LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c03530
Nurafni Annisa Achmad, Rachmatya W. Tuna, Irfan Kurniawan, Khairiyah, Muhammad Bisfain Asaf, Latifah Rahman, Marianti A. Manggau, Aliyah, Juan Dominguez-Robles, Muhammad Aswad, Andi Dian Permana
{"title":"Development of Thermosensitive Mucoadhesive Gel Based Encapsulated Lipid Microspheres as Nose-to-Brain Rivastigmine Delivery System","authors":"Nurafni Annisa Achmad, Rachmatya W. Tuna, Irfan Kurniawan, Khairiyah, Muhammad Bisfain Asaf, Latifah Rahman, Marianti A. Manggau, Aliyah, Juan Dominguez-Robles, Muhammad Aswad, Andi Dian Permana","doi":"10.1021/acs.langmuir.4c03530","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03530","url":null,"abstract":"Alzheimer’s disease (ALZ) is a neurodegenerative disease that damages neuronal cells and causes decline in cognitive abilities. Administration of cholinesterase inhibitor compounds is the primary choice in the treatment of ALZ, one of which is rivastigmine (RVT). Several routes of administration of RVT are available, such as oral and transdermal. However, in the oral route, RVT has low bioavailability, undergoes first-pass metabolism, and the presence of the blood-brain barrier (BBB) reduces the therapeutic concentration of RVT. The transdermal route is nonselective target in the brain. This study aims to combine thermosensitive mucoadhesive gel (TG) and lipid microspheres (LM) as a drug delivery system to improve the efficacy of RVT. Combining these will prevent systemic side effects of RVT and increase drug concentration in the brain. LM was formulated with varying concentrations of Compritol polymer. The results of LM evaluation showed the values of particle size, PDI, and %EE and %DL were 8.519 μm, 0.018 ± 0.004, 72.54%, and 76.43%, respectively. The TG formulation can provide a liquid form at room temperature (25 °C) and a gel at nasal temperature (35 °C). Hemolytic and HET-CAM tests confirmed TG RVT LM’s safety for use. <i>Ex vivo</i> studies showed controlled and sustained release of TG RVT LM, and <i>in vivo</i> studies showed TG RVT LM a higher pharmacokinetic profile in the brain than oral formulations and injections. The <i>C</i><sub>max</sub> was found to be 7.05 ± 0.55 μg/cm<sup>3</sup>, <i>T</i><sub>max</sub> was 24 h, and AUC<sub>0–24</sub>, which is related to the effectiveness of brain targeting, was 225.73 μg/cm<sup>3</sup>. In conclusion, this study shows the successful development of TG RVT LM, as evidenced by improved drug delivery to the brain, which is characterized by higher concentrations of RVT in the brain compared with oral and injectable RVT, this delivery system shows potential as a future treatment for Alzheimer’s disease.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"92 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874364","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c03229
Vikram P. Wanjari, Pawan Kumar, Siddhartha P. Duttagupta, Swatantra P. Singh
{"title":"Adsorption-Enhanced Sensitivity for Electrochemical Sensing of Diclofenac by Poly(ether sulfone)-Based Laser-Induced Graphene","authors":"Vikram P. Wanjari, Pawan Kumar, Siddhartha P. Duttagupta, Swatantra P. Singh","doi":"10.1021/acs.langmuir.4c03229","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03229","url":null,"abstract":"Emerging contaminants are a matter of growing concern for environmental and human health and safety, requiring efficient and affordable sensing platforms. Laser-induced graphene (LIG) is a novel material with a 3D porous graphene structure that can be fabricated in a simple one-step fabrication process. However, most LIG-based works in electrochemical sensors are limited to polyimide (PI)-based platforms, thus limiting the purview of properties of LIG dependent on the substrate–laser interaction. Diclofenac (DCF), a nonsteroidal anti-inflammatory drug, is an emerging contaminant in water and wastewater that threatens aquatic and terrestrial life. Furthermore, LIG-based sensors have not been used to sense DCF. In this work, we demonstrate the spontaneous adsorption behavior of LIG toward DCF without applying any external potential. This spontaneous adsorption phenomenon can enhance the sensitivity per the characteristics of the tested water samples and permissible standards to be followed. Poly(ether sulfone)-based LIG (PES-LIG) is found to be more responsive to laser irradiation than PI-LIG due to its highly porous surface and fibrous nature, imparting more electrochemical sites and adsorption area for DCF. These characteristics lead to a higher sensitivity of 0.2774 μA μM<sup>–1</sup> toward DCF sensing for PES-LIG with a limit of detection of 0.1 μM. The sensors were applied for DCF measurement in wastewater and tap water samples with appreciable selectivity. The specific adsorption behavior of LIG toward DCF could pave the way for new pathways in emerging contaminant sensing and removal as well as for other applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"13 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874362","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c04040
Li Wang, Chunqiu Han, Xin Ying Kong, Liqun Ye, Yingping Huang
{"title":"Piezoelectric Activation of Peroxymonosulfate by CoMn2O4 for Highly Efficient Tetracycline Degradation","authors":"Li Wang, Chunqiu Han, Xin Ying Kong, Liqun Ye, Yingping Huang","doi":"10.1021/acs.langmuir.4c04040","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04040","url":null,"abstract":"Advanced oxidation processes employing peroxymonosulfate (PMS) show significant promise for wastewater treatment. However, PMS activation typically relies on energy- and chemically intensive techniques due to its relatively low reactivity. Hence, the exploration of novel and energy-efficient approaches, such as the piezoelectric effect, for PMS activation is of paramount importance. Herein, we prepared a piezoelectric material (CoMn<sub>2</sub>O<sub>4</sub>) via a simple hydrothermal method followed by calcination. The degradation experiments of tetracycline (TC) demonstrated that CoMn<sub>2</sub>O<sub>4</sub> exhibited excellent performance under ultrasound, the apparent rate constant <i>k</i> is 0.191 min<sup>–1</sup>, and its degradation rate reached 83.63% after 10 min. Piezo force microscopy (PFM) tests confirmed that CoMn<sub>2</sub>O<sub>4</sub> exhibited a piezotronic effect under ultrasound. <i>In situ</i> electron paramagnetic resonance (<i>in situ</i> EPR) tests revealed that PMS could be activated to form hydroxyl radicals (<sup>•</sup>OH) and sulfate radicals (SO<sub>4</sub><sup>•–</sup>) under ultrasound, which are active species for TC degradation. Consequently, CoMn<sub>2</sub>O<sub>4</sub> effectively activated PMS into <sup>•</sup>OH and SO<sub>4</sub><sup>•–</sup> active species, enabling the effective TC degradation. Moreover, biotoxicity experiments using germination tests showed that CoMn<sub>2</sub>O<sub>4</sub> was capable of effectively degrading TC, thereby reducing environmental toxicity. This work not only provides mechanistic insights into piezoelectric material-activated PMS for pollutants degradation but also establishes a basis for the application of piezoelectric materials in pollutant degradation.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"26 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c03704
Hao Zhang, Xiaoyan Zhuang, Yutong Wang, Zhen Zhao, Lijuan Yan, Guangyong Li, Jun Li, Hui Yan
{"title":"Molecular Dynamics Simulation on the Conformational Change of a pH-Switchable Lipid","authors":"Hao Zhang, Xiaoyan Zhuang, Yutong Wang, Zhen Zhao, Lijuan Yan, Guangyong Li, Jun Li, Hui Yan","doi":"10.1021/acs.langmuir.4c03704","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03704","url":null,"abstract":"pH-sensitive lipids are important components of lipid nanoparticles, which enable the targeted delivery and controlled release of drugs. Understanding the mechanism of pH-triggered drug release at the molecular level is important for the rational design of ionizable lipids. Based on a recently reported pH-switchable lipid, named SL2, molecular dynamics (MD) simulations were employed to explore the microscopic mechanism behind the membrane destabilization induced by the conformational change of pH-switchable lipids. The simulated results showed that, at neutral pH, the neutral SL2 lipids assembled with other components (helper lipids and cholesterol) to form a structurally ordered bilayer structure. At this moment, the two hydrocarbon chains of SL2 were closely aligned and inserted in an orderly manner inside of the membrane. With a decrease in pH, the protonation of the pyridinium ring caused a large degree of molecular structural change. The pyridinium ring preferred to form intramolecular H-bonds with the methoxy groups and intermolecular H-bonds with water, resulting in the flip of the pyridinium ring. Meanwhile, due to the structural flip, the two alkane chains showed a more open state, which perturbed the arrangement of molecules within the membrane. The perturbations caused local collapse of the membrane and the formation of water molecule channels, which contributed to the pH-induced drug release. Our results verified the experimentally proposed mechanism at the molecular level and provided more complementary information, which are expected to have deeper insights into the pH-triggered drug release.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"24 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c03611
Hassane Lgaz, Savas Kaya, Dong-Eun Lee, Ali Aldalbahi, Han-seung Lee
{"title":"Functional Group Effects on the Interfacial Adsorption of Arylquinoline-3-Carbonitriles on Iron: A DFT-D3 Investigation of Surface Interaction Mechanisms","authors":"Hassane Lgaz, Savas Kaya, Dong-Eun Lee, Ali Aldalbahi, Han-seung Lee","doi":"10.1021/acs.langmuir.4c03611","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03611","url":null,"abstract":"Reliable corrosion inhibition systems are crucial for extending the lifespan of industrial metal structures. Quinolines, with their high adsorption capacity and protective efficiency, are promising next-generation inhibitors. However, the impact of substitutions on their coordination with iron surfaces requires deeper understanding. Herein, we investigate the influence of various functional groups on the adsorption behavior of three 2-amino-4-arylquinoline-3-carbonitriles (AACs) on iron surfaces using first-principles density functional theory calculations. Results reveal that nitrophenyl and hydroxyphenyl significantly enhance the adsorption strength of AACs on the Fe(110) surface, facilitated by donor–acceptor interactions. Neutral molecules were more stable than their protonated counterparts. Key results show strong adsorption energies, with values ranging from −2.005 to −1.809 eV for the AACs, along with significant electron gains across carbon atoms as indicated by Bader charge analysis. These strong interactions result in notable charge redistribution and bond formation, as shown by projected density of states and electron density difference iso-surfaces. Furthermore, electron localization function analysis indicates that van der Waals interactions, influenced by multiple nitrogen atoms, play a crucial role in stabilizing the adsorbed molecules. Stronger adsorption through electron donation and retro-donation mechanisms suggests enhanced corrosion protection efficiency of these substituted quinolines. The conductor-like screening model for real solvents analysis provides complementary insights into the solvation characteristics. Overall, the findings demonstrate the specific role functional groups play in the coordination of arylquinoline-3-carbonitriles with iron surfaces.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"3 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874535","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c03420
Telma Domingues, Chun-Da Liao, Marta Prado, M. Fátima Cerqueira, Dmitri Y. Petrovykh, Pedro Alpuim, Jérôme Borme, Joana Rafaela Guerreiro
{"title":"Tailoring DNA Surface Interactions on Single-Layer Graphene: Comparative Analysis of Pyrene, Acridine, and Fluorenyl Methyl Linkers","authors":"Telma Domingues, Chun-Da Liao, Marta Prado, M. Fátima Cerqueira, Dmitri Y. Petrovykh, Pedro Alpuim, Jérôme Borme, Joana Rafaela Guerreiro","doi":"10.1021/acs.langmuir.4c03420","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03420","url":null,"abstract":"This study investigates the effect of different linkers and solvents on the immobilization of DNA probes on graphene surfaces, which are crucial for developing high-performance biosensors. Quartz crystal microbalance with dissipation (QCM-D) measurements were used to characterize in situ and real-time the immobilization of ssDNA and hybridization efficiency on model graphene surfaces. The DNA probes immobilization kinetics and thermodynamics were systematically investigated for all the pairings between three bifunctional linkers─1-pyrenebutyric acid succinimidyl ester (PBSE), Fluorenylmethylsuccinimidyl carbonate (FSC), and Acridine Orange (AO) succinimidyl ester─and three organic solvents (DMF, DMSO, and 10% DMF/ethanol). The linker’s spatial orientation and effective surface modification for DNA probe attachment were also evaluated based on footprints and DNA probe surface coverage. Graphene surfaces functionalized with PBSE in DMF achieved the highest DNA probe surface density (up to 1.31 × 10<sup>13</sup> molecules cm<sup>–2</sup>) and fastest kinetic, <i>p</i> values above 4, and hybridization efficiencies of at least 70%, with 20 to 30% of ssDNA directly adsorbed nonspecifically on the functionalized graphene surface, which has significant implications for the design of sensitive biosensors. The efficiency of the ethanolamine-NHS blocking reaction was estimated to be 80%. The surface packing density of the linker was estimated at 25% of the entire surface coverage for PBSE, and about 22 and 13% for AO and FSC, respectively. Overall, the surface coverage achieved for probe DNA was in the same order of magnitude as that obtained on flat gold surfaces (≥10<sup>13</sup> molecules cm<sup>–2</sup>), typically used in biosensors. These findings highlight the importance of the selected conditions for graphene surface modification to achieve high DNA probe surface density on graphene materials. These results underscore the critical role of interface engineering in achieving target functional outcomes in biosensing technology.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"83 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Alkaline-Assisted Excessive Impregnation for Enhancing Au Nanoparticle Loading on the TS-1 Zeolite","authors":"Chenyang Zhao, Yujia Liu, Yahui Li, Yupeng Tian, Haiyuan Jia, Wei Xu, Zhe Yang, Bing Sun","doi":"10.1021/acs.langmuir.4c04101","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04101","url":null,"abstract":"Direct epoxidation of propylene (C<sub>3</sub>H<sub>6</sub>) with hydrogen (H<sub>2</sub>) and oxygen (O<sub>2</sub>) over the Au/TS-1 catalyst is known as the “Holy Grail” reaction for propylene oxide (PO) synthesis. However, Au nanoparticle loading on TS-1 was limited by traditional deposition precipitation, impregnation and could not achieve ideal catalytic results. In this report, alkaline-assisted excessive impregnation helped to remove Cl<sup>–</sup> from the Au impregnation precursor, improve the loading efficiency of Au nanoparticles and overcome the abnormal growth of nanograins. Better hydrophobicity, surface acidity and an oxygen-containing free radical environment helped Au/TS-1-AEI achieve much better C<sub>3</sub>H<sub>6</sub> conversion (8.0%), PO selectivity (96.7%) and stability (>100 h).","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"149 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-23DOI: 10.1021/acs.langmuir.4c03727
Qianqian Yin, Yuanhe Gao, Wenbo Zhang, Ruikun Wang, Xiaoxun Zhu, Xiaoxia Gao, Peng Gao, Kai Ma
{"title":"Theoretical Study on the Adsorption of Hexavalent Chromium by Metal-Modified and Nitrogen-Doped Carbon Materials","authors":"Qianqian Yin, Yuanhe Gao, Wenbo Zhang, Ruikun Wang, Xiaoxun Zhu, Xiaoxia Gao, Peng Gao, Kai Ma","doi":"10.1021/acs.langmuir.4c03727","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03727","url":null,"abstract":"Cr(VI) can cause great harm to human beings and the environment and often exists in the form of HCrO<sub>4</sub>̅ in aqueous environments. The adsorption characteristics of HCrO<sub>4</sub>̅ on nitrogen-doped and iron–nickel-modified carbon substrates were systematically investigated using first principles. The properties of electron transfer and orbital hybridization of the substrates and HCrO<sub>4</sub>̅ during the adsorption process were analyzed by electron deformation density and density of states. The electrons were donated by the metal atoms and gained by the oxygen atoms involved in the adsorption of HCrO<sub>4</sub><sup>–</sup>. The binding energies of the substrates and metal atoms were larger than the cohesive energies of the metal atoms, indicating excellent structural stability. Both mono- and bimetallic modifications of the carbon materials by Fe/Ni were favorable for the adsorption of HCrO<sub>4</sub><sup>–</sup>. The increased number of doped nitrogen atoms could promote the adsorption. Among them, (Fe,Ni)/N–C possesses the optimal adsorption of HCrO<sub>4</sub><sup>–</sup>, with an adsorption energy of −4.64 eV. This is mainly attributed to the fact that the Fe–Ni bimetallic atoms simultaneously participate in the electron transfer and orbital hybridization, providing a new perspective for the adsorption of Cr(VI) on bimetallic-modified substrates.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"32 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874363","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
LangmuirPub Date : 2024-12-22DOI: 10.1021/acs.langmuir.4c04332
Shu Tian, Yi Li, Hao Zhang, Guangming Lu, Ruiqi Li, Junyu Yu, Chao Zhao, Jing Yang, Lei Zhang
{"title":"Amphiphilic Marine Antifouling Coatings Based on Zwitterion-Modified Silicone Polymers","authors":"Shu Tian, Yi Li, Hao Zhang, Guangming Lu, Ruiqi Li, Junyu Yu, Chao Zhao, Jing Yang, Lei Zhang","doi":"10.1021/acs.langmuir.4c04332","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04332","url":null,"abstract":"Silicone coatings are widely employed in marine antifouling applications due to their low surface energy. However, in static marine environments, pure silicone coatings are ineffective in preventing the adhesion of marine biofilms, which consist of proteins, marine bacteria, and extracellular matrices, ultimately promoting the attachment of macrofouling organisms. To address the limitations in antifouling performance under static conditions, this study introduces a silicone-based antifouling coating modified with zwitterionic polymers. Sulfobetaine (SB) zwitterionic segments were grafted onto the side chains of poly(dimethylsiloxane) (PDMS) to synthesize the amphiphilic polymer P(DMS-SB), which was incorporated into the PDMS network to create an interpenetrating network-structured silicone coating. The zwitterionic segments effectively inhibited the adhesion of proteins, bacteria, and algae through hydration effects. Compared to pure PDMS coatings, the adhesion of proteins, bacteria, and algae was reduced by 88%, 98.9%, and 99.3%, respectively. Additionally, the coating demonstrated excellent fouling-release properties, achieving a 91.3% removal rate for settled algae under water flow conditions and reducing the simulated barnacle adhesion strength by 68.4%. This coating presents a promising antifouling solution for ships, offshore structures, and aquaculture facilities in static marine environments with significant potential for widespread application.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"61 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874540","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Excellent Electrochemical Performance and Air Storage Stability of Na-Ion Layered Oxide Cathodes Benefiting from Enhanced Ce–O Binding Energy","authors":"Xiangnan Li, Xinyu Tang, Mengdan Zhang, Xiaojian Liu, Yiwei Xu, Zhenpu Shi, Huishuang Zhang, Yanhong Yin, Shu-Ting Yang","doi":"10.1021/acs.langmuir.4c03801","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03801","url":null,"abstract":"The widespread application of layered oxides is constrained by their low electrochemical performance and complex irreversible phase transition. The high entropy oxide NaNi<sub>0.25</sub>Fe<sub>0.15</sub>Mn<sub>0.3</sub>Ti<sub>0.1</sub>Sn<sub>0.05</sub>Co<sub>0.05</sub>Li<sub>0.1</sub>O<sub>2</sub> (HEO) is synthesized by leveraging the entropy stabilization effect, which offers a partial solution to this issue, but electrochemical performance and air stability imperative to be improved. On the high entropy oxide HEO, due to the strong bond energy of Ce–O, the introduction of Ce<sup>4+</sup> improves the specific discharge capacity and reduces the battery gas production problem. It also improves the air stability. NaNi<sub>0.25</sub>Fe<sub>0.15</sub>Mn<sub>0.3</sub>Ti<sub>0.1</sub>Sn<sub>0.03</sub>Ce<sub>0.02</sub>Co<sub>0.05</sub>Li<sub>0.1</sub>O<sub>2</sub> (HEO-Ce2) demonstrated a specific discharge capacity of 160 mA h g<sup>–1</sup> at 0.1 C. The discharge-specific capacity retention rate of the material is 86%, after air exposure for 10 days. The high entropy effect and introduction of Ce<sup>4+</sup> provide a viewpoint for a layered oxide of sodium-ion batteries.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"20 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}