Angewandte Chemie最新文献

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Metabolism-inspired chemical reaction networks for chemically driven dissipative oligoesterification
Angewandte Chemie Pub Date : 2025-02-15 DOI: 10.1002/ange.202425407
Yeonsoo Lim, Gyunam Park, Hojin An, Jonghwa Han, Joonhyun Bae, Ji-Hyun Kim, Yan Lee, Kyungtae Kang, Jaeyoung Sung, Sunbum Kwon
{"title":"Metabolism-inspired chemical reaction networks for chemically driven dissipative oligoesterification","authors":"Yeonsoo Lim,&nbsp;Gyunam Park,&nbsp;Hojin An,&nbsp;Jonghwa Han,&nbsp;Joonhyun Bae,&nbsp;Ji-Hyun Kim,&nbsp;Yan Lee,&nbsp;Kyungtae Kang,&nbsp;Jaeyoung Sung,&nbsp;Sunbum Kwon","doi":"10.1002/ange.202425407","DOIUrl":"https://doi.org/10.1002/ange.202425407","url":null,"abstract":"<p>Metabolism is a complex network of chemical reactions in which transient biomolecules are continuously produced and degraded. Mimicking this dynamic process in synthetic systems poses a considerable challenge, as it requires designs that enable the exchange of energy and matter among transient molecules. In this study, we explored a chemically driven oligoesterification process operating within a highly intricate reaction network and constructed a dynamic library of transient oligoesters. Our kinetic analysis uncovered an intriguing phenomenon: oligoesters undergo parasitic exchanges, consuming one another to sustain the system's dynamics before reaching thermodynamic equilibrium. This discovery opens new opportunities for designing synthetic systems that replicate the complexity and self-sustaining behavior of metabolic processes.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 14","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202425407","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143761987","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
Electrocatalytic Acetylene Semi-Hydrogenation to Ethylene with High Energy Efficiency
Angewandte Chemie Pub Date : 2025-02-15 DOI: 10.1002/ange.202423381
Cong Dou, Yanmei Huang, Bohang Zhao, Weiwei Lei, Prof. Bin Zhang, Prof. Yifu Yu
{"title":"Electrocatalytic Acetylene Semi-Hydrogenation to Ethylene with High Energy Efficiency","authors":"Cong Dou,&nbsp;Yanmei Huang,&nbsp;Bohang Zhao,&nbsp;Weiwei Lei,&nbsp;Prof. Bin Zhang,&nbsp;Prof. Yifu Yu","doi":"10.1002/ange.202423381","DOIUrl":"https://doi.org/10.1002/ange.202423381","url":null,"abstract":"<p>Electrocatalytic acetylene semi-hydrogenation (EASH) provides a petroleum-independent strategy for ethylene production. However, the challenges of high overpotentials and strong hydrogen evolution competition reaction over conventional electrocatalysts at industrial current densities result in substantial energy consumption, limiting the practical application of EASH technology. Herein, zinc-doped copper catalysts are designed and prepared via a facile impregnation and electroreduction relay method. The as-prepared Cu-2.7Zn catalyst exhibits an ethylene partial current density of −0.29 A cm<sup>−2</sup> with a Faradaic efficiency of 96 % and a reaction potential of −0.62 V versus reversible hydrogen electrode (RHE), surpassing the previously reported electrocatalysts. The combined results of experimental tests and theoretical calculations demonstrate zinc doping significantly enhances acetylene adsorption and accelerates reaction kinetics, leading to a notable decrease in overpotential. Furthermore, the increased *H-*H binding energy barrier and the improved ethylene desorption on Cu-2.7Zn effectively suppress hydrogen evolution and acetylene over-hydrogenation, contributing to the enhancement of ethylene Faradaic efficiency.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 14","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143761941","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
Rücktitelbild: Air-Mediated Biomimetic Synthesis of Polyhydroxyalkanoate with C4 Diol (Angew. Chem. 8/2025)
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502402
Huilin Xie, Kaibin Zhong, Shihao Niu, Xiaoxu Li, Zexu Hu, Guang Xiao, Prof. Yifu Huang, Prof. Hongjie Zhang, Prof. Yuan Liu, Prof. Hefeng Zhang, Prof. Qiuquan Cai
{"title":"Rücktitelbild: Air-Mediated Biomimetic Synthesis of Polyhydroxyalkanoate with C4 Diol (Angew. Chem. 8/2025)","authors":"Huilin Xie,&nbsp;Kaibin Zhong,&nbsp;Shihao Niu,&nbsp;Xiaoxu Li,&nbsp;Zexu Hu,&nbsp;Guang Xiao,&nbsp;Prof. Yifu Huang,&nbsp;Prof. Hongjie Zhang,&nbsp;Prof. Yuan Liu,&nbsp;Prof. Hefeng Zhang,&nbsp;Prof. Qiuquan Cai","doi":"10.1002/ange.202502402","DOIUrl":"https://doi.org/10.1002/ange.202502402","url":null,"abstract":"<p>A strategy for the biomimetic synthesis of polyhydroxyalkanoates (PHA) using C4 diol and air, catalyzed by a synergistic catalyst, was presented by Qiuquan Cai and co-workers in their Research Article (e202417660). The resulting PHA can reversibly convert back to a small-molecule monomer in the form of a five-membered ring, demonstrating excellent ecological sustainability. This study highlights the potential for large-scale synthesis of high-value PHAs from diverse non-grain-based diols.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202502402","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431567","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
BERICHTIGUNG: Correction to “Tandem Methanolysis and Catalytic Transfer Hydrogenolysis of Polyethylene Terephthalate to p-Xylene Over Cu/ZnZrOx Catalysts”
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502639
{"title":"BERICHTIGUNG: Correction to “Tandem Methanolysis and Catalytic Transfer Hydrogenolysis of Polyethylene Terephthalate to p-Xylene Over Cu/ZnZrOx Catalysts”","authors":"","doi":"10.1002/ange.202502639","DOIUrl":"https://doi.org/10.1002/ange.202502639","url":null,"abstract":"<p>This Research Article has been corrected and republished because an author (Michelle Bishop) was accidentally removed at issue publication stage. Michelle Bishop has been included to the list of authors in the corrected publication.</p><p>We apologize for this error.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 11","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202502639","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581685","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
Innentitelbild: Bridging Electrolyte Bulk and Interfacial Chemistry: Dynamic Protective Strategy Enable Ultra-Long Lifespan Aqueous Zinc Batteries (Angew. Chem. 10/2025)
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502397
Qing Wu, Jinlong Zhang, Song Yang, Fusheng Luo, Zeyu Yan, Xiude Liu, Haibo Xie, Prof. Jun Huang, Prof. Yiwang Chen
{"title":"Innentitelbild: Bridging Electrolyte Bulk and Interfacial Chemistry: Dynamic Protective Strategy Enable Ultra-Long Lifespan Aqueous Zinc Batteries (Angew. Chem. 10/2025)","authors":"Qing Wu,&nbsp;Jinlong Zhang,&nbsp;Song Yang,&nbsp;Fusheng Luo,&nbsp;Zeyu Yan,&nbsp;Xiude Liu,&nbsp;Haibo Xie,&nbsp;Prof. Jun Huang,&nbsp;Prof. Yiwang Chen","doi":"10.1002/ange.202502397","DOIUrl":"https://doi.org/10.1002/ange.202502397","url":null,"abstract":"<p>The main bottleneck of rechargeable aqueous zinc batteries (AZBs) is their limited cycle lifespans stemming from the unhealthy electrolyte bulk and fragile interface. In their Research Article (e202418524), Jun Huang, Yiwang Chen et al. report a dynamic protective strategy to bridge electrolyte bulk and interfacial chemistry for ultra-long lifespan AZBs, which greatly unlocks the potential for an extended service lifespan for advanced AZBs.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 10","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202502397","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143530758","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
Rücktitelbild: Monodisperse Chemical Oligophosphorylation of Peptides via Protected Oligophosphorimidazolide Reagents (Angew. Chem. 11/2025)
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502765
Kevin Qian, Björn Hanf, Prof. Christopher Cummins, Prof. Dorothea Fiedler
{"title":"Rücktitelbild: Monodisperse Chemical Oligophosphorylation of Peptides via Protected Oligophosphorimidazolide Reagents (Angew. Chem. 11/2025)","authors":"Kevin Qian,&nbsp;Björn Hanf,&nbsp;Prof. Christopher Cummins,&nbsp;Prof. Dorothea Fiedler","doi":"10.1002/ange.202502765","DOIUrl":"https://doi.org/10.1002/ange.202502765","url":null,"abstract":"<p>Oligophosphorylated peptides were prepared by Kevin Qian, Björn Hanf, Christopher Cummins, and Dorothea Fiedler in their Research Article (e202419147). Oligophosphorimidazolide reagents are presented that enable the conjugation of multiple phosphates to phosphopeptides, yielding derivatives with monodisperse phosphate chain lengths. The picture illustrates different peptides with varying phosphate chain lengths, bearing either a terminal protecting group or a free oligophosphate moiety.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 11","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202502765","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581686","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
Innentitelbild: In/Outside Catalytic Sites of the Pore Walls in One-Dimensional Covalent Organic Frameworks for Oxygen Reduction Reaction (Angew. Chem. 11/2025)
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502955
Shuai Yang, Zejin He, Xuewen Li, Bingbao Mei, Yifan Huang, Qing Xu, Zheng Jiang
{"title":"Innentitelbild: In/Outside Catalytic Sites of the Pore Walls in One-Dimensional Covalent Organic Frameworks for Oxygen Reduction Reaction (Angew. Chem. 11/2025)","authors":"Shuai Yang,&nbsp;Zejin He,&nbsp;Xuewen Li,&nbsp;Bingbao Mei,&nbsp;Yifan Huang,&nbsp;Qing Xu,&nbsp;Zheng Jiang","doi":"10.1002/ange.202502955","DOIUrl":"https://doi.org/10.1002/ange.202502955","url":null,"abstract":"<p>Pore channels play an essential role in the catalytic process. In their Research Article (e202418347), Zheng Jiang, Qing Xu, Yifan Huang, and co-workers precisely designed one-dimensional covalent organic frameworks to compare the catalytic sites inside or outside the pore walls to enlighten heterogeneous catalysis structural engineering.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 11","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202502955","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581699","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
Selective and Efficient Upcycling of Polyesters from Waste Plastic Blends Enabled by a Rationally Designed Manganese Pincer Catalyst
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502923
Dr. Yue Hu, Dr. Yanwei Gu, Yongjing Dong, Yiqing Wang, Juanfang Xu, Yingying Han, Dr. Chijian Zhang, Prof. Dr. Yinjun Xie
{"title":"Selective and Efficient Upcycling of Polyesters from Waste Plastic Blends Enabled by a Rationally Designed Manganese Pincer Catalyst","authors":"Dr. Yue Hu,&nbsp;Dr. Yanwei Gu,&nbsp;Yongjing Dong,&nbsp;Yiqing Wang,&nbsp;Juanfang Xu,&nbsp;Yingying Han,&nbsp;Dr. Chijian Zhang,&nbsp;Prof. Dr. Yinjun Xie","doi":"10.1002/ange.202502923","DOIUrl":"https://doi.org/10.1002/ange.202502923","url":null,"abstract":"<p>Herein, we report a new class of earth-abundant pincer manganese catalysts that not only enable the efficient conversion of single-component post-consumer polyesters with a turnover number (TON) of up to 5300, but more importantly, allow the selective upcycling of polyesters from waste plastic blends (e.g., nylon, PA; polyethylene, PE; polyurethane, PU; polyvinyl chloride, PVC; cotton) or contaminants such as pigment, aluminum, or glass into highly valuable oxygenated products under mild conditions. Detailed mechanistic studies combined with DFT calculations revealed that the exceptional efficiency of this protocol is due to the use of rationally designed quinaldine-based PNN<sup>H</sup>-type Mn complexes with an extended π-system and an N−H moiety on the side arm to simultaneously enhance the stability and reactivity of the catalyst. In addition, the incorporation of dual metal-ligand cooperation (MLC) relay catalysis more effectively facilitates the key steps of this transformation, including H<sub>2</sub> activation and hydrogen bond-assisted hydride transfer.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 14","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143762071","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
Rücktitelbild: Diastereoselective Polypseudorotaxane Formation with Planar Chiral Pillar[5]arenes via Co-crystallization Processes (Angew. Chem. 12/2025)
Angewandte Chemie Pub Date : 2025-02-14 DOI: 10.1002/ange.202502767
Kiichi Yasuzawa, Dr. Keisuke Wada, Prof. Dr. Shixin Fa, Prof. Dr. Yuuya Nagata, Dr. Kenichi Kato, Dr. Shunsuke Ohtani, Prof. Dr. Motohiro Mizuno, Prof. Dr. Tomoki Ogoshi
{"title":"Rücktitelbild: Diastereoselective Polypseudorotaxane Formation with Planar Chiral Pillar[5]arenes via Co-crystallization Processes (Angew. Chem. 12/2025)","authors":"Kiichi Yasuzawa,&nbsp;Dr. Keisuke Wada,&nbsp;Prof. Dr. Shixin Fa,&nbsp;Prof. Dr. Yuuya Nagata,&nbsp;Dr. Kenichi Kato,&nbsp;Dr. Shunsuke Ohtani,&nbsp;Prof. Dr. Motohiro Mizuno,&nbsp;Prof. Dr. Tomoki Ogoshi","doi":"10.1002/ange.202502767","DOIUrl":"https://doi.org/10.1002/ange.202502767","url":null,"abstract":"<p>Diastereoselective polypseudorotaxane formation via co-crystallization of stereodynamic planar chiral pillar[5]arene and polyethylene glycol is reported by Tomoki Ogoshi et al. in their Research Article (e202420115). In the image, the bracelet represents the polypseudorotaxane, with blue and red stones depicting the pS and pR forms of the pillar[5]arene ring, respectively. The crystals between the stones imply the crystallization method. As the number of stones increases, the possible combinations multiply, making selection more difficult, but ultimately, you will find the bracelet that suits you best.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 12","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202502767","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143639011","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
An Organic Crystalline Ternary Pseudo-Heterojunction with Contrasting Luminescent and Mechanical Properties Prepared by Thermotropic Phase Transition
Angewandte Chemie Pub Date : 2025-02-13 DOI: 10.1002/ange.202500151
Jianqun Qi, Dr. Linfeng Lan, Prof. Dr. Hongyu Zhang
{"title":"An Organic Crystalline Ternary Pseudo-Heterojunction with Contrasting Luminescent and Mechanical Properties Prepared by Thermotropic Phase Transition","authors":"Jianqun Qi,&nbsp;Dr. Linfeng Lan,&nbsp;Prof. Dr. Hongyu Zhang","doi":"10.1002/ange.202500151","DOIUrl":"https://doi.org/10.1002/ange.202500151","url":null,"abstract":"<p>Advancements in crystal engineering have enabled the precise tuning of the physical properties of organic crystals, thereby enhancing their potential in advanced optoelectronics. Here, we design an organic compound which crystallizes into distinct polymorphs with contrasting luminescent and mechanical behaviors. Controlled growth conditions yield flexible (Cry-<b>O</b>: orange fluorescence) and brittle (Cry-<b>Y</b>: yellow fluorescence) crystals which exhibit unique fluorescence shifts and reversible spectral changes between room and low temperatures, alongside unidirectional phase transitions upon thermal stimulation. The optical and mechanical differences between the polymorphs <b>O</b> and <b>Y</b> stem from their distinct molecular packing arrangements and intermolecular interactions. Notably, Cry-<b>O</b> undergoes sequential phase transitions upon heating to 98 and 132 °C, enabling the creation of a ternary “pseudo-heterojunction” structure, facilitating the integration of multiple functional phases into a single material. These findings not only enhance the understanding of structure–property relationships of organic materials but also demonstrate the potential of polymorphism-driven property tuning for optoelectronic devices, thermal management systems, and optical sensors.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 13","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143688714","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
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