Angewandte Chemie International Edition最新文献_第2页

Co-Regulation of Interface and Bulk for Enhanced Localized High-Concentration Electrolytes in Stable and Practical Zinc Metal Batteries. 在稳定实用的锌金属电池中增强局部高浓度电解质的界面和体积协同调节。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202501183

Tao Li,Hange Yang,Xinji Dong,Hexian Ma,Jinghua Cai,Chenyu Wei,Tao Zhang,Shicong Zhang,Fuqiang Huang,Tianquan Lin

{"title":"Co-Regulation of Interface and Bulk for Enhanced Localized High-Concentration Electrolytes in Stable and Practical Zinc Metal Batteries.","authors":"Tao Li,Hange Yang,Xinji Dong,Hexian Ma,Jinghua Cai,Chenyu Wei,Tao Zhang,Shicong Zhang,Fuqiang Huang,Tianquan Lin","doi":"10.1002/anie.202501183","DOIUrl":"https://doi.org/10.1002/anie.202501183","url":null,"abstract":"Rechargeable zinc metal batteries (RZMBs) are promising for energy storage due to their high capacity and cost-effectiveness. However, their commercialization is hindered by challenges including dendrite growth, parasitic reactions, and cathode degradation, particularly under low current densities and negative/positive (N/P) capacity ratios. Localized high-concentration electrolytes offer potential solutions, but their reliance on high salt concentrations to replicate solvation structures of high-concentration electrolytes limits their practicality, due to diluent's inherent inertness that limits its role in interfacial chemistry. Here, we present a co-regulation strategy that integrates bulk and interfacial properties to develop an interfacial-enhanced localized high-concentration electrolyte (ILHCE). By incorporating non-coordinating 1,4-dioxane diluent and 1-ethyl-3-methylimidazolium (emim+) cations into dilute aqueous electrolytes, dioxane molecules are pulled into electric double layer (EDL) through the interaction between emim+ and dioxane, achieving a pronounced dilution effect from bulk electrolyte to the EDL. This generates an anion-rich and water-depleted EDL at both anode and cathode interfaces, enhancing Zn2+ transport dynamics, ensuring cathode stability and deriving a robust anion-derived solid-electrolyte interphase. Full batteries using Mn0.5V6O13 cathodes with a low N/P ratio of 1.77 demonstrate 80% capacity retention over 300 cycles at 0.2 A g-1, highlighting ILHCE as a transformative electrolyte design toward real-world applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":"e202501183"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087625","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

Modulating the Polarity of Imine Bonds in Donor-Acceptor Covalent Organic Frameworks for Enhanced Photocatalytic H2 Production. 调节供体-受体共价有机框架中亚胺键的极性以增强光催化制氢。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202509444

Zixuan Li,Bingzi Cai,Qun Li,Di Zhang,Yizhao Liang,Yuanyuan Liu,Yalong Jiao,Arne Thomas,Xiaojia Zhao

{"title":"Modulating the Polarity of Imine Bonds in Donor-Acceptor Covalent Organic Frameworks for Enhanced Photocatalytic H2 Production.","authors":"Zixuan Li,Bingzi Cai,Qun Li,Di Zhang,Yizhao Liang,Yuanyuan Liu,Yalong Jiao,Arne Thomas,Xiaojia Zhao","doi":"10.1002/anie.202509444","DOIUrl":"https://doi.org/10.1002/anie.202509444","url":null,"abstract":"The development of imine-linked covalent organic frameworks (COFs) has also drawn attention to the influence of the nature of imine binding, including its orientation and possible protonation, on the chemical and physical properties of imine COFs. However, the influence of the polarity of imine bond (C=N) on the photocatalytic performance of COFs has not yet been described. In this work, we synthesized a series of imine COFs with differently polarized C=N bonds by altering the C=N bond orientation and regulating the donor-acceptor (D-A) strength, respectively. The less polarized C=N bond for one of the COFs possesses a faster charge separation with a decrease of exciton binding energy (Eb). In contrast, the imine COF with more polarized C=N bond exhibits a stronger internal electric field contributing to a more efficient charge transfer. Taking into account this trade-off between binding energy and charge transfer concerning the effect of C=N polarity on the photocatalytic performances, the imine COF with moderately polarized C=N bond shows the highest hydrogen evolution performance of 28.1 mmol h-1 g-1. This work provides evidence that the polarity of C=N should be taken into account when designing and tuning the properties of imine COFs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"56 1","pages":"e202509444"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087563","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

Ultrahigh-Voltage Lithium Metal Batteries Enabled by Single-Ion and Weakly-Solvating Nanometric Aggregates. 单离子和弱溶剂化纳米聚集体实现的超高压锂金属电池。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202502465

Chenxi Xiao,Peng Wen,Feiyu Luo,Dengxiang Yu,Huaijiao Wang,Zhirong Zhou,Weiping Li,Xinxing Zhang,Xinrong Lin

{"title":"Ultrahigh-Voltage Lithium Metal Batteries Enabled by Single-Ion and Weakly-Solvating Nanometric Aggregates.","authors":"Chenxi Xiao,Peng Wen,Feiyu Luo,Dengxiang Yu,Huaijiao Wang,Zhirong Zhou,Weiping Li,Xinxing Zhang,Xinrong Lin","doi":"10.1002/anie.202502465","DOIUrl":"https://doi.org/10.1002/anie.202502465","url":null,"abstract":"The urgent need for high energy density (> 400 Wh kg-1) has driven advancements in lithium metal batteries (LMBs) with high-voltage cathodes. However, degradation of traditional electrolytes restricts high cut-off voltage < 4.4 V, while low lithium transference numbers (tLi+) lead to polarization and early charge/discharge termination, which typically necessitate use of multiple solvents or salt-concentrated electrolytes to enable high-voltage chemistry. To address this challenge, we developed a single-solvent, single-salt electrolyte with tris(2,2,2-trifluoroethyl)phosphate (TFEP), achieving a high tLi+ of 0.82 and enabling ultra-high-voltage LMB operation up to 5.0 V. Large molecular sterics and electron density delocalization of TFEP enabled dominant presence of local aggregates (AGGs), which further populated to form large and ion-rich weakly-solvating nanometric aggregates (n-AGGs), changing redox properties and promoting the interfacial stabilities to a greater extent. As a result, we showed suppressed dendrite formation with stable cycling for over 1,500 hours, and full-cell operations paired with LiNi0.8Mn0.1Co0.1O2 (NCM811) at 4.7 V and with LiNi0.5Mn1.5O4 (LNMO) at 5.0 V. The tuning of bulk electrolyte properties from the scale of microscopic electronic structures to mesoscopic solvation structures has effectively enhanced thermodynamic and kinetic stabilities of the electrolyte, paving the way for lithium metal batteries with high-voltage tolerance.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"54 1","pages":"e202502465"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087611","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

Kelvin Probe Force Microscopy Reveals Spatially Resolved Charge-Transfer Mechanism in CdS/BiOBr S-scheme Heterojunction Photocatalyst. 开尔文探针力显微镜揭示CdS/BiOBr S-scheme异质结光催化剂的空间分辨电荷转移机制。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202505456

Zheng Meng,Jianjun Zhang,Haoyu Long,Hermenegildo García,Liuyang Zhang,Bicheng Zhu,Jiaguo Yu

{"title":"Kelvin Probe Force Microscopy Reveals Spatially Resolved Charge-Transfer Mechanism in CdS/BiOBr S-scheme Heterojunction Photocatalyst.","authors":"Zheng Meng,Jianjun Zhang,Haoyu Long,Hermenegildo García,Liuyang Zhang,Bicheng Zhu,Jiaguo Yu","doi":"10.1002/anie.202505456","DOIUrl":"https://doi.org/10.1002/anie.202505456","url":null,"abstract":"S-scheme heterojunctions hold great promise for photocatalysis, yet a comprehensive understanding of their charge-transfer mechanisms remains limited. While time-resolved techniques have provided valuable insights, the spatial resolution of charge transfer at the material surface remains underexplored. Here, we employ Kelvin probe force microscopy (KPFM) to investigate the charge-transfer dynamics in S-scheme heterojunctions, revealing spatially resolved details. Our findings show that upon illumination, the Fermi level (Ef) of n-type semiconductors increases, but a built-in electric field (IEF) persists within the heterojunction. Electrons accumulate on the surface of the reduction semiconductor (RS), resulting in a surface photovoltage (SPV) lower than that of the individual semiconductor, while holes accumulate on the oxidation semiconductor (OS) surface, producing an SPV higher than that of the bare material. The S-scheme heterojunction leads to a remarkable increase in charge separation, with 11 additional photogenerated electrons and 3,722 additional holes compared to the bare CdS and BiOBr. These results offer critical insights into the spatially resolved charge-transfer mechanisms of S-scheme heterojunctions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":"e202505456"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087620","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

Unlocking Precision in Biomass Conversion through Functional Ligand Engineering of Lewis Acidic MOFs. 通过Lewis酸性mof的功能配体工程解锁生物质转化精度。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202508256

Qingchong Xu,Xingjie Wang,Yao Liu,Lihong Zhao,Feng Peng,Junli Ren

{"title":"Unlocking Precision in Biomass Conversion through Functional Ligand Engineering of Lewis Acidic MOFs.","authors":"Qingchong Xu,Xingjie Wang,Yao Liu,Lihong Zhao,Feng Peng,Junli Ren","doi":"10.1002/anie.202508256","DOIUrl":"https://doi.org/10.1002/anie.202508256","url":null,"abstract":"The catalytic isomerization of glucose to fructose is a key factor in cellulosic biomass utilization. Thus, achieving high-efficient fructose production and understanding the dominant reaction route remain crucial goals. Hereby, this study refines a precise ligand engineering strategy applied to the typical metal-organic framework, UiO-66, generating a series of Lewis acidic UiO-66-based catalysts with only subtle structural adjustments. Among all, UiO-66-pCl-SBA possessed the strongest Lewis acidity and exhibited the best glucose isomerization performance. Further investigation elaborates the crucial contribution of both the amount of Lewis acid and the nature of specific acid sites to enhanced catalytic reactivity, given a high fructose yield of 47% at a glucose conversion of 63%, achieved with a UiO-66 catalyst substituted by 49% monosodium 2-sulfoterephthalate. The increased acid density with specific Lewis acid strength is computationally identified to promote the polarization of glucose molecules, facilitating the isomerization process. Density functional theory calculations reveal that incorporating functionalized ligands and increasing their proportion markedly decrease both the electron density at Zr sites and the material's band gap, which in turn benefits the Lewis acid strength and catalytic activity enhancement. This work highlights the significance of Lewis sites'nature and its effect on glucose isomerization performance.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":"e202508256"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087661","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

The Role of Reducibility of PtGaO x -based Catalysts for Efficient and Durable Propane Dehydrogenation. PtGaO x基催化剂的还原性在丙烷高效持久脱氢中的作用。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202506704

Kai Wu,Vita A Kondratenko,Mingxia Zhou,Dmitry Doronkin,Stephan Bartling,Qiyang Zhang,Shanlei Han,Xin Jia,Qi Liu,Dong Xiong,Chunming Xu,Guiyuan Jiang,Dan Zhao,Uwe Rodemerck,David Linke,Evgenii V Kondratenko

{"title":"The Role of Reducibility of PtGaO x -based Catalysts for Efficient and Durable Propane Dehydrogenation.","authors":"Kai Wu,Vita A Kondratenko,Mingxia Zhou,Dmitry Doronkin,Stephan Bartling,Qiyang Zhang,Shanlei Han,Xin Jia,Qi Liu,Dong Xiong,Chunming Xu,Guiyuan Jiang,Dan Zhao,Uwe Rodemerck,David Linke,Evgenii V Kondratenko","doi":"10.1002/anie.202506704","DOIUrl":"https://doi.org/10.1002/anie.202506704","url":null,"abstract":"Although PtGaOx-containing catalysts are active and selective in the non-oxidative dehydrogenation of propane (PDH) to propylene, they suffer from rapid deactivation and, especially, inability to recover their initial performance in a series of PDH/oxidative regeneration cycles, characteristics that are highly relevant to commercialization. Herein, we identified reducibility of GaOx as the key descriptor affecting the above catalyst features. Oxidized GaOx species are more active than reduced GaOx in the recombination of two H species formed from propane, which is the rate-limiting step in the PDH reaction. This process is further accelerated by Pt. The reduction of GaOx with time on propane stream leads to catalyst deactivation. Easily reducible GaOx also tend to form PtGaOx under PDH conditions, from which Pt atoms present in fresh catalysts cannot be completely recovered during oxidative regeneration, which is detrimental to catalyst durability. Regardless of the reaction atmosphere, Pt single atoms exist on the surface of PtGaOx-containing catalysts with hardly reducible GaOx. Based on the knowledge derived, we developed a catalyst with 500 ppm Pt on the surface of mixed GaAlOx, which outperforms almost all previous PtGaOx-containing catalysts in terms of space-time yield of propylene formation and shows durable operation under industrially relevant conditions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"62 1","pages":"e202506704"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087667","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

Atomic Cu-O-Zr sites for highly selective production of p-xylene from tandem upcycling of PET and CO2. 通过PET和CO2的串联升级循环制备高选择性对二甲苯的Cu-O-Zr原子位点。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202507309

Qizhuang Zou,Tairen Long,Ruiqi Fang,Xin Zhao,Fengliang Wang,Yingwei Li

{"title":"Atomic Cu-O-Zr sites for highly selective production of p-xylene from tandem upcycling of PET and CO2.","authors":"Qizhuang Zou,Tairen Long,Ruiqi Fang,Xin Zhao,Fengliang Wang,Yingwei Li","doi":"10.1002/anie.202507309","DOIUrl":"https://doi.org/10.1002/anie.202507309","url":null,"abstract":"Exploring an efficient catalytic system for tandem upcycling of CO2 and polyethylene terephthalate (PET) is highly desirable for achieving efficient resource utilization of wastes. However, the high activation energy for C=O bonds (in both PET and CO2) and the difficulty in regulating the reaction pathways restricted PET recovery efficiency. Here, we demonstrated the rational design of a single-atom Cu catalyst for precisely catalyzing the hydrogenation of CO2 to methanol and tandem PET upcycling to ethylene glycol (EG) and p-xylene (PX). In the Cu/UiO-66-NH2-A catalyst, Cu atoms are selectively anchored to the Zr-oxo nodes of UiO-66-NH2 to form Cu-O-Zr sites. The Cu-O-Zr sites can effectively activate both CO2 and H2 by reducing the activation energy and accelerate the transformation of PET to dimethyl terephthalate (DMT), which is further hydro-deoxygenated to yield PX. As a result, 20.4% CO2 conversion was obtained within 36 h, with 89.5% and 92.1% yields of PX and EG, respectively. Rapid and precise hydrogen spillover from Cu atoms to adsorbed reactants/intermediates at the Cu-O-Zr sites also drives the reaction process.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":"e202507309"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087613","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

A Cerium-Naphthazarin Catecholate MOF as a Heterogeneous Photocatalyst for Selective Functionalization of Alkanes. 铈-萘杂酚儿茶酚酸MOF作为烷烃选择性功能化的非均相光催化剂。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202503328

Sharath Kandambeth,Rajesh Kancherla,Kuntal Pal,Taslim Melliti,Mostafa Zeama,Vinayak S Kale,Issatay Nadinov,Abdulaziz M Alali,Osama Shekhah,Omar F Mohammed,Magnus Rueping,Mohamed Eddaoudi

{"title":"A Cerium-Naphthazarin Catecholate MOF as a Heterogeneous Photocatalyst for Selective Functionalization of Alkanes.","authors":"Sharath Kandambeth,Rajesh Kancherla,Kuntal Pal,Taslim Melliti,Mostafa Zeama,Vinayak S Kale,Issatay Nadinov,Abdulaziz M Alali,Osama Shekhah,Omar F Mohammed,Magnus Rueping,Mohamed Eddaoudi","doi":"10.1002/anie.202503328","DOIUrl":"https://doi.org/10.1002/anie.202503328","url":null,"abstract":"In this work we have successfully synthesized a series of novel semiconducting 2D catecholate metal-organic frameworks (MOFs) based on naphthazarin ligands by utilizing unraveled metal-acetyl acetonate linkage chemistry. The synthesized Ce-Naph MOF exhibited excellent light absorption properties and chemical stability across various solvents. Its insoluble and stable framework, combined with an optimal band gap, enabled its use as a photocatalyst for organic transformations. For the first time, Ce-Naph MOF is explored as a heterogeneous catalyst for photocatalytic applications specifically for the selective C-H amination of alkanes, achieving yields of up to 89% under ambient conditions. We propose that the initial metal-to-ligand charge transfer in Ce-Naph MOF, promoted by light, is essential for forming an active alkoxy-Ce(IV)-species. This species subsequently undergoes ligand-to-metal charge transfer to generate the alkoxy radical, which acts as a hydrogen atom transfer reagent to activate alkanes. Furthermore, Ce-Naph MOF demonstrated long-term cyclic stability, maintaining its catalytic activity and structural integrity over five cycles, highlighting its durability as a heterogeneous catalyst. We are confident that this straightforward and practical methodology opens new avenues for industrial applications, significantly advancing the fields of metal catalysis, photocatalysis, and sustainable chemistry.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"17 1","pages":"e202503328"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087619","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

Fluoridation-assisted Interfacial Dipole for CsPbI3 Perovskite Solar Cells with over 22% Efficiency. 氟化辅助CsPbI3钙钛矿太阳能电池界面偶极子，效率超过22%。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202506282

Junming Qiu,Xinyi Mei,Mingxu Zhang,Guoliang Wang,Lixin Pan,Shengwen Zou,Jianmei Huang,Xiaoliang Zhang

{"title":"Fluoridation-assisted Interfacial Dipole for CsPbI3 Perovskite Solar Cells with over 22% Efficiency.","authors":"Junming Qiu,Xinyi Mei,Mingxu Zhang,Guoliang Wang,Lixin Pan,Shengwen Zou,Jianmei Huang,Xiaoliang Zhang","doi":"10.1002/anie.202506282","DOIUrl":"https://doi.org/10.1002/anie.202506282","url":null,"abstract":"Inorganic CsPbI3 perovskite attracts remarkable interest in photovoltaic applications due to its outstanding thermal stability and optoelectronic properties. However, CsPbI3 perovskite solar cells (PSCs) significantly suffer from severe energy losses due to interface nonradiative recombination and poor charge carrier transport, predominantly affecting their photovoltaic performance and operational stability. Herein, an interfacial dipole engineering is introduced for CsPbI3 PSCs, in which azetidinium chloride (Az) and its fluorinated derivative 3,3-difluoroazetidinium chloride (DFAz) are employed to manipulate the interface properties of PSCs and thus diminish energy losses. Systematically theoretical calculations and experimental studies reveal that the fluoridation-assisted ammonium molecule could form a stronger interaction with perovskites and thereby arrange the dipole alignment on the superficial layer of perovskites, which could simultaneously ameliorate passivation effect and energy level alignment of the perovskite and hole transport layers, thereby suppressing interface recombination. Meanwhile, the coordinated bonding between the ammonium and hole transport layer facilitates charge transport at the heterojunction interface by offering additional carrier transport channels. Consequently, the CsPbI3 PSCs deliver a high efficiency of up to 22.05%. This work provides important design principles of interface engineering for high-performance solar cells to minimize energy losses.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"151 1","pages":"e202506282"},"PeriodicalIF":16.6,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087567","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

Au6Cu2 Clusters with High Electron Affinity and Oxygen-Mimetic Properties for Hypoxic Tumor Radiosensitization. 具有高电子亲和和模拟氧特性的Au6Cu2簇在低氧肿瘤放射增敏中的应用。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-19 DOI: 10.1002/anie.202504524

Xueli Zhao,Jingpeng Han,Junqi Liu,Zhao-Yang Wang,Xiaoyuan Chen,Shuang-Quan Zang

引用次数: 0