Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.10.002
Dongsheng Mao , Wenxing Li , Xueliang Liu , Jingqi Chen , Dali Wei , Lei Luo , Qianqin Yuan , Yu Yang , Xiaoli Zhu , Weihong Tan
Enzymes with ingenious structures and diverse functions are crucial for biomedical applications but face challenges like instability, limited targetability, and delivery complexity. We developed core-shell DNA-enzyme conjugates using rolling circle amplification (RCA), creating RCA-based DNA-enzyme nanostructure (RCA-DEN) for efficient enzyme immobilization and functionalization. RCA-DEN, characterized by densely packed nucleic acids and negligible disruption of enzyme activity, increases the stability of enzymes and nucleic acids while reducing technical difficulties, making it a versatile platform for diverse biomedical applications. This approach facilitates the modular customization of enzymes and the incorporation of functionalities such as aptamers and DNAzymes. The efficacy of RCA-DEN has been demonstrated in several areas, including selective catalysis, cascade catalysis, dynamic monitoring of intracellular chemical processes, and synergistic therapeutic interventions against tumors. Overall, this work provides a new perspective on enzyme immobilization and functionalization, paving the way for broader biomedical applications of enzymes.
具有巧妙结构和多样化功能的酶对生物医学应用至关重要，但也面临着不稳定性、靶向性有限和传递复杂性等挑战。我们利用滚动圆扩增（RCA）技术开发了核壳DNA-酶共轭物，形成了基于RCA的DNA-酶纳米结构（RCA-DEN），实现了酶的高效固定和功能化。RCA-DEN 的特点是核酸密集包装，对酶活性的干扰微乎其微，在增加酶和核酸稳定性的同时降低了技术难度，使其成为一个可用于多种生物医学应用的多功能平台。这种方法有利于对酶进行模块化定制，并加入适配体和 DNA 酶等功能。RCA-DEN 的功效已在多个领域得到证实，包括选择性催化、级联催化、细胞内化学过程的动态监测以及针对肿瘤的协同治疗干预。总之，这项工作为酶的固定化和功能化提供了一个新的视角，为酶更广泛的生物医学应用铺平了道路。
{"title":"Rolling-circle-amplification-based DNA-enzyme nanostructure for immobilization and functionalization of enzymes","authors":"Dongsheng Mao , Wenxing Li , Xueliang Liu , Jingqi Chen , Dali Wei , Lei Luo , Qianqin Yuan , Yu Yang , Xiaoli Zhu , Weihong Tan","doi":"10.1016/j.chempr.2024.10.002","DOIUrl":"10.1016/j.chempr.2024.10.002","url":null,"abstract":"<div><div>Enzymes with ingenious structures and diverse functions are crucial for biomedical applications but face challenges like instability, limited targetability, and delivery complexity. We developed core-shell DNA-enzyme conjugates using rolling circle amplification (RCA), creating RCA-based DNA-enzyme nanostructure (RCA-DEN) for efficient enzyme immobilization and functionalization. RCA-DEN, characterized by densely packed nucleic acids and negligible disruption of enzyme activity, increases the stability of enzymes and nucleic acids while reducing technical difficulties, making it a versatile platform for diverse biomedical applications. This approach facilitates the modular customization of enzymes and the incorporation of functionalities such as aptamers and DNAzymes. The efficacy of RCA-DEN has been demonstrated in several areas, including selective catalysis, cascade catalysis, dynamic monitoring of intracellular chemical processes, and synergistic therapeutic interventions against tumors. Overall, this work provides a new perspective on enzyme immobilization and functionalization, paving the way for broader biomedical applications of enzymes.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102335"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536375","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}
Enzymes are highly efficient, chemoselective, and sustainable biocatalysts, standing out as eco-friendly tools to advance the circular plastics economy. Herein, we explored enzymatic reactions of poly(ε-caprolactone)-poly(urethane) (PCL-PUs) in organic solvent under different reaction conditions using Novozym 435 (immobilized lipase) as the enzyme. PCL-PUs with triacetylated γ-cyclodextrin (TAcγCD)-based movable crosslinks (PCL-γCD-PU) not only exhibited excellent mechanical properties due to effective energy dissipation, but also efficient enzymatic degradation that was optimized for increases in TAcγCD content. Under reaction time control, molecular weight and mechanical properties of PCL-γCD-PU were enhanced by a novel enzymatic reinforcement strategy. Without sorting, the degraded products are versatile resources that can be enzymatically closed-loop recycled by switching reaction concentration or enzymatically upcycled into value-added polymers by mixing with selective substrates. The facile polymer structure design combined with enzymatic reactions is expected to provide a broad approach for toughening various polymeric materials and advancing their development as sustainable resources.
{"title":"Exploring enzymatic degradation, reinforcement, recycling, and upcycling of poly(ester)-poly(urethane) with movable crosslinks","authors":"Jiaxiong Liu , Ryohei Ikura , Kenji Yamaoka , Akihide Sugawara , Yuya Takahashi , Bunsho Kure , Naomi Takenaka , Junsu Park , Hiroshi Uyama , Yoshinori Takashima","doi":"10.1016/j.chempr.2024.09.026","DOIUrl":"10.1016/j.chempr.2024.09.026","url":null,"abstract":"<div><div>Enzymes are highly efficient, chemoselective, and sustainable biocatalysts, standing out as eco-friendly tools to advance the circular plastics economy. Herein, we explored enzymatic reactions of poly(<em>ε</em>-caprolactone)-poly(urethane) (PCL-PUs) in organic solvent under different reaction conditions using Novozym 435 (immobilized lipase) as the enzyme. PCL-PUs with triacetylated γ-cyclodextrin (TAcγCD)-based movable crosslinks (PCL-γCD-PU) not only exhibited excellent mechanical properties due to effective energy dissipation, but also efficient enzymatic degradation that was optimized for increases in TAcγCD content. Under reaction time control, molecular weight and mechanical properties of PCL-γCD-PU were enhanced by a novel enzymatic reinforcement strategy. Without sorting, the degraded products are versatile resources that can be enzymatically closed-loop recycled by switching reaction concentration or enzymatically upcycled into value-added polymers by mixing with selective substrates. The facile polymer structure design combined with enzymatic reactions is expected to provide a broad approach for toughening various polymeric materials and advancing their development as sustainable resources.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102327"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.102389
Ali Omidkar , Avinash Alagumalai , Razieh Es’haghian , Hua Song
Producing clean, high-calorific fuels is challenging because of poor bio-oil quality, low yields, high costs, and environmental impacts. A new upgrading plant using methane instead of hydrogen offers a promising solution to address these issues effectively and sustainably.
{"title":"Producing economically viable renewable diesel by upgrading organic solid waste with natural gas","authors":"Ali Omidkar , Avinash Alagumalai , Razieh Es’haghian , Hua Song","doi":"10.1016/j.chempr.2024.102389","DOIUrl":"10.1016/j.chempr.2024.102389","url":null,"abstract":"<div><div>Producing clean, high-calorific fuels is challenging because of poor bio-oil quality, low yields, high costs, and environmental impacts. A new upgrading plant using methane instead of hydrogen offers a promising solution to address these issues effectively and sustainably.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102389"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987071","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}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2025.102443
Xin Jiang , Yunyan Qiu
The large-scale and sustainable production of high-quality graphene and its derivatives encounters significant challenges. Recently in Nature Sustainability, Wang et al. reported an economical and green approach for the preparation of reduced graphene oxide from biomass waste. This method is highlighted by its room-temperature operation and minimal energy consumption.
{"title":"Biomass waste valorization: Ambient synthesis of reduced graphene oxide","authors":"Xin Jiang , Yunyan Qiu","doi":"10.1016/j.chempr.2025.102443","DOIUrl":"10.1016/j.chempr.2025.102443","url":null,"abstract":"<div><div>The large-scale and sustainable production of high-quality graphene and its derivatives encounters significant challenges. Recently in <em>Nature Sustainability</em>, Wang et al. reported an economical and green approach for the preparation of reduced graphene oxide from biomass waste. This method is highlighted by its room-temperature operation and minimal energy consumption.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102443"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143072042","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}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2025.102454
Xianbao Li , Qi Li , Junbai Li
In the January issue of Chem, Kriebisch et al. presented a peptide-assembled nanoribbon capable of mimicking flagellar motion. The nanoribbon exhibits a novel movement mechanism wherein motion is induced by a chemically powered morphological transition. This work could pave the way for the development of advanced supramolecular nanomachines.
{"title":"Morphological-transition-induced motion","authors":"Xianbao Li , Qi Li , Junbai Li","doi":"10.1016/j.chempr.2025.102454","DOIUrl":"10.1016/j.chempr.2025.102454","url":null,"abstract":"<div><div>In the January issue of <em>Chem</em>, Kriebisch et al. presented a peptide-assembled nanoribbon capable of mimicking flagellar motion. The nanoribbon exhibits a novel movement mechanism wherein motion is induced by a chemically powered morphological transition. This work could pave the way for the development of advanced supramolecular nanomachines.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102454"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124917","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}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2025.102435
Yuanbo Liu , Haohong Duan
Functionalizing conventional polyvinyl chloride (PVC) into leach-resistant PVC with a well-defined structure is challenging owing to uncontrollable side reactions such as elimination and chain scission. Recently in Chem, Sevov and coworkers developed an electrocatalytic strategy for covalently grafting plasticizers into PVC backbone, endowing the material with new properties.
{"title":"Electrocatalysis enables polyvinyl chloride functionalization","authors":"Yuanbo Liu , Haohong Duan","doi":"10.1016/j.chempr.2025.102435","DOIUrl":"10.1016/j.chempr.2025.102435","url":null,"abstract":"<div><div>Functionalizing conventional polyvinyl chloride (PVC) into leach-resistant PVC with a well-defined structure is challenging owing to uncontrollable side reactions such as elimination and chain scission. Recently in <em>Chem</em>, Sevov and coworkers developed an electrocatalytic strategy for covalently grafting plasticizers into PVC backbone, endowing the material with new properties.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102435"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077416","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}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.09.018
Tristan H. Borchers , Filip Topić , Mihails Arhangelskis , Michael Ferguson , Cameron B. Lennox , Patrick A. Julien , Tomislav Friščić
Low-frequency Raman, also known as terahertz-Raman (THz-Raman), spectroscopy offers a laboratory benchtop-based alternative to synchrotron X-ray diffraction for real-time, in situ monitoring of ball-milling mechanochemical reactions. Although direct monitoring of the long-range structure of materials during mechanochemical reactions is generally challenging by conventional Raman spectroscopy, and typically requires synchrotron X-ray diffraction, here we use THz-Raman spectroscopy to monitor mechanosynthesis of cocrystals, stoichiomorphs, and polymorphs, detect multi-step sequences, and discover solid-state phases in systems difficult to differentiate using fingerprint-region Raman spectroscopy—all through real-time observation of changes in lattice vibrational models. The methodology is augmented by periodic density functional theory (DFT), which enables structural interpretation of spectroscopic changes, notably the identification of THz-Raman bands associated with halogen bond transformations. Simultaneous monitoring of mechanochemical processes in both the fingerprint and low-frequency Raman regions enables real-time observation of changes to extended as well as molecular structure during milling, in a single laboratory benchtop experiment, without synchrotron radiation.
低频拉曼（又称太赫兹-拉曼，THz-Raman）光谱法为实验室台式同步辐射 X 射线衍射法提供了一种替代方法，可用于实时、原位监测球磨机械化学反应。虽然在机械化学反应过程中直接监测材料的长程结构通常是传统拉曼光谱法所无法实现的，而且通常需要同步辐射 X 射线衍射法，但在这里，我们使用太赫兹-拉曼光谱法监测共晶体、共晶和多晶体的机械合成，检测多步序列，并在使用指纹区拉曼光谱法难以区分的系统中发现固态相--所有这些都是通过实时观测晶格振动模型的变化实现的。周期性密度泛函理论（DFT）对该方法进行了增强，从而能够对光谱变化进行结构解释，特别是识别与卤素键转化相关的太赫兹-拉曼带。同时监测指纹区和低频拉曼区的机械化学过程，可在实验室台式实验中实时观察研磨过程中扩展分子结构的变化，而无需同步辐射。
{"title":"Terahertz-Raman spectroscopy for in situ benchtop monitoring of changes to extended, supramolecular structure in milling mechanochemistry","authors":"Tristan H. Borchers , Filip Topić , Mihails Arhangelskis , Michael Ferguson , Cameron B. Lennox , Patrick A. Julien , Tomislav Friščić","doi":"10.1016/j.chempr.2024.09.018","DOIUrl":"10.1016/j.chempr.2024.09.018","url":null,"abstract":"<div><div>Low-frequency Raman, also known as terahertz-Raman (THz-Raman), spectroscopy offers a laboratory benchtop-based alternative to synchrotron X-ray diffraction for real-time, <em>in situ</em> monitoring of ball-milling mechanochemical reactions. Although direct monitoring of the long-range structure of materials during mechanochemical reactions is generally challenging by conventional Raman spectroscopy, and typically requires synchrotron X-ray diffraction, here we use THz-Raman spectroscopy to monitor mechanosynthesis of cocrystals, stoichiomorphs, and polymorphs, detect multi-step sequences, and discover solid-state phases in systems difficult to differentiate using fingerprint-region Raman spectroscopy—all through real-time observation of changes in lattice vibrational models. The methodology is augmented by periodic density functional theory (DFT), which enables structural interpretation of spectroscopic changes, notably the identification of THz-Raman bands associated with halogen bond transformations. Simultaneous monitoring of mechanochemical processes in both the fingerprint and low-frequency Raman regions enables real-time observation of changes to extended as well as molecular structure during milling, in a single laboratory benchtop experiment, without synchrotron radiation.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102319"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489464","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.08.019
Eunhye Hwang , Unhyeok Jo , Jiyeon Kim , Deok-Ho Roh , Seung Chan Kim , Minseok Kim , Hyun-Chul Ki , Wonyoung Choe , Jun Yeob Lee , Tae-Hyuk Kwon
Despite the emergence of interlayers with high triplet energies (T1) to stabilize blue phosphorescent organic light-emitting diodes (PhOLEDs), a limited understanding of their molecular structures poses a challenge in preventing triplet exciton leakage while maintaining charge balance. Here, we report a rational design strategy for interlayers aimed at concurrently controlling T1 and molecular arrangements conducive to charge transport. Four interlayer materials having high T1 (∼3.0 eV) are developed as electron-blocking materials (EBMs), utilizing asymmetric orthogonal geometries with varying torsion angles and dipole moments. X-ray crystallographic analyses reveal that the EBM, featuring the most asymmetric charge distributions, exhibits a herringbone packing and a face-on orientation through dipole-induced anisotropic interactions, thereby promoting hole transport. The power efficiency and operational lifetime of the corresponding blue PhOLEDs increase by 24% and 21%, respectively, compared with a conventional EBM. This study offers extensive insights into designing interlayers with versatile applicability in optoelectronics harnessing triplets.
{"title":"Anisotropy-guided interface molecular engineering for stable blue electroluminescence","authors":"Eunhye Hwang , Unhyeok Jo , Jiyeon Kim , Deok-Ho Roh , Seung Chan Kim , Minseok Kim , Hyun-Chul Ki , Wonyoung Choe , Jun Yeob Lee , Tae-Hyuk Kwon","doi":"10.1016/j.chempr.2024.08.019","DOIUrl":"10.1016/j.chempr.2024.08.019","url":null,"abstract":"<div><div>Despite the emergence of interlayers with high triplet energies (T<sub>1</sub>) to stabilize blue phosphorescent organic light-emitting diodes (PhOLEDs), a limited understanding of their molecular structures poses a challenge in preventing triplet exciton leakage while maintaining charge balance. Here, we report a rational design strategy for interlayers aimed at concurrently controlling T<sub>1</sub> and molecular arrangements conducive to charge transport. Four interlayer materials having high T<sub>1</sub> (∼3.0 eV) are developed as electron-blocking materials (EBMs), utilizing asymmetric orthogonal geometries with varying torsion angles and dipole moments. X-ray crystallographic analyses reveal that the EBM, featuring the most asymmetric charge distributions, exhibits a herringbone packing and a face-on orientation through dipole-induced anisotropic interactions, thereby promoting hole transport. The power efficiency and operational lifetime of the corresponding blue PhOLEDs increase by 24% and 21%, respectively, compared with a conventional EBM. This study offers extensive insights into designing interlayers with versatile applicability in optoelectronics harnessing triplets.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102296"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142246235","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}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.09.005
Rui Qiao , Yan Zhao , Shijie Zhou , Huijun Zhang , Fuzhu Liu , Tianhong Zhou , Baoyu Sun , Hao Fan , Chao Li , Yanhua Zhang , Feng Liu , Xiangdong Ding , Jang Wook Choi , Ali Coskun , Jiangxuan Song
Electrolyte engineering plays a critical role in enabling lithium (Li) metal batteries. However, the simultaneous realization of anion-rich solvation structure and high ionic conductivity of electrolytes via solvation structure design remains challenging. Here, we report a low-cost, non-fluorinated electrolyte with a micelle-like solvation structure by introducing amphiphilic n-butyl methyl ether (MNBE) into Li bis(fluorosulfonyl)imide (LiFSI)/1,2-dimethoxyethane (DME) for stable Li metal batteries (LMBs). MNBE can effectively promote Li+-FSI− coordination through steric crowding. Meanwhile, the inert alkyl chains of MNBE can mitigate the reaction between electrolyte and Li metal due to their lithiophobicity. Specifically, the micelle-like, non-fluorinated electrolyte exhibits an ionic conductivity as high as 12.55 mS cm−1, and its anion-rich solvation structure promotes the formation of LiF-rich solid-electrolyte interphase. We constructed a 7.3 Ah Li||NMC811 pouch cell employing this electrolyte under harsh conditions, exhibiting ultra-high specific energy of 503.7 Wh kg−1 with impressive cycling stability of 84.1% capacity retention after 100 cycles.
{"title":"Non-fluorinated electrolytes with micelle-like solvation for ultra-high-energy-density lithium metal batteries","authors":"Rui Qiao , Yan Zhao , Shijie Zhou , Huijun Zhang , Fuzhu Liu , Tianhong Zhou , Baoyu Sun , Hao Fan , Chao Li , Yanhua Zhang , Feng Liu , Xiangdong Ding , Jang Wook Choi , Ali Coskun , Jiangxuan Song","doi":"10.1016/j.chempr.2024.09.005","DOIUrl":"10.1016/j.chempr.2024.09.005","url":null,"abstract":"<div><div>Electrolyte engineering plays a critical role in enabling lithium (Li) metal batteries. However, the simultaneous realization of anion-rich solvation structure and high ionic conductivity of electrolytes via solvation structure design remains challenging. Here, we report a low-cost, non-fluorinated electrolyte with a micelle-like solvation structure by introducing amphiphilic n-butyl methyl ether (MNBE) into Li bis(fluorosulfonyl)imide (LiFSI)/1,2-dimethoxyethane (DME) for stable Li metal batteries (LMBs). MNBE can effectively promote Li<sup>+</sup>-FSI<sup>−</sup> coordination through steric crowding. Meanwhile, the inert alkyl chains of MNBE can mitigate the reaction between electrolyte and Li metal due to their lithiophobicity. Specifically, the micelle-like, non-fluorinated electrolyte exhibits an ionic conductivity as high as 12.55 mS cm<sup>−1</sup>, and its anion-rich solvation structure promotes the formation of LiF-rich solid-electrolyte interphase. We constructed a 7.3 Ah Li||NMC811 pouch cell employing this electrolyte under harsh conditions, exhibiting ultra-high specific energy of 503.7 Wh kg<sup>−1</sup> with impressive cycling stability of 84.1% capacity retention after 100 cycles.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102306"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142369578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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