Angewandte Chemie最新文献_第10页

Branched Alkyl Chains Tunable Organic-Inorganic Hybrid Manganese Halides for Anti-counterfeiting, White Light-emitting Diode and X-ray Imaging Applications 支链烷基链可调有机-无机杂化卤化锰防伪，白光发光二极管和x射线成像应用

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202508536

Jing-Hua Chen, Jian-Bin Luo, Qing-Peng Peng, Zi-Lin He, Jun-Hua Wei, Prof. Dai-Bin Kuang

{"title":"Branched Alkyl Chains Tunable Organic-Inorganic Hybrid Manganese Halides for Anti-counterfeiting, White Light-emitting Diode and X-ray Imaging Applications","authors":"Jing-Hua Chen, Jian-Bin Luo, Qing-Peng Peng, Zi-Lin He, Jun-Hua Wei, Prof. Dai-Bin Kuang","doi":"10.1002/ange.202508536","DOIUrl":"https://doi.org/10.1002/ange.202508536","url":null,"abstract":"Manganese-based organic–inorganic metal halides (Mn-based OIMHs) scintillators have aroused a research upsurge due to their outstanding photoluminescence performance, low toxicity, and tunable structures. Herein, we demonstrate a molecular engineering strategy that synergistically enhances luminescence efficiency and radiation sensitivity by systematic elongation of branched alkyl chains in phosphonium-based cations. The (4-DEATBP)MnBr4 (4-DEATBP = (4-(diethylamino)butyl)triphenylphosphonium) crystal exhibits remarkable thermochromic luminescence properties and anti-thermal quenching effect, highlighting the application potential in high-temperature anti-counterfeiting and information encryption. Through effective chain elongation, the (4-DBATBP)MnBr4 (4-DBATBP = (4-(dibutylamino)butyl)triphenylphosphonium) single crystal achieves an impressive photoluminescence quantum yield (PLQY) of 100% and exhibits superior performance under X-ray irradiation, with a high light yield of 67953 photons MeV−1 and a low limit of detection (LOD) of 10.45 nGy s−1. Additionally, the glassy (4-DBATBP)MnBr4 demonstrates an impressive spatial resolution of 25 lp mm−1. (4-DBATBP)MnBr4 shows great application potential in the fields of white light-emitting diode (WLED) and express security check due to its outstanding luminescence performance. This work not only offers two kinds of new Mn-based OIMH materials but also authenticates the role of extending the branched alkyl chain for improving the photoluminescence performance.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624460","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-Entropy Modulated High-Spin Localized Cobalt Sites Enhance Catalytic Ozonation for Efficient Odor Control 高熵调制的高自旋定位钴位点增强催化臭氧化有效控制气味

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202507109

Rumeng Zhang, Hao Zhou, Tao Shao, Qiyu Lian, Mengliang Hu, Ji Mei, Shulin Zuo, Jiahao Huang, Zhuoyun Tang, Dehua Xia

{"title":"High-Entropy Modulated High-Spin Localized Cobalt Sites Enhance Catalytic Ozonation for Efficient Odor Control","authors":"Rumeng Zhang, Hao Zhou, Tao Shao, Qiyu Lian, Mengliang Hu, Ji Mei, Shulin Zuo, Jiahao Huang, Zhuoyun Tang, Dehua Xia","doi":"10.1002/ange.202507109","DOIUrl":"https://doi.org/10.1002/ange.202507109","url":null,"abstract":"Catalytic ozonation technology is crucial for environmental remediation due to its exceptional efficiency and capability for complete mineralization of organic pollutants. However, hindered by spin-forbidden transitions, effective catalytic ozonation remains contingent upon the electronic properties and interfacial interactions of the catalyst. Recent studies identify interfacial atomic metal-oxygen species (*O) as a key descriptor in catalytic ozonation, determining the derivation of reactive species and subsEquationuent reactivity. Herein, we modulated the high-spin localized Co active sites in HE-Co3O4 via a high-entropy strategy, which selectively stabilizes *O surface species, thereby enhancing catalytic ozonation efficiency. HE-Co3O4 exhibits a five-fold higher degradation rate than Co3O4 for 50 ppm CH3SH elimination (63-fold the mass activity compared to commercial MnO2) while maintaining exceptional stability over 24 h at 298 K. Electron paramagnetic resonance (EPR) and magnetization hysteresis (M-H) measurements confirm the transition of Co3+ to high-spin states in HE-Co3O4. Density functional theory (DFT) calculations reveal that unpaired electrons enhance the hybridization of Co 3d with O 2p orbitals, thereby establishing a *O-mediated interfacial pathway. This mechanism is directly observed through in situ Raman spectroscopy. These findings provide insights into the targeted modulation of catalyst electronic structures for ozone-catalyzed environmental remediation.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624462","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Outside Back Cover: Photoredox Autocatalysis: Towards a Library of Generally Applicable Reductive Photocatalysts (Angew. Chem. 22/2025) 外封底：光氧化还原自催化：走向一个普遍适用的还原性光催化剂库（新）。化学22/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202509841

Jaspreet Kaur, Mark John P. Mandigma, Nakul Abhay Bapat, Joshua P. Barham

引用次数: 0

A Dynamic Self-Healing Protective Layer Enabling Stable Zinc Ion Batteries through Strong Zn-S Affinity and Intramolecular Hydrogen Bonding 一种动态自愈保护层，通过强Zn-S亲和力和分子内氢键使锌离子电池稳定

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202503345

Bao Li, Bo Zhang, Xiang Bai, Jiahui Zhang, Xinyue Chang, Lifeng Hou, Hao Huang, Tiantian Lu, Shi Wang, Zhong Jin, Qian Wang

{"title":"A Dynamic Self-Healing Protective Layer Enabling Stable Zinc Ion Batteries through Strong Zn-S Affinity and Intramolecular Hydrogen Bonding","authors":"Bao Li, Bo Zhang, Xiang Bai, Jiahui Zhang, Xinyue Chang, Lifeng Hou, Hao Huang, Tiantian Lu, Shi Wang, Zhong Jin, Qian Wang","doi":"10.1002/ange.202503345","DOIUrl":"https://doi.org/10.1002/ange.202503345","url":null,"abstract":"Aqueous Zn-ion batteries (AZIBs) are promising for large-scale energy storage, yet Zn metal anodes face issues like hydrogen evolution, dendrite growth, and corrosion. Herein, we develop a self-healable, adhesive polymer layer for AZIBs by polymerizing thioctic acid (TA) on Zn surfaces. Thanks to the strong and spontaneous affinity between Zn metal surface and S atoms on polymer chains, this protective layer can firmly and dynamically adhere to the Zn surface. Thus, even at a thickness of <1 µm, the protective layer exhibits a strong adhesion force of up to 10.5 N with Zn surface, while the abundant carboxyl groups in the protective layer can form intramolecular hydrogen bonds, endowing its high self-healing property and enhancing its strength (Young's modulus reaches 15.1 GPa). Such a protective layer effectively inhibits the dendrite growth physically and regulates the Zn2+ migration and deposition behavior chemically. Therefore, the symmetric cells can be cycled for more than 1000 h at the current densities of 1.0 and 5.0 mA cm−2, respectively. Full cells with NH4V4O10 also run stably for 1000 cycles with a high capacity retention. This work offers a promising strategy for designing multifunctional polymer coating towards high-stability and long-cycling AZIBs.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

2D/2D MOF/MXene Schottky Junction: Prolonged Carrier Lifetime and Enhanced Hydrogen Evolution Efficiency 2D/2D MOF/MXene Schottky结：延长载流子寿命和提高析氢效率

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202503860

María Cabrero-Antonino, Andrés Uscategui-Linares, Rubén Ramírez-Grau, Pablo García-Aznar, Prof. German Sastre, Dr. Jianjun Zhang, Dr. Sara Goberna-Ferrón, Dr. Josep Albero, Prof. Jiaguo Yu, Prof. Hermenegildo García, Dr. Feiyan Xu, Prof. Ana Primo

{"title":"2D/2D MOF/MXene Schottky Junction: Prolonged Carrier Lifetime and Enhanced Hydrogen Evolution Efficiency","authors":"María Cabrero-Antonino, Andrés Uscategui-Linares, Rubén Ramírez-Grau, Pablo García-Aznar, Prof. German Sastre, Dr. Jianjun Zhang, Dr. Sara Goberna-Ferrón, Dr. Josep Albero, Prof. Jiaguo Yu, Prof. Hermenegildo García, Dr. Feiyan Xu, Prof. Ana Primo","doi":"10.1002/ange.202503860","DOIUrl":"https://doi.org/10.1002/ange.202503860","url":null,"abstract":"Harnessing sunlight for photocatalytic overall water splitting offers a sustainable approach to renewable hydrogen (H2) production, addressing global energy and environmental challenges. However, the development of efficient and durable photocatalysts remains a significant obstacle. This study introduces the design and performance of a 2D/2D Schottky heterojunction composed of Cu2[CuTCPP] MOF of nanometric size and exfoliated Ti3C2 MXene for visible-light-driven overall water splitting. By leveraging the extensive interfacial contact between the two components, an interfacial electric field is generated, promoting efficient charge migration and prolonging carrier lifetimes, as confirmed through systematic density functional theory simulations, in situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and X-ray absorption spectroscopy. Ti3C2 MXene, acting as a cocatalyst for photohole transport and accumulation, reduces oxidative degradation and slows catalyst deactivation. The synergistically enhanced light absorption properties of the Cu2[CuTCPP]/Ti3C2 heterojunction result in an impressive H2 evolution rate exceeding 5000 µmol gcat⁻1, underscoring its potential for next-generation photocatalytic systems in renewable energy applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202503860","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624463","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

π–π Stacking as Electron-Transfer Channels in Hydrogen-Bonded Organic Frameworks for Boosting Photocatalysis 氢键有机骨架中π -π堆叠作为电子传递通道促进光催化

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202507332

Jian-Hua Mei, Ya-Ru Zeng, Dr. Yun-Nan Gong, Dr. Wen-Jie Shi, Prof. Dr. Di-Chang Zhong, Prof.Dr. Tong-Bu Lu

{"title":"π–π Stacking as Electron-Transfer Channels in Hydrogen-Bonded Organic Frameworks for Boosting Photocatalysis","authors":"Jian-Hua Mei, Ya-Ru Zeng, Dr. Yun-Nan Gong, Dr. Wen-Jie Shi, Prof. Dr. Di-Chang Zhong, Prof.Dr. Tong-Bu Lu","doi":"10.1002/ange.202507332","DOIUrl":"https://doi.org/10.1002/ange.202507332","url":null,"abstract":"Photocatalysis provides a promising approach to produce green energy, by which the intermittent solar energy can be converted into storable chemical energy. It is well-known that the electron-transfer rate has great influence on the photocatalytic efficiency. Revealing the influence of electron-transfer rate on the photocatalytic efficiency from a molecular level is of great significance but a challenge. Herein, we give solid evidence to show that the π–π stacking can serve as an electron-transfer channel to boost photocatalysis. Specifically, two hydrogen-bonded organic frameworks (HOFs) with similar structures but slightly different intermolecular interactions have been weaved. Interestingly, the HOF with π–π stacking interactions shows much higher photocatalytic activity for hydrogen evolution than the one without. Further structural and spectroscopic analyses revealed that the much-enhanced photocatalytic activity of the former can be attributed to the π–π stacking, which can really serve as an electron-transfer channel, thus accelerating the electron transfer and achieving a remarkably enhanced activity in photocatalytic hydrogen evolution. The work, from a molecular level, reveals the role of π–π stacking in photocatalysis and gives new insights into the electron-transfer in photocatalysts.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624439","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Achieving Uniform Phase Structure for Layer-by-Layer Processed Binary Organic Solar Cells with 20.2% Efficiency 以20.2%的效率实现逐层加工二元有机太阳能电池的均匀相结构

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202508257

Hao Wang, Busheng Zhang, Liming Wang, Xia Guo, Le Mei, Bo Cheng, Wei Sun, Lixuan Kan, Xinxin Xia, Xiaotao Hao, Thomas Geue, Feng Liu, Maojie Zhang, Xian-Kai Chen

{"title":"Achieving Uniform Phase Structure for Layer-by-Layer Processed Binary Organic Solar Cells with 20.2% Efficiency","authors":"Hao Wang, Busheng Zhang, Liming Wang, Xia Guo, Le Mei, Bo Cheng, Wei Sun, Lixuan Kan, Xinxin Xia, Xiaotao Hao, Thomas Geue, Feng Liu, Maojie Zhang, Xian-Kai Chen","doi":"10.1002/ange.202508257","DOIUrl":"https://doi.org/10.1002/ange.202508257","url":null,"abstract":"Layer-by-layer (LBL) deposition has become a facile and promising method to fabricate highly efficient organic solar cells (OSCs). However, characterization and optimization of 3D morphology remain a grand challenge for LBL-processed active layers, and their correlation with photovoltaic properties of OSC devices is not clear to date. Here, to address this issue, the morphology and its formation mechanisms of LBL-processed active layer based on the classical D18/L8-BO blend were investigated systematically. Intriguingly, a unique 3D nanomorphology is achieved and uncovered within the LBL processed active layer, which highlights a highly uniform and “zigzag”-shaped phase structure formed by the intersection of donor and acceptor aggregates along horizontal direction in the middle-depth layer, rarely found in bulk heterojunction (BHJ) films processed by blend casting. Our results revealed that solid additive DBM with a twisted conformation plays a crucial role in achieving the uniform phase structure of LBL-deposited active layer. Consequently, the characteristic 3D morphology of LBL-processed device significantly improves short-circuit current and fill factor, enabling an impressive PCE of 20.2% in such binary device. Therefore, this work unambiguously demonstrates a unique 3D nanomorphology within LBL active layer, unveils the morphology manipulation mechanism, and their correlation with optoelectronic properties of OSCs.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624440","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Outside Front Cover: Direct Observation of Cyclo-Pentazolate Anion Decomposition in a Tailored Molecular Trap (Angew. Chem. 22/2025) 外封面：直接观察环戊唑酸阴离子在定制分子阱中的分解（新）。化学22/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202510027

Jinjin Zhang, Mingjie Tang, Siyuan Yang, Hongqing Li, Guangbin Cheng, Yongxing Tang, Ming Liu

引用次数: 0

Inside Front Cover: Indole-Quinoline Transmutation Enabled by Formal Rhodium-Carbynoid (Angew. Chem. 25/2025) 内封面：吲哚-喹啉转化的形式铑-羰基(新。化学25/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202510007

Lu-Jie Liu, Meng-Yang Tian, Zhi-Yu Lang, Yong-Li Wang, Chun-Yang He, Yong-Zheng Chen, Wen-Yong Han

引用次数: 0

Inside Back Cover: Rare Earth Single-Atomic Hybrid Glasses for Near-Infrared II Optical Waveguides (Angew. Chem. 27/2025) 内封底：稀土单原子杂化玻璃用于近红外II光波导。化学27/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202510009

Meiqi Dai, Bo Zhou, Dongpeng Yan

引用次数: 0