Journal of the American Chemical Society最新文献_第4页

Unraveling the Roles of Amines in Atom Transfer Radical Polymerization in the Dark

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.4c18496

Arman Moini Jazani, Gorkem Yilmaz, Mitchell Baumer, Julian Sobieski, Stefan Bernhard, Krzysztof Matyjaszewski

{"title":"Unraveling the Roles of Amines in Atom Transfer Radical Polymerization in the Dark","authors":"Arman Moini Jazani, Gorkem Yilmaz, Mitchell Baumer, Julian Sobieski, Stefan Bernhard, Krzysztof Matyjaszewski","doi":"10.1021/jacs.4c18496","DOIUrl":"https://doi.org/10.1021/jacs.4c18496","url":null,"abstract":"Multidentate amines have been widely used as ligands (L) for Cu-catalysts in atom transfer radical polymerization (ATRP) and as electron donors in photochemically induced polymerizations. However, mechanistic aspects of the role of amines in ATRP in the dark have remained elusive. Herein, the structure–activity relationship and the related electron transfer reactions with Br–CuII/L complexes and/or with alkyl bromides (R-Br) were investigated for 25 amines. Amines function as electron donors and reducing agents for Br–CuII/L complexes via an outer sphere electron transfer (OSET) mechanism, enabling slow but continuous generation of CuI/L activators and inducing controlled ATRP. However, two amines, diazabicyclo(5.4.0)undec-7-ene (DBU) and 1,1,3,3-tetramethylguanidine (TMG), reduced Br–CuII/L faster, suggesting an inner sphere electron transfer (ISET) process. ATRP, starting with initial deactivators (Br–CuII/L) species, proceeded in the dark in the presence of an excess of tertiary amines, such as tris[2-(dimethylamino)ethyl]amine (Me6TREN), 1,4-diazabicyclo[2.2.2]octane (DABCO), and TMG at room temperature and afforded polymers with low dispersities (Đ ≤ 1.15). With copper(II) triflate complex (CuII/L+2, –(OTf)2), which has a more positive reduction potential, ATRP proceeded at room temperature with several inexpensive secondary and tertiary amines including triethylamine (TEA) and dimethylethanolamine (DMAE). Interestingly, multidentate amines also served as direct R-Br activators at elevated temperatures (60 °C). In all cases, chains were initiated with R-Br and not by the amine radical cations as byproducts of electron transfer. Amines also enabled ATRP in the presence of residual air in flasks with a large headspace, underpinning them as a robust and accessible reducing agent for practical applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"41 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766761","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

Role of Site-Specific Iron in Fe-Doped Nickel Hydroxide Toward Water Oxidation Revealed by Spatially Resolved Imaging at the Single-Particle Level

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c00438

Jie Wei, Jing Zhu, Rong Jin, Yan Liu, Guiliang Liu, Ming-Hui Fan, Mingkai Liu, Dechen Jiang, Jie Zeng

{"title":"Role of Site-Specific Iron in Fe-Doped Nickel Hydroxide Toward Water Oxidation Revealed by Spatially Resolved Imaging at the Single-Particle Level","authors":"Jie Wei, Jing Zhu, Rong Jin, Yan Liu, Guiliang Liu, Ming-Hui Fan, Mingkai Liu, Dechen Jiang, Jie Zeng","doi":"10.1021/jacs.5c00438","DOIUrl":"https://doi.org/10.1021/jacs.5c00438","url":null,"abstract":"Water electrolysis driven by renewable electricity is limited by the slow-kinetic oxygen evolution reaction (OER). NiFe-based hydroxides are considered promising non-noble electrocatalysts toward the OER but require profound insight into the role of site-specific iron incorporation. Herein, we determined the critical role of edge sites on single-crystalline NiFe-based hydroxide toward the OER using spatially resolved in situ single-particle imaging techniques. The potential-driven incorporation of Fe into the specific edge or plane sites was achieved on two-dimensional (2D) Ni layer double hydroxide (LDH) single crystals. The spatially resolved scanning electrochemical cell microscopy imaging illustrated that Fe-doped edge sites dominated the activity of the OER rather than Fe-doped plane sites. In situ Raman spectroscopy imaging of single particles was used to monitor the evolution of edge and plane sites, revealing that the incorporation of Fe impeded the oxidation of Ni. Moreover, spatially resolved 18O-isotope-labeling experiments demonstrated that Fe doping hindered the oxygen exchange between Ni LDH and the electrolyte, inducing the switch of partial active sites from Ni to Fe. Combined with theoretical calculations, the Fe–Obridge–Ni sites contributed to the enhanced OER activity on Ni LDH with Fe doping at the edge, whereas the Ohollow (NiNiFe) sites induced by the infiltration of Fe into the plane were detrimental to the OER performance. This work provides direct spectroscopic evidence for understanding the specific sites at the single-particle level and guides the rational design of optimal electrocatalysts.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"34 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766762","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

Visualizing the Sliding Motion of Dynamic Rotaxanes by Surface Wrinkles

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c00968

Shuzhen Yan, Mengling Yang, Xinlu Deng, Guoquan Liu, Xiaxin Gao, Shuai Chen, Lin Cheng, Tiantian Li, Tianjiao Ma, Mengda Xu, Jin Li, Zhaoming Zhang, Li Yang, Wei Yu, Xuzhou Yan, Xuesong Jiang

{"title":"Visualizing the Sliding Motion of Dynamic Rotaxanes by Surface Wrinkles","authors":"Shuzhen Yan, Mengling Yang, Xinlu Deng, Guoquan Liu, Xiaxin Gao, Shuai Chen, Lin Cheng, Tiantian Li, Tianjiao Ma, Mengda Xu, Jin Li, Zhaoming Zhang, Li Yang, Wei Yu, Xuzhou Yan, Xuesong Jiang","doi":"10.1021/jacs.5c00968","DOIUrl":"https://doi.org/10.1021/jacs.5c00968","url":null,"abstract":"Visualizing the sliding dynamics of a topological network can provide critical insight into determining the design and properties of mechanically interlocked materials. Although several auxiliary techniques have been proposed to infer the microscopic motion of rotaxanes, employing intuitive and convenient methods to explore the microscopic dynamics of a mechanically interlocked polymer remains a significant challenge. Herein, this work introduces a mechanically interlocked network (MIN) into the patterned surfaces for visualizing and regulating the sliding process of [2]rotaxane units through the evolution of surface wrinkles. Upon the photodimerization of the anthracene-functionalized polymer chain, the surface wrinkle can be formed after thermal treatment and subsequent cooling to room temperature. Specifically, the cross-linked films exhibit visible changes in wrinkle topography through the disruption of host–guest recognition by alkaline stimuli. Moreover, by leveraging the unique mechanical properties of surface wrinkles, we prolonged and amplified the originally extremely transient and difficult-to-detect sliding motion of rotaxane units in terms of time scale. Through statistical analysis of the changes in wrinkle morphology, we were able to correspondingly deconstruct the three processes of the rotaxane sliding motion: (I) unrestricted rapid sliding following host–guest dissociation; (II) restricted sliding; and (III) termination of sliding. The novel approach we propose opens a new avenue for studying the microscopic molecular motion of mechanically interlocked materials, facilitating the advancement and application of mechanically interlocked structures. In addition to using macroscopic surface patterns to visualize and explore microscopic molecular motion, the motion of microscopic molecules can also be used to regulate macroscopic surface patterns.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"16 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766764","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

In Situ Neutron Reflectometry Reveals the Interfacial Microenvironment Driving Electrochemical Ammonia Synthesis

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.4c16636

Valerie A. Niemann, Mathieu Doucet, Peter Benedek, Niklas H. Deissler, Jon Bjarke Valbaek Mygind, Sang-Won Lee, Isabela Rios Amador, Wrayzene L. Willoughby, Ib Chorkendorff, Adam C. Nielander, William A. Tarpeh, Thomas F. Jaramillo

{"title":"In Situ Neutron Reflectometry Reveals the Interfacial Microenvironment Driving Electrochemical Ammonia Synthesis","authors":"Valerie A. Niemann, Mathieu Doucet, Peter Benedek, Niklas H. Deissler, Jon Bjarke Valbaek Mygind, Sang-Won Lee, Isabela Rios Amador, Wrayzene L. Willoughby, Ib Chorkendorff, Adam C. Nielander, William A. Tarpeh, Thomas F. Jaramillo","doi":"10.1021/jacs.4c16636","DOIUrl":"https://doi.org/10.1021/jacs.4c16636","url":null,"abstract":"Electrified interfaces are critical to the performance of energy systems and often demonstrate substantial complexity under operating conditions. A nanoscale understanding of the interfacial microenvironment, i.e., the solid-electrolyte interphase (SEI), in lithium-mediated nitrogen reduction (Li–N2R) is key for realizing efficient ammonia (NH3) production. Herein, we used time-resolved neutron reflectometry (NR) to observe SEI formation under Li–N2R conditions. We found that the LiBF4-based electrolyte provided a substantially more well-defined SEI layer than previous SEI NR interrogations that used LiClO4, highlighting the underlying chemistry that dictates electrolyte design and enabling new NR-based studies. Using in situ NR, we found that the LiBF4-derived SEI under Li–N2R conditions comprises a thick, diffuse outer layer and a thin, compact inner layer at low current cycling (<2 mA/cm2), revealing a structure which ex situ studies have not been able to probe. Increased current cycling and sustained current cycling led to the merging of the layers into a single-layer SEI. We used isotope contrast methods with d6-EtOH and d8-THF to drive time-resolved tracking of SEI growth at low current cycling, revealing that the proton donor modifies the inner layer, and the solvent modifies the outer layer. Li dendritic growth was observed in the absence of a proton donor. Neutron absorption also indicated the presence of boron in the SEI, underscoring the value of neutron-based interrogation. Our results inform Li-based systems and reaction microenvironments, and these methods can be applied broadly to interfacial energy technologies.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"58 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758723","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

Magnetic Field-Enhanced Acidic CO2 Electroreduction Reaction on Single Nickel-Site Catalysts

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c00858

Jia Song, Dayin He, Xianhui Ma, Peigen Liu, Wenxin Guo, Rongbo Sun, Feng Li, Zhicheng Zhong, Huang Zhou, Jun Tang, Jie Xu, Tongwei Wu, Lin Hu, Yuen Wu

{"title":"Magnetic Field-Enhanced Acidic CO2 Electroreduction Reaction on Single Nickel-Site Catalysts","authors":"Jia Song, Dayin He, Xianhui Ma, Peigen Liu, Wenxin Guo, Rongbo Sun, Feng Li, Zhicheng Zhong, Huang Zhou, Jun Tang, Jie Xu, Tongwei Wu, Lin Hu, Yuen Wu","doi":"10.1021/jacs.5c00858","DOIUrl":"https://doi.org/10.1021/jacs.5c00858","url":null,"abstract":"The synergistic integration of electrochemical reactions with an external magnetic field offers a powerful strategy for enhancing reaction performance. Herein, we introduce a flexible and continuously adjustable external magnetic field to enhance acidic CO2 reduction reaction (CO2RR) performance. In an acidic electrolyte (pH = 0.91), the initial Faradaic efficiency (FE) of the CO2RR for CO is only 18%, which can be increased to 63.2% when a 2 T magnetic field is applied. More importantly, the introduction of this external magnetic field enables the continuous switching of CO2 reduction products in a noncontact magnetic switching mode. Theoretical calculations demonstrate that the application of a magnetic field promotes CO2 adsorption at Ni sites and inhibits the hydrogen evolution reaction (HER), ultimately enhancing CO2RR activity and selectivity. This work provides fresh insight into how an external magnetic field promotes CO2RR performance.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"37 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766765","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

Reactive ZIF-L Crystal Surface for Organophosphorous Degradation and Acetylcholinesterase Reactivation.

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 Epub Date: 2025-03-10 DOI: 10.1021/jacs.5c00382

Emilio Borrego-Marin, Pablo Garrido-Barros, Gregory W Peterson, Rebecca Vismara, Francisco J Carmona, Elisa Barea, Jorge A R Navarro

{"title":"Reactive ZIF-L Crystal Surface for Organophosphorous Degradation and Acetylcholinesterase Reactivation.","authors":"Emilio Borrego-Marin, Pablo Garrido-Barros, Gregory W Peterson, Rebecca Vismara, Francisco J Carmona, Elisa Barea, Jorge A R Navarro","doi":"10.1021/jacs.5c00382","DOIUrl":"10.1021/jacs.5c00382","url":null,"abstract":"The importance of crystal surface reactivity of reticular materials is exemplified by exfoliation of nonporous layered zeolitic imidazolate framework Zn(mIm)2·0.5mImH (ZIF-L, mImH = 2-methylimidazole). Sonication of ZIF-L ethanolic suspensions leads to exfoliation of microcrystals along the 2 0 0 planes, giving rise to 1.5 μm wide × 25 nm thick flakes, which we term ZIF-L_exf. ZIF-L_exf exhibits a high reactivity toward hydrolytic degradation of extremely toxic G-type nerve agents, Soman (GD), and simulant diisopropylfluorophosphate (DIFP). The reactivity of the crystal surface of ZIF-L_exf toward P-F bond breakdown gives rise to framework structural degradation, releasing nucleophilic mImH molecules that reactivate organophosphate-inhibited acetylcholinesterase within 10 min. This detoxification process can be taken as a proof of concept for reversing organophosphorous poisoning. More generally, this approach underscores the importance of the crystal surface nature and composition to control the reactivity of reticular materials.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"10834-10839"},"PeriodicalIF":14.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143595909","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

Engineered Artificial Nanochannels with Cell Membrane Nanointerface for Ultrasensitive Detection and Discrimination of Multiple Bacterial Infections

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c01542

Jin Wang, Chengcheng Zhu, Jing Tan, Jing-Juan Xu, Chen Wang

{"title":"Engineered Artificial Nanochannels with Cell Membrane Nanointerface for Ultrasensitive Detection and Discrimination of Multiple Bacterial Infections","authors":"Jin Wang, Chengcheng Zhu, Jing Tan, Jing-Juan Xu, Chen Wang","doi":"10.1021/jacs.5c01542","DOIUrl":"https://doi.org/10.1021/jacs.5c01542","url":null,"abstract":"Bacterial infection is a major threat to global public health, which urgently require rapid and reliable analytical techniques for complex biological samples but remains a challenge. Herein, we developed an artificial affinity nanochannel with a cell membrane nanointerface, which enables broad-spectrum capture and specifically discriminates multiple pathogens. The macrophage membrane is pre-engineered with azide groups by a biometabolic process and then modified on a porous anodized aluminum oxide substrate via click reactions, preserving dynamic lateral fluidity and broad-spectrum recognition capacity. The macrophage membrane/anodized aluminum oxide membrane is evaluated with remarkable ion current rectification performance with a distinct current response upon bacterial binding, which realizes ultrasensitive detection of bacteria. Moreover, discrimination of bacterial species is achieved by further introducing specific antibodies. The nanochannel-based biosensor allows accurately capturing and quantifying multiple bacteria over a broad linear range, with a detection limit as low as 2.7 CFU/mL. Finally, this nanoplatform is successfully applied for broad-spectrum capture of bacterial species in several practical application scenarios including water, serum, and blood samples, achieving ultrasensitive detection and identification of bacteria below 10 CFU/mL. Overall, the proposed nanochannel with cell membrane nanointerface shows broad applicability in bacterial analysis, highlighting its potential in diagnosing infectious diseases.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"33 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766771","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

Chiral Lewis Acid-Catalyzed Intramolecular [2 + 2] Photocycloaddition: Enantioselective Synthesis of Azaarene-Functionalized Azabicyclo[2.1.1]hexanes and Bicyclo[1.1.1]pentanes

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c03542

Dong Tian, Yixing Pan, Xiaowei Zhao, Yanli Yin, Zhiyong Jiang

引用次数: 0

Excess Cations Alter *CO Intermediate Configuration and Product Selectivity of Cu in Acidic Electrochemical CO2 Reduction Reaction

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c02954

Suhwan Yoo, Sejin Park, Jihoon Son, Jiseon Kim, Hyeyoung Shin, Yun Jeong Hwang

{"title":"Excess Cations Alter *CO Intermediate Configuration and Product Selectivity of Cu in Acidic Electrochemical CO2 Reduction Reaction","authors":"Suhwan Yoo, Sejin Park, Jihoon Son, Jiseon Kim, Hyeyoung Shin, Yun Jeong Hwang","doi":"10.1021/jacs.5c02954","DOIUrl":"https://doi.org/10.1021/jacs.5c02954","url":null,"abstract":"Concentrated cations are often employed to promote electrochemical CO2 reduction reaction (CO2RR) selectivity in acidic electrolytes. Here, we investigate the influence of excess cations on the *CO adsorption configuration and the product distribution of the CO2RR. Operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals that increasing the Cs+ concentration shifts the preference of the *CO intermediate on the Cu surface from the atop (*COatop) to the bridge (*CObridge) configuration. This transition leads to a sharp decline in C–C coupling and an increase in the hydrogen evolution reaction at high Cs+ concentrations (0.7 and 1.0 M) under acidic conditions. Time-resolved SEIRAS scans show that *COatop is kinetically dominant and the proportion of *CObridge increases gradually only at high cation concentrations. Density functional theory simulations confirm that Cs+ on the Cu surface can interact electrostatically with *CO and stabilize *CObridge over *COatop on the Cu surface. The evolution of *CObridge is also observed on Ag catalysts, indicating that the effect at high concentrations is not limited to Cu. Furthermore, polymeric binders on the Cu surface mitigate these detrimental effects on the CO2RR and restore C2H4 production by preventing the cation from altering the *CO adsorption sites on the catalyst surface. This study provides new insights into the effects of cations on catalyst performance, with implications for catalyst design and operation.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"8 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758551","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

Enzyme-Mimic Activities of RuCo Bimetallic Nanosheets for Inflammatory Bowel Disease Treatment

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-02 DOI: 10.1021/jacs.5c00100

Zhixin Chen, Ya-Xuan Zhu, Yanling You, Min Ge, Yihan Chen, Han Lin, Jianlin Shi

{"title":"Enzyme-Mimic Activities of RuCo Bimetallic Nanosheets for Inflammatory Bowel Disease Treatment","authors":"Zhixin Chen, Ya-Xuan Zhu, Yanling You, Min Ge, Yihan Chen, Han Lin, Jianlin Shi","doi":"10.1021/jacs.5c00100","DOIUrl":"https://doi.org/10.1021/jacs.5c00100","url":null,"abstract":"The presence of abnormal levels of reactive oxygen species (ROS) is a recognized pathological feature of inflammatory bowel disease (IBD). Therefore, the development of orally administered antioxidants with high antioxidative capacity and gastric acid tolerance for the treatment of IBD is of great significance. Here, we present the design and synthesis of a bimetallic ruthenium–cobalt (RuCo) nanosheet for the treatment of IBD. The Ru–Co atoms within the nanosheet structure exhibit significant electron transfer properties owing to their electronegativity feature. Density functional theory calculations indicate that the RuCo nanosheets have higher d-band centers than the corresponding Ru and Co metal monoliths, which increases the catalytic activity. Such RuCo nanosheets exhibit superoxide dismutase and catalase-like cascade enzyme activities and show robust stability in gastric fluid over a 4 h period when exposed to simulated gastric fluid, ensuring desirable retention of antioxidative activity. Cellular and animal studies show that RuCo nanosheets are capable of effectively reducing oxidative stress, preventing inflammatory responses triggered by an abnormal increase in ROS at intestinal sites, and thus protecting cells from inflammatory damages. This research presents a gastric-acid-stabilized antioxidative nanocatalytic platform for the efficient treatment of inflammatory diseases of the digestive system.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"10 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766760","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