{"title":"Ether-Anchored MOFs Enable Stable Pseudosuspension Electrolytes for High-Energy Lithium Metal Batteries.","authors":"Yu Han,Yong Chen,Tonghui Zhang,Zhiye Hao,Lianlian He,Weiting Ma,Taolue Wen,Shunshun Zhao,Qimin Peng,Zhenzhen Shen,Robin Wang,Guoxiu Wang,Shimou Chen","doi":"10.1002/anie.202518384","DOIUrl":"https://doi.org/10.1002/anie.202518384","url":null,"abstract":"Rational electrolyte design, capable of simultaneously accelerating bulk ion transport and stabilizing interfacial chemistry, is indispensable for achieving high-energy-density lithium metal batteries (LMBs). Here, we demonstrate that short-chain ether-functionalized metal-organic frameworks (S@MOFs) meet these requirements by efficiently tailoring Li⁺ coordination and reconstructing the electrode/electrolyte interphase, achieving durable interfacial ion transport kinetics. Synergistic experimental and theoretical investigations demonstrate that the S@MOF-based electrolyte features distinctive pseudosuspension characteristics, harnessing ether chemistry that affords Li-metal compatibility and Li-salt coordination in concert with MOF's abundant binding sites and ordered rigid frameworks. The resultant S@MOF-based electrolyte delivers robust thermodynamic stability across -10 to 60 °C, even in LiNi0.8Co0.1Mn0.1O2 (NCM811)||Li full-cell configurations. Under lean-electrolyte and 50 µm-thick Li-metal configurations, it achieves 92.40% capacity retention for LiCoO2||Li after 1000 cycles. Remarkably, 90.70% for quasi-solid-state NCM811||Li (500 cycles), and 93.21% for Na3V2(PO4)3||Na (3000 cycles) were obtained, confirming its broad applicability across alkali-metal battery chemistries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"59 1","pages":"e202518384"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145338581","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}
{"title":"A Sonosensitive Heterometallic Polyoxometalate for Highly Efficient Chemo-Sonodynamic Synergistic Cancer Therapy.","authors":"Man-Yi Du,Hui-Ping Xiao,Ruo-Fei Xu,Xian-Bin Sun,Xin-Yi Wang,Dong-Miao Li,Sheng-Nan Yue,Zi-Zhong Zhang,Xing Huang,Yu Gao,Xiu-Ling Shang,Xin-Xiong Li,Shou-Tian Zheng","doi":"10.1002/anie.202514859","DOIUrl":"https://doi.org/10.1002/anie.202514859","url":null,"abstract":"Chemo-sonodynamic synergistic therapy (CSDT) integrates the advantages of both chemodynamic therapy (CDT) and sonodynamic therapy (SDT), including specificity, non-invasiveness, high penetration, and controllability, and it is especially suitable for deep-seated tumors. However, there is still a lack of effective CSDT agents with long-term stability, excellent water solubility, biocompatibility, and highly efficient catalytic activities. To address these challenges, we report a rare sonosensitive polyoxometalate (POM), H11[Er2Sb2W7O23(OH)(DMF)2(SbW9O33)2]·17H2O (ErSbW), featuring an atomically precise capsule-like structure with good solubility, molecular stability, and biosafety under physiological conditions. In vitro studies reveal ErSbW's remarkable CDT efficiency in catalyzing the generation of reactive oxygen species (ROS). More importantly, the efficiency can be further distinctly augmented by three times with the presence of ultrasound irradiation, suggesting a pronounced synergistic enhancement effect in ErSbW. Most notably, ErSbW-mediated CSDT achieved complete eradication of deep-seated tumors in a melanoma model at the dose of 35 µg kg-1. This work not only provides a unique POM-based molecular agent for CSDT but also demonstrates the great potential of POM materials in synergistic cancer therapies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"12 1","pages":"e202514859"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331883","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}
{"title":"Molecular Design-Driven Interface Engineering Enabling Simultaneous Defect Passivation and Enhanced Hole Extraction in Perovskite Solar Cells.","authors":"Wei Jia,Riming Sun,Jingyuan Qiao,Guangchao Shi,Qiangqiang Zhao,Ziyan Gong,Siming Zheng,Ruida Xu,Jingzhi Shang,Lin Song,Kai Wang,Wei Huang,Ruihao Chen,Yiyun Fang,Hongqiang Wang,Zi-Qiang Rong","doi":"10.1002/anie.202513869","DOIUrl":"https://doi.org/10.1002/anie.202513869","url":null,"abstract":"Interface engineering has emerged as an effective strategy to address interface defects and energy level misalignment between the perovskite and hole transport layer (HTL). Herein, three novel multifunctional hole interface molecules with distinct substituents were designed to passivate defects at the perovskite/HTL interface. These molecules integrate hole-transporting groups with passivating units, enabling effective defect passivation, improved energy level alignment, and facilitating efficient carrier extraction. Among the three hole transport interface molecules (HTIMs), the 3-(3,6-bis(4-(bis(4-(methylthio)phenyl)amino)phenyl)-9H-carbazol-9-yl)hexan-1-amine hydroiodide (MeS-TPA-Cbz-HAI), comprising -MeS and HAI units, exhibited superior interface passivation capability and greater chemical compatibility with 2,2',7,7'-Tetrakis (N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (Spiro-OMeTAD), leading to a reduction in defect density and enhanced hole transport. Consequently, the device based on MeS-TPA-Cbz-HAI achieved a notable power conversion efficiency (PCE) of 25.83%. Moreover, the unencapsulated device maintained 94% of its initial efficiency after 1000 hours of continuous operation under ambient conditions (30%-65% relative humidity), demonstrating remarkable long-term stability. This design strategy for hole interface molecules presents a promising avenue for achieving both high efficiency and operational stability in perovskite solar cells.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"11 1","pages":"e202513869"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145338554","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}
{"title":"Rapid Fabrication of Defective CuInP2S6 Nanosheets for Efficient CO2-to-Formate Conversion over Wide Current Densities.","authors":"Ya Liu,Meng Zhang,Xitang Qian,Guoyu Hou,Yicheng Li,Yanxiu Liu,Xingqiu Li,Shixian Guan,Junjie Chen,Minhua Shao,Yu Zhang","doi":"10.1002/anie.202516041","DOIUrl":"https://doi.org/10.1002/anie.202516041","url":null,"abstract":"Electrochemical CO2 reduction reaction (CO2RR) to produce value-added chemicals offers a promising approach to mitigate global warming and address the energy crisis. However, the development of highly selective and durable catalysts that perform reliably across varying operational conditions remains challenging. In this work, we report the synthesis of lithium-intercalated CuInP2S6 (Li-CIPS) with a layered structure via a one-step chemical vapor transport method. Compared to pristine CuInP2S6, lithium intercalation in Li-CIPS facilitates the rapid production of ultrathin CuInP2S6 nanosheets through simple soaking in water. Experimental and theoretical investigations reveal that these ultrathin Li-CIPS nanosheets contain abundant sulfur vacancies (Vs), which can substantially enhance the CO2RR activity while suppressing the competing hydrogen evolution reaction. As a result, the Li-CIPS catalyst achieves over 90% Faradaic efficiency (FE) for formate production across wide current densities ranging from 100 to 800 mA cm-2, and it maintains stable operation over 100 h at 200 mA cm-2. This study highlights a promising and selective AMP2X6-based electrocatalyst for efficient CO2-to-formate conversion in practical applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"129 1","pages":"e202516041"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331789","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}
Christoph Fornacon-Wood,Luca Steiner,Chengzhang Xu,Beate Paulus,Alex J Plajer
{"title":"Recoverable Fluorination Accelerates Ring-Opening Copolymerisation and Enables Post-Polymerisation-Modification of Polyesters.","authors":"Christoph Fornacon-Wood,Luca Steiner,Chengzhang Xu,Beate Paulus,Alex J Plajer","doi":"10.1002/anie.202515104","DOIUrl":"https://doi.org/10.1002/anie.202515104","url":null,"abstract":"Fluorination of polymers is a powerful strategy to enhance chemical or material properties yet integrating these benefits into degradable polymers remains underexplored. Here, we report a new class of fluorinated polyesters synthesized via ring-opening copolymerisation of pentafluoro styrene oxide with phthalic anhydride. The pendant C6F5 groups accelerate catalysis through fluorine-specific π-stacking interactions and improve obtained molecular weights compared to the non-fluorinated variant giving access to high weight materials (Mn,max. > 100 kg mol-1) with thermal and mechanical properties competitive with commodity plastics. These C6F5 groups then act as reactive handles in the material for efficient post-polymerisation modification (PPM) in solution, allowing fine-tuning of thermal, mechanical, optical, and solubility properties. PPM can even be performed on material surfaces, films and fibres can be selectively modified without dissolution. Lastly, degradation enables quantitative recovery of fluorine centres as sodium fluoride, offering a sustainable end-of-life option for the incorporated fluorine. Our work demonstrates how targeted fluorination of degradable polyesters can simultaneously enhance catalysis and unlock advanced material functionality.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"49 1","pages":"e202515104"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331725","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}
Yun-Ke Zhao,Zi-Rui Liu,Zhen-Chao Long,Wan-Qi Shi,Quan-Ming Wang
{"title":"Superatomic or Not? A Case Study on Isostructural Au3Ag2 and Au3Cu2 Nanoclusters.","authors":"Yun-Ke Zhao,Zi-Rui Liu,Zhen-Chao Long,Wan-Qi Shi,Quan-Ming Wang","doi":"10.1002/anie.202519135","DOIUrl":"https://doi.org/10.1002/anie.202519135","url":null,"abstract":"Two bimetal nanoclusters, [Au3Ag2(Ppy3)6](NO3)3 (Au3Ag2) and [Au3Cu2(Ppy3)6](BF4)3 (Au3Cu2) have been synthesized with tri(2-pyridyl)phosphine (Ppy3). Single crystal X-ray structural analysis reveals that both have trigonal bipyramidal structures with three Au atoms at the waist and Ag/Cu atoms at the top and bottom vertices. Au3Ag2 demonstrates much better stability than Au3Cu2 in solution. Theoretical calculations indicate that Au3Ag2 is the smallest well-defined superatom while Au3Cu2 is nonsuperatomic, even though they are isostructural and have the same number of valence electrons. This work highlights the influence of atom doping on the electronic structures and superatomic properties of metal nanoclusters.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"54 1","pages":"e202519135"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331730","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}
{"title":"Metal-Hydroxide-Porphin Framework Membrane for Almost Perfectly Selective Li+ Retention.","authors":"Min Jian,Tingting Ma,Zixin Wang,Xuan Ding,Hongfei Gao,Shangfa Pan,Bo Wang,Lijun Yang,Lei Jiang,Jun Gao","doi":"10.1002/anie.202515502","DOIUrl":"https://doi.org/10.1002/anie.202515502","url":null,"abstract":"Membrane separation of Li+ from other ions, particularly alkaline ions, offers a green way toward direct lithium extraction from various brines. Here we report a metal-hydroxide-porphin framework membrane, allowing the passage of all major competing cations (Na+, K+, Ca2+, and Mg2+) while only retaining Li+. The crystalline nature of the membrane allows periodically arranged porphin molecules, enabling stable molecular recognition effect. By density functional theory calculations, we found that the porphin molecules had a strong interaction with Li+ and prevented their translocation through the porphin cavity. As a result, the membrane allows Na+ and K+ transport but rejects the transport of Li+ completely. Notably, due to the much higher mobility of divalent ions, the membrane also allows the passage of Ca2+ and Mg2+ while still retaining Li+ under a low external voltage (0.8 V). We expect that this work establishes metal-hydroxide-porphin framework membrane as a promising and versatile platform for ion sieving studies and applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"15 1","pages":"e202515502"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331740","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}
{"title":"Mechanism of the Stoltz-Grubbs (KOtBu/Et3SiH) Silylation: Single-Electron Transfer is the Missing Link between the Heterolytic and Radical Pathways.","authors":"Ian D Jenkins,Ka Ho Chow,Elizabeth H Krenske","doi":"10.1002/anie.202517336","DOIUrl":"https://doi.org/10.1002/anie.202517336","url":null,"abstract":"A new mechanism for the Stoltz-Grubbs (KOtBu/Et3SiH) silylation of heteroarenes is reported that successfully resolves the important unexplained experimental features of the reaction. The mechanism combines hydride transfer, hydrogen atom transfer (HAT), and single electron transfer (SET) steps (with the substrate hydride adduct being identified as a new SET donor) and is supported by extensive theoretical calculations. Previously proposed heterolytic and radical mechanisms do not involve SET. The discovery of a mechanistic role for SET explains why the silylation reaction simultaneously displays both heterolytic and radical character, and why it does not require free silyl radicals. Previously unexplained experimental results from reactions of isotopically labelled reactants and on the inhibitory effects of electron-accepting additives can also be understood based on the SET mechanism.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":"e202517336"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331661","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}
Wenbo Zhao,Yuliang Tang,Yihui Gao,Qi Ding,Qiang Li,Wenyang Li,Xiaoguang Lei
{"title":"Quantitative Reactivity Profiling of Functional Arginine Residues in Human Cancer Cell Line Proteomes.","authors":"Wenbo Zhao,Yuliang Tang,Yihui Gao,Qi Ding,Qiang Li,Wenyang Li,Xiaoguang Lei","doi":"10.1002/anie.202515603","DOIUrl":"https://doi.org/10.1002/anie.202515603","url":null,"abstract":"Arginine, a critical amino acid for protein structure and function, is involved in enzyme catalysis and macromolecular interactions. However, selectively targeting its reactive guanidine group has been challenging. Here, we utilized a probe, AP-1, based on phenylglyoxal, which demonstrated remarkable chemical selectivity and reactivity toward arginine residues. Using activity-based protein profiling (ABPP), we explored the human proteome across four cancer cell lines, obtaining quantitative data for approximately 17 000 arginine residues. This analysis led to the identification of several previously unreported hyperreactive arginine residues, including R43 of PKM, R171 of LDHA, R172 of LDHB, R341 of CKB, R168 of EIF4A1, and R118 of FUBP1, which are crucial for protein function. Notably, the mutation of CKB's R341 inhibited cell proliferation and migration by downregulating energy supply. We also introduced ArGO-LDHA-1, a covalent inhibitor targeting LDHA's hyperreactive arginine residues, showing potential to enhance chemotherapy efficacy. This work highlights the biological significance of arginine residues and provides a platform for large-scale profiling of arginine reactivity.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"54 1","pages":"e202515603"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331648","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}
Sukanta Saha,Yashwant Pratap Kharwar,Santanu Ghorai,Harshini V Annadata,Suhana Karim,Arnab Dutta
{"title":"A Heterogenised Molecular Electrocatalyst for Round-the-Clock Green Hydrogen Production by Solar-Electrolyser and Zinc-Air Batteries.","authors":"Sukanta Saha,Yashwant Pratap Kharwar,Santanu Ghorai,Harshini V Annadata,Suhana Karim,Arnab Dutta","doi":"10.1002/anie.202516482","DOIUrl":"https://doi.org/10.1002/anie.202516482","url":null,"abstract":"Solar energy-driven seawater electrolysis presents a sustainable method for producing high-purity green hydrogen to address the energy crisis. Developing a robust electrocatalyst for seawater splitting is crucial for green fuel production with solar integration. This study introduces a silica-anchored cobaloxime system as a multifunctional electrocatalyst for overall seawater splitting in conjunction with photovoltaic cells. The system achieves a solar-to-hydrogen generation efficiency of 14%, a power conversion efficiency of 17.4%, and a round-trip energy efficiency of 80%. A single-stack electrolyser using this catalyst produces an average of 0.82 mmol h-1 of green hydrogen and 0.44 mmol h-1 of oxygen, with a hydrogen conversion efficiency of approximately 80 kWh kg-1 under natural sunlight. The same catalyst also shows bidirectional O2 reduction and evolution activity, enabling solar energy storage through a rechargeable zinc-air battery (RZAB). A photovoltaic-RZAB-electrolyser triad was established for indirect green hydrogen production using stored renewable energy. The catalyst-containing RZAB system is effectively charged by a photovoltaic (PV) cell, achieving 25% energy efficiency, and facilitates seawater splitting without sunlight at an energy conversion efficiency of 84%. The strategic application of the catalyst as a multifunctional electrocatalyst enables sustainable green hydrogen production both during the day and night under practical conditions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"17 1","pages":"e202516482"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331663","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}