Zhaoyu Zhang, Xiaojia Lan, Guoli Liao, Wencheng Du, Yufei Zhang, Minghui Ye, Zhipeng Wen, Yongchao Tang, Xiaoqing Liu, Cheng Chao Li
A major dilemma faced by Zn anodes at high zinc utilization rate (ZUR) is the insufficient supply of ionic carriers that initiate the space charge layer (SCL) subject to rampant growth of Zn dendrites. Herein, an ‘anion-cation co-regulation’ strategy, associated with a fundamental principle for screening potential electrolyte additives coupling the Zn2+ ferrying effect with anion-retention capability, are put forward to construct dendrite-free, high-ZUR Zn anode. Taking ninhydrin-modified ZnSO4 system as a proof-of-concept, the multiple zincophilic polar groups of ninhydrin facilitate the transport of Zn2+ ions while its electron-deficient aromatic ring retains SO42- counterions via anion-π interaction, constructing an ion-rich interface that minimizes the SCL-driven Zn deterioration. Consequently, the Zn anode can endure ~240 h continuous cycling at an ultrahigh ZUR of 87.3%. The superiority brought by ninhydrin is further reflected by the ultralong cycling durability of Zn-I2 batteries (over 100000 cycles at 10 A g-1, ~20-fold lifespan extension). Even at an ultralow N/P ratio of 1.1 (~90.6% ZUR), the battery with a capacity of ~5.27 mAh cm-2 can still sustain for 350 cycles, which has been hardly achieved in aqueous Zn batteries. Furthermore, the effectiveness of this strategy is fully validated by a series of additives sharing similar fundamentals.
{"title":"Coupling Zn2+ Ferrying Effect with Anion-π Interaction to Mitigate Space Charge Layer Enables Ultra-High Utilization Rate Zn Anode","authors":"Zhaoyu Zhang, Xiaojia Lan, Guoli Liao, Wencheng Du, Yufei Zhang, Minghui Ye, Zhipeng Wen, Yongchao Tang, Xiaoqing Liu, Cheng Chao Li","doi":"10.1002/anie.202503396","DOIUrl":"https://doi.org/10.1002/anie.202503396","url":null,"abstract":"A major dilemma faced by Zn anodes at high zinc utilization rate (ZUR) is the insufficient supply of ionic carriers that initiate the space charge layer (SCL) subject to rampant growth of Zn dendrites. Herein, an ‘anion-cation co-regulation’ strategy, associated with a fundamental principle for screening potential electrolyte additives coupling the Zn2+ ferrying effect with anion-retention capability, are put forward to construct dendrite-free, high-ZUR Zn anode. Taking ninhydrin-modified ZnSO4 system as a proof-of-concept, the multiple zincophilic polar groups of ninhydrin facilitate the transport of Zn2+ ions while its electron-deficient aromatic ring retains SO42- counterions via anion-π interaction, constructing an ion-rich interface that minimizes the SCL-driven Zn deterioration. Consequently, the Zn anode can endure ~240 h continuous cycling at an ultrahigh ZUR of 87.3%. The superiority brought by ninhydrin is further reflected by the ultralong cycling durability of Zn-I2 batteries (over 100000 cycles at 10 A g-1, ~20-fold lifespan extension). Even at an ultralow N/P ratio of 1.1 (~90.6% ZUR), the battery with a capacity of ~5.27 mAh cm-2 can still sustain for 350 cycles, which has been hardly achieved in aqueous Zn batteries. Furthermore, the effectiveness of this strategy is fully validated by a series of additives sharing similar fundamentals.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"59 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672716","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}
Rechargeable magnesium (Mg) batteries represent a promising energy storage system by offering low cost and dendrite-less propensity. However, the limited selection of cathode materials, and often with low voltage and capacity, constrain Mg batteries. Herein, by exploiting the ion-docking effect between two halogen species — iodine cations (I+) and chlorine anions (Cl-) — we activate the cathodic activity of halogens and develop a magnesium-iodine/chlorine (Mg-I/Cl) battery prototype with high energy and power density. The ion-docking effect enables I+ and Cl- to mutually balance and disperse their charges, weakens the coordination strength between Cl- and Mg2+ while enhances the stability of I+, thus facilitating the multi-electron (2+1/3) redox reactions of halogens. We also find the solvation state of iodine species determine the reaction process of the I0/I3-/I- redox couples. The here-developed magnesium-iodine/chlorine battery features an impressively high discharge plateau of up to 3.0 V with a high capacity exceeding 400 mAh g-1, and demonstrates a stable lifespan for 500 cycles, with the ability of ultra-fast charging at 20C and low-temperature cycling under -30 °C. These findings may provide new insights for developing high-energy-density Mg battery systems.
{"title":"Ion-Docking Effect Enabling Rechargeable High-Voltage Magnesium-Iodine/Chlorine Battery","authors":"Longyuan Guo, Tong Li, Ting Yang, Zhenglin Hu, Aoxuan Wang, Jiayan Luo","doi":"10.1002/anie.202503209","DOIUrl":"https://doi.org/10.1002/anie.202503209","url":null,"abstract":"Rechargeable magnesium (Mg) batteries represent a promising energy storage system by offering low cost and dendrite-less propensity. However, the limited selection of cathode materials, and often with low voltage and capacity, constrain Mg batteries. Herein, by exploiting the ion-docking effect between two halogen species — iodine cations (I+) and chlorine anions (Cl-) — we activate the cathodic activity of halogens and develop a magnesium-iodine/chlorine (Mg-I/Cl) battery prototype with high energy and power density. The ion-docking effect enables I+ and Cl- to mutually balance and disperse their charges, weakens the coordination strength between Cl- and Mg2+ while enhances the stability of I+, thus facilitating the multi-electron (2+1/3) redox reactions of halogens. We also find the solvation state of iodine species determine the reaction process of the I0/I3-/I- redox couples. The here-developed magnesium-iodine/chlorine battery features an impressively high discharge plateau of up to 3.0 V with a high capacity exceeding 400 mAh g-1, and demonstrates a stable lifespan for 500 cycles, with the ability of ultra-fast charging at 20C and low-temperature cycling under -30 °C. These findings may provide new insights for developing high-energy-density Mg battery systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"16 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672722","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}
Liquid crystal elastomers (LCEs) are versatile soft actuators known for their flexible texture, low density, and ability to undergo reversible deformations that mimic the behavior of skeletal muscles. These properties make them highly attractive for applications in exoskeletons, soft robotics, and medical devices. However, their functionality is typically limited to simple and discontinuous deformations. This study introduces a novel structural design that enables precise control of both the mode and amplitude of deformation. This design integrates photo‐reactive o‐nitrobenzyl moieties and temperature‐dependent hydrogen bonds into the LCE structure. The o‐nitrobenzyl moieties enable irreversible reconfiguration of the LCE crosslinked network through photoreactions, allowing for easy alignment and reshaping of the material. Meanwhile, the hydrogen bonds act as "temperature‐dependent locks", regulating the mobility of polymer chains during thermal deformation. By adjusting the heating temperature, the deformation amplitude can be finely tuned across a wide range (0~103%). The synergy of these two mechanisms—light‐induced irreversible reconfiguration and temperature‐induced reversible H‐bond exchanges—empowers LCEs to achieve customizable and continuous deformations. This represents a significant advancement in bridging the gap between synthetic actuators and biological motion systems.
{"title":"Controlled Deformation Mode and Amplitude of Liquid Crystal Actuators through Orthogonal Light and Heat‐Induced Exchanges","authors":"Jian Ding, Tuan Liu, Jinwen Zhang, Yuzhan Li, Xuepei Miao, Caicai Li, Wanqi Chen, Baihang Chen, Xinyi Huang, Liangdong Zhang, Kun Wang, Zhixiang Dong, Bingkun Bao, Linyong Zhu, Qiuning Lin","doi":"10.1002/anie.202505172","DOIUrl":"https://doi.org/10.1002/anie.202505172","url":null,"abstract":"Liquid crystal elastomers (LCEs) are versatile soft actuators known for their flexible texture, low density, and ability to undergo reversible deformations that mimic the behavior of skeletal muscles. These properties make them highly attractive for applications in exoskeletons, soft robotics, and medical devices. However, their functionality is typically limited to simple and discontinuous deformations. This study introduces a novel structural design that enables precise control of both the mode and amplitude of deformation. This design integrates photo‐reactive o‐nitrobenzyl moieties and temperature‐dependent hydrogen bonds into the LCE structure. The o‐nitrobenzyl moieties enable irreversible reconfiguration of the LCE crosslinked network through photoreactions, allowing for easy alignment and reshaping of the material. Meanwhile, the hydrogen bonds act as \"temperature‐dependent locks\", regulating the mobility of polymer chains during thermal deformation. By adjusting the heating temperature, the deformation amplitude can be finely tuned across a wide range (0~103%). The synergy of these two mechanisms—light‐induced irreversible reconfiguration and temperature‐induced reversible H‐bond exchanges—empowers LCEs to achieve customizable and continuous deformations. This represents a significant advancement in bridging the gap between synthetic actuators and biological motion systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"183 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672411","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}
Jihong Yu, Ruobing Bai, Nana Yan, Guangyuan He, Yingchun Ye, Risheng Bai, Dan Li, Peng Guo, Donghai Mei, Wenfu Yan
Efficient ethylene/ethane (C2H4/C2H6) separation using low-energy technologies is crucial for the chemical industry yet remains challenging due to the lack of industrially applicable adsorbents. Cu(I)-based adsorbents show significant potential; however, traditional synthesis methods often involve complex procedures or reduction steps. Herein, we report that Cu@SAPO-RHO zeolite, synthesized for the first time via a one-pot method with cyclam as the Cu(II) ligand, exhibits a remarkable C2H4/C2H6 selectivity of 22.6, a C2H4 uptake of 3.08 mmol/g, and a separation factor of 9.4 under ambient conditions by using a C2H4 pretreatment, placing it among the best-performing zeolitic materials. The C2H4 pretreatment enhances separation efficiency by partially reducing Cu(II) to Cu(I) and water resistance through the formation of carbon species during pretreatment. Structural analysis using Rietveld refinement reveals that Cu2+ ions occupy the corners of elliptical single 8-rings (s8r). X-ray absorption near-edge structure (XANES) analysis confirms a reduction in Cu oxidation state, while X-ray photoelectron spectroscopy (XPS) corroborates the partial conversion of Cu(II) to Cu(I). Periodic density functional theory (DFT) calculations further reveal that Cu(I) interacts more strongly with C2H4 than Cu(II). With its straightforward synthesis and enhanced performance through C2H4 pretreatment, Cu@SAPO-RHO zeolite presents a promising solution for industrial-scale C2H4/C2H6 separation.
{"title":"Ethylene Pretreatment Enhances Ethylene Adsorption and Separation over Cu@SAPO-RHO Zeolite","authors":"Jihong Yu, Ruobing Bai, Nana Yan, Guangyuan He, Yingchun Ye, Risheng Bai, Dan Li, Peng Guo, Donghai Mei, Wenfu Yan","doi":"10.1002/anie.202501053","DOIUrl":"https://doi.org/10.1002/anie.202501053","url":null,"abstract":"Efficient ethylene/ethane (C2H4/C2H6) separation using low-energy technologies is crucial for the chemical industry yet remains challenging due to the lack of industrially applicable adsorbents. Cu(I)-based adsorbents show significant potential; however, traditional synthesis methods often involve complex procedures or reduction steps. Herein, we report that Cu@SAPO-RHO zeolite, synthesized for the first time via a one-pot method with cyclam as the Cu(II) ligand, exhibits a remarkable C2H4/C2H6 selectivity of 22.6, a C2H4 uptake of 3.08 mmol/g, and a separation factor of 9.4 under ambient conditions by using a C2H4 pretreatment, placing it among the best-performing zeolitic materials. The C2H4 pretreatment enhances separation efficiency by partially reducing Cu(II) to Cu(I) and water resistance through the formation of carbon species during pretreatment. Structural analysis using Rietveld refinement reveals that Cu2+ ions occupy the corners of elliptical single 8-rings (s8r). X-ray absorption near-edge structure (XANES) analysis confirms a reduction in Cu oxidation state, while X-ray photoelectron spectroscopy (XPS) corroborates the partial conversion of Cu(II) to Cu(I). Periodic density functional theory (DFT) calculations further reveal that Cu(I) interacts more strongly with C2H4 than Cu(II). With its straightforward synthesis and enhanced performance through C2H4 pretreatment, Cu@SAPO-RHO zeolite presents a promising solution for industrial-scale C2H4/C2H6 separation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"8 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672719","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}
Proton exchange is a fundamental chemical event, and NMR provides the most direct readout of protonation events with site-specific resolution. Conventional approaches require manual titration of sample pH to collect a series of NMR spectra at different pH values. This requires extensive sample handling and often results in significant sample loss, leading to reduced signal or the need to prepare additional samples. Here, we introduce a novel approach to control pH in NMR samples using water soluble photoacids, which alter the pH of the solution from near neutral to acidic pH upon in situ photo-illumination. We show that the solution pH can be precisely controlled by choice of illumination wavelength and intensity and sufficient protons are released from the photoacid to achieve meaningful pH change in samples where the molecule of interest has significant buffering capacity, such as a >100 µM protein sample. The pH is monitored in situ using internal standards with pH-sensitive chemical shifts. This method enables precise, calibrated, non-invasive change of sample pH within an NMR magnet, dramatically reducing the necessary sample handling. These findings highlight the potential of light-induced pH control in NMR experiments and increase the robustness and reliability of pH-dependent studies.
{"title":"In situ light-driven pH modulation for NMR studies","authors":"Ravula Thirupathi","doi":"10.1002/anie.202501440","DOIUrl":"https://doi.org/10.1002/anie.202501440","url":null,"abstract":"Proton exchange is a fundamental chemical event, and NMR provides the most direct readout of protonation events with site-specific resolution. Conventional approaches require manual titration of sample pH to collect a series of NMR spectra at different pH values. This requires extensive sample handling and often results in significant sample loss, leading to reduced signal or the need to prepare additional samples. Here, we introduce a novel approach to control pH in NMR samples using water soluble photoacids, which alter the pH of the solution from near neutral to acidic pH upon in situ photo-illumination. We show that the solution pH can be precisely controlled by choice of illumination wavelength and intensity and sufficient protons are released from the photoacid to achieve meaningful pH change in samples where the molecule of interest has significant buffering capacity, such as a >100 µM protein sample. The pH is monitored in situ using internal standards with pH-sensitive chemical shifts. This method enables precise, calibrated, non-invasive change of sample pH within an NMR magnet, dramatically reducing the necessary sample handling. These findings highlight the potential of light-induced pH control in NMR experiments and increase the robustness and reliability of pH-dependent studies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"93 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672715","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}
Xulong Fan, Lidan Lan, Yuanyu Chang, Long Yang, Yun Huang, Yi Dan, Long Jiang
Photoconversion of waste plastics into valuable CO and CH3COOH represents a ground-breaking strategy for addressing plastic pollution issues. However, this process currently encounters significant challenges, primarily due to the limitation of catalyst activity and the difficulty in breaking C–C bonds. Herein, we present a novel approach that integrates multi-step charge transfer pathways with photothermal-driven reactions to improve photoconversion efficiency. By incorporating Bi0/Bi3+ metal as an electron transport mediator for multi-step charge transfer, we markedly enhanced the separation and transport of photoelectrons, thereby accelerating the generation of active species. Meanwhile, the heat generated by the localized surface plasmon resonance effect of Bi0 drove the reactions related to the photoconversion of polypropylene. Subsequently, the photo-conversion rates of PP into CO by Bi0@Bi3+-KNbO3 reached 209.41 μmol gcat-1 h-1, which is 27.55 times higher than that achieved with KNbO3. Furthermore, the dual Bi-Nb sites effectively stabilize the key intermediate *COOH, thereby promoting the production of CH3COOH at a rate of 213.00 μmol gcat-1 h-1. This strategy of boosting photoconversion activity of PP into CO and CH3COOH offers an effective green solution to the serious issue of plastic pollution.
{"title":"Construction of Multi-step Charge Transfer Pathways in Bi0@Bi3+-KNbO3 for Significantly Accelerated Photoconversion of Waste Plastics","authors":"Xulong Fan, Lidan Lan, Yuanyu Chang, Long Yang, Yun Huang, Yi Dan, Long Jiang","doi":"10.1002/anie.202502874","DOIUrl":"https://doi.org/10.1002/anie.202502874","url":null,"abstract":"Photoconversion of waste plastics into valuable CO and CH3COOH represents a ground-breaking strategy for addressing plastic pollution issues. However, this process currently encounters significant challenges, primarily due to the limitation of catalyst activity and the difficulty in breaking C–C bonds. Herein, we present a novel approach that integrates multi-step charge transfer pathways with photothermal-driven reactions to improve photoconversion efficiency. By incorporating Bi0/Bi3+ metal as an electron transport mediator for multi-step charge transfer, we markedly enhanced the separation and transport of photoelectrons, thereby accelerating the generation of active species. Meanwhile, the heat generated by the localized surface plasmon resonance effect of Bi0 drove the reactions related to the photoconversion of polypropylene. Subsequently, the photo-conversion rates of PP into CO by Bi0@Bi3+-KNbO3 reached 209.41 μmol gcat-1 h-1, which is 27.55 times higher than that achieved with KNbO3. Furthermore, the dual Bi-Nb sites effectively stabilize the key intermediate *COOH, thereby promoting the production of CH3COOH at a rate of 213.00 μmol gcat-1 h-1. This strategy of boosting photoconversion activity of PP into CO and CH3COOH offers an effective green solution to the serious issue of plastic pollution.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"183 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672717","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}
Yinuo Zheng, Elvis Wang Hei NG, Antonio Rizzo, Pauline Chiu
We present the first reductive kinetic resolution of racemic 2H-azirines to prepare optically enriched N-H aziridine-2-carboxylates, which are bench stable and easily diversifiable building blocks, concomitantly with the corresponding enantiomerically enriched 2H-azirines. The N-H aziridines were obtained with excellent diastereoselectivity (>20:1) and high enantioselectivity (up to 94%). A Hammett study revealed a linear free energy relationship between the ΔΔG⧧ of the diastereomeric transition states and the σp- values. DFT calculations and non-covalent interaction analysis suggested that non-classical H–bonding interactions and edge-to-face aromatic interactions between the substrate and the ligand are responsible for the stereoselectivity and also for the substrate electronic effects observed in the Hammett study.
{"title":"Enantiomerically Enriched Aziridine-2-carboxylates via Copper-Catalyzed Reductive Kinetic Resolution of 2H-Azirines","authors":"Yinuo Zheng, Elvis Wang Hei NG, Antonio Rizzo, Pauline Chiu","doi":"10.1002/anie.202423645","DOIUrl":"https://doi.org/10.1002/anie.202423645","url":null,"abstract":"We present the first reductive kinetic resolution of racemic 2H-azirines to prepare optically enriched N-H aziridine-2-carboxylates, which are bench stable and easily diversifiable building blocks, concomitantly with the corresponding enantiomerically enriched 2H-azirines. The N-H aziridines were obtained with excellent diastereoselectivity (>20:1) and high enantioselectivity (up to 94%). A Hammett study revealed a linear free energy relationship between the ΔΔG⧧ of the diastereomeric transition states and the σp- values. DFT calculations and non-covalent interaction analysis suggested that non-classical H–bonding interactions and edge-to-face aromatic interactions between the substrate and the ligand are responsible for the stereoselectivity and also for the substrate electronic effects observed in the Hammett study.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"20 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672720","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}
Chenglong Liu, Tian Liu, Ruiqi Liu, Yuying Liu, Jin Ma, Qianqian Ji, Na Li, Chao Wang, Qichong Zhang, Wensheng Yan
Aqueous Zinc-based batteries provide promising opportunities for next-generation rechargeable batteries. Nevertheless, Zn anode encounters severe challenges, such as Zn dendrite formation, surface corrosion, and hydrogen evolution reaction (HER). Here, we report a strategy to spontaneously construct a boron-fluoride dual-atom regulated SEI (ZnBOF), which involves the formation of a B-compound coating through etching process and followed by an in-situ F substitution during the initial electrochemical cycling. The ZnBOF/Zn anode benefit preferential deposition of Zn2+ along the (002) plane without Zn dendrite, and the side reaction including by-product and HER are dramatically suppressed. A combination of characterization methods, such as X-ray absorption spectroscopy, show that the B-containing passivation layer facilitates the transport of Zn2+ and mitigates water-related side reactions, and the F atoms serve as zincophilic sites that enhance the transfer kinetics of Zn2+. As expected, the well-designed ZnBOF/Zn anode exhibits ultra-stable Zn plating/stripping for 5000 h at 2 mA cm-2. The assembled ZnBOF/Zn||MnO2 batteries show impressive cycling stability, remaining 96.2% of the initial capacity (234.3 mAh g-1) after 1700 cycles at 1.0 A g-1. Therefore, this work reveals a dual-atom synergistic regulated strategy to fabricate a robust SEI for Zn anode, which contributes to the development of aqueous zinc-based batteries.
{"title":"Boron-Fluoride Dual-atom Synergistic Regulated Interface Coating Enables Stable Zn-metal Anodes","authors":"Chenglong Liu, Tian Liu, Ruiqi Liu, Yuying Liu, Jin Ma, Qianqian Ji, Na Li, Chao Wang, Qichong Zhang, Wensheng Yan","doi":"10.1002/anie.202503376","DOIUrl":"https://doi.org/10.1002/anie.202503376","url":null,"abstract":"Aqueous Zinc-based batteries provide promising opportunities for next-generation rechargeable batteries. Nevertheless, Zn anode encounters severe challenges, such as Zn dendrite formation, surface corrosion, and hydrogen evolution reaction (HER). Here, we report a strategy to spontaneously construct a boron-fluoride dual-atom regulated SEI (ZnBOF), which involves the formation of a B-compound coating through etching process and followed by an in-situ F substitution during the initial electrochemical cycling. The ZnBOF/Zn anode benefit preferential deposition of Zn2+ along the (002) plane without Zn dendrite, and the side reaction including by-product and HER are dramatically suppressed. A combination of characterization methods, such as X-ray absorption spectroscopy, show that the B-containing passivation layer facilitates the transport of Zn2+ and mitigates water-related side reactions, and the F atoms serve as zincophilic sites that enhance the transfer kinetics of Zn2+. As expected, the well-designed ZnBOF/Zn anode exhibits ultra-stable Zn plating/stripping for 5000 h at 2 mA cm-2. The assembled ZnBOF/Zn||MnO2 batteries show impressive cycling stability, remaining 96.2% of the initial capacity (234.3 mAh g-1) after 1700 cycles at 1.0 A g-1. Therefore, this work reveals a dual-atom synergistic regulated strategy to fabricate a robust SEI for Zn anode, which contributes to the development of aqueous zinc-based batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"27 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672718","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}
Miaomiao Ding, Bin Chen, Daniela A. Wilson, Yingfeng Tu, Fei Peng
{"title":"Inside Back Cover: From Autonomous Chemical Micro‐/Nanomotors to Rationally Engineered Bio‐Interfaces","authors":"Miaomiao Ding, Bin Chen, Daniela A. Wilson, Yingfeng Tu, Fei Peng","doi":"10.1002/anie.202505569","DOIUrl":"https://doi.org/10.1002/anie.202505569","url":null,"abstract":"","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"56 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672410","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":"Inside Back Cover: Reinventing the High‐rate Energy Storage of Hard Carbon: the Order‐degree Governs the Trade‐off of Desolvation–Solid Electrolyte Interphase at Interfaces","authors":"Meiqi Liu, Zhou Jiang, Xiangyu Wu, Fuxi Liu, Wenwen Li, Detian Meng, Aofei Wei, Ping Nie, Wei Zhang, Weitao Zheng","doi":"10.1002/anie.202505563","DOIUrl":"https://doi.org/10.1002/anie.202505563","url":null,"abstract":"","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"24 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672408","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}
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