noncovalently interfaced flipper controls are much less responsive. In light of the importance their fluorogenic compression has reached in biology, synthetic access to flippers that can be stretched rather than compressed and use in materials rather than life sciences opens up significant, fundamentally new perspectives for flipper research.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3944–3950"},"PeriodicalIF":8.7,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00579","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual-Ligand Metal–Organic Framework for Ultrasensitive Fluorescence Detection of Uranium: An In Situ Trace Enrichment Strategy to Overcome Concentration Limitations 超灵敏荧光检测铀的双配体金属-有机框架：一种克服浓度限制的原位微量富集策略

IF 8.7

JACS Au Pub Date : 2025-08-01 DOI: 10.1021/jacsau.5c00663

Mengtao Fu, Chengkai Mao, Changhong Wei, Chunxiao Wang, Qihui Kan, Shipeng Dong and Liang Mao*,

{"title":"Dual-Ligand Metal–Organic Framework for Ultrasensitive Fluorescence Detection of Uranium: An In Situ Trace Enrichment Strategy to Overcome Concentration Limitations","authors":"Mengtao Fu, Chengkai Mao, Changhong Wei, Chunxiao Wang, Qihui Kan, Shipeng Dong and Liang Mao*, ","doi":"10.1021/jacsau.5c00663","DOIUrl":"https://doi.org/10.1021/jacsau.5c00663","url":null,"abstract":"The development of trace analysis technology for uranium pollution has become crucial for ecological protection, owing to the extensive utilization of uranium in the nuclear industry. Fluorescence method has been widely used for the detection of uranium in water, but current research still suffers from insufficient sensitivity, sluggish detection speed, and interference from coexisting ions. This is mainly due to the poor selective enrichment ability of the sensors for trace uranium. Herein, a fluorescent metal–organic framework (MOF) named dual-ligand MOF-AO (DMOF-AO) with high uranium affinity was synthesized via a mixed ligand strategy. The incorporated amidoxime groups served as specific recognition sites, achieving a high quenching selectivity against at least 17 interfering ions. The biomimetic flower-like structure coupled with the second ligand intercalation strategy greatly improves the mass transfer rate, enabling the rapid in situ enrichment of uranium even at trace concentrations. This synergistic design and trace uranium enrichment strategy resulted in high detection sensitivity (LOD of 2.72 nmol L–1) and ultrashort response time (10 s), surpassing most reported fluorescent sensors. Mechanistic investigations elucidated the coordination configuration and revealed the underlying fluorescence quenching mechanism caused by photoinduced electron transfer. The uranium concentrations in the actual water samples from different regions tested by DMOF-AO were consistent with the gold-standard ICP-MS results, validating the practical reliability. This study demonstrates the promoting effect of improving enrichment ability at trace concentrations on detection sensitivity and establishes an efficient, instantaneous, visualization, and reliable strategy for uranium detection using fluorescent MOF.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"4044–4054"},"PeriodicalIF":8.7,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00663","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

DNA-Programmable Protein Degradation: Dynamic Control of Proteolysis-Targeting Chimera Activity via DNA Hybridization and Strand Displacement DNA可编程蛋白降解：通过DNA杂交和链位移对蛋白水解靶向嵌合体活性的动态控制

IF 8.7

JACS Au Pub Date : 2025-07-31 DOI: 10.1021/jacsau.5c00422

Disha Kashyap, Shozeb Haider, Thomas A. Milne* and Michael J. Booth*,

{"title":"DNA-Programmable Protein Degradation: Dynamic Control of Proteolysis-Targeting Chimera Activity via DNA Hybridization and Strand Displacement","authors":"Disha Kashyap, Shozeb Haider, Thomas A. Milne* and Michael J. Booth*, ","doi":"10.1021/jacsau.5c00422","DOIUrl":"https://doi.org/10.1021/jacsau.5c00422","url":null,"abstract":"Targeted protein degradation is a powerful therapeutic approach: expanding the druggable proteome, providing enhanced selectivity, and having the ability to overcome conventional resistance mechanisms. A major class of such molecules is proteolysis-targeting chimeras (PROTACs). PROTACs are catalytic heterobifunctional small molecules that simultaneously bind a protein of interest (POI) and an E3 ligase. And thus, PROTACs induce a proximity-dependent ubiquitination of the POI and its subsequent degradation by the ubiquitin–proteasome system. While PROTACs have successfully transitioned from academia to industry, increasing awareness of off-target effects and related toxicities highlights the urgent need for precise control mechanisms over activity. Achieving this level of control, however, remains challenging, with traditional chemistries. DNA nanotechnology, with its unparalleled programmability and structural versatility, presents a powerful tool for achieving such control. Here, we report the design and characterization of oligonucleotide-linked PROTACs (OligoPROTACs). These constructs comprise PROTAC warheads covalently linked to separate complementary DNA strands, brought together in space via DNA hybridization. OligoPROTACs are able to degrade the POI in a distance-dependent manner. Furthermore, we demonstrate the first instance of a dynamic off-switch mechanism for PROTAC activity, enabled by toehold-mediated strand displacement using a third DNA strand. This work highlights the potential of DNA nanotechnology combined with the clinical emergence of nucleic acid therapeutics to enhance the safety and functionality of PROTAC systems, paving the way for more refined and translatable therapeutic strategies.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3799–3807"},"PeriodicalIF":8.7,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00422","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892624","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Fluorinating the Sugar and the Nucleotide: Exploring Fluorination Within GDP-Mannose Probes Using Chemoenzymatic Synthesis 糖和核苷酸的氟化：利用化学酶合成探索gdp -甘露糖探针中的氟化

IF 8.7

JACS Au Pub Date : 2025-07-31 DOI: 10.1021/jacsau.5c00626

Jonathan P. Dolan, Sean T. Evans, Caecilie M. M. Benckendorff, Suat Sari, Aisling Ní Cheallaigh and Gavin J. Miller*,

{"title":"Fluorinating the Sugar and the Nucleotide: Exploring Fluorination Within GDP-Mannose Probes Using Chemoenzymatic Synthesis","authors":"Jonathan P. Dolan, Sean T. Evans, Caecilie M. M. Benckendorff, Suat Sari, Aisling Ní Cheallaigh and Gavin J. Miller*, ","doi":"10.1021/jacsau.5c00626","DOIUrl":"https://doi.org/10.1021/jacsau.5c00626","url":null,"abstract":"Fluorinated glycans offer a prime opportunity to study the intricacies of their associated binding events with proteins, invoke resistance toward enzymatic hydrolysis, and modulate carbohydrate physicochemical properties. Sugar nucleotides are the key building blocks used by glycosyltransferases and associated enzymes to assemble glycans and, as such, represent a considerable landscape of opportunity to develop fluorinated motifs and enable structure-to-function understanding. Herein, we target the isosteric inclusion of fluorine within the nucleoside diphosphate sugar framework of GDP-mannose using a chemoenzymatic approach. Utilizing chemical synthesis to incorporate bespoke fluorine modifications and a promiscuous pyrophosphorylase, to assemble the sugar nucleotide, enables first-in-class access to GDP-mannoses containing fluorine within the nucleotide alongside double fluorination, within both the pyranose and nucleotide. These materials are utilized to probe a guanosine diphosphate mannose dehydrogenase critical to mucoid Pseudomonas aeruginosa alginate biosynthesis. This work provides an exemplar framework for incorporating fluorine within the nucleotide of derived sugar nucleotides and thus the capability to study glycosyltransferesase utilizing GDP-mannose more broadly.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3994–4001"},"PeriodicalIF":8.7,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00626","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892623","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thick ZnS Shells on CsPbBr3 Quantum Dots by Colloidal-Atomic Layer Deposition for Enhanced Photoluminescence and Stability 胶体-原子层沉积在CsPbBr3量子点上的厚ZnS壳增强光致发光和稳定性

IF 8.7

JACS Au Pub Date : 2025-07-31 DOI: 10.1021/jacsau.5c00651

Justice A. Teku, Derrick A. Taylor and Jong-Soo Lee*,

{"title":"Thick ZnS Shells on CsPbBr3 Quantum Dots by Colloidal-Atomic Layer Deposition for Enhanced Photoluminescence and Stability","authors":"Justice A. Teku, Derrick A. Taylor and Jong-Soo Lee*, ","doi":"10.1021/jacsau.5c00651","DOIUrl":"https://doi.org/10.1021/jacsau.5c00651","url":null,"abstract":"The colloidal-atomic layer deposition (c-ALD) method is employed to grow a zinc sulfide (ZnS) shell on CsPbBr3 perovskite quantum dots (PeQDs) to form CsPbBr3/ZnS core/shell heterostructures to address the intrinsic stability challenges of PeQDs. The c-ALD process offers layer by layer control over the thickness of the shell, enabling uniform and conformal encapsulation, which significantly passivates the surface defects and enhances the optical properties of the PeQDs. This approach significantly improves photoluminescence quantum yield, increases environmental stability, and prolongs the average radiative lifetime of the CsPbBr3 PeQDs. The structural and spectroscopic analysis confirms the formation of a thick and uniform ZnS shell. Furthermore, the resulting core/shell PeQDs exhibit exceptional thermal, photostability, and aqueous durability, surpassing the limitations of pristine CsPbBr3 PeQDs. This work opens new opportunities for the c-ALD method to be integrated into perovskite core/shell heterostructures for advancing optoelectronic technologies.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"4036–4043"},"PeriodicalIF":8.7,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00651","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892622","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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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