Angewandte Chemie最新文献_第6页

Anion-π Interactions on Functionalized Porous Aromatic Cages for Gold Recovery from Complex Aqueous with High Capacity

Angewandte Chemie Pub Date : 2025-01-18 DOI: 10.1002/ange.202410665

Dr. Jianzhu Jiang, Dr. Junning Kou, Dr. Qi Wu, Dr. Li Chen, Prof. Dr. Yun Geng, Prof. Dr. Guogang Shan, Prof. Dr. Chunyi Sun, Prof. Dr. Zhongmin Su, Prof. Dr. Xinlong Wang

引用次数: 0

Nikolaos Eleftheriadis

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202423044

引用次数: 0

In-Situ Formation of Three-Dimensional Network Intrinsic Microporous Ladder Polymer Membranes with Ultra-High Gas Separation Performance and Anti-Trade-Off Effect

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202420742

Luxin Sun, Wei Xu, Prof. Hongjun Zhang, Jiachen Chu, Mengtao Wang, Kai Song, Wenjie Wu, Prof. Jianxin Li, Dr. Yingge Wang, Prof. Ingo Pinnau, Prof. Xiaohua Ma

{"title":"In-Situ Formation of Three-Dimensional Network Intrinsic Microporous Ladder Polymer Membranes with Ultra-High Gas Separation Performance and Anti-Trade-Off Effect","authors":"Luxin Sun, Wei Xu, Prof. Hongjun Zhang, Jiachen Chu, Mengtao Wang, Kai Song, Wenjie Wu, Prof. Jianxin Li, Dr. Yingge Wang, Prof. Ingo Pinnau, Prof. Xiaohua Ma","doi":"10.1002/ange.202420742","DOIUrl":"https://doi.org/10.1002/ange.202420742","url":null,"abstract":"The global quest for clean energy and sustainable processes makes advanced membrane extremely attractive for energy-intensive industrial gas separations. Here, we disclose a series of ultra-high-performance gas separation membranes (PIM-3D-TB) from novel network polymers of intrinsic microporosity (PIM) that combine the advantages of solution processible PIM and small pore size distribution (PSD) of porous organic polymers (POP), which was synthesized by in situ copolymerization of triptycene-2,6-diamine as linear part and triptycene-2,6,13(14)-triamine (TTA) as crosslinker. The resulting PIM-3D-TB membranes demonstrated outstanding separation properties that outperformed the latest trade-off lines for H2/CH4 and O2/N2. They also showed an anti-trade-off effect by simultaneously enhancing gas permeability and gas-pair selectivity with increasing TTA content. The TTA crosslinking node increased the microporosity, and, shifted the PSD from the ultramicropore (<7 Å) toward the more size sieving submicropore (<4 Å) region. The post-treated TTA-75 displayed an exceptional H2 permeability of 8000 Barrer and H2/CH4 selectivity of 208. These PIM-3D-TB membranes and their design protocol have unparalleled potential in the next generation of membranes for hydrogen purification and air separations.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143252717","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

Sprayed Aqueous Microdroplets for Spontaneous Synthesis of Functional Microgels 用于自发合成功能性微凝胶的喷雾水性微滴

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202420926

Dr. Xin Li, Wenjing Zhang, Dr. Helin Li, Prof. Dr. Qi Shuai, Prof. Dr. Xingcai Zhang, Prof. Dr. Andrij Pich

{"title":"Sprayed Aqueous Microdroplets for Spontaneous Synthesis of Functional Microgels","authors":"Dr. Xin Li, Wenjing Zhang, Dr. Helin Li, Prof. Dr. Qi Shuai, Prof. Dr. Xingcai Zhang, Prof. Dr. Andrij Pich","doi":"10.1002/ange.202420926","DOIUrl":"https://doi.org/10.1002/ange.202420926","url":null,"abstract":"The development of sustainable synthesis route to produce functional and bioactive polymer colloids has attracted much attention. Most strategies are based on the polymerization of monomers or crosslinking of prepolymers by enzyme- or cell-mediated reactions or specific catalysts in confined emulsions. Herein, a facile solution spray method was developed for spontaneous synthesis of microgels without use of confined emulsion, additional initiators/catalysts and deoxygenation, which addresses the challenges in traditional microgel synthesis. The polarization of air-water interface of the microdroplets can spontaneously split hydroxide ions in water to produce hydroxyl radicals, thereby initiating polymerization and crosslinking in air environment. This synthesis strategy is applicable to a variety of monomers and enables the fabrication of microgels with tunable chemical structures and variable sizes. Importantly, the synthesis route also allows for the preparation of enzyme- or drug-loaded microgels via the in situ encapsulation, which also display high enzymatic activity and stimuli-triggered drug release. Therefore, this work not only is of great significance to macromolecular science and microdroplet chemistry, but also may bring new insights into cellular biochemistry and even prebiotic chemistry due to the prevalence of microdroplets in the environment.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202420926","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Elaborate Designed Three-Dimensional Hierarchical Conductive MOF/LDH/CF Nanoarchitectures for Superior Capacitive Deionization

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202420295

Dr. Chang He, Jun Zhang, Prof. Dionissios Mantzavinos, Prof. Alexandros Katsaounis, Dr. Duan-Hui Si, Dr. Zhang Yan, Dr. Hong-Yu Zhang, Prof. Zhu-Wu Jiang

{"title":"Elaborate Designed Three-Dimensional Hierarchical Conductive MOF/LDH/CF Nanoarchitectures for Superior Capacitive Deionization","authors":"Dr. Chang He, Jun Zhang, Prof. Dionissios Mantzavinos, Prof. Alexandros Katsaounis, Dr. Duan-Hui Si, Dr. Zhang Yan, Dr. Hong-Yu Zhang, Prof. Zhu-Wu Jiang","doi":"10.1002/ange.202420295","DOIUrl":"https://doi.org/10.1002/ange.202420295","url":null,"abstract":"Rational exploration of cost-effective, durable, and high-performance electrode materials is imperative for advancing the progress of capacitive deionization (CDI). The integration of multicomponent layered double hydroxides (LDHs) with conjugated conductive metal–organic frameworks (c-MOFs) to fabricate bifunctional heterostructure electrode materials is considered a complex but promising strategy. Herein, the fabrication of elaborately designed three-dimensional hierarchical conductive MOF/LDH/CF nanoarchitectures (M–CAT/LDH/CF) as CDI anodes via a controllable grafted-growth strategy is reported. In this assembly, carbon fiber (CF) provides exceptional electrical conductivity facilitating rapid ion transfer and acts as a sturdy foundation for even distribution of NiCoCu-LDH nanosheets. Moreover, the well-ordered NiCoCu-LDH further acts as interior templates to create an interface by embedding c-MOFs and aligning two crystal lattice systems, facilitating the graft growth of c-MOFs/LDH heterostructures along the LDH nanosheet arrays on CF, leading to accelerated ion diffusion kinetics. Density functional theory (DFT) confirms the unique structure of M–CAT/LDH/CF promotes interfacial charge transfer from NiCoCu-LDH to M–CAT. This enhancement accelerates ion transfer, decreases ion migration energy, and leads to better ion diffusion kinetics and a smoother Cl− shuttle. Accordingly, the asymmetrical M–CAT/LDH/CF cell exhibited superior specific capacitance (315 F g−1), excellent salt adsorption capacity (147.8 mg g−1), rapid rate (21.1 mg g−1 min−1), and impressive cyclic stability (91.4 % retention rate). This work offers valuable insights for designing heterostructure electrode materials based on three-dimensional interconnected networks, contributing to further advancements in CDI technology.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431333","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

Deciphering and Enhancing Rate-Determining Step of Sodium Deposition towards Ultralow-Temperature Sodium Metal Batteries

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202416720

Yuxiang Niu, Jinlin Yang, Fanbin Meng, Zejun Sun, Chonglai Jiang, Yuan Liu, Hongfei Xu, Meng Wang, Haotian Yang, Yupeng Zhu, Gang Wu, Prof. Wei Chen

{"title":"Deciphering and Enhancing Rate-Determining Step of Sodium Deposition towards Ultralow-Temperature Sodium Metal Batteries","authors":"Yuxiang Niu, Jinlin Yang, Fanbin Meng, Zejun Sun, Chonglai Jiang, Yuan Liu, Hongfei Xu, Meng Wang, Haotian Yang, Yupeng Zhu, Gang Wu, Prof. Wei Chen","doi":"10.1002/ange.202416720","DOIUrl":"https://doi.org/10.1002/ange.202416720","url":null,"abstract":"Achieving high ionic conductivity and stable performance at low temperatures remains a significant challenge in sodium-metal batteries (SMBs). In this study, we propose a novel electrolyte design strategy that elucidates the solvation structure-function relationship within mixed solvent systems. A mixture of diglyme and 1,3-dioxolane was developed to optimize the solvation structure towards superior low-temperature electrolyte. Molecular dynamics simulations and Raman spectra results reveal the solvent-separated ion pairs and contact ion pairs dominated solvation structure in the designed electrolyte, displaying a superior ionic conductivity of 1.78×10−3 S cm−1 at −40 °C. Besides, comprehensive kinetic analysis shows Na+ transportation in the electrolyte shows a greater impact on sodium plating than Na+ transport through the solid electrolyte interphase or charge transfer. As a result, the electrolyte enables stable operation for over 12,000 hours in Na<math></math>\u0000Na cells at −40 °C. In Na<math></math>\u0000Na2/3Ni1/4Cu1/12Mn2/3O2 full cells, it maintains a high capacity retention of 92.4 % over 600 cycles with an initial specific capacity of 89.4 mAh g−1 at −40 °C, and achieves 81.7 % capacity retention after 50 cycles with an initial specific capacity of 75.3 mAh g−1 at −78 °C. These results pave the way for the development of high-performance SMBs capable of operating under ultralow temperatures.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202416720","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Multivariate Approaches Boosting Lithium-Mediated Ammonia Electrosynthesis in Different Electrolytes

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202416027

Anna Mangini, Jon Bjarke Valbæk Mygind, Sara Garcia Ballesteros, Alessandro Pedico, Marco Armandi, Ib Chorkendorff, Federico Bella

{"title":"Multivariate Approaches Boosting Lithium-Mediated Ammonia Electrosynthesis in Different Electrolytes","authors":"Anna Mangini, Jon Bjarke Valbæk Mygind, Sara Garcia Ballesteros, Alessandro Pedico, Marco Armandi, Ib Chorkendorff, Federico Bella","doi":"10.1002/ange.202416027","DOIUrl":"https://doi.org/10.1002/ange.202416027","url":null,"abstract":"Ammonia electrosynthesis through the lithium-mediated approach has recently reached promising results towards high activity and selectivity in aprotic media, reaching high Faradaic efficiency (FE) values and NH3 production rates. To fasten the comprehension and optimization of the complex lithium-mediated nitrogen reduction system, for the first time a multivariate approach is proposed as a powerful tool to reduce the number of experiments in comparison with the classical one-factor-at-a-time approach. Doehlert design and surface response methodology are employed to optimize the electrolyte composition for a batch autoclaved cell. The method is validated with the common LiBF4 salt, and the correlations between the FE and the amount of lithium salt and ethanol as proton donor are elucidated, also discussing their impact on the solid electrolyte interphase (SEI) layer. Moreover, a new fluorinated salt is proposed (i.e., lithium difluoro(oxalate) borate (LiFOB)), taking inspiration from lithium batteries. This salt is chosen to tailor the SEI layer, with the aim of obtaining a bifunctional interfacial layer, both stable and permeable to N2, the latter being an essential characteristic for batch systems. The SEI layer composition is confirmed strategic and its tailoring with LiFOB boosts FE values.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202416027","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

From Natural Product Derivative to Hexagonal Prism Supermolecule: Potent Biofilm Disintegration, Enhanced Foliar Affinity, and Effective Management of Tomato Bacterial Canker

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202416079

Xue Chen, Run Yang, Prof. Dr. Kongjun Liu, Min Liu, Qingchuan Shi, Jinghan Yang, Prof. Gefei Hao, Prof. Dr. Laixin Luo, Prof. Dr. Fengpei Du, Prof. Dr. Peiyi Wang

{"title":"From Natural Product Derivative to Hexagonal Prism Supermolecule: Potent Biofilm Disintegration, Enhanced Foliar Affinity, and Effective Management of Tomato Bacterial Canker","authors":"Xue Chen, Run Yang, Prof. Dr. Kongjun Liu, Min Liu, Qingchuan Shi, Jinghan Yang, Prof. Gefei Hao, Prof. Dr. Laixin Luo, Prof. Dr. Fengpei Du, Prof. Dr. Peiyi Wang","doi":"10.1002/ange.202416079","DOIUrl":"https://doi.org/10.1002/ange.202416079","url":null,"abstract":"Clavibacter michiganensis (Cmm), designated as an A2 quarantine pest by the European and Mediterranean Plant Protection Organization (EPPO), incites bacterial canker of tomato, which presently eludes rapid and effective control methodologies. Dense biofilms formed by Cmm shield internal bacteria from host immune defenses and obstruct the ingress of agrochemicals. Even when agrochemicals disintegrate biofilms, splashing and bouncing during application disperse active ingredients away from target sites. Herein, we present a supramolecular strategy to fabricate a hexagonal prism-shaped material, BPGA@CB[8], assembled from an 18β-glycyrrhetinic acid derivative (PBGA) and host molecule—cucurbit[8]uril (CB[8]) via host–guest recognition. This positively charged material manifests multifaceted functionalities, notably the ability to surmount biofilm barriers, annihilate the encased pathogenic bacteria, and enhance foliar affinity of droplets. The strong in vitro potency and effective deposition of BPGA@CB[8] foster optimal conditions for robust in vivo efficacy, demonstrating superior protective and curative activities (56.9 %/53.4 %) against canker of tomato at a low-dose of 100 μg⋅mL−1 compared to BPGA (44.6 %/42.2 %), kasugamycin (30.1 %/28.4 %), and thiodiazole copper (35.4 %/31.0 %). This supramolecular material, based on natural product derivatives, provides a potent treatment for high-risk canker of tomato, and exemplifies the utility of supramolecular strategies in optimizing the attributes of natural products for managing plant bacterial diseases.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431724","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

Activatable Photosensitizer Prodrug for Self-Amplified Immune Therapy Via Pyroptosis

Angewandte Chemie Pub Date : 2025-01-17 DOI: 10.1002/ange.202419376

Ping-Zhao Liang, Li-Li Ren, Ying-Hong Yan, Zhe Li, Fei-Yu Yang, Tian-Bing Ren, Lin Yuan, Xiao-Bing Zhang

{"title":"Activatable Photosensitizer Prodrug for Self-Amplified Immune Therapy Via Pyroptosis","authors":"Ping-Zhao Liang, Li-Li Ren, Ying-Hong Yan, Zhe Li, Fei-Yu Yang, Tian-Bing Ren, Lin Yuan, Xiao-Bing Zhang","doi":"10.1002/ange.202419376","DOIUrl":"https://doi.org/10.1002/ange.202419376","url":null,"abstract":"Immunotherapy is a promising cancer treatment, but its application is hindered by tumors’ low immunogenicity and the difficulty of immune cell infiltration. Here, to address above issues and achieve targeted tumor treatment, we designed the first activated small molecule photosensitizer immune-prodrug HDIM based on pyroptosis, and proposed a self-amplified immune therapy strategy (SITS) for enhanced tumor therapy. HDIM can be specifically activated by the tumor hypoxia and then simultaneously initiate immuno-therapy and photodynamic therapy (PDT)-induced pyroptosis with NIR laser irradiation. Mechanism study demonstrated that the immunogenicity in tumor can be significantly enhanced by HDIM-induced pyroptosis and immune cells are recruited, thus effectively amplifying the therapeutic effect of the released immune drugs. As proof of application, we have utilized HDIM for primary tumor and distant tumor therapy. And the experiment results showed that compared to current monotherapy as well as simple combination therapy, the photosensitizer prodrug HDIM exhibited much superior tumor treatment effect owing to its synchronous activation of pyroptosis and immuno-therapy in tumor.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475676","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

Titelbild: Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure (Angew. Chem. 8/2025)

Angewandte Chemie Pub Date : 2025-01-16 DOI: 10.1002/ange.202500499

Chang-An Lo, Yixian Wang, Varun R. Kankanallu, Aditya Singla, Dean Yen, Xiaoyin Zheng, Kaustubh G. Naik, Bairav S. Vishnugopi, Callum Campbell, Vikalp Raj, Chonghang Zhao, Lu Ma, Jianming Bai, Feipeng Yang, Ruipeng Li, Mingyuan Ge, John Watt, Partha P. Mukherjee, David Mitlin, Yu-chen Karen Chen-Wiegart

{"title":"Titelbild: Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure (Angew. Chem. 8/2025)","authors":"Chang-An Lo, Yixian Wang, Varun R. Kankanallu, Aditya Singla, Dean Yen, Xiaoyin Zheng, Kaustubh G. Naik, Bairav S. Vishnugopi, Callum Campbell, Vikalp Raj, Chonghang Zhao, Lu Ma, Jianming Bai, Feipeng Yang, Ruipeng Li, Mingyuan Ge, John Watt, Partha P. Mukherjee, David Mitlin, Yu-chen Karen Chen-Wiegart","doi":"10.1002/ange.202500499","DOIUrl":"https://doi.org/10.1002/ange.202500499","url":null,"abstract":"Electrodeposition of sodium metal in an anode-free battery can be dendritic. The tree at the center of the cover image represents a single crystalline dendrite, branched and complex in its morphology, originating at the support and growing towards the cathode. Its multicolor leaves are the solid electrolyte interphase (SEI) that cover the metal surface. The SEI is a complex mosaic containing crystalline sodium fluoride, sodium hydride and sodium hydroxide, as well as organic constituents. Details of this study are reported by David Mitlin, Yu-chen Karen Chen-Wiegart et al. in their Research Article (e202412550).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202500499","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0