Angewandte Chemie International Edition最新文献

Modulating Adsorption Behavior by Single-site Pt on RuO2 for Efficient Electrosynthesis of Glycolic Acid from Plastic Wastes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202422183

Yong Chen, Fulai Liu, Jingtao Zhou, Xutao Gao, Rui Shi, Zhengxiao Guo, Edmund C. M. Tse

{"title":"Modulating Adsorption Behavior by Single-site Pt on RuO2 for Efficient Electrosynthesis of Glycolic Acid from Plastic Wastes","authors":"Yong Chen, Fulai Liu, Jingtao Zhou, Xutao Gao, Rui Shi, Zhengxiao Guo, Edmund C. M. Tse","doi":"10.1002/anie.202422183","DOIUrl":"https://doi.org/10.1002/anie.202422183","url":null,"abstract":"Electrochemical upcycling of polyethylene terephthalate (PET) wastes into valuable glycolic acid (GA) is an ideal solution for resource utilization. However, simultaneously achieving high activity and selectivity remains challenging due to the over-oxidation and C-C cleavage during ethylene glycol (EG) oxidation in PET hydrolysate. Herein, we develop an atomically isolated Pt on RuO2 (Pt1/RuO2) catalyst composed of high-density Pt-Ru interfaces that ensure single-site adsorption of EG, enrich surface *OH coverage and weaken *CO−CH2OH intermediate adsorption, thereby synergistically promoting GA generation. Specifically, Pt1/RuO2 delivers a remarkable mass activity of 8.09 A/mgPt, as well as a high GA Faradaic efficiency (95.3%) and selectivity (96.9%). Under membrane electrode assembly conditions, Pt1/RuO2 realizes a stable electrolysis over 500 h at 6 A with a GA yield rate of 4.06 g h-1. In-depth theoretical and in situ spectroscopic investigations reveal the synergy between isolated Pt and oxophilic RuO2 plays a crucial role in high-efficiency EG-to-GA conversion. This study offers valuable insights for the rational design of advanced catalysts for GA synthesis from PET wastes via a single-site doped bimetallic strategy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"23 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471057","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

Stefan‐Boltzmann Water Catalyzed Propane Dehydrogenation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202424800

Xue Ding, Zichan Zheng, Chengyuan Liu, Junchuan Sun, Yongcai Zhang, Chen Huang, Wenguang Tu, Long Zhao, Zhixin Hu, Zhigang Zou, Lu Wang

引用次数: 0

A Druglike Ferrostatin‐1 Analogue as a Ferroptosis Inhibitor and Photoluminescent Indicator

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202502195

Jiangkun Yan, Luo Bao, Huicong Liang, Li Zhao, Ming Liu, Lingxiu Kong, Xuejing Fan, Chunhui Liang, Tongtong Liu, Xinyu Han, Kangnan Wang, Chuanbin Shen, Wanyang Sun, Xin Zhou, Bo Chu, Michael McGlinchey, Ximing Xu, Xue Qiu, Yong Wang

{"title":"A Druglike Ferrostatin‐1 Analogue as a Ferroptosis Inhibitor and Photoluminescent Indicator","authors":"Jiangkun Yan, Luo Bao, Huicong Liang, Li Zhao, Ming Liu, Lingxiu Kong, Xuejing Fan, Chunhui Liang, Tongtong Liu, Xinyu Han, Kangnan Wang, Chuanbin Shen, Wanyang Sun, Xin Zhou, Bo Chu, Michael McGlinchey, Ximing Xu, Xue Qiu, Yong Wang","doi":"10.1002/anie.202502195","DOIUrl":"https://doi.org/10.1002/anie.202502195","url":null,"abstract":"Redox‐based diagnostic and therapeutic applications have long suffered from a shortage of suitable drugs and probes of high specificity. In the context of anti‐ferroptosis research for neurological diseases, the inaccessibility of a blood‐brain barrier permeable (BBB) small molecular ferroptosis inhibitor, and the lack of specific ferroptosis probes seriously impeded a deeper understanding of the mechanism of ferroptosis and the development of clinically applicable drugs. We here report a novel 1,3,4‑thiadiazole‐functionalized drug‐like ferrostatin analogue entitled Ferfluor‐1 with superior anti‐ferroptosis potency, favorable BBB permeability and in vivo activity against stroke and Parkinson’s disease. Moreover, the exclusive pseudo excited‐state intramolecular proton‐transfer (ESIPT) property of Ferfluor‐1 via a long‐distance hydrogen‐bonding network facilitated it as the first sensitive ratiometric photoluminescent probe to detect phospholipid hydroperoxides and a specific indicator for the fluctuation of ferroptosis. These unprecedented advantages not only engendered Ferfluor‐1 as a potential tool for ferroptosis‐related diagnostic and therapeutic applications in the central nervous system, but also paved the way to developing new theragnostic agents for precision redox detection and regulation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"21 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470671","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

Nanofabrication via SEM Electron‐beam Stimulated Suzuki‐Miyura Type Reaction: Fingerprints of Carbazole Derivative Revealed by Synchrotron‐IR Nanospectroscopy and Mass Spectrometry

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202425591

Matheus Costa Ximenes, Luiz Phelipe de Souza Tomaso, Igor Zanetti, Amanda Beatriz Silva Quirgo dos Reis, Eustáquio de Souza Baêta Júnior, Leticia dos Santos Aguilera, Suzana Bottega Peripolli, Lucyano Jefferson Alves Macedo, Raul de Oliveira Freitas, Luiz Fernando Brum Malta, José Brant de Campos, Jaqueline Dias Senra

{"title":"Nanofabrication via SEM Electron‐beam Stimulated Suzuki‐Miyura Type Reaction: Fingerprints of Carbazole Derivative Revealed by Synchrotron‐IR Nanospectroscopy and Mass Spectrometry","authors":"Matheus Costa Ximenes, Luiz Phelipe de Souza Tomaso, Igor Zanetti, Amanda Beatriz Silva Quirgo dos Reis, Eustáquio de Souza Baêta Júnior, Leticia dos Santos Aguilera, Suzana Bottega Peripolli, Lucyano Jefferson Alves Macedo, Raul de Oliveira Freitas, Luiz Fernando Brum Malta, José Brant de Campos, Jaqueline Dias Senra","doi":"10.1002/anie.202425591","DOIUrl":"https://doi.org/10.1002/anie.202425591","url":null,"abstract":"Carbazole‐based compounds have demonstrated interesting physical and chemical properties for OLED devices. 3,6‐diphenylcarbazole has a direct application in the composition of structures with potential to suppress the loss of efficiency under high luminance conditions along with its use in the emitting layer. In this study, we reveal and explore the conditions in which a triggered electron beams (e‐beams) solid state Suzuki‐Miyaura type reaction between 3,6‐diiodocarbazole and phenylboronic acid could be carried out. Applying typical SEM acceleration voltage (30 keV), sufficient energy transfer enabled the activation of the reaction. Synchrotron Infrared Nano Spectroscopy (SINS) was used to acquire nanoscale molecular vibrational spectra and compare with conventional FTIR absorption spectra for chemical characterization. Evidences obtained by mass spectrometry confirmed the formation of the 3,6‐diphenyl‐9H‐carbazole under higher e‐beam dose (30 keV, 10 minutes), when compared to 5 and 10 keV. In addition, the phenylboronic acid seems to have a role in the reaction outcome. Both samples irradiated in the presence and in the absence of palladium exhibited the fingerprints of the expected product 3,6‐diphenylcarbazole shedding light on possible alternative mechanisms and the straightforward construction of nanodevices.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"47 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470670","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

Aqueous Zinc-Ion Batteries with Boosted Stability and Kinetics Under a Wide Temperature Range

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202500434

Lei Zhang, Yu Han, Yaheng Geng, Hui Zhang, Hongguang Liu, Yan He, Zichao Yan, Zhiqiang Zhu

{"title":"Aqueous Zinc-Ion Batteries with Boosted Stability and Kinetics Under a Wide Temperature Range","authors":"Lei Zhang, Yu Han, Yaheng Geng, Hui Zhang, Hongguang Liu, Yan He, Zichao Yan, Zhiqiang Zhu","doi":"10.1002/anie.202500434","DOIUrl":"https://doi.org/10.1002/anie.202500434","url":null,"abstract":"Sustainable aqueous zinc ion batteries (AZIBs) necessitate a wide operational temperature range to ensure practicability, yet achieving this often compromises either reaction kinetics at low temperatures or cycling stability at high temperatures. Here we present an electrolyte design that balances this trade-off, enhancing the stability and kinetics of AZIBs across −60 to 60 °C. Our approach incorporates silk fibroin as a multifunctional additive into ZnCl2-based “water-in-salt” electrolyte, which modifies both electrolyte structure and electrode interphase. Specifically, Zn||Zn half-cells with this electrolyte realize low hysteresis (180 mV at 1 mA cm–2) at −60 °C, and stable operation (200 hours at 2 mA cm–2) at 60 °C. This electrolyte is compatible with both inorganic and organic cathode materials. Remarkably, an ampere-hour-level Zn||V2O5·nH2O pouch cell with this electrolyte achieves an energy density of ∼72W h L–1 with minimal capacity decay after 50 cycles at 0.5 A g–1. Furthermore, the pouch cell stably cycles across −60 to 60 °C. This strategy provides a powerful solution to the challenges of aqueous metal-ion batteries at extreme temperatures.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"6 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471106","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

Photoexcited Transition‐Metal Catalyzed Carbon‐Halogen Bond Formation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202500929

Ramon Arora, Philip Samokhin, Mark Lautens

引用次数: 0

Enabling Solid‐Electrolyte Interphase Formation Prior to Water Reduction in Aqueous Zinc Batteries by Mild Protic Chemistry

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202424642

Taiqiang Chen, Yunfei Wang, Xin Li, Tao Yuan, Yuepeng Pang, Shiyou Zheng

{"title":"Enabling Solid‐Electrolyte Interphase Formation Prior to Water Reduction in Aqueous Zinc Batteries by Mild Protic Chemistry","authors":"Taiqiang Chen, Yunfei Wang, Xin Li, Tao Yuan, Yuepeng Pang, Shiyou Zheng","doi":"10.1002/anie.202424642","DOIUrl":"https://doi.org/10.1002/anie.202424642","url":null,"abstract":"Challenges like hydrogen evolution reaction (HER) and dendrite formation on zinc anodes hinder the practical application of aqueous zinc batteries (AZBs), primarily due to the lack of an exceptional passivating solid‐electrolyte interphase (SEI). To effectively prevent water decomposition, it is essential to in‐situ construct SEI prior to water reduction. This study shifts the focus from aprotic to protic SEI chemistry and predicts reduction potentials of mild protic compounds using thermodynamics. Based on this insight, mild protic 2‐mercapto‐1‐methylimidazole (MMI) is introduced and found to be reduced prior to water at higher electrode potentials, as MMI exhibits slightly higher proton activity than water due to its thiol group. The reduction of MMI produces isothiocyanate species via a proposed electrocatalytic ring cleavage mechanism, which deposit on zinc anodes to form an SEI predominantly composed of organic compounds supplemented with Zn(OH)2. Benefiting from the unique advantage of preferential reduction before water, the MMI‐derived SEI exhibits a superior passivating effect, as evidenced by a two‐order‐of‐magnitude reduction in corrosion current of zinc anodes from 1170 μA cm‐2 to 13.6 μA cm‐2. The SEI effectively suppresses HER, and ensures dendrite‐free zinc deposition, leading to high reversible zinc anodes with exceptional electrochemical performances.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470692","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

Super-Assembled Lamellar Conductive Heterochannels with Optical-Electrical Coupling Sensitivity for Smart Ion Transport

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202500116

Yaxin Guo, Xin Zhang, Shan Zhou, Qirui Liang, Hui Zeng, Yeqing Xu, Abuduheiremu Awati, Kang Liang, Dazhang Zhu, Mingxian Liu, Lei Jiang, Biao Kong

{"title":"Super-Assembled Lamellar Conductive Heterochannels with Optical-Electrical Coupling Sensitivity for Smart Ion Transport","authors":"Yaxin Guo, Xin Zhang, Shan Zhou, Qirui Liang, Hui Zeng, Yeqing Xu, Abuduheiremu Awati, Kang Liang, Dazhang Zhu, Mingxian Liu, Lei Jiang, Biao Kong","doi":"10.1002/anie.202500116","DOIUrl":"https://doi.org/10.1002/anie.202500116","url":null,"abstract":"Artificial nanofluidic devices for light-driven ion transport in biological systems based on the photoelectric effect have attracted extensive attention in signal transduction and smart ion transport. However, effective separation of photogenerated carriers in traditional p-n junction interface can be hindered by energy band structure of different semiconductor materials. Here, we present a novel approach using conductive polypyrrole (PPy) to modify GO, creating polypyrrole-graphene oxide (PyGO) functional lamellar conductive nanochannels with tailored channel-sized gradients and inherent optical-electrical coupling sensitivity via a facile super-assembly strategy. This design facilitates the PyGO own conductive lamellar channels and efficient separation of photogenerated carriers, resulting in significantly enhanced selective ion transport behavior. Coupling the conductivity and photosensitivity of PPy contributes to a peak power density of 14.1 W m-2 under a salinity differential of 0.5/0.01 M NaCl, which is 35.6% higher than that under dark conditions. Additionally, combing the salinity gradients with optical-electrical coupling sensitivity of the nanofludic devices, we demonstrate the application of PyGO in a real-time detection device for monitoring ion concentrations in nutrient solutions, paving the way for smart irrigation systems in agriculture. This work presents a novel and effective strategy for light-driven ion transport with potential applications in energy conversion and beyond.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"27 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471055","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

6H-Intermediate Phase Enabled Slow Crystal Growth of Tin Halide Perovskites for Indoor Photovoltaics

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202421547

Muhammad Abdel-Shakour, Junfang Wang, Junjie Huang, Zhen Gao, Yongle Pan, Xiangyue Meng

{"title":"6H-Intermediate Phase Enabled Slow Crystal Growth of Tin Halide Perovskites for Indoor Photovoltaics","authors":"Muhammad Abdel-Shakour, Junfang Wang, Junjie Huang, Zhen Gao, Yongle Pan, Xiangyue Meng","doi":"10.1002/anie.202421547","DOIUrl":"https://doi.org/10.1002/anie.202421547","url":null,"abstract":"The rapid expansion of Big Data and Internet of Things (IoT) has driven significant advancements in indoor photovoltaics (IPVs), which provide power to wireless IoT devices. Tin halide perovskites (THPs) have garnered significant attention for IPVs due to their excellent optoelectronic properties without the environmental risks of lead exposure. However, THPs face challenges in controlling their fast crystallization process. Here, we introduce a novel approach to precisely control the crystallization kinetics of FASnI2Br perovskite via the formation of the 6H-intermediate phase, supported by the mesomeric (+M) interaction effect of 4-aminopyridine hydrochloride (4APCl) in the perovskite precursor. The grazing-incidence wide-angle X-ray scattering measurements indicated the formation of 6H-intermediate phase for the FASnI2Br-4APCl perovskite during the crystallization process. The in-situ ultraviolet-visible absorption spectroscopy during the spin coating and annealing process confirmed the reduction of crystal growth rate after the 6H-intermediate phase formation. Thus, high-quality perovskite films were obtained with reduced defects. The resulting IPVs achieved an efficiency of 21.55% under indoor illumination at 1000 lux, exceeding all types of lead-free perovskite IPVs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"50 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471058","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

Elucidating the Boundary of Intercalation vs. Sequestration in Supramolecular Polymers by Retrosynthetic Design Towards the Construction of Complex Supramolecular Systems

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202501693

Nils Bäumer, Soichiro Ogi, Shigehiro Yamaguchi

{"title":"Elucidating the Boundary of Intercalation vs. Sequestration in Supramolecular Polymers by Retrosynthetic Design Towards the Construction of Complex Supramolecular Systems","authors":"Nils Bäumer, Soichiro Ogi, Shigehiro Yamaguchi","doi":"10.1002/anie.202501693","DOIUrl":"https://doi.org/10.1002/anie.202501693","url":null,"abstract":"Controlled social self‐sorting by intercalation can offer distinct properties at the supramolecular level that go beyond the sum of its parts. Likewise, controlling narcissistic self‐sorting by sequestration can induce unique system properties such as dilution‐induced self‐assembly. In contrast, the interface between the two extreme cases has hitherto remained underexplored and clear design rules remain elusive. Herein we demonstrate that by fine‐tuning the molecular similarity of supramolecular synthons in a complex system, intricate control over concerted supramolecular equilibria can be achieved. By reducing the molecular similarity, a former intercalator can be tuned to become a strong or weak sequestrator. Understanding these roles in binary mixtures allows us to rationalize more complex tertiary systems. Consequently, we show here in‐depth the influence of an uncommon dual sequestration mechanism. Further, an unprecedented hybrid mechanism between supramolecular intercalation and sequestration could be demonstrated. We are hopeful that the results presented herein will contribute to the development and understanding of concerted processes in complex supramolecular systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"8 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470659","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