Angewandte Chemie (International ed. in English)最新文献

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Atomic-Level Design of Acid-Base Pairs in Oxides for Selective Catalytic Reduction of Nitrogen Oxides with Ammonia. 氨选择性催化还原氮氧化物中酸碱对的原子水平设计。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202509362
Guoquan Liu, He Zhang, Pengfei Wang, Chao Gao, Zechao Zhuang, Dingsheng Wang, Sihui Zhan
{"title":"Atomic-Level Design of Acid-Base Pairs in Oxides for Selective Catalytic Reduction of Nitrogen Oxides with Ammonia.","authors":"Guoquan Liu, He Zhang, Pengfei Wang, Chao Gao, Zechao Zhuang, Dingsheng Wang, Sihui Zhan","doi":"10.1002/anie.202509362","DOIUrl":"10.1002/anie.202509362","url":null,"abstract":"<p><p>Selective catalytic reduction of nitrogen oxides (NO<sub>x</sub>) with NH<sub>3</sub> (NH<sub>3</sub>-SCR) poses considerable potential in the abatement of NO<sub>x</sub> emissions. However, the efficient adsorption and speedy reaction of reactants following the specific mechanism in a favorable way is still a challenge for enhancing catalysis. Herein, we propose the strategy aimed at adjusting electronic properties of Ce-O<sub>v</sub>-W acid-base pairs through constructing oxygen vacancies on Ce/WO<sub>x</sub>, thereby fostering SCR activity. Experimental and theoretical results reveal that Ce-O<sub>v</sub>-W acid-base pairs not only provide more Ce<sup>3+</sup> sites for promoting the reactivity of adsorbed NO, but also accelerate the reaction between NH<sub>3</sub> and gaseous NO owing to the generation of W<sup>5+</sup> species with superior surface acidity, which enhance Langmuir-Hinshelwood and Eley-Rideal mechanisms, respectively. Consequently, the designed catalysts achieve over 90% NO<sub>x</sub> conversion above 250 °C and exhibit higher activity than normal Ce/WO<sub>3</sub> and V/W-TiO<sub>2</sub> commercial catalysts, with anti-poisoning of SO<sub>2</sub> and H<sub>2</sub>O under harsh working conditions, expecting to provide the guidance for promoting de-NO<sub>x</sub> industrial application.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202509362"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586133","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
Metastable Macrocyclic Bis-Meisenheimer Adduct. 亚稳态大环双-迈森海默加合物。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202511037
Simon Pascal, Angélina Torres Ruiz, Aerin E Baker, Douglas A Vander Griend, Michel Giorgi, Aurélien Planchat, Denis Jacquemin, Olivier Siri
{"title":"Metastable Macrocyclic Bis-Meisenheimer Adduct.","authors":"Simon Pascal, Angélina Torres Ruiz, Aerin E Baker, Douglas A Vander Griend, Michel Giorgi, Aurélien Planchat, Denis Jacquemin, Olivier Siri","doi":"10.1002/anie.202511037","DOIUrl":"10.1002/anie.202511037","url":null,"abstract":"<p><p>An electron-deficient tetranitroazacalixarene is shown to undergo reversible cyanide capture via nucleophilic aromatic substitution, yielding an unprecedented class of metastable dianionic macrocycle incorporating two Meisenheimer units, fully characterized by single-crystal X-ray diffraction, NMR, and electronic absorption spectroscopies. Acting as a chemical fuel, cyanide transiently drives the formation of this adduct, which can spontaneously regenerate the parent macrocycle under mild conditions, representing a rare demonstration of metastability in a Meisenheimer complex. The dynamic behavior of this system, reminiscent of out-of-equilibrium assemblies, is finely tunable through macrocycle concentration, counterion nature, solvent, and temperature. Detailed crystallographic, spectroscopic, and computational analyses reveal that intramolecular hydrogen bonding plays a key role in stabilizing the adduct. Comparative studies with simpler analogues further highlight the importance of macrocyclic preorganization and non-covalent interactions in governing this reversible reactivity.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202511037"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586148","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
Molecular Engineering of Plant Polyphenols Into Amorphous Room-Temperature Phosphorescent Materials. 植物多酚制备非晶室温磷光材料的分子工程研究。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202511218
Guobin Yang, Yajing Zhang, Chuang Lei, Yunxiang He, Yizhen Wang, Huijing Li, Yanchao Wu, Junling Guo
{"title":"Molecular Engineering of Plant Polyphenols Into Amorphous Room-Temperature Phosphorescent Materials.","authors":"Guobin Yang, Yajing Zhang, Chuang Lei, Yunxiang He, Yizhen Wang, Huijing Li, Yanchao Wu, Junling Guo","doi":"10.1002/anie.202511218","DOIUrl":"10.1002/anie.202511218","url":null,"abstract":"<p><p>Room-temperature phosphorescent (RTP) materials have potential applications in optoelectronics and bioimaging but encounter significant challenges. Traditional heavy-metal-based and crystalline systems are often toxic and environmentally sensitive, while strategies involving host-guest doping and encapsulation frequently suffer from phase separation and limited controllability-ultimately resulting in poor repeatability and restricted applications. Here, we developed a novel polyphenol-mediated molecular splicing and ring-locking strategy to incorporate benzo[c][1,2,5]thiadiazole (BZT) into polyphenol molecules, yielding a range of eco-friendly and processable amorphous single-component systems with a lifetime of up to 124 ms. Experimental and calculational analyses confirm that phosphorescence arises from synergistic interactions between polyphenol and BZT. Furthermore, phosphorescent nanoparticles (NPs) were synthesized via nanoprecipitation in tetrahydrofuran with 30% water content. These well-dispersed, metal-free NPs demonstrate excellent biocompatibility and low cytotoxicity, facilitating time-resolved luminescence imaging with minimal background fluorescence interference both in vitro and in vivo. This research establishes a versatile and sustainable design strategy for developing high-performance amorphous RTP materials using plant polyphenols, offering promising prospects for advanced biomedical applications.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202511218"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586149","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
SmI2-Catalyzed Coupling of Alkyl Housane Ketones and Alkenes in an Approach to Norbornanes. sm2催化的烷基侯烷酮与烯烃偶联制备降硼烷。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202512018
Debayan Roy, Jack I Mansell, Giorgia Barison, Song Yu, Rocco Katavic, Ciro Romano, Nikolas Kaltsoyannis, David John Procter
{"title":"SmI2-Catalyzed Coupling of Alkyl Housane Ketones and Alkenes in an Approach to Norbornanes.","authors":"Debayan Roy, Jack I Mansell, Giorgia Barison, Song Yu, Rocco Katavic, Ciro Romano, Nikolas Kaltsoyannis, David John Procter","doi":"10.1002/anie.202512018","DOIUrl":"10.1002/anie.202512018","url":null,"abstract":"<p><p>Cross-coupling strategies involving strain-release have gained significant recent attention for the construction of complex molecular frameworks, particularly in the context of preparing bioisosteres for medicinal chemistry. While the reactivity of cyclopropanes and bicyclo[1.1.0]butanes (BCBs) has been extensively studied, higher homologues are emerging as valuable substrates for synthesis. For example, methods for the fragmentation and coupling of bicyclo[2.1.0]pentane, or housane, ketones show promise, but are currently limited in substrate scope. Here, we describe a mild, atom-economical, samarium diiodide (SmI2) catalyzed fragmentation and coupling of alkyl and aryl housane ketones with alkenes that grants access to functionalized norbornane structural motifs, not easily accessible by classical cycloaddition approaches, and with considerable potential for further manipulation.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202512018"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586157","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
Sub-Ångstrom Pore Engineering in Carbon Molecular Sieves Realizes Diffusion-Gated Kinetic Sieving of Alkenes from Alkanes. 碳分子筛的亚-Ångstrom孔工程实现了从烷烃中分离烯烃的扩散门控动力学筛分。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202513448
Fuqiang Chen, Hua Shang, Guangtong Hai, Xinlei Huang, Zhe Chu, Haoran Sun, Liu Yang, Qiwei Yang, Zhiguo Zhang, Qilong Ren, Zongbi Bao
{"title":"Sub-Ångstrom Pore Engineering in Carbon Molecular Sieves Realizes Diffusion-Gated Kinetic Sieving of Alkenes from Alkanes.","authors":"Fuqiang Chen, Hua Shang, Guangtong Hai, Xinlei Huang, Zhe Chu, Haoran Sun, Liu Yang, Qiwei Yang, Zhiguo Zhang, Qilong Ren, Zongbi Bao","doi":"10.1002/anie.202513448","DOIUrl":"10.1002/anie.202513448","url":null,"abstract":"<p><p>Sub-ångstrom pore engineering offers a new paradigm for molecular separations. Here, we report sucrose-derived carbon molecular sieves with precisely tailored sub-ångstrom slit pores that enable diffusion-gated kinetic sieving for the challenging separation of alkenes from alkanes. The optimized materials, C-Suc-650 and C-Suc-750, set new industry-leading standards for the kinetic separation of C3H6/C3H8 and C2H4/C2H6, respectively. Through a combination of breakthrough experiments, pressure swing adsorption (PSA) simulations, and molecular dynamics modeling, we demonstrate that these sieves consistently achieve >99.9% alkene purity, with outstanding selectivity, rapid uptake kinetics, and remarkably low energy consumption. Mechanistic studies reveal that slit pore architecture uniquely enhances alkene diffusion while hindering alkane movement, establishing a clear design principle for next-generation, energy-efficient gas separations. These results provide a blueprint for exploiting diffusion-gated kinetic sieving at the sub-ångstrom scale to address longstanding challenges in industrial gas purification.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202513448"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586160","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
Synthesis and Reactivity of a Mono-Coordinated Triplet Bismuthinidene. 单配位三态铋的合成及其反应性。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202508250
Yannick Schulte, Timo Freese, Christoph Wölper, Jan Schulte, Gebhard Haberhauer, Stephan Schulz
{"title":"Synthesis and Reactivity of a Mono-Coordinated Triplet Bismuthinidene.","authors":"Yannick Schulte, Timo Freese, Christoph Wölper, Jan Schulte, Gebhard Haberhauer, Stephan Schulz","doi":"10.1002/anie.202508250","DOIUrl":"10.1002/anie.202508250","url":null,"abstract":"<p><p>The triplet bismuthinidene Ar*Bi (4) stabilized by a very bulky septiphenyl ligand (Ar* = 3,5-i-Pr<sub>2</sub>-2,6-(2,6-Me<sub>2</sub>-3,5-(2,6-i-Pr<sub>2</sub>C<sub>6</sub>H<sub>3</sub>)<sub>2</sub>-C<sub>6</sub>H)-C<sub>6</sub>H) was synthesized by dehydrogenation of in situ formed bismuth dihydride Ar*BiH<sub>2</sub> (3). Oxidative addition reactions of 4 with alkyl halides (MeI, EtBr, i-PrBr) yielded bismuthanes Ar*Bi(Me)I (5), Ar*Bi(Et)Br (6), and Ar*Bi(i-Pr)Br (7), which reacted with LiAlH<sub>4</sub> and LiAlD<sub>4</sub> to the thermally robust bismuth monohydrides Ar*Bi(R)H (R = Me 8, Et 10, i-Pr 12) and monodeuterides Ar*Bi(R)D (R = Me 9, Et 11, i-Pr 13). Ar*Bi(NMe<sub>2</sub>)<sub>2</sub> 1 and Ar*BiH<sub>2</sub> 3 were characterized in situ by <sup>1</sup>H NMR spectroscopy and sc-XRD (1), whereas the other compounds were characterized by heteronuclear NMR (<sup>1</sup>H/<sup>2</sup>H (D), <sup>13</sup>C) and IR spectroscopy, elemental analysis (Ar*-2, Ar*-3, Ar*-5, Ar*-7, Ar*I, Ar*H, 2, 4-7), as well as by UV-vis (4) and sc-XRD (Ar*-7, Ar*I, Ar*Li·Lit-Bu, Ar*H, 1, 2, 4, 12). Quantum chemical calculations revealed the triplet character of the bismuthinidine 4.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202508250"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586161","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
Bipyridine-Thiosumanene Isomeric Lewis Bases for Synergistic Defect Passivation and Hole Extraction Enables over 26% Efficient Perovskite Solar Cells. 协同缺陷钝化和空穴提取的联吡啶-硫苏烯异构路易斯碱使钙钛矿太阳能电池的效率超过26%。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202510255
Zhongquan Wan, Yuanxi Wang, Yao Ma, Muhammad Azam, Boxue Zhang, Xiangfeng Shao, Runmin Wei, Haomiao Yin, Huaibiao Zeng, Junsheng Luo, Chunyang Jia
{"title":"Bipyridine-Thiosumanene Isomeric Lewis Bases for Synergistic Defect Passivation and Hole Extraction Enables over 26% Efficient Perovskite Solar Cells.","authors":"Zhongquan Wan, Yuanxi Wang, Yao Ma, Muhammad Azam, Boxue Zhang, Xiangfeng Shao, Runmin Wei, Haomiao Yin, Huaibiao Zeng, Junsheng Luo, Chunyang Jia","doi":"10.1002/anie.202510255","DOIUrl":"10.1002/anie.202510255","url":null,"abstract":"<p><p>Interface defects between the perovskite layer and the hole transport layer (HTL) seriously limit the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs). Herein, we designed two isomers, 4BT and 5BT, based on 2,2'-bipyridine-thiosumanene-functionalized polycyclic aromatic hydrocarbons as novel Lewis bases with dual capabilities for deep-level defects (Pb2+, VI) passivation and promoting hole extraction. By shifting the pyridine bridging unit from the tetra to the penta positions, these molecules undergo a configurational transformation from an orthogonal (4BT) to a planar structure (5BT). The configuration-functionality relationship was comprehensively investigated through theorical and experimental analyses. The planar configuration of 5BT enables more Lewis base sites to interact with perovskite, exhibiting more pronounced deep-level defect passivation effect, while improving hole extraction capability. Consequently, the 5BT-modified n-i-p PSCs achieved a champion PCE of 26.15% (certified at 26.12%) and superior operational stability by retaining 94.0% of the initial PCE according to ISOS-L-2 protocol. This work offers a unique molecular designing mechanism to address the interfacial-related issues for high-performance PSCs.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202510255"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144593704","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
Advancing Solid-State Calcium Batteries: Achieving Fast Ionic Conductivity at Near Ambient Conditions in Calcium Hydridoborates. 推进固态钙电池:在氢化硼酸钙接近环境条件下实现快速离子导电性。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202510493
Jakob B Grinderslev, Lasse N Skov, Lasse R Kristensen, Torben R Jensen
{"title":"Advancing Solid-State Calcium Batteries: Achieving Fast Ionic Conductivity at Near Ambient Conditions in Calcium Hydridoborates.","authors":"Jakob B Grinderslev, Lasse N Skov, Lasse R Kristensen, Torben R Jensen","doi":"10.1002/anie.202510493","DOIUrl":"10.1002/anie.202510493","url":null,"abstract":"<p><p>All-solid-state batteries based on abundant elements, such as calcium, offer a promising route to safer, cheaper, and more sustainable energy storage. Here, we report a series of fast Ca<sup>2+</sup>-conducting compounds of methylamine calcium tetrahydridoborates, Ca(BH<sub>4</sub>)<sub>2</sub>·xCH<sub>3</sub>NH<sub>2</sub> (0 < x < 4.9) and related nanocomposites stabilized by inert MgO nanoparticles. Three new crystal structures are identified: a three-dimensional network of octahedrally coordinated Ca<sup>2+</sup> complexes for x = 1, a molecular structure of neutral complexes for x = 4, and a structure of cationic complexes for x = 6. The thermal stability generally decreases with increasing CH<sub>3</sub>NH<sub>2</sub> content, and samples with x > 2 slowly release CH<sub>3</sub>NH<sub>2</sub> in \"open\" atmosphere at room temperature, but are stabilized in \"closed\" environments, e.g. capillaries. The ionic conductivity increases with CH<sub>3</sub>NH<sub>2</sub> content and correlates with increased void space and structural flexibility, reaching σ(Ca<sup>2+</sup>) = 5.0·10<sup>-5</sup> S cm<sup>-1</sup> at 60 °C for x = 4. Moreover, the effect of nanocomposite formation provides mechanical stability and a doubling of the ionic conductivity for Ca(BH<sub>4</sub>)<sub>2</sub>·4CH<sub>3</sub>NH<sub>2 </sub>- MgO (50 wt%), reaching σ(Ca<sup>2+</sup>) = 1.3·10<sup>-4</sup> S cm<sup>-1</sup> at 60 °C. These findings demonstrate how local structure and nanoscale interfacial effects govern calcium transport, offering new design principles for functional calcium solid electrolytes.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202510493"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586131","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
Amplifying Circularly Polarized Luminescence with High Dissymmetry Factor over 10-2 Based on Robust Point Chirality Triptycene Derivatives. 基于鲁棒点手性的三甲烯衍生物放大高不对称系数大于10-2的圆偏振发光。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202511414
Yufeng Xie, Songkun Zeng, Wenbin Huang, Chenlong Wei, Zikai He
{"title":"Amplifying Circularly Polarized Luminescence with High Dissymmetry Factor over 10<sup>-2</sup> Based on Robust Point Chirality Triptycene Derivatives.","authors":"Yufeng Xie, Songkun Zeng, Wenbin Huang, Chenlong Wei, Zikai He","doi":"10.1002/anie.202511414","DOIUrl":"10.1002/anie.202511414","url":null,"abstract":"<p><p>Chiral organic luminescent materials are promising candidates as direct emitting layers (EMLs) in circularly polarized organic light-emitting diodes (CP-OLEDs). However, most conventional systems suffered poor thermal stability of chiral configurations and low luminescent dissymmetry factors. Herein, we reported a pair of triptycene-bridged enantiomers with a point chirality and a donor-acceptor architecture. Robust point chirality, originating from quaternary bridgehead-carbons, prevented the common racemization during thermal sublimation. Thanks to the reduced electric transition dipole moment (µ<sub>e</sub>) in donor-acceptor architecture, tuned parallel alignment between the further reduced µ<sub>e</sub> and magnetic transition dipole moment (µ<sub>m</sub>) in the exciplex emitter, and the utilized chiral exciplex host for energy transfer to phosphor, the corresponding dissymmetry factors of emitters were sequentially amplified from 3.3 × 10<sup>-4</sup> to 4.5 × 10<sup>-3</sup>, and to 8.1 × 10<sup>-3</sup>. Remarkably, the CP-OLED device simultaneously achieved outstanding electroluminescence performance with a high external quantum efficiency of 31.8% and a large dissymmetry factor of 2.2 × 10<sup>-2</sup>. This work provided a viable pathway for developing high-performance CP-OLED materials through synergistic structural, material, and device engineering.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202511414"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586132","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
Polycation Engineering in Polymeric Metal Halides Enables Tunable and Multicolor Emission from Single Transition-Metals. 聚合金属卤化物的多阳离子工程使单一过渡金属的可调多色发射成为可能。
Angewandte Chemie (International ed. in English) Pub Date : 2025-07-08 DOI: 10.1002/anie.202502210
Shun-Shun Li, Pengfei Cheng, Huaxin Liu, Juntao Li, Jianyong Liu, Junsheng Chen, Kaifeng Wu
{"title":"Polycation Engineering in Polymeric Metal Halides Enables Tunable and Multicolor Emission from Single Transition-Metals.","authors":"Shun-Shun Li, Pengfei Cheng, Huaxin Liu, Juntao Li, Jianyong Liu, Junsheng Chen, Kaifeng Wu","doi":"10.1002/anie.202502210","DOIUrl":"10.1002/anie.202502210","url":null,"abstract":"<p><p>Zero-dimensional metal halides have emerged as a versatile platform for the development of light-emitting materials, but achieving tunable or even multicolor emission from a material containing a single type of metal has proven highly challenging. Here, we leverage the \"structural tolerance\" of recently-developed polymeric metal halides to integrate two distinct coordination units of a single metal into a material, thereby achieving highly tunable optical properties in single-phase metal halides. By manipulating the steric hindrance of polycations, facilely adjustable green, red or bicolor emission can be realized in manganese bromides, which originates from controllable transformation from manganese-bromine tetrahedra into octahedra. This design principle is further extended to polymeric copper halides, wherein broad self-trapped exciton emissions derived from distinct copper-iodine polyhedrons allow the emission colors to be linearly tunable from blue to yellow, encompassing pure white light, by tailoring the composition, excitation wavelength, or temperature. This study opens avenues for facile and precise modulation of the optical properties of metal halides by exploiting the intrinsic coordinative diversity of metal elements.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202502210"},"PeriodicalIF":0.0,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144586153","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
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