Chemical Science最新文献_第9页

Electrolyte design weakens lithium-ion solvation for a fast-charging and long-cycling Si anode.

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-07 DOI: 10.1039/d4sc08125k

Min Li, Shuai Li, Dong Yan, Yuhao Ma, Xiaobin Niu, Liping Wang

{"title":"Electrolyte design weakens lithium-ion solvation for a fast-charging and long-cycling Si anode.","authors":"Min Li, Shuai Li, Dong Yan, Yuhao Ma, Xiaobin Niu, Liping Wang","doi":"10.1039/d4sc08125k","DOIUrl":"10.1039/d4sc08125k","url":null,"abstract":"Silicon (Si) is considered a promising anode material for next-generation lithium-ion batteries due to its high theoretical specific capacity and earth-abundancy. However, challenges such as significant volume expansion, unstable solid electrolyte interphase (SEI) formation in incompatible electrolytes, and slow lithium-ion transport lead to its poor cycling and rate performance. In this work, it is demonstrated that superior cyclability and rate capability of Si anodes can be achieved using ethyl fluoroacetate (EFA) and fluoroethylene carbonate (FEC) solvents with low binding energy with Li+ but with sufficiently high relative dielectric constants. By weakening the interaction between Li+ and the solvent, the energy barrier for the Li+ desolvation process is lowered, while ensuring the conductivity and diffusion of Li+. As a result, the silicon-carbon anode with the optimized electrolyte exhibits excellent cycling and rate performance, and can work reversibly with a high capacity of 1709.1 mAh g-1 that proceeds for over 250 cycles and retains 85.2% of its capacity at 0.2C. Furthermore, the Si/C‖LiFePO4 (LFP) full cell shows an extended service life of more than 500 cycles. This work offers valuable insights into the design of weakly solvating electrolytes for high-performance Si-based batteries.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11728059/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982659","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}

引用次数: 0

Correction: Radical ligand transfer: mechanism and reactivity governed by three-component thermodynamics

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-07 DOI: 10.1039/D4SC90254H

Zuzanna Wojdyla and Martin Srnec

引用次数: 0

Dibenzyl isophthalates as versatile hosts in room temperature phosphorescence host-guest systems.

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-07 DOI: 10.1039/d4sc07768g

Martin Molkenthin, Emanuel Hupf, Boris J Nachtsheim

引用次数: 0

Rapid (≤25 °C) cycloisomerization of anhydride-tethered triynes to benzynes - origin of a remarkable anhydride linker-induced rate enhancement.

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-07 DOI: 10.1039/d4sc07232d

Dorian S Sneddon, Paul V Kevorkian, Thomas R Hoye

{"title":"Rapid (≤25 °C) cycloisomerization of anhydride-tethered triynes to benzynes - origin of a remarkable anhydride linker-induced rate enhancement.","authors":"Dorian S Sneddon, Paul V Kevorkian, Thomas R Hoye","doi":"10.1039/d4sc07232d","DOIUrl":"https://doi.org/10.1039/d4sc07232d","url":null,"abstract":"The hexadehydro-Diels-Alder (HDDA) reaction is a cycloisomerization between a conjugated diyne and a tethered diynophile that generates ortho-benzyne derivatives. Considerable fundamental understanding of aryne reactivity has resulted from this body of research. The multi-yne cycloisomerization substrate is typically pre-formed and the (rate-limiting) closure of this diyne/diynophile pair to produce the isomeric benzyne generally requires thermal input, often requiring reaction temperatures of >100 °C and times of 16-48 h to achieve near-full conversion. We report here that diynoic acids can be dimerized and that the resulting substrate, having a 3-atom anhydride linker (i.e., O[double bond, length as m-dash]COC[double bond, length as m-dash]O), then undergoes HDDA cyclization within minutes at or below room temperature. This allows for the novel in situ assembly and cyclization of HDDA benzyne precursors in an operationally simple protocol. Experimental kinetic data along with DFT computations are used to identify the source of this surprisingly huge rate acceleration afforded by the anhydride linker: >107 faster than the analogous multi-yne having, instead, a CH2OCH2 ether linker.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11734507/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143000658","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}

引用次数: 0

In situ synthesis of degradable polymer prodrug nanoparticles.

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-07 DOI: 10.1039/d4sc07746f

Chen Zhu, Hannah Beauseroy, Julie Mougin, Maëlle Lages, Julien Nicolas

{"title":"In situ synthesis of degradable polymer prodrug nanoparticles.","authors":"Chen Zhu, Hannah Beauseroy, Julie Mougin, Maëlle Lages, Julien Nicolas","doi":"10.1039/d4sc07746f","DOIUrl":"https://doi.org/10.1039/d4sc07746f","url":null,"abstract":"The in situ synthesis of degradable polymer prodrug nanoparticles is still a challenge to be met, which would make it possible to remedy both the shortcomings of traditional formulation of preformed polymers (e.g., low nanoparticle concentrations) and those of the physical encapsulation of drugs (e.g., burst release and poor drug loadings). Herein, through the combination of radical ring-opening polymerization (rROP) and polymerization-induced self-assembly (PISA) under appropriate experimental conditions, we report the successful preparation of high-solid content, degradable polymer prodrug nanoparticles, exhibiting multiple drug moieties covalently linked to a degradable vinyl copolymer backbone. Such a rROPISA process relied on the chain extension of a biocompatible poly(ethylene glycol)-based solvophilic block with a mixture of lauryl methacrylate (LMA), cyclic ketene acetal (CKA) and drug-bearing methacrylic esters by reversible addition fragmentation chain transfer (RAFT) copolymerization at 20 wt% solid content. This novel approach was exemplified with two different CKA monomers and two different anticancer drugs, namely paclitaxel and gemcitabine, to demonstrate its versatility. After transferring to water, remarkably stable aqueous suspensions of core-degradable polymer prodrug nanoparticles, 56-225 nm in diameter, with tunable amounts of CKA units (7-26 mol%) and drug loadings of up to 33 wt% were obtained. The incorporation of ester groups in the copolymers was demonstrated by hydrolytic degradation of both the copolymers and the nanoparticles under accelerated conditions. The nanoparticles showed significant cytotoxicity against A549 cells, used as a lung cancer model. Fluorescence labeling of the solvophilic block also enabled effective monitoring of cell internalization by confocal microscopy, with potential for theranostic applications.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11733764/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143000948","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}

引用次数: 0

A two-dimensional fluorescence and chemiluminescence orthogonal probe for discriminating and quantifying similar proteins.

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-07 DOI: 10.1039/d4sc07714h

Juan Li, Xiuyan Zhao, Yutao Zhang, Yao Lu, Haoyun Xue, Dan Li, Qiang Liu, Chenxu Yan, Weijie Chi, Xingqing Xiao, Wei-Hong Zhu, Zhiqian Guo

{"title":"A two-dimensional fluorescence and chemiluminescence orthogonal probe for discriminating and quantifying similar proteins.","authors":"Juan Li, Xiuyan Zhao, Yutao Zhang, Yao Lu, Haoyun Xue, Dan Li, Qiang Liu, Chenxu Yan, Weijie Chi, Xingqing Xiao, Wei-Hong Zhu, Zhiqian Guo","doi":"10.1039/d4sc07714h","DOIUrl":"https://doi.org/10.1039/d4sc07714h","url":null,"abstract":"Given that proteins with minor variations in amino acid sequences cause distinct functional outcomes, identifying and quantifying similar proteins is crucial, but remains a long-standing challenge. Herein, we present a two-dimensional orthogonal fluorescence and chemiluminescence design strategy for the probe DCM-SA, which is sequentially activated by albumin-mediated hydrolysis, exhibiting light-up fluorescence and photo-induced cycloaddition generating chemiluminescence, enabling orthogonal signal amplification for discrimination of subtle differences between similar proteins. By orthogonalizing these dual-mode signals, a two-dimensional work curve of fluorescence and chemiluminescence is established to distinguish and quantify similar proteins HSA and BSA. Importantly, the dual-mode signals of DCM-SA exhibit contrary incremental trends towards HSA and BSA. Molecular docking and femtosecond transient absorbance spectroscopy reveal that the lower K D value of DCM-SA with HSA and the longer excited-state lifetime of DCM-SA with BSA underlie the distinct dual-mode responses. Using two-dimensional orthogonal signals, for the first time, we precisely measure the HSA/BSA ratio in mixed serum. This method facilitates rapid blood source identification and trace HSA quantitation in human urine. Our two-dimensional orthogonal amplification approach offers a powerful tool for distinguishing and quantifying subtle differences among highly similar proteins, demonstrating great potential for both basic life science research and clinical applications.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11744679/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143000957","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}

引用次数: 0

A focus on phosphinophosphination of apolar bonds by a structurally constrained P–P bonded system

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-06 DOI: 10.1039/D4SC90251C

Tyler J. Hannah and Saurabh S. Chitnis

引用次数: 0

A focus on microporous perovskites: new tricks for an old dog

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-06 DOI: 10.1039/D4SC90244K

Miriam Segundo-Osorio, A. Paulina Gómora-Figueroa and Diego Solis-Ibarra

引用次数: 0

Chemical modulation and defect engineering in high-performance GeTe-based thermoelectrics

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-06 DOI: 10.1039/D4SC06615D

Yilin Jiang, Jincheng Yu, Hezhang Li, Hua-Lu Zhuang and Jing-Feng Li

{"title":"Chemical modulation and defect engineering in high-performance GeTe-based thermoelectrics","authors":"Yilin Jiang, Jincheng Yu, Hezhang Li, Hua-Lu Zhuang and Jing-Feng Li","doi":"10.1039/D4SC06615D","DOIUrl":"10.1039/D4SC06615D","url":null,"abstract":"Thermoelectric technology plays an important role in developing sustainable clean energy and reducing carbon emissions, offering new opportunities to alleviate current energy and environmental crises. Nowadays, GeTe has emerged as a highly promising thermoelectric candidate for mid-temperature applications, due to its remarkable thermoelectric figure of merit (ZT) of 2.7. This review presents a thorough overview of the advancements in GeTe thermoelectric materials, meticulously detailing the crystal structure, chemical bonding characteristics, band structure, and phonon dynamics to elucidate the underlying mechanisms that contribute to their exceptional performance. Moreover, the phase transition in GeTe introduces unique degrees of freedom that enable multiple pathways for property optimization. In terms of electrical properties, noticeable enhancement can be realized through strategies such as band structure modulation, carrier concentration engineering, and vacancy engineering. For phonon transport properties, by incorporating defect structures with varying dimensions and constructing multi-scale hierarchical architectures, phonons can be effectively scattered across different wavelengths. Additionally, we provide a summary of current research on devices and modules of GeTe. This review encapsulates historical progress while projecting future development trends that will facilitate the practical application of GeTe in alignment with environmentally sustainable objectives.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" 4","pages":" 1617-1651"},"PeriodicalIF":7.6,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/sc/d4sc06615d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929688","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}

引用次数: 0

Correction: Reconstructing the phase of vanadium oxides enables redox-catalysis manipulated reversible sulfur conversion for stable Zn–S batteries

IF 7.6 1区化学

Chemical Science Pub Date : 2025-01-06 DOI: 10.1039/D4SC90253J

Hao Luo, Fan Li, Mingli Wang, Shang Sun, Min Zhou, Wenjing Zhang, Hengrui Guo, Xueyin Su, Xiaolong Li and Lina Ma

引用次数: 0