Angewandte Chemie (International ed. in English)最新文献_第6页

Kinetic Control of Anisotropic Grain Growth in Ni-Rich Layered Cathodes. 富镍层状阴极各向异性晶粒生长的动力学控制。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202516715

Shuli Zheng, Lang Qiu, Mengke Zhang, Yiyang Zhao, Jiayang Li, Weibo Hua, Yao Xiao, Fang Wan, Zhenguo Wu, Xiaodong Guo

{"title":"Kinetic Control of Anisotropic Grain Growth in Ni-Rich Layered Cathodes.","authors":"Shuli Zheng, Lang Qiu, Mengke Zhang, Yiyang Zhao, Jiayang Li, Weibo Hua, Yao Xiao, Fang Wan, Zhenguo Wu, Xiaodong Guo","doi":"10.1002/anie.202516715","DOIUrl":"https://doi.org/10.1002/anie.202516715","url":null,"abstract":"The particle morphology governed by anisotropic grain growth of Ni-rich layered oxide cathodes plays a crucial role in electrochemical stability and can be tuned via element doping during the high-temperature lithiation process. However, the fundamental impact of dopants on the anisotropic grain growth kinetics remains unclear. Herein, this work systematically investigates how dopants with different valences (Mg2+, Al3+, Zr4+, Ta5+, and Mo6+) affect the anisotropic grain growth during the high-temperature lithiation process. The findings demonstrate that the grain growth rate along the [104] and [110] directions is initially faster, followed by a higher growth rate along the [003] direction. The coarsening exponents n for the grain growth (along the [003], [104], and [110] directions) with low-valence ions (Mg2+, Al3+) dopants are approximately equal to 2, indicating that the grain growth depends solely on short-range diffusion at the grain boundary. Interestingly, the n value along the [003] direction enlarges with an increase in valence. Notably, the higher valence of Mo6+ results in a significant elevation of the exponent n along the [003] direction to 4.5, indicating a strong pinning effect due to Mo6+ segregation at the grain boundary. This pinning impedes grain boundary migration, inhibits grain coarsening, and effectively enhances cycle stability.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202516715"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077169","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

Spillover Hydrogen Boosts Nitroarene Hydrogenation to Industrial Activity with Ppm-Level Platinum Single Atoms. 溢出氢促进硝基芳烃加氢工业活动与ppm级铂单原子。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202514332

Nai-Liang Wang, Tong-Hui Li, Xin Wang, Xiang-Lin Kong, Wen-Hao Xie, Lin Xu, Yu-Rong He, Peng-Fei Zhang, Zheng-Hong Luo

{"title":"Spillover Hydrogen Boosts Nitroarene Hydrogenation to Industrial Activity with Ppm-Level Platinum Single Atoms.","authors":"Nai-Liang Wang, Tong-Hui Li, Xin Wang, Xiang-Lin Kong, Wen-Hao Xie, Lin Xu, Yu-Rong He, Peng-Fei Zhang, Zheng-Hong Luo","doi":"10.1002/anie.202514332","DOIUrl":"https://doi.org/10.1002/anie.202514332","url":null,"abstract":"The application of noble single-atom catalysts (SACs) at trace loadings is constrained by a low space-time yield, presenting a formidable challenge in elevating the activity of SACs to be comparable to industrial catalysts in nitroarene hydrogenation. In this study, the spillover hydrogen from a carbon-coated nickel support (Ni@C) coupled with 300 ppm platinum results in a 25.7-fold enhancement in turnover frequency (TOF, 44.1 s-1), thereby achieving a space-time yield equivalent to 1 wt.% Pd/C industrial hydrogenation catalyst. Remarkably, the Pt1/Ni@C catalyst preserves excellent stability under rigorous conditions, including acidic, basic, and oxidative environments. Density functional theory (DFT) calculations reveal that spillover hydrogen effectively reduces the hydrogenation energy barrier, with the energy barrier height inversely correlated to the density of adsorbed spillover hydrogen on Pt single atom. Extrapolating the enhanced hydrogenation effect to other SACs and nitroarene substrates shows that spillover hydrogen can either promote or inhibit hydrogenation processes. The density of adsorbed spillover hydrogen serves as a predictive descriptor for discerning the direction of the synergistic effect in single-atom catalyzed hydrogenation. This study provides insightful guidance for the rational design of more efficient and industrially viable SACs exploiting hydrogen spillover.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202514332"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145076699","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

Fully Sensitized Upconversion Nanoparticles as Efficient Catalysts for NIR-Driven UV Photochemistry. 全敏化上转化纳米颗粒作为nir驱动的紫外光化学的高效催化剂。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202511247

Naomi Weitzel, Armaz Tsutskiridze, Julia Bramowski, Burkhard König, Thomas Hirsch

{"title":"Fully Sensitized Upconversion Nanoparticles as Efficient Catalysts for NIR-Driven UV Photochemistry.","authors":"Naomi Weitzel, Armaz Tsutskiridze, Julia Bramowski, Burkhard König, Thomas Hirsch","doi":"10.1002/anie.202511247","DOIUrl":"https://doi.org/10.1002/anie.202511247","url":null,"abstract":"Biological photosynthesis harnesses energy from multiple photons to drive complex chemical transformations. In contrast, chemical photocatalysis typically relies on single-photon excitation, limiting its applicability in high-energy-demanding reactions. Upconversion nanoparticles (UCNPs), which can convert multiple low-energy near-infrared (NIR) photons into a single higher-energy photon, offer a promising solution. We synthesized and systematically improved NaYbF4:Tm@NaYF4 nanoparticles, focusing on sensitizer concentration, dopant spacing, and shell thickness to enhance ultraviolet (UV) and blue emission. Compared to low doped NaYF4:Yb, Tm systems, our nanoparticles exhibited significantly improved brightness, with a 210-fold enhancement in UV emission at 345 nm. Using these UCNPs as heterogeneous photocatalysts, we achieved efficient [2 + 2] photocycloadditions and Paternò-Büchi reactions under 980 nm excitation, with turnover numbers (TON) exceeding 290,000 and turnover frequencies (TOF) up to 8.52 s-1. Additionally, the UCNP catalysts were readily recoverable. Our results provide a rational framework for tailoring UCNPs for energy-demanding photochemical reactions and establish their potential in synthetic and biomedical applications that require deep-tissue, low-phototoxicity excitation.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202511247"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077100","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

Probing and Enhancing DNA Ligase Specificity via Se-Atom-Mutagenesis of ATP for Accurate Gene Synthesis and Detection. 通过ATP的硒原子诱变来探测和增强DNA连接酶的特异性，用于精确的基因合成和检测。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202424948

Dejin Xu, Bei Hu, Xiaoling Ding, Tong Qin, Ting Li, Jiaxin Li, Danyan Luo, Lu Chen, Yunfan Xu, Jun Zhang, Han Kang, Yang Zhang, Zhen Huang

{"title":"Probing and Enhancing DNA Ligase Specificity via Se-Atom-Mutagenesis of ATP for Accurate Gene Synthesis and Detection.","authors":"Dejin Xu, Bei Hu, Xiaoling Ding, Tong Qin, Ting Li, Jiaxin Li, Danyan Luo, Lu Chen, Yunfan Xu, Jun Zhang, Han Kang, Yang Zhang, Zhen Huang","doi":"10.1002/anie.202424948","DOIUrl":"https://doi.org/10.1002/anie.202424948","url":null,"abstract":"Discriminating against base-pair mismatches by nucleic acid-related enzymes is essential for DNA replication, RNA replication, nucleic acid repair, transcription, and translation. However, the discrimination mechanisms at the atomic level remain poorly understood, limited by the availability of atom-probing methods. Herein, we developed a single-Se-atom strategy (using ATPαSe) to explore mismatch discrimination in the DNA ligase system. We found that the Se-atom (substituting O) in ATPαSe played a key role in the mismatch discrimination of DNA ligase, and ATPαSe significantly improved the ligation specificity, achieving up to 1000-fold enhancement and expanding the region of mismatch discrimination up to 8 nt. Sequencing ligation products of various substrates generally confirmed the specificity enhancement using ATPαSe. Our mechanistic studies indicated that the specificity increase was correlated with the kcat reduction in mismatch ligations and with the disruption of the key interactions, supported by the site-specific ligase mutations. Further, using ATPαSe, we achieved over 200-fold increase in gene assembly efficiency and accomplished mismatch suppression in the single-nucleotide-polymorphism (SNP) detection. In conclusion, our Se-atom-probing strategy enables the atomic-level studies on mismatch discrimination and offers a useful tool for accuracy enhancement, highlighting its broad potential for exploring molecular recognition and specificity.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202424948"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145076740","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

Unraveling the Role of Triplet-Triplet Annihilation and Photodegradation in Difluoroboron-Based Organic Laser Gain Materials. 揭示三重态湮灭和光降解在二氟硼基有机激光增益材料中的作用。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202509535

Suman Kuila, Hector Miranda-Salinas, Chunyong Li, Natalie E Pridmore, Martin R Bryce, Christel M Marian, Andrew P Monkman

{"title":"Unraveling the Role of Triplet-Triplet Annihilation and Photodegradation in Difluoroboron-Based Organic Laser Gain Materials.","authors":"Suman Kuila, Hector Miranda-Salinas, Chunyong Li, Natalie E Pridmore, Martin R Bryce, Christel M Marian, Andrew P Monkman","doi":"10.1002/anie.202509535","DOIUrl":"https://doi.org/10.1002/anie.202509535","url":null,"abstract":"In this study, we investigate the triplet exciton dynamics of a series of difluoroboron-based organic gain molecules. We synthesized three previously reported molecules from the difluoroboron family and examined their photophysical properties using time-resolved emission spectroscopy and high-level theoretical calculations. Our results reveal that emission from these materials arises predominantly from the singlet manifold via prompt and triplet-triplet annihilation (TTA)-driven delayed fluorescence, rather than from phosphorescence, challenging the earlier assumptions of amplified spontaneous emission (ASE) originating from the triplet manifold. In highly concentrated solutions, the emission shows strong resemblance to that of the crystalline phase, confirming its origin from aggregate singlet states rather than monomeric pathways. Further, the materials are prone to photodegradation, which gives rise to new high-energy fluorescence and phosphorescence bands adding to the complexity of the photophysics of this family of materials.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202509535"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077095","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

Thiazole-2-Carbaldehyde-Based Covalent Organic Frameworks. 噻唑-2-乙醛基共价有机框架。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202516013

Xuefeng Wang, Jing Ning, Jianping Zhang, Lingyu Ge, Hongtao Wei, Shitao Wang, Long Hao, Dapeng Cao

{"title":"Thiazole-2-Carbaldehyde-Based Covalent Organic Frameworks.","authors":"Xuefeng Wang, Jing Ning, Jianping Zhang, Lingyu Ge, Hongtao Wei, Shitao Wang, Long Hao, Dapeng Cao","doi":"10.1002/anie.202516013","DOIUrl":"https://doi.org/10.1002/anie.202516013","url":null,"abstract":"We first synthesize a novel aldehyde-substituted benzo[1,2-d:4,5-d']bis(thiazole) monomer (BBTC) via a facile method with a high yield, and the BBTC is used for the first time as a building block for synthesis of imine-linked COFs. By using linkage transformation strategy, we further synthesize an imidazole N-heterocyclic carbene precursor COF (BBTC-INP COF) and the imidazole-2-thione COF (BBTC-IT COF). Interestingly, the BBTC-INP and BBTC-IT COFs exhibit 2620- and 1810-fold enhancements in photoluminescence quantum yields, respectively, compared to the parent BBTC COF. This linkage transformation not only optimizes the optical performance but also enables effective Hg2⁺ detection through the strategic incorporation of thione (C═S) groups as specific binding sites. In particular, the BBTC-IT COF presents outstanding selectivity and sensitivity for toxic Hg2⁺ detection, and the limit of detection reaches 60 nM, highlighting the advantage of as-synthesized BBTC-IT COFs in fluorescence sensing applications. In short, this work reports a series of novel thiazole-2-carbaldehyde-based COFs, which largely enriches the diversity of COFs and would also stimulate the synthesis of more BBTC-based COFs for different applications.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202516013"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071505","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

NIR-Activatable, Sequence-Specific Metal-Nucleic Acid Scaffolds for Responsive Uncaging. nir可激活，序列特异性金属核酸支架反应性剥离。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202514717

Arpit Sharma, Man Kshetri, Deepak Karna, Md Al Amin, Shirin Akter, Hanbin Mao, Yao-Rong Zheng

{"title":"NIR-Activatable, Sequence-Specific Metal-Nucleic Acid Scaffolds for Responsive Uncaging.","authors":"Arpit Sharma, Man Kshetri, Deepak Karna, Md Al Amin, Shirin Akter, Hanbin Mao, Yao-Rong Zheng","doi":"10.1002/anie.202514717","DOIUrl":"https://doi.org/10.1002/anie.202514717","url":null,"abstract":"Precise molecular activation with both analyte specificity and spatiotemporal control remains a major challenge in responsive diagnostics, targeted therapies, and the study of complex biological systems. Traditional photo-uncaging strategies offer excellent temporal resolution but suffer from limited tissue penetration and poor biological specificity, while analyte-responsive platforms provide molecular selectivity without external control. Here, we introduce sequence-responsive diagnostic uncaging-a unique approach that integrates nucleic acid recognition with near-infrared (NIR)-triggered molecular activation within a metal-nucleic acid scaffold. This platform is built upon a first-of-its-kind Pt(IV)-DNA molecular scaffold, modularly assembled via click chemistry, and integrates a Pt(IV)-caged reporter, a nucleic acid recognition domain, and an NIR antenna (e.g., IR800). Notably, DNA-mediated electron transfer (DNA-MET) provides a long-range ET pathway to direct photoreduction of the Pt(IV) centers, enabling \"responsive uncaging\" that occurs only upon hybridization with a fully complementary DNA or miRNA strand. Upon NIR irradiation, the duplexed nucleic acid system facilitates electron transfer from the excited antenna to Pt(IV), triggering the release of fluorescent reporters. Using two Pt(IV)-caged fluorophores (MCA and BDP), we demonstrate efficient uncaging and high sequence specificity in both solution and live cells. This platform offers a powerful and versatile photochemical tool that seamlessly bridges diagnostics and molecular activation, with broad implications for precision medicine, targeted drug delivery, and next-generation biosensing technologies.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202514717"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145076765","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

BN/BO Doping of peri-Acenoacenes: Modulating Excited States in Trapeziumene Congeners. BN/BO掺杂对梯形烯同系物激发态的调节。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202517114

Daniele Poletto, Mauro Marongiu, David Hernández-Castillo, Rúben R Ferreira, Martina Crosta, Pradip Kumar Mondal, Leticia González, Davide Bonifazi

{"title":"BN/BO Doping of peri-Acenoacenes: Modulating Excited States in Trapeziumene Congeners.","authors":"Daniele Poletto, Mauro Marongiu, David Hernández-Castillo, Rúben R Ferreira, Martina Crosta, Pradip Kumar Mondal, Leticia González, Davide Bonifazi","doi":"10.1002/anie.202517114","DOIUrl":"https://doi.org/10.1002/anie.202517114","url":null,"abstract":"The rational design of polycyclic aromatic hydrocarbons that combine chemical and physical robustness with finely tuned optoelectronic properties remains a key challenge in materials science. As an initial step toward this goal, we report the synthesis and comprehensive characterization of a new class of boron-, nitrogen-, and oxygen-doped peri-acenoacenes, termed (2,5,4)-trapeziumene congeners. Analysis of these systems provides chemical descriptors that could guide the rational tailoring of their properties through peripheral doping. The target trapeziumene congeners were obtained via a sequence of Suzuki-Miyaura and Buchwald-Hartwig couplings, followed by directed borylation, giving both phenylborane and borinic derivatives with diverse peripheral doping sequences. Single-crystal X-ray diffraction revealed planar to slightly twisted backbones, with peripheral heteroatomic motifs that modulate π-conjugation and intermolecular packing. Photophysical studies showed bright fluorescence (ΦF up to 0.99), narrow Stokes shifts, and structured phosphorescence at 77 K. Electrochemical analysis demonstrated p-type behavior and a progressive HOMO-LUMO gap widening upon N→O substitution. Theoretical investigations revealed that N→O substitution asymmetrically affects the excited states, blue-shifting fluorescence while red-shifting phosphorescence, through an asymmetric charge stabilization in the S1 and T1 excited states. This is accompanied by a progressive widening of the T1-T2 energy gap.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202517114"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077107","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

Topologically Tunable α-Helix Mimetics for Targeting Protein-Protein Interactions. 靶向蛋白-蛋白相互作用的拓扑可调α-螺旋模拟物。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202508209

Tae-Kyung Lee, Luxi Chen, Chia-Yuan Chen, Henry Neal, Jung-Mo Ahn

引用次数: 0

Unveiling the Influence of Formation Voltage on Li-Rich Layered Oxide Cathode. 揭示形成电压对富锂层状氧化物阴极的影响。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202515719

Kang Zhang, Yichun Zheng, Jianhua Yin, Yawen Yan, Yilong Chen, Yuan Tian, Yizhen Huang, Lianpeng Li, Jiyuan Xue, Wen Jiao, Na Liu, Lirong Zheng, Huan Huang, Jing Zhang, Deniz Wong, Bodry Tegomo Chiogo, Christian Schulz, Yang Sun, Chongheng Shen, Qingsong Wang, Yu Qiao, Shi-Gang Sun

{"title":"Unveiling the Influence of Formation Voltage on Li-Rich Layered Oxide Cathode.","authors":"Kang Zhang, Yichun Zheng, Jianhua Yin, Yawen Yan, Yilong Chen, Yuan Tian, Yizhen Huang, Lianpeng Li, Jiyuan Xue, Wen Jiao, Na Liu, Lirong Zheng, Huan Huang, Jing Zhang, Deniz Wong, Bodry Tegomo Chiogo, Christian Schulz, Yang Sun, Chongheng Shen, Qingsong Wang, Yu Qiao, Shi-Gang Sun","doi":"10.1002/anie.202515719","DOIUrl":"https://doi.org/10.1002/anie.202515719","url":null,"abstract":"Lithium-rich layered oxide (LRLO) cathodes are recognized for their high energy densities, primarily driven by oxygen-related anionic redox activities, yet substantial activation of this process simultaneously induces structural instability. The typical voltage range in academic studies spans 2.0-4.8 V. Although 2.5-4.5 V are generally considered in industrial applications for enhanced capacity retention and electrolyte compatibility, this moderate voltage window leads to reduced capacity. To address energy density limitations, several top battery suppliers propose to separately increase the formation voltage during the initial cycle to enhance capacity, while other companies (e.g., Contemporary Amperex Technology Co., Ltd., CATL) claim that this high-voltage formation protocol would exacerbate cycling capacity fading. Herein, we systemically demonstrate that high-voltage formation promotes substantial Li+ extraction from the transition metal (TM) layers, creating vacancies (in TM layer) that drive in-plane TM migration. This migration triggers a transformation in the OM6 (M, cation) configuration from O4 (OLixTM2) to O5 (OLiyTM1). Such evolution simultaneously enhances both anionic and cationic redox activity, collectively boosting capacity. Nonetheless, the induced in-plane TM migration would further aggravate out-of-plane TM migration, leading to progressive structural degradation, which has been elucidated as the main reason for cycling capacity fading.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515719"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077120","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