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学者姓名:林立森
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Real-time monitoring of hydroxyl radical (& sdot;OH) generation is crucial for both the efficacy and safety of chemodynamic therapy (CDT). Although & sdot;OH probe-integrated CDT agents can track & sdot;OH production by themselves, they often require complicated synthetic procedures and suffer from self-consumption of & sdot;OH. Here, we report the facile fabrication of a self-monitored chemodynamic agent (denoted as Fc-CD-AuNCs) by incorporating ferrocene (Fc) into beta-cyclodextrin (CD)-functionalized gold nanoclusters (AuNCs) via host-guest molecular recognition. The water-soluble CD served not only as a capping agent to protect AuNCs but also as a macrocyclic host to encapsulate and solubilize hydrophobic Fc guest with high Fenton reactivity for in vivo CDT applications. Importantly, the encapsulated Fc inside CD possessed strong electron-donating ability to effectively quench the second near-infrared (NIR-II) fluorescence of AuNCs through photoinduced electron transfer. After internalization of Fc-CD-AuNCs by cancer cells, Fenton reaction between redox-active Fc quencher and endogenous hydrogen peroxide (H2O2) caused Fc oxidation and subsequent NIR-II fluorescence recovery, which was accompanied by the formation of cytotoxic & sdot;OH and therefore allowed Fc-CD-AuNCs to in situ self-report & sdot;OH generation without undesired & sdot;OH consumption. Such a NIR-II fluorescence-monitored CDT enabled the use of renal-clearable Fc-CD-AuNCs for efficient tumor growth inhibition with minimal side effects in vivo. A NIR-II fluorescence-monitored chemodynamic therapy agent (Fc-CD-AuNCs) is prepared by integrating ferrocene (Fc) into beta-cyclodextrin-functionalized gold nanoclusters via host-guest interaction. In addition to producing & sdot;OH, Fenton reaction between redox-active Fc quencher and H2O2 causes Fc oxidation and consequent NIR-II fluorescence recovery, allowing renal-clearable Fc-CD-AuNCs to self-monitor & sdot;OH formation without undesired & sdot;OH consumption.image
Keyword :
Antitumor Agents Antitumor Agents Chemodynamic Therapy Chemodynamic Therapy Ferrocene Ferrocene Host-Guest Systems Host-Guest Systems NIR-II Fluorescence NIR-II Fluorescence
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GB/T 7714 | Yu, Meili , Ye, Zhuangjie , Liu, Siqin et al. Redox-Active Ferrocene Quencher-Based Supramolecular Nanomedicine for NIR-II Fluorescence-Monitored Chemodynamic Therapy [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (10) . |
MLA | Yu, Meili et al. "Redox-Active Ferrocene Quencher-Based Supramolecular Nanomedicine for NIR-II Fluorescence-Monitored Chemodynamic Therapy" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 10 (2024) . |
APA | Yu, Meili , Ye, Zhuangjie , Liu, Siqin , Zhu, Yang , Niu, Xuegang , Wang, Jun et al. Redox-Active Ferrocene Quencher-Based Supramolecular Nanomedicine for NIR-II Fluorescence-Monitored Chemodynamic Therapy . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (10) . |
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Chemodynamic therapy (CDT) is a potential cancer treatment strategy, which relies on Fenton chemistry to transform hydrogen peroxide (H2O2) into highly cytotoxic reactive oxygen species (ROS) for tumor growth suppression. Although overproduced H2O2 in cancerous tissues makes CDT a feasible and specific tumor therapeutic modality, the treatment outcomes of traditional chemodynamic agents still fall short of expectations. Reprogramming cellular metabolism is one of the hallmarks of tumors, which not only supports unrestricted proliferative demands in cancer cells, but also mediates the resistance of tumor cells against many antitumor modalities. Recent discoveries have revealed that various cellular metabolites including H2O2, iron, lactate, glutathione, and lipids have distinct effects on CDT efficiency. In this perspective, we intend to provide a comprehensive summary of how different endogenous molecules impact Fenton chemistry for a deep understanding of mechanisms underlying endogenous regulation-enhanced CDT. Moreover, we point out the current challenges and offer our outlook on the future research directions in this field. We anticipate that exploring CDT through manipulating metabolism will yield significant advancements in tumor treatment. A comprehensive summary of how different endogenous molecules' metabolic processes (including H2O2, iron, lactate, GSH, and lipid metabolisms) impact Fenton chemistry is provided in this perspective for advancing chemodynamic therapy against cancer.
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GB/T 7714 | Wang, Jun , Liu, Yina , Cui, Tingting et al. Current progress in the regulation of endogenous molecules for enhanced chemodynamic therapy [J]. | CHEMICAL SCIENCE , 2024 , 15 (26) : 9915-9926 . |
MLA | Wang, Jun et al. "Current progress in the regulation of endogenous molecules for enhanced chemodynamic therapy" . | CHEMICAL SCIENCE 15 . 26 (2024) : 9915-9926 . |
APA | Wang, Jun , Liu, Yina , Cui, Tingting , Yang, Huanghao , Lin, Lisen . Current progress in the regulation of endogenous molecules for enhanced chemodynamic therapy . | CHEMICAL SCIENCE , 2024 , 15 (26) , 9915-9926 . |
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Traditional cancer chemotherapy suffers from low efficacy and severe side effects, limiting its use as a first-line treatment. To address this issue, we investigated a novel way to induce lipid peroxidation (LPO), which plays an essential role in ferroptosis and may be useful against cancer cells and tumors. In this study, a pH-responsive synergistic cancer therapy nanoplatform was prepared using CaCO3 co-loaded with oleanolic acid (OA) and lipoxygenase (LOX), resulting in the formation OLCaP NP. This nanoplatform exhibited good drug release properties in an acidic tumor environment owing to the presence of CaCO3. As a result of acidic stimulation at tumor sites, the OLCaP NP released OA and LOX. OA, a chemotherapeutic drug with anticancer activity, is already known to promote the apoptosis of cancer cells, and LOX is a natural enzyme that catalyzes the oxidation of polyunsaturated fatty acids, leading to the accumulation of lipid peroxides and promoting the apoptosis of cancer cells. More importantly, OA upregulated the expression of acyl-coenzyme A synthetase long-chain family member 4 (ACSL4), which promoted enzyme-mediated LPO. Based on our combined chemotherapy and nanocatalytic therapy, the OLCaP NP not only had remarkable antitumor ability but also upregulated ACSL4 expression, allowing further amplification of LPO to inhibit tumor growth. These findings demonstrate the potential of this nanoplatform to enhance the therapeutic efficacy against tumors by inducing oxidative stress and disrupting lipid metabolism, highlighting its clinical potential for improved cancer treatment. Statement of significance: This study presents a novel nanoplatform that combines oleanolic acid (OA), a chemotherapeutic drug, and lipoxygenase (LOX), which oxidizes polyunsaturated fatty acids to trigger apoptosis, for targeted cancer therapy. Unlike traditional treatments, our nanoplatform exhibits pH-responsive drug release, specifically in acidic tumor environments. This innovation enhances the therapeutic effects of OA and LOX, upregulating acyl-CoA synthetase long-chain family member 4 expression and amplifying lipid peroxidation to promote tumor cell apoptosis. Our findings significantly advance the existing literature by demonstrating a synergistic approach that combines chemotherapy and nanocatalytic therapy. The scientific impact of this work lies in its potential to improve cancer treatment efficacy and specificity, offering a promising strategy for clinical applications and future research in cancer therapy. © 2024 Acta Materialia Inc.
Keyword :
Double emulsion Double emulsion Lipid peroxidation Lipid peroxidation Mitochondrial damage Mitochondrial damage Nanocatalytic tumor therapy Nanocatalytic tumor therapy
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GB/T 7714 | Zhuge, X. , Tang, R. , Jiang, Y. et al. A multifunctional nanoplatform for chemotherapy and nanocatalytic synergistic cancer therapy achieved by amplified lipid peroxidation [J]. | Acta Biomaterialia , 2024 , 184 : 419-430 . |
MLA | Zhuge, X. et al. "A multifunctional nanoplatform for chemotherapy and nanocatalytic synergistic cancer therapy achieved by amplified lipid peroxidation" . | Acta Biomaterialia 184 (2024) : 419-430 . |
APA | Zhuge, X. , Tang, R. , Jiang, Y. , Lin, L. , Xi, D. , Yang, H. . A multifunctional nanoplatform for chemotherapy and nanocatalytic synergistic cancer therapy achieved by amplified lipid peroxidation . | Acta Biomaterialia , 2024 , 184 , 419-430 . |
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Radiodynamic therapy that employs X-rays to trigger localized reactive oxygen species (ROS) generation can tackle the tissue penetration issue of phototherapy. Although calcium tungstate (CaWO4) shows great potential as a radiodynamic agent benefiting from its strong X-ray absorption and the ability to generate electron-hole (e(-)-h(+)) pairs, slow charge carrier transfer and fast e(-)-h(+) recombination greatly limit its ROS-generating performance. Herein, via a one-pot wet-chemical method, oxygen vacancy-rich amorphous/crystalline heterophase CaWO4 nanoparticles (Ov-a/c-CaWO4 NPs) with enhanced radiodynamic effect are synthesized for radiodynamic-immunotherapy of cancer. The phase composition and oxygen vacancy content of CaWO4 can be easily tuned by adjusting the solvothermal temperature. More intriguingly, the amorphous/crystalline interfaces and abundant oxygen vacancies accelerate charge carrier transfer and suppress e(-)-h(+) recombination, respectively, enabling synergistically improved ROS production from X-ray-irradiated Ov-a/c-CaWO4 NPs. In addition to directly inducing oxidative damage of cancer cells, radiodynamic generation of ROS also boosts immunogenic cell death to provoke a systemic antitumor immune response, thereby allowing the inhibition of both primary and distant tumors as well as cancer metastasis. This study establishes a synergistic enhancement strategy involving the integration of phase and defect engineering to improve the ROS generation capacity of radiodynamic-immunotherapeutic anticancer nanoagents.
Keyword :
CaWO4 nanoparticles CaWO4 nanoparticles enhanced radiodynamic effect enhanced radiodynamic effect heterophase heterophase oxygen vacancies oxygen vacancies radiodynamic-immunotherapy radiodynamic-immunotherapy
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GB/T 7714 | Peng, Shanshan , Chen, Zhen , Wang, Jun et al. One-Pot Synthesis of Oxygen Vacancy-Rich Amorphous/Crystalline Heterophase CaWO4 Nanoparticles for Enhanced Radiodynamic-Immunotherapy [J]. | ADVANCED SCIENCE , 2024 , 12 (7) . |
MLA | Peng, Shanshan et al. "One-Pot Synthesis of Oxygen Vacancy-Rich Amorphous/Crystalline Heterophase CaWO4 Nanoparticles for Enhanced Radiodynamic-Immunotherapy" . | ADVANCED SCIENCE 12 . 7 (2024) . |
APA | Peng, Shanshan , Chen, Zhen , Wang, Jun , Yu, Meili , Niu, Xuegang , Cui, Tingting et al. One-Pot Synthesis of Oxygen Vacancy-Rich Amorphous/Crystalline Heterophase CaWO4 Nanoparticles for Enhanced Radiodynamic-Immunotherapy . | ADVANCED SCIENCE , 2024 , 12 (7) . |
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As a rising generation of nanozymes, single atom enzymes show significant promise for cancer therapy, due to their maximum atom utilization efficiency and well-defined electronic structures. However, it remains a tremendous challenge to precisely produce a heteroatom-doped single atom enzyme with an expected coordination environment. Herein, we develop an anion exchange strategy for precisely controlled production of an edge-rich sulfur (S)-and nitrogen (N)-decorated nickel single atom enzyme (S-N/Ni PSAE). In particular, sulfurized S-N/Ni PSAE exhibits stronger peroxidase-like and glutathione oxidase-like activities than the nitrogen-monodoped nickel single atom enzyme, which is attributed to the vacancies and defective sites of sulfurized nitrogen atoms. Moreover, both in vitro and in vivo results demonstrate that, compared with nitrogen-monodoped N/Ni PSAE, sulfurized S-N/Ni PSAE more effectively triggers ferroptosis of tumor cells via inactivating glutathione peroxidase 4 and inducing lipid peroxidation. This study highlights the enhanced catalytic efficacy of a polynary heteroatom-doped single atom enzyme for ferroptosis-based cancer therapy.
Keyword :
ferroptosis ferroptosis heteroatom doping heteroatom doping lipid peroxidation lipid peroxidation single atom enzyme single atom enzyme tumor therapy tumor therapy
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GB/T 7714 | Zhu, Yang , Wang, Wenyu , Gong, Peng et al. Enhancing Catalytic Activity of a Nickel Single Atom Enzyme by Polynary Heteroatom Doping for Ferroptosis-Based Tumor Therapy [J]. | ACS NANO , 2023 . |
MLA | Zhu, Yang et al. "Enhancing Catalytic Activity of a Nickel Single Atom Enzyme by Polynary Heteroatom Doping for Ferroptosis-Based Tumor Therapy" . | ACS NANO (2023) . |
APA | Zhu, Yang , Wang, Wenyu , Gong, Peng , Zhao, Yafei , Pan, Yuanbo , Zou, Jianhua et al. Enhancing Catalytic Activity of a Nickel Single Atom Enzyme by Polynary Heteroatom Doping for Ferroptosis-Based Tumor Therapy . | ACS NANO , 2023 . |
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Lipid peroxidation (LPO) is one of the most damaging processes in chemodynamic therapy (CDT). Although it is well known that polyunsaturated fatty acids (PUFAs) are much more susceptible than saturated or monounsaturated ones to LPO, there is no study exploring the effect of cell membrane unsaturation degree on CDT. Here, we report a self-reinforcing CDT agent (denoted as OA@Fe-SAC@EM NPs), consisting of oleanolic acid (OA)-loaded iron single-atom catalyst (Fe-SAC)-embedded hollow carbon nanospheres encapsulated by an erythrocyte membrane (EM), which promotes LPO to improve chemodynamic efficacy via modulating the degree of membrane unsaturation. Upon uptake of OA@Fe-SAC@EM NPs by cancer cells, Fe-SAC-catalyzed conversion of endogenous hydrogen peroxide into hydroxyl radicals, in addition to initiating the chemodynamic therapeutic process, causes the dissociation of the EM shell and the ensuing release of OA that can enrich cellular membranes with PUFAs, enabling LPO amplification-enhanced CDT.
Keyword :
Antitumor Agents Antitumor Agents Chemodynamic Therapy Chemodynamic Therapy Lipid Peroxidation Lipid Peroxidation Polyunsaturated Fatty Acids Polyunsaturated Fatty Acids Single-Atom Catalysts Single-Atom Catalysts
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GB/T 7714 | Zhu, Yang , Gong, Peng , Wang, Jun et al. Amplification of Lipid Peroxidation by Regulating Cell Membrane Unsaturation To Enhance Chemodynamic Therapy [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (12) . |
MLA | Zhu, Yang et al. "Amplification of Lipid Peroxidation by Regulating Cell Membrane Unsaturation To Enhance Chemodynamic Therapy" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 12 (2023) . |
APA | Zhu, Yang , Gong, Peng , Wang, Jun , Cheng, Junjie , Wang, Wenyu , Cai, Huilan et al. Amplification of Lipid Peroxidation by Regulating Cell Membrane Unsaturation To Enhance Chemodynamic Therapy . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (12) . |
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Mild photothermal therapy (mPTT) has emerged as a highly promising approach for tumor ablation. However, the heat-induced overexpression of heat shock proteins (HSPs) limits its efficacy by increasing cellular temperature tolerance. Herein, a self-catalytically enhanced mild PTT strategy that directly disrupts the structure of HSPs to restore tumor cell sensitivity is proposed. In the proof-of-concept study, AgFeCu nanoparticles (AgFeCu NPs) with dual-active catalytic centers (Fe-Cu) and near-infrared photothermal properties are developed. The AgFeCu NPs can efficiently catalyze the conversion of endogenous hydrogen peroxide into hydroxyl radicals in situ, leading to the degradation of HSPs and enhancing the therapeutic effects of mild PTT mediated by their Ag-based substrates. Furthermore, AgFeCu NPs can also induce oxidative stress by depleting intracellular glutathione and promoting lipid peroxidation, thereby triggering tumor ferroptosis and resulting in significant tumor elimination in a U87MG murine tumor model. This self-catalytically enhanced strategy maximizes the efficacy of mild PTT while minimizing damage to healthy tissues, which is expected to provide valuable insights for the development of next-generation photothermal nanoagents for improved tumor therapeutics.
Keyword :
catalytic therapy catalytic therapy ferroptosis ferroptosis heat shock proteins heat shock proteins mild photothermal therapy mild photothermal therapy reactive oxygen species reactive oxygen species
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GB/T 7714 | Niu, Xuegang , Zhu, Yang , Ding, Chenyu et al. Dual-Active Center AgFeCu Nanocatalyst for Tumor Destruction via Self-Catalytically Enhanced Mild Photothermal Therapy [J]. | ADVANCED FUNCTIONAL MATERIALS , 2023 , 33 (51) . |
MLA | Niu, Xuegang et al. "Dual-Active Center AgFeCu Nanocatalyst for Tumor Destruction via Self-Catalytically Enhanced Mild Photothermal Therapy" . | ADVANCED FUNCTIONAL MATERIALS 33 . 51 (2023) . |
APA | Niu, Xuegang , Zhu, Yang , Ding, Chenyu , Ma, Jing , Wei, Penghui , Lin, Yuanxiang et al. Dual-Active Center AgFeCu Nanocatalyst for Tumor Destruction via Self-Catalytically Enhanced Mild Photothermal Therapy . | ADVANCED FUNCTIONAL MATERIALS , 2023 , 33 (51) . |
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Ferrous iron (Fe2+) has more potent hydroxyl radical ((OH)-O-center dot)-generating ability than other Fenton-type metal ions, making Fe-based nanomaterials attractive for chemodynamic therapy (CDT). However, because Fe2+ can be converted by ferritin heavy chain (FHC) to nontoxic ferric form and then sequestered in ferritin, therapeutic outcomes of Fe-mediated CDT agents are still far from satisfactory. Here we report the synthesis of siRNA-embedded Fe-0 nanoparticles (Fe-0-siRNA NPs) for self-reinforcing CDT via FHC downregulation. Upon internalization by cancer cells, pH-responsive Fe-0-siRNA NPs are degraded to release Fe2+ and FHC siRNA in acidic endo/lysosomes with the aid of oxygen (O-2). The accompanied O-2 depletion causes an intracellular pH decrease, which further promotes the degradation of Fe-0-siRNA NPs. In addition to initiating chemodynamic process, Fe2+-catalyzed (OH)-O-center dot generation facilitates endo/lysosomal escape of siRNA by disrupting the membranes, enabling FHC downregulation-enhanced CDT.
Keyword :
Chemodynamic Therapy Chemodynamic Therapy Fenton Reaction Fenton Reaction Ferritin Heavy Chain Ferritin Heavy Chain Iron Nanoparticles Iron Nanoparticles Small Interfering RNA Small Interfering RNA
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GB/T 7714 | Wang, Jun , Ding, Hongye , Zhu, Yang et al. Iron-siRNA Nanohybrids for Enhanced Chemodynamic Therapy via Ferritin Heavy Chain Downregulation [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
MLA | Wang, Jun et al. "Iron-siRNA Nanohybrids for Enhanced Chemodynamic Therapy via Ferritin Heavy Chain Downregulation" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 22 (2023) . |
APA | Wang, Jun , Ding, Hongye , Zhu, Yang , Liu, Yina , Yu, Meili , Cai, Huilan et al. Iron-siRNA Nanohybrids for Enhanced Chemodynamic Therapy via Ferritin Heavy Chain Downregulation . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
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Nanomaterials with enzyme-mimicking properties, coined as nanozymes, are a promising alternative to natural enzymes owing to their remarkable advantages, such as high stability, easy preparation, and favorable catalytic performance. Recently, with the rapid development of nanotechnology and characterization techniques, single atom nanozymes (SAzymes) with atomically dispersed active sites, well-defined electronic and geometric structures, tunable coordination environment, and maximum metal atom utilization are developed and exploited. With superior catalytic performance and selectivity, SAzymes have made impressive progress in biomedical applications and are expected to bridge the gap between artificial nanozymes and natural enzymes. Herein, the recent advances in SAzyme preparation methods, catalytic mechanisms, and biomedical applications are systematically summarized. Their biomedical applications in cancer therapy, oxidative stress cytoprotection, antibacterial therapy, and biosensing are discussed in depth. Furthermore, to appreciate these advances, the main challenges, and prospects for the future development of SAzymes are also outlined and highlighted in this review.
Keyword :
antibacterial therapy antibacterial therapy biosensing biosensing cancer therapy cancer therapy oxidative-stress cytoprotection oxidative-stress cytoprotection reactive oxygen species reactive oxygen species single-atom nanozymes single-atom nanozymes
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GB/T 7714 | Zhu, Yang , Liao, Yaxin , Zou, Jianhua et al. Engineering Single-Atom Nanozymes for Catalytic Biomedical Applications [J]. | SMALL , 2023 , 19 (30) . |
MLA | Zhu, Yang et al. "Engineering Single-Atom Nanozymes for Catalytic Biomedical Applications" . | SMALL 19 . 30 (2023) . |
APA | Zhu, Yang , Liao, Yaxin , Zou, Jianhua , Cheng, Junjie , Pan, Yuanbo , Lin, Lisen et al. Engineering Single-Atom Nanozymes for Catalytic Biomedical Applications . | SMALL , 2023 , 19 (30) . |
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The practical applications of solid-state electrolytes in lithium-ion batteries (LIBs) are hindered by their low ionic conductivity and high interfacial resistance. Herein, an ethoxylated trimethylolpropane triacrylate based quasi-solid-state electrolyte (ETPTA-QSSE) with a three-dimensional (3D) network is prepared by a one-step in-situ photopolymerization method. The 3D network is designed to overcome the contradiction between the plasticizer-related ionic conductivity and the thickness-dependent mechanical property of quasi-solid-state electrolytes. The ETPTA-QSSE achieves superb room-temperature ionic conductivity up to 4.55x10(-3) S cm(-1), a high lithium ion transference number of 0.57, along with a wide electrochemical window of 5.3 V (vs. Li+/Li), which outperforms most ever of the reported solid-state electrolytes. Owing to the robust network structure and the cathode-electrolyte integrated electrode design, Li metal symmetrical cells show reduced interface resistance and reinforced electrode/ electrolyte interface stability. When applying the ETPTA-QSSE in LiFePO4 parallel to Li cells, the quasi-solid-state cell demonstrates an enhanced initial discharge capacity (155.5 mAh g(-1) at 0.2 C) accompanied by a high average Coulombic efficiency of greater than 99.3%, offering capacity retention of 92% after 200 cycles. Accordingly, this work sheds light on the strategy of enhancing ionic conductivity and reducing interfacial resistance of quasi-solid-state electrolytes, which is promising for high-voltage LIBs.
Keyword :
electrochemical window electrochemical window ionic conductivity ionic conductivity lithium-ion batteries lithium-ion batteries photopolymerization photopolymerization quasi-solid-state electrolyte quasi-solid-state electrolyte
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GB/T 7714 | Zhang WenJing , Li SenLin , Zhang YuRong et al. A quasi-solid-state electrolyte with high ionic conductivity for stable lithium-ion batteries [J]. | SCIENCE CHINA-TECHNOLOGICAL SCIENCES , 2022 , 65 (10) : 2369-2379 . |
MLA | Zhang WenJing et al. "A quasi-solid-state electrolyte with high ionic conductivity for stable lithium-ion batteries" . | SCIENCE CHINA-TECHNOLOGICAL SCIENCES 65 . 10 (2022) : 2369-2379 . |
APA | Zhang WenJing , Li SenLin , Zhang YuRong , Wang XingHui , Liu JingDong , Zheng YuanHui . A quasi-solid-state electrolyte with high ionic conductivity for stable lithium-ion batteries . | SCIENCE CHINA-TECHNOLOGICAL SCIENCES , 2022 , 65 (10) , 2369-2379 . |
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