Chemical Science最新文献_第2页

Synergistic catalysis between In single atoms and In nanoparticles for highly selective electrocatalytic CO2 reduction to formate with high current densities In单原子和In纳米颗粒之间的协同催化在高电流密度下高选择性电催化CO2还原生成甲酸盐

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d5sc01580d

Yuxin Chen, Junyoung Choi, Fangkui Liang, Xinyi Tan, Yudi Chen, Jiahui Yang, Song Hong, Xin Zhang, Alex Robertson, Yousung Jung, Zhenyu Sun

{"title":"Synergistic catalysis between In single atoms and In nanoparticles for highly selective electrocatalytic CO2 reduction to formate with high current densities","authors":"Yuxin Chen, Junyoung Choi, Fangkui Liang, Xinyi Tan, Yudi Chen, Jiahui Yang, Song Hong, Xin Zhang, Alex Robertson, Yousung Jung, Zhenyu Sun","doi":"10.1039/d5sc01580d","DOIUrl":"https://doi.org/10.1039/d5sc01580d","url":null,"abstract":"The practical realization of the electrocatalytic reduction of CO2 to formate is limited by the lack of suitable highly active and selective electrocatalysts, particularly candidates compatible with operation at high current densities. Herein, we report a dual-active sites electrocatalyst consisting of In single atoms and In nanoparticles supported on N, S-codoped porous carbon (In−NSC/NPs), which enables a remarkable formate faradaic efficiency (FE) of 92% with a large absolute partial current density for formate of up to 1.1 A·cm−2. By using membrane electrode assembly cells, a formate FE exceeding 90% and an energy conversion efficiency of over 44% are attainable within a wide cell voltage range of 2.4–3 V. The maximum formate generation rate reaches 10.5 mmol·cm−2·h−1 at a cell voltage of 2.9 V. By coupling with anodic glycerol oxidation, the formate yield rate in a full electrolytic cell is significantly improved to 23.2 mmol·cm−2·h−1 while using the same reaction conditions as the standard anodic oxygen evolution reaction. A combination of control experiments and in situ characterizations reveals that In nanoparticles facilitate the generation of the *OCHO and the subsequent hydrogenation step to generate formate while the In single atoms boost H2O dissociation. The generated *H migrates to the surface of the In nanoparticles, increasing the proton concentration and promoting the hydrogenation reaction.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"55 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143945957","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

Inhibition of ferroptosis by N-oxide-based fluorescent probes via selective oxidation of ferrous ion 基于n -氧化物的荧光探针通过选择性氧化亚铁离子抑制铁下垂

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d4sc07972h

Kanta Kawai, Rie Haruki, Shunsuke Nozawa, Hideko Nagasawa, Tasuku Hirayama

引用次数: 0

Spiro-Fluorene Locked Multi-Resonance Delayed Fluorescence Helical Framework: Efficient Circularly Polarized Electroluminescent Material 螺芴锁定多共振延迟荧光螺旋框架：高效圆极化电致发光材料

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d5sc01958c

Xinliang Cai, Jinbei Wei, Zhiqiang Li, Yexuan Pu, Youwei Wu, Yue Wang

{"title":"Spiro-Fluorene Locked Multi-Resonance Delayed Fluorescence Helical Framework: Efficient Circularly Polarized Electroluminescent Material","authors":"Xinliang Cai, Jinbei Wei, Zhiqiang Li, Yexuan Pu, Youwei Wu, Yue Wang","doi":"10.1039/d5sc01958c","DOIUrl":"https://doi.org/10.1039/d5sc01958c","url":null,"abstract":"Due to their excellent optical properties, circularly polarized multiple resonance thermally activated delayed fluorescence (CP-MR-TADF) compounds are highly suitable for applications as chiral emitters with high efficiencies and high color purity. However, the challenges of limited molecular design strategies often hinder their application in circularly polarized organic light-emitting diodes (CP-OLEDs). In this work, based on an intramolecular-locking strategy, a carbon bridge was introduced to fuse the tert-butyl carbazole moiety within the MR skeleton, which merges the intrinsically helical chirality into the MR framework. The designed molecule was modified by incorporating a locking group with significant spatial hindrance, named Spiro-3TCzBN. Consequently, the optimized CP-OLEDs with (P/M)-Spiro-3TCzBN emitters achieve remarkable maximum external quantum efficiencies of 34.6% and 34.9%, respectively, accompanied by clear circularly polarized electroluminescence signals with electroluminescence dissymmetry factors of −3.51 × 10−4 and +4.26 × 10−4. Furthermore, the electroluminescence spectra of Spiro-3TCzBN-based OLEDs show a notably stable profile as the doping level increases from 1-10 wt%. These results indicate that the conformational locking strategy is a compelling design approach for helicene, which is expected to be a potential chiral optical material for next-generation high-resolution CP-OLED displays.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"231 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946012","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

Synthesis of Polysubstituted Cyclobutanes through Photoredox Strain-Release/[3,3]-Rearrangement Cascade 光氧化还原-释放/[3,3]-重排级联合成多取代环丁烷

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d5sc01431j

Fangqing Zhang, Chun Xu, Zichun Zhang, Zhuang Yang, Tao Peng, Wen Shao, Xiaoming Feng, Yangbin Liu

引用次数: 0

A Strategy of Chiral Cation Coordination to Achieve Large Luminescence Dissymmetry Factor in 1D Hybrid Manganese Halides 一维杂化卤化锰中实现大发光不对称因子的手性阳离子配位策略

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d5sc01615k

Fei Wang, Xingjun Li, Tianqi Chen, Liqing Wang, Chenliang Li, Wei Zhang, Wen Yuan, Shan Lu, Lina Li, Xueyuan Chen

{"title":"A Strategy of Chiral Cation Coordination to Achieve Large Luminescence Dissymmetry Factor in 1D Hybrid Manganese Halides","authors":"Fei Wang, Xingjun Li, Tianqi Chen, Liqing Wang, Chenliang Li, Wei Zhang, Wen Yuan, Shan Lu, Lina Li, Xueyuan Chen","doi":"10.1039/d5sc01615k","DOIUrl":"https://doi.org/10.1039/d5sc01615k","url":null,"abstract":"Chiral organic-inorganic metal halides (OIMHs) have emerged as a new class of promising circularly polarized luminescence (CPL) materials owing to their structural tunability and fascinating optoelectronic properties. However, the development of high-performance chiral hybrid OIMHs remains a critical challenge, largely attributed to the absence of effective strategies for modulating chiroptical activity. Herein, we present enantiomeric hybrid manganese bromides, denoted as R/S-DACAMnBr3, featuring organic cations alternately coordinated one-dimensional chain structure via edge-sharing MnOBr5 octahedra, which establishes a robust chiral transfer pathway from organic cations to inorganic emissive centers. This structural design synergizes with the high intrinsic emission efficiency of Mn²⁺ centers to achieve intense orange CPL at 626 nm, yielding a highest luminescence dissymmetry factor (glum) of 0.292 for S-DACAMnBr3, which surpasses most reported chiral OIHMs by 1-3 orders of magnitude. Remarkably, positive magneto-chiroptical effect under a 1.6 T magnetic field amplifies the glum value to 0.321 at room temperature, demonstrating the first example of magnetic-field-enhanced CPL in lead-free OIMHs. The practical viability is further evidenced by S-DACAMnBr3-based circularly polarized light-emitting diodes exhibiting a strong CPL signal at 620 nm with a glum of 6.4 × 10-3, alongside single-crystal photodetectors achieving a switching ratio of 7.72. These findings contribute valuable insights for amplifying chiroptical activity of hybrid OIMHs via a strategy of chiral cation coordination, which may pave the way for the development of effective CPL materials toward diverse applications in the future.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"122 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946078","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

Inter-Cluster-Linker-Absence-Enabled Sub-Ångstrom Pore Modulation in Metal-Organic Framework for Multi-Scenario CO2 Capture 簇间连接缺失使能的亚-Ångstrom多孔调制在金属-有机框架中用于多场景二氧化碳捕获

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d5sc02144h

Jia-Wen Wang, Shucong Fan, Wenyu Yuan, Ying Wang, Quan-Guo Zhai

{"title":"Inter-Cluster-Linker-Absence-Enabled Sub-Ångstrom Pore Modulation in Metal-Organic Framework for Multi-Scenario CO2 Capture","authors":"Jia-Wen Wang, Shucong Fan, Wenyu Yuan, Ying Wang, Quan-Guo Zhai","doi":"10.1039/d5sc02144h","DOIUrl":"https://doi.org/10.1039/d5sc02144h","url":null,"abstract":"Ultrafine aperture control of carbon capture adsorbents is first and foremost important but inscrutable. Herein an inter-cluster-linker-absence-enabled sub-Ångstrom pore modulation strategy is proposed through the efficient transitivity of coordination bonds in metal-organic framework (MOF). The feasibility of this strategy is well-demonstrated in SNNU-98-M materials composed of directly-connected [M8(TAZ)9] (M = Cd or Cu, TAZ = tetrazolate) triangular prism clusters. The removal of inter-cluster linkers effectively transfers the difference of coordination bond length (~2.3 Å for Cd(II)-N and ~2.1 Å for Cu(II)-N) to the size of secondary building blocks (~6.5 × 6.5 × 6.7 Å3 for [Cd8(TAZ)9] and ~6.2 × 6.2 × 6.3 Å3 for [Cu8(TAZ)9]), and to the final MOF pore (~5.5 Å for SNNU-98-Cd and ~5.1 Å for SNNU-98-Cu). Rational and hyperfine pore control together with optimized Lewis basic N sites endow SNNU-98-M with benchmark multi-scenario CO2 capture performance varying from binary flue gas (CO2/N2) to ternary biogas (CO2/CH4/N2) and even to quinary coal gas (CO2/CH4/N2/CO/H2) mixtures by a one-step process. Low-cost raw materials, easy scalablity in synthesis, ultra-high stability, top-level selective adsorption ability as well as multi-scenario adaptability make SNNU-98-Cu ideal carbon capture material for practical applications.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"4 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946010","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

Copper-Catalyzed Asymmetric Carbonylative Hydroallylation of Vinylarenes 铜催化乙烯烯的不对称羰基化水解烯丙基化反应

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-14 DOI: 10.1039/d5sc02421h

Sufang Shao, Yuan Yang, Alban Schmoll, Xiao-Feng Wu

引用次数: 0

Enhancing the Nucleophilicity of Aluminyl Anions: Targeting Selective C–H Activation 增强铝基阴离子的亲核性：靶向选择性C-H活化

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-13 DOI: 10.1039/d5sc02682b

Fabian Kallmeier, Gareth Roland Nelmes, Claire Louise McMullin, Alison J. Edwards, Jamie Hicks

引用次数: 0

Fast Emission Color Switching of Circularly Polarized Luminescence in Platinum(II) Liquid Crystalline Co-Assembly 铂（II）液晶共组装中圆偏振发光的快速发射色开关

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-13 DOI: 10.1039/d5sc02285a

Guo Zou, Qihuan Li, Zhenhao Jiang, Wentong Gao, Yixiang Cheng

{"title":"Fast Emission Color Switching of Circularly Polarized Luminescence in Platinum(II) Liquid Crystalline Co-Assembly","authors":"Guo Zou, Qihuan Li, Zhenhao Jiang, Wentong Gao, Yixiang Cheng","doi":"10.1039/d5sc02285a","DOIUrl":"https://doi.org/10.1039/d5sc02285a","url":null,"abstract":"Developing stimuli-responsive circularly polarized luminescence (CPL) materials that feature fast emission color switching for advanced information encryption presents a scientifically significant yet formidable challenge. Herein, we construct a supramolecular co-assembly system demonstrating transiently responsive CPL emission color switching, enabling mechanically-modulated information encryption. Combining a highly luminescent Pt(II) liquid crystal (Pt8) with the anchored binaphthyl inducers (R/S-M) form chiral co-assemblies (R/S-M)0.03-(Pt8)0.97, which assembles into twisted nanobelts (180 ºC) and helical nanofibers (260 ºC) exhibiting green (λem = 545 nm, gem = 0.038) and red CPL (λem = 640 nm, gem = 0.133), respectively. Notably, mechanical grinding transforms the 180 ºC-annealed (R/S-M)0.03-(Pt8)0.97 into nanoparticles, resulting in a fast dynamic switching of CPL emission color from green to orange-red (λem: 545 → 625 nm, gem: 0.038 → 0.058). Reheating the grinding films (R/S-M)0.03-(Pt8)0.97 to 180 ºC restores the initial green CPL of the nanobelts. Based on the fast CPL emission color switching, we demonstrate the applications of these supramolecular chiral co-assemblies for mechanically-modulated information encryption.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"112 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143939750","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

Emerging Techniques and Scenarios of Scanning Electrochemical Microscopy for the Characterization of Electrocatalytic Reactions 扫描电化学显微镜表征电催化反应的新技术和场景

IF 8.4 1区化学

Chemical Science Pub Date : 2025-05-13 DOI: 10.1039/d5sc01854d

Jinming Xu, Ran Chen, Juanxian Song, Songqin Liu, Yanfei Shen, Yuanjian Zhang

{"title":"Emerging Techniques and Scenarios of Scanning Electrochemical Microscopy for the Characterization of Electrocatalytic Reactions","authors":"Jinming Xu, Ran Chen, Juanxian Song, Songqin Liu, Yanfei Shen, Yuanjian Zhang","doi":"10.1039/d5sc01854d","DOIUrl":"https://doi.org/10.1039/d5sc01854d","url":null,"abstract":"To fulfill the evergrowing energy consumption demands and the pursuit of sustainable and renewable energy, electrocatalytic reactions such as water electrocatalysis, O2 reduction, N2 reduction (NRR), CO2 reduction (CO2RR), etc., have drawn a lot of attention. Scanning electrochemical microscopy (SECM) is a powerful technique for in-situ surface characterization, providing critical information about the local reactivity of electrocatalysts and unveiling key information about the reaction mechanisms, which are essential for the rational design of novel electrocatalysts. There has been a growing trend of SECM-based study in electrocatalytic reactions, with a major focus on water splitting and O2 reduction reactions, and relying mostly on conventional SECM techniques. Recently, novel operation modes of SECM have emerged, adding new features to the functionality of SECM and successfully expanding the scope of SECM to other electrocatalytic reactions, i.e., NRR, NO3- reduction (NO3RR), CO2RR and so on, as well as more complicated electrolysis systems, i.e. gas diffusion electrodes. In this perspective, we summarized recent progresses in the development of novel SECM techniques and recent SECM-based researches in NRR, NO3RR, CO2RR, and so on, where quantitative information on the reaction mechanism and catalyst reactivity were uncovered through SECM. The development of novel SECM techniques and the application of these techniques can provide new insights into the reaction mechanisms of diverse electrocatalytic reactions as well as the in-situ characterization of electrocatalysts, facilitating the pursuit of sustainable and renewable energy.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"5 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143939746","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