The Journal of Physical Chemistry C最新文献

{"title":"Detecting Reactive Products in Carbon Capture Polymers with Chemical Shift Anisotropy and Machine Learning","authors":"Maxwell A. T. Marple, Sichi Li, Elwin Hunter-Sellars, Simon H. Pang","doi":"10.1021/acs.jpcc.4c07459","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07459","url":null,"abstract":"Aminopolymers are attractive sorbents for CO₂ direct air capture applications due to their high density of amine groups, which can readily react with atmospheric levels of CO₂ to form chemisorbed species. The identity of these chemisorbed species and the functional groups that form upon oxidative degradation depends on both material properties and processing conditions, forming a variety of carbonyl-type sites such as ammonium carbamates, bicarbonates, carbonates, carbamic acids, ureas, and amides. ¹³C solid-state nuclear magnetic resonance (NMR) is often used to help elucidate the identity of these reacted species, but it is challenging due to the narrow chemical shift range of carbonyl sites. Herein, we demonstrate the application of a two-dimensional (2D) chemical shift anisotropy (CSA) recoupling pulse sequence (ROCSA) to obtain CSA tensor values at each isotropic chemical shift, overcoming limitations of isotropic peak resolution. CSA tensor values describe the local chemical environment and can readily differentiate between the chemisorbed and degradation products. To aid identification, we also developed a <i>k</i>-nearest neighbor (kNN) classification model to distinguish the functional groups via their CSA tensor parameters. This methodology was demonstrated on poly(ethylenimine) in γ-Al₂O₃ exposed to CO₂ and showed that the chemisorbed products are ammonium carbamate and a mixed carbamate–carbamic acid species. The sample was analyzed again after desorption at 100 °C inducing mild degradation, and the remaining products were strongly bound carbamate and urea species. The combination of 2D CSA measurements coupled with a kNN classification model enhances the ability to accurately identify chemisorbed or degradation products in complex carbon capture materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"9 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044488","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"What Spectro-electrochemical Studies Tell about the Interactions between Antimicrobial Peptides and Biomimetic Membranes at Electrode Surfaces","authors":"Zhangfei Su, Aicheng Chen, Jacek Lipkowski","doi":"10.1021/acs.jpcc.4c07961","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07961","url":null,"abstract":"This feature article provides a summary of spectro-electrochemical studies of selected antimicrobial peptides in model biomimetic membranes deposited at a gold electrode surface. This metal support allows for varying transmembrane potential acting on the membrane and investigating its effect on the properties of the biomimetic membranes and the peptides incorporated into the membrane. The responses of gramicidin (channel-forming peptide), alamethicin (pore-forming peptide), valinomycin (ionophore) and polymyxin (peptide disrupting the outer membrane of the Gram-negative bacteria) to changes in the transmembrane potential are described. The properties of these peptides were investigated in three model membranes: supported bilayer membrane (sBLM), tethered bilayer membrane (tBLM) and floating bilayer membrane (fBLM). Polarization modulation infrared reflection absorption spectroscopy (PM IRRAS) was used to provide information about changes in the orientation and conformation of biomolecules and electrochemical impedance spectroscopy (EIS) was employed to monitor the membrane conductivity. The materials described in this article have been published in several papers over the past decade. This feature article provides a comprehensive and comparative analysis of the assembled information.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"120 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044489","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Zinc Deposition Tuned by Single-Layer Graphene on Copper","authors":"Xiaolan Wang, Minghao Guo, Jiahui Xu, Wenshan Jia, Hengxing Ji, Kun Ni, Yanwu Zhu","doi":"10.1021/acs.jpcc.4c06348","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06348","url":null,"abstract":"Using carbon as a substrate or scaffold has been considered as an efficient strategy to improve the uniformity of zinc deposition, which may boost the anode performance of metal zinc batteries. However, the essential role of the carbon substrate remains unclear. Here, single-layer graphene grown on copper is used as a model material to investigate the interaction between zinc and carbon. The morphology and crystallinity of early-stage zinc deposition with galvanostatic or potentiostatic electrochemical plating are discussed. By using an electrochemical quartz crystal microbalance study, we verify the difference in energy dissipation of the zinc deposition with or without single-layer graphene. Density functional theory simulations show that the presence of graphene reduces the difference in the binding energy of zinc on different sites of defective copper surfaces, thus improving the uniformity of zinc electrodeposition. Our study shows that single-layer graphene can act as the passivation layer of copper to reduce the probability of dendrite growth.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"4 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Pressure-Driven Structural Transition in the Charge Density Wave Material SrAl4","authors":"Shihu Zhang, Yi-Chi Li, Yang Chen, Yonghui Zhou, Shuyang Wang, Ying Zhou, Min Zhang, Chao An, Yong Fang, Jian Zhou, Zhaorong Yang","doi":"10.1021/acs.jpcc.4c08594","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c08594","url":null,"abstract":"SrAl&lt;sub&gt;4&lt;/sub&gt;, which possesses a BaAl&lt;sub&gt;4&lt;/sub&gt;-type tetragonal structure (&lt;i&gt;I&lt;/i&gt;4/&lt;i&gt;mmm&lt;/i&gt;, No. 139), exhibits both a charge density wave (CDW) order and a topological semimetal state at ambient pressure. Here, the electronic and structural properties of SrAl&lt;sub&gt;4&lt;/sub&gt; were systematically investigated with pressure up to 49.4 GPa through electrical transport, X-ray diffraction (XRD), and Raman scattering measurements, as well as theoretical calculations. With increasing pressure, the &lt;i&gt;T&lt;/i&gt;&lt;sub&gt;CDW&lt;/sub&gt; is monotonically decreased, and the CDW state is eventually suppressed to zero temperature at ∼10 GPa based on the linear extrapolation. At ambient pressure, three Raman vibrational modes are identified, which are assigned to &lt;i&gt;B&lt;/i&gt;&lt;sub&gt;1&lt;i&gt;g&lt;/i&gt;&lt;/sub&gt; (230.9 cm&lt;sup&gt;–1&lt;/sup&gt;), &lt;i&gt;&lt;/i&gt;&lt;span style=\"color: inherit;\"&gt;&lt;/span&gt;&lt;span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\"&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;E&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;g&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"&gt;&lt;nobr aria-hidden=\"true\"&gt;&lt;span style=\"width: 1.539em; display: inline-block;\"&gt;&lt;span style=\"display: inline-block; position: relative; width: 1.232em; height: 0px; font-size: 122%;\"&gt;&lt;span style=\"position: absolute; clip: rect(1.181em, 1001.23em, 2.769em, -999.997em); top: -2.2em; left: 0em;\"&gt;&lt;span&gt;&lt;span&gt;&lt;span style=\"display: inline-block; position: relative; width: 1.232em; height: 0px;\"&gt;&lt;span style=\"position: absolute; clip: rect(3.179em, 1000.77em, 4.152em, -999.997em); top: -3.993em; left: 0em;\"&gt;&lt;span&gt;&lt;span style=\"font-family: MathJax_Math-italic;\"&gt;E&lt;span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.054em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; width: 0px; height: 3.998em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"position: absolute; clip: rect(3.384em, 1000.41em, 4.152em, -999.997em); top: -4.403em; left: 0.822em;\"&gt;&lt;span&gt;&lt;span style=\"font-size: 70.7%; font-family: MathJax_Main;\"&gt;2&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; width: 0px; height: 3.998em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"position: absolute; clip: rect(3.537em, 1000.41em, 4.306em, -999.997em); top: -3.737em; left: 0.72em;\"&gt;&lt;span&gt;&lt;span style=\"font-size: 70.7%; font-family: MathJax_Math-italic;\"&gt;g&lt;span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.003em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; width: 0px; height: 3.998em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; width: 0px; height: 2.205em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; overflow: hidden; vertical-align: -0.559em; border-left: 0px solid; width: 0px; height: 1.691em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;/nobr&gt;&lt;span role=\"presentation\"&gt;&lt;math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;E&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;g&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"39 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050294","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unraveling the Influence of Al Addition and Location on the Catalytic Mechanism and Performance of the TS-1 Catalyst toward Ethylene Glycol Synthesis","authors":"Tian Liu, Xiaowa Nie, Wenchao Yang, Chunshan Song, Xinwen Guo","doi":"10.1021/acs.jpcc.4c05512","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05512","url":null,"abstract":"In this work, the reaction mechanism of ethylene glycol (EG) synthesis from the oxidation hydration of ethylene catalyzed by Al/TS-1 was studied by density functional theory calculations, based on which the optimal energy pathway, rate-limiting step, and the underlying effect of Al addition and location were identified. The calculation results showed that the introduction of Al increased the catalytic activity of the Ti(IV) site of TS-1. The relative position of Al to Ti had an obvious influence on the reaction properties over the Ti(IV) site but had a minor effect on the catalytic activity of the Al(H) Brønsted acid site toward EG generation. In the optimal energy pathway of ethylene oxidation hydration to EG over Al/TS-1, the H₂O₂ activation and ethylene epoxidation occurred at the Ti(IV) site with barriers of 0.85 and 0.54 eV, respectively, while the hydration of EO to EG preferentially took place at the Al(H) Brønsted acid site with a barrier of 1.33 eV, exhibiting bifunctional actions of Ti–Al(H) sites. The Al/TS-1 catalyst showed a high selectivity to the EG product with the formation of the diethylene glycol byproduct suppressed by slow kinetics.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"25 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Naphthalene Decomposition on Fe(110)─Adsorption, Dehydrogenation, Surface Carbon Formation and the Influence of Coadsorbed Oxygen","authors":"Lea Hohmann, Franziska Dahlmann, Giorgio Bruno Braghin, Léonie Laviron, Layal Hussein, Jakob Martinez, Anton Harrer, Haley Robertson, Jona Guiborat, Xiaoming Hu, Jonas Weissenrieder, Klas Engvall, Jerry LaRue, Tony Hansson, Mats Göthelid, Amirreza Ghassami, Dan J. Harding, Henrik Öström","doi":"10.1021/acs.jpcc.4c06619","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06619","url":null,"abstract":"Tar is an undesirable byproduct of biomass gasification, which can be removed through catalytic reforming to syngas components. Iron is a promising, abundant alternative to highly active but toxic nickel catalysts. The results observed so far in catalytic studies with iron have been mixed. In this paper, the decomposition of naphthalene, a representative model compound of tar, was studied on the catalytic Fe(110) surface using temperature-programmed desorption (TPD), sum frequency generation spectroscopy (SFG), and X-ray photoelectron spectroscopy (XPS). Napthalene adsorption, dehydrogenation and the formation of surface carbon were investigated, as well as the influence of oxygen. In comparison with previous studies on Ni(111), a similar dehydrogenation activity was found for Fe(110) with two main H₂ TPD peaks at 450 and 550 K. The reaction of naphthalene on Fe(110) resulted in the predominant formation of carbidic and atomically adsorbed carbon on the surface, which did not dissolve into the bulk even at high temperatures. A moderately carbon-covered surface was shown to still be active toward naphthalene decomposition. Similarly to Ni(111), large amounts of oxygen inhibited the reaction but, at low oxygen doses, very high hydrogen yields were observed, suggesting that Fe(110) could be a valid alternative for tar decomposition.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"72 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Copper-Doped CsPbI3 Nanocrystals: Improved Stability and Ultrafast Photophysical Dynamics","authors":"Yusheng He, Xiaohu Zhao, Junwei Zhou, Qingyuan Zhou, Yuanchen Jiang, Jianhui Sun, Zhen Liu, Kai Pan","doi":"10.1021/acs.jpcc.4c07798","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07798","url":null,"abstract":"CsPbI₃ nanocrystals (NCs) are highly promising for optoelectronic applications due to their excellent photoluminescence quantum yield (PLQY), adjustable emission wavelength, and high color purity. However, their poor stability poses significant challenges for practical applications and further development. In this study, we synthesized CsPbI₃ NCs doped with copper ions (Cu²⁺) using a hot-injection method, with Cl^– ions effectively passivating surface defects. We then examined the effects of varying Cu²⁺ doping levels (0%, 5%, 10%, and 15%) on their properties. X-ray diffraction (XRD) analysis showed that Cu²⁺ doping caused the main diffraction peak to shift to higher angles, indicating the successful substitution of Pb²⁺ by Cu²⁺ in the crystal structure. Specifically, doping with 10% Cu²⁺ increased the photoluminescence quantum efficiency from 53.88% to 94.24% and extended the exciton lifetime from 36.60 to 50.26 ns. From 17.72 to 50.11 ps, the bleach recovery rate for Cu²⁺-doped samples is approximately 25%, while that for undoped samples is 28%. Additionally, the environmental stability of the NCs was greatly improved. This study highlights the potential of using transition metal ion doping to enhance the optoelectronic properties and stability of the photoluminescence quantum efficiency.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"13 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044784","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High Anisotropic Optoelectronics and Robust Transport Performance in Two-Dimensional Single-Layer and Bilayer As4P6","authors":"Tingting Duan, Zheng Zhang, Ying Yao, Wangping Xu, Juexian Cao, Xiaolin Wei","doi":"10.1021/acs.jpcc.4c07460","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07460","url":null,"abstract":"Two-dimensional black arsenic phosphorus has attracted significant interest due to its extraordinary electronic, optical, and transport properties. Therefore, in this work, we go through all the possibilities, including 3297 nonrepetitive configurations, and demonstrate the lowest energy structure of the As_<i>x</i>P_1–<i>x</i> (<i>x</i> = 0.4) monolayer by first-principles calculations. Our results indicate that both single-layer and bilayer As₄P₆ host direct and indirect bandgap semiconductors with bandgaps of 1.94 and 1.26 eV, respectively, which exhibit good light adsorption within the visible light and infrared region. Moreover, both single-layer and bilayer As₄P₆ possess high electron and hole mobilities (up to 2.6 × 10⁴ cm² v^–1 s^–1), which also exhibit extreme carrier anisotropy originating from their high in-plane lattice anisotropy. Furthermore, bilayer As₄P₆ exhibits exceptional device characteristics including a lower threshold voltage, higher on-state current, and higher conductance. In addition, the transmission coefficient spectrum of bilayer As₄P₆ is three times greater than that of the monolayer owing to an increased number of electronic channels. Additionally, the extinction ratio of single-layer As₄P₆ exhibits high anisotropy, indicating enhanced polarization sensitivity in the zigzag direction. Our findings provide two excellent candidate materials for the application of optoelectronic devices.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"116 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual Effects of LiF on Enhancing the Synthesis and Electrochemical Stability of Amorphous Nano/Micro Ce2Mg17/Ni Composite Electrodes","authors":"Zhuocheng Liu, Qilong Fan, Yiming Li, Boshuo Wang, Fei Ruan, Ming Zhao, Fei Yang","doi":"10.1021/acs.jpcc.4c07162","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07162","url":null,"abstract":"Amorphous nano/microstructured rare earth (RE)-Mg-based alloys exhibit outstanding hydrogen storage capacity and charge–discharge kinetics. However, precisely controlling the composition to ensure the formation of a uniform microstructure with finely dispersed amorphous or nano/micro phases remains challenging. Simultaneously, the rapid corrosion of nano- and microsized Mg particles in an alkali solution reduces the battery lifespan. Therefore, a LiF catalyst was used to enhance the corrosion resistance of the electrode alloy. Subsequently, a simulation calculation was performed based on the extended Miedema thermodynamic theory. The calculation results show that to ensure Δ<i>H</i>_amor ≤ 0 for amorphous enthalpy, the enthalpy difference between the amorphous and solid states |Δ<i>H</i>_sol^m – Δ<i>H</i>_amor| ≤ 5 is essential for the successful formation of amorphous phases. Moreover, the optimal ranges for Li concentration and corresponding enthalpy differences were determined as 3–5 wt % and −4.55 and −4.41 kJ/mol, respectively. Based on the simulation results, Ce₂Mg₁₇/Ni (1:1) + <i>x</i> wt % LiF (<i>x</i> = 0, 1, 3, 5, and 10) composite electrode materials were prepared through mechanical ball-milling, with the results revealing that the Ce₂Mg₁₇/Ni (1:1) composite material with 3 wt % LiF exhibits the best discharge capacity (526.22 mAh·g^–1). The microstructural observation results indicated that LiF effectively inhibited the propagation of cracks along the grain boundaries. These experimental findings were consistent with our theoretical predictions. Hence, the findings of this study may serve as a reference for future development of novel Ce–Mg-based electrode alloys.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"5 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044491","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"First-Principles Insight into the Antiperovskite c-Na3HS Solid-State Electrolyte","authors":"Sananya Chakraborty, Nidhi Verma, Ashok Kumar","doi":"10.1021/acs.jpcc.4c05533","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05533","url":null,"abstract":"We explore the potential of the novel antiperovskite c-Na₃HS to be a solid-state electrolyte for sodium-ion batteries. To investigate the dynamical stability, phase stability, thermal stability, mechanical stability, and ionic, electronic, and diffusive properties of c-Na₃HS, first-principles methods based on density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations have been employed. c-Na₃HS has no imaginary phonon modes, indicating its dynamical stability. Key findings include a small energy above the hull, a wide band gap of 4.25 eV, and a mechanical stability analysis that indicates the moderately hard and a little brittle nature of c-Na₃HS. The activation energy of Na in c-Na₃HS is calculated to be ∼300 meV, which reduces to ∼100 meV upon introducing Na vacancy. The ionic conductivity can be enhanced by up to ∼3 orders of magnitude by vacancy and halogen doping in the c-Na₃HS structure. Thus, the obtained results indicate that c-Na₃HS can be a viable option to be utilized as a solid-state electrolyte in sodium-ion batteries.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"108 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143027107","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}