The Journal of Physical Chemistry C最新文献_第10页

Molecular Simulation Study of Elasticity of Fluid-Saturated Zeolites 饱和沸石弹性的分子模拟研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c04839

Santiago A. Flores Roman, Alina Emelianova, Gennady Y. Gor

引用次数: 0

First-Principles Study on the Monomolecular Isomerization of Ethylbenzene within H-BEA Zeolite 乙苯在H-BEA分子筛内单分子异构化的第一性原理研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c07471

Peng Liu, Donghai Mei

{"title":"First-Principles Study on the Monomolecular Isomerization of Ethylbenzene within H-BEA Zeolite","authors":"Peng Liu, Donghai Mei","doi":"10.1021/acs.jpcc.4c07471","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07471","url":null,"abstract":"To decipher the reaction network involving ethylbenzene in the petrochemical industry, the monomolecular isomerization process of ethylbenzene to xylene has been studied using density functional theory. With a combination of ab initio molecular dynamics simulations and metadynamics, free energy landscapes characterizing eight elementary steps, viz., ethylidene/methylene transfer, Buchner and retro-Buchner ring expansion, intramolecular hydride transfer, deprotonation of cationic bicyclo[4.1.0] hydrocarbon, and protonation of norcaradiene, have been determined. The Buchner and retro-Buchner ring expansions are found to be the rate-limiting step with the highest free energy barrier of 205 kJ/mol. While the destruction of the cationic diaryl intermediate via the reverse Friedel–Crafts alkylation step is kinetically comparable. Further charge analysis reveals that the highest free energy barrier for the Buchner and retro-Buchner ring expansion step can be attributed to the electron transfer between two strongly positively charged atom groups. This comprehensive computational study offers valuable insights into the intricate details of the ethylbenzene isomerization process, shedding light on the underlying mechanisms of this important reaction in the petrochemical industry.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"12 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975629","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}

引用次数: 0

Electrochemical Oxidative Desorption of Adsorbed Sulfur Species on (111) Surfaces of Single Crystals of Pure Pt and Pt-Based Bimetallic Alloys 纯Pt及Pt基双金属合金（111）单晶表面吸附硫的电化学氧化脱附

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c06652

Makoto Aoki, Tamao Shishido, Tetsuro Morooka, Takuya Nakanishi, Takuya Masuda

{"title":"Electrochemical Oxidative Desorption of Adsorbed Sulfur Species on (111) Surfaces of Single Crystals of Pure Pt and Pt-Based Bimetallic Alloys","authors":"Makoto Aoki, Tamao Shishido, Tetsuro Morooka, Takuya Nakanishi, Takuya Masuda","doi":"10.1021/acs.jpcc.4c06652","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06652","url":null,"abstract":"The adsorption/desorption behavior of sulfur species at the (111) surfaces of pure Pt and various Pt-based bimetallic alloys, denoted as Pt3M (M = Co, Cu, Fe, Pd), was investigated by electrochemical measurements and X-ray photoelectron spectroscopy (XPS). After the adsorption of elemental sulfur, the current responses characteristic of the adsorption/desorption of hydrogen and hydroxyl species at the sulfur-free bare (111) surfaces completely disappeared, and a doublet peak corresponding to the elemental sulfur appeared in the S 2p region of XPS spectra. The characteristic current responses gradually recovered, simultaneously with the decrease of the S 2p peak, by repeating the potential cycling between −0.2 and 0.8 V vs Ag/AgCl, indicating the oxidative desorption of S species. Except for the Pt3Pd(111) surface, in which Pd has a similar atomic radius to Pt and fully occupied 4d orbitals, the Pt3M(111) surfaces showed higher oxidative desorption capability than those of the pure Pt(111) surface; electrochemically active surface area recovered at the Pt3M(111) surfaces by fewer potential cycles than at the Pt(111) surface. Among the various factors, the downshift of the d-band center due to the ligand effect of foreign metal and the electronic interaction between adsorbed S and Pt are the dominant factors promoting the oxidative desorption of sulfur as well as the strain effect of foreign metal with an atomic radius smaller than Pt.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"22 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975676","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}

引用次数: 0

Theoretical Insight into the Transition-Metal-Embedded Boron Nitride-Doped Graphene Single-Atom Catalysts for Electrochemical Nitrogen Reduction Reaction 过渡金属嵌入氮化硼掺杂石墨烯单原子电化学氮还原反应催化剂的理论研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c04481

Yuan-Hui Xiao, Zi-Wei Ma, Xin-Wei Wu, Lai-Ke Chen, Zubia Sajid, Rajkumar Devasenathipathy, Jian-De Lin, De-Yin Wu, Zhong-Qun Tian

{"title":"Theoretical Insight into the Transition-Metal-Embedded Boron Nitride-Doped Graphene Single-Atom Catalysts for Electrochemical Nitrogen Reduction Reaction","authors":"Yuan-Hui Xiao, Zi-Wei Ma, Xin-Wei Wu, Lai-Ke Chen, Zubia Sajid, Rajkumar Devasenathipathy, Jian-De Lin, De-Yin Wu, Zhong-Qun Tian","doi":"10.1021/acs.jpcc.4c04481","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c04481","url":null,"abstract":"Single-atom catalysts (SACs) have become attractive options for the efficient nitrogen reduction reaction (NRR) because of their unique properties in the activation of nitrogen molecules. As a novel two-dimensional material, boron nitride (BN)-doped graphene has attracted much attention due to its electronic structure, which can be regulated with boron nitride coverage. In the current work, we first screened potential SACs for NRR from various single transition metal atoms embedded in BN-doped graphene (BNC) by using density functional theory (DFT) calculations. Excellent catalytic activity for NRR is demonstrated by the V, Mo, Ru, and Os anchored on the B vacancy and generated SACs, with overpotentials of −0.56, −0.52, −0.60, and −0.61 V vs the standard hydrogen electrode (SHE). Taking advantage of BN-doped graphene electronic structures that can be modified, we further investigated the effect of boron nitride coverage on the SACs’ NRR performance. The electronic structure of the metal center can be altered by controlling the boron nitride coverage, which can further affect the catalytic performance. The potential determining step (PDS) and also the maximal free energy difference vary by modulating the boron nitride coverage. A larger energy range than the hydrogen evolution reaction (HER) is covered by the maximum energy shift between the PDSs, which can reach 0.29 eV. This indicates that by changing the coverage of the BN of the substrate, it is expected to improve the SACs’s catalytic activity and selectivity of NRR. Moreover, it is possible for a pathway to change from one that is adsorption favorable to another one that is thermodynamically favorable of the intermediate NNH. Our results help to clarify the structure–performance correlations and expedite the creation of SACs for ammonia synthesis.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"127 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981713","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}

引用次数: 0

Theoretical Investigation of Polarization-Sensitive Photoresponse in the Donor–Acceptor Interface of Organic Photovoltaic Devices 有机光伏器件施主-受主界面极化敏感光响应的理论研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c06061

Fuzhen Bi, Chiyung Yam, Wu Yang, Junhao Chu, Xichang Bao

{"title":"Theoretical Investigation of Polarization-Sensitive Photoresponse in the Donor–Acceptor Interface of Organic Photovoltaic Devices","authors":"Fuzhen Bi, Chiyung Yam, Wu Yang, Junhao Chu, Xichang Bao","doi":"10.1021/acs.jpcc.4c06061","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06061","url":null,"abstract":"Understanding the photoelectric conversion process is of great significance for the design and preparation of organic photovoltaic devices. In this work, we investigated the intermolecular and intramolecular photoelectric conversion processes and charge transfer characteristics of donor (D) and acceptor (A) materials at the molecular level by using simulation methods. The nonequilibrium Green’s function method is used to calculate the photocurrents excited by incident photons with different polarization directions. The results show that the photocurrents are optical anisotropy, and the maximum responsivity appears along the specific direction that depends on the incident photon energy. The polarization-sensitive photocurrents are attributed to the anisotropic distribution of photogenerated electrons and holes. Moreover, the integrated photocurrents decrease exponentially with the increase in the π–π stacking distance. However, for the photoexcitation by photons with specific energy, such as 1.18 eV, the photocurrents would increase at first and then decrease as the stacking distance increases; this is due to the energy level splitting caused by the π–π stacking of donor and acceptor molecules. This study proposes a new perspective for understanding photoresponse of the D/A interface, which provides theoretical insights for the advancement of polarized light detection and organic optoelectronics.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"91 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975574","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}

引用次数: 0

Solvatochromic Dyes Increase the Sensitivity of Nanosensors 溶剂致变色染料提高纳米传感器的灵敏度

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c07273

Chen Ma, Tanuja Kistwal, Bjoern F. Hill, Krisztian Neutsch, Sebastian Kruss

{"title":"Solvatochromic Dyes Increase the Sensitivity of Nanosensors","authors":"Chen Ma, Tanuja Kistwal, Bjoern F. Hill, Krisztian Neutsch, Sebastian Kruss","doi":"10.1021/acs.jpcc.4c07273","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c07273","url":null,"abstract":"Organic dyes can be chemically tailored to bind specific molecules and act as molecular sensors or probes. However, they bleach, and most of them fluoresce in the UV–vis range. In contrast, nanomaterials such as single-wall carbon nanotubes (SWCNTs) fluoresce in the near-infrared (NIR) tissue transparency window and are extremely stable. Here, we combine solvatochromic dyes with SWCNTs to create molecular sensors and increase their sensitivity. We find that the dyes trans-4-[4-(dimethylamino)styryl]-1-methylpyridinium iodide (t-DSMI) and Reichardt’s dye (Betaine 30) increase the fluorescence responses of DNA-modified SWCNTs to target analytes. With t-DSMI the fluorescence of (GC)15-SWCNT decreases 4 times more in response to pH changes compared to SWCNTs alone. Betaine 30 also boosts the sensitivity of T20-SWCNT for the lipid linoleic acid (LA) more than 2-fold. A kinetic model shows that not the affinity for the analyte but mainly the fluorescence change is increased by the presence of the solvatochromic dyes. This approach provides a flexible design framework to increase the sensitivity of SWCNTs-based biosensors and combines the best of two worlds.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"36 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975583","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}

引用次数: 0

Out-of-Plane Piezoelectricity of V2CXY (X/Y = O, S, Se) MXenes Monolayers for Wearable Devices 可穿戴器件用V2CXY (X/Y = O， S, Se) MXenes单层膜的面外压电性

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c06201

Jiao Zhao, Hao-Hao Yang, Kun Xu, Yan-Ru Kang, Han-Wei Li, Shi-Yun Zheng, Fan Xin, Sheng-Xian Wei, Qi Chen, Fang-Biao Wang, Yi-Ming Cao

{"title":"Out-of-Plane Piezoelectricity of V2CXY (X/Y = O, S, Se) MXenes Monolayers for Wearable Devices","authors":"Jiao Zhao, Hao-Hao Yang, Kun Xu, Yan-Ru Kang, Han-Wei Li, Shi-Yun Zheng, Fan Xin, Sheng-Xian Wei, Qi Chen, Fang-Biao Wang, Yi-Ming Cao","doi":"10.1021/acs.jpcc.4c06201","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06201","url":null,"abstract":"Due to the characteristics of two-dimensional materials, they have demonstrated unique advantages in fields such as piezoelectric devices. Unfortunately, most piezoelectric materials currently do not simultaneously possess excellent piezoelectric effects and mechanical properties. Since the emergence of MXenes, their excellent electrical conductivity and good dynamic and mechanical stability have garnered widespread attention in the energy storage field. Consequently, MXenes are also considered candidates for piezoelectric materials. In this study, the piezoelectric properties and mechanical stability of V2CXY (V2COS, V2CSO, V2COSe, V2CSeO) MXenes monolayers were predicted using first-principles methods based on density functional theory. The results indicate that these four materials exhibit good dynamic, thermodynamic, and mechanical stability. It is noteworthy that due to the structural inversion asymmetry and differences in electronegativity, the structure exhibits strong in-plane piezoelectric effects and excellent out-of-plane piezoelectric effects. In particular, the d33 piezoelectric strain coefficient is 2 to 3 orders of magnitude higher than d22 and d31, with the d33 coefficient of V2CSO reaching up to 313.01 pm/V. This makes these materials highly promising for potential applications in wearable and piezoelectric devices.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"17 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975575","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}

引用次数: 0

Evaluating the Dehydrogenation Performance of Cyclohexane on Pt-Skin AgPt3(111) and Ag3Pt(111) Surface Slabs: A Density Functional Theory Approach 评价环己烷在pt -蒙皮AgPt3（111）和Ag3Pt（111）表面板上的脱氢性能：密度泛函理论方法

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c05825

Desalegn Nigatu Gemechu, Kingsley Onyebuchi Obodo, Ahmed Mustefa Mohammed, Yedilfana Setarge Mekonnen

{"title":"Evaluating the Dehydrogenation Performance of Cyclohexane on Pt-Skin AgPt3(111) and Ag3Pt(111) Surface Slabs: A Density Functional Theory Approach","authors":"Desalegn Nigatu Gemechu, Kingsley Onyebuchi Obodo, Ahmed Mustefa Mohammed, Yedilfana Setarge Mekonnen","doi":"10.1021/acs.jpcc.4c05825","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05825","url":null,"abstract":"The development of highly effective dehydrogenation catalysts presents significant potential for storing hydrogen solutions with favorable economic advantages. In this study, we examined the dehydrogenation of cyclohexane on Pt-skin AgPt3(111) and Ag3Pt(111) surfaces in comparison with that on a Pt(111) pristine surface by applying density functional theory. We assessed the performance of various exchange–correlation functionals (PBE, BEEF-vdW, optPBE-vdW, and PBE-D3) in predicting the adsorption energy of cyclohexane on Pt–AgPt3(111), Pt–Ag3Pt(111), and Pt(111) surfaces and compared them to the experimental data. Through systematic calculations, we analyzed the electronic and structural properties of catalysts, adsorption energies of cyclohexane and intermediate molecules on various Ag–Pt alloy surfaces, surface charge distribution, dehydrogenation processes, and the effect of Ag concentration on its activity. The findings indicate that an increase in the Ag content leads to a closer shift of the d-band center of the Pt atom toward the Fermi level, moving from −2.31 to −1.81 eV. This shift increases surface charge accumulation. This gradual accumulation enhances the adsorption of cyclohexane. Notably, the dehydrogenation of cyclohexane on Pt-skin Ag3Pt exhibited a lower reaction energy, with a value of 1.31 eV compared to the pristine Pt(111) catalyst. This study revealed that the Pt-skin Ag3Pt(111) catalyst exhibits enhanced performance for the dehydrogenation of cyclohexane, which should stimulate additional experimental studies.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"82 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975573","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}

引用次数: 0

Unraveling the Effects of Reducing and Oxidizing Pretreatments and Humidity on the Surface Chemistry of the Ru/CeO2 Catalyst during Propane Oxidation 还原氧化预处理和湿度对丙烷氧化过程中Ru/CeO2催化剂表面化学性质的影响

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c08033

Thu Ngan Dinhová, Oleksii Bezkrovnyi, Lesia Piliai, Ivan Khalakhan, Samiran Chakraborty, Maciej Ptak, Piotr Kraszkiewicz, Mykhailo Vaidulych, Michal Mazur, Štefan Vajda, Leszek Kepinski, Michael Vorochta, Iva Matolínová

{"title":"Unraveling the Effects of Reducing and Oxidizing Pretreatments and Humidity on the Surface Chemistry of the Ru/CeO2 Catalyst during Propane Oxidation","authors":"Thu Ngan Dinhová, Oleksii Bezkrovnyi, Lesia Piliai, Ivan Khalakhan, Samiran Chakraborty, Maciej Ptak, Piotr Kraszkiewicz, Mykhailo Vaidulych, Michal Mazur, Štefan Vajda, Leszek Kepinski, Michael Vorochta, Iva Matolínová","doi":"10.1021/acs.jpcc.4c08033","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c08033","url":null,"abstract":"This work investigates the surface chemistry of the Ru/CeO2 catalyst under varying pretreatment conditions and during the oxidation of propane, focusing on both dry and humid environments. Our results show that the Ru/CeO2 catalyst calcined in O2 at 500 °C initiates propane oxidation at 200 °C, achieves high conversion rates above 400 °C, and demonstrates almost no change in activity in the presence of water vapor across the entire studied temperature range of 200–500 °C. Prereduction of the oxidized Ru/CeO2 catalyst in H2 significantly enhances its activity, though this enhancement diminishes at higher temperatures. Adding water to the reaction mixture boosts the low-temperature activity of the prereduced catalyst but decreases it at 300–400 °C. Several ex-situ analytical techniques in combination with the in-situ NAP-XPS analysis reveal that while exposed to oxygen, Ru nanoparticles on the ceria surface oxidize to form RuO2 below 200 °C and volatile RuOx (x > 2) at higher temperatures. The presence of water vapor in the reaction mixture leads to the transformation of RuO2 into ruthenium hydroxide at 200 °C, which, in turn, facilitates propane oxidation. At higher temperatures, the water does not have much influence on the oxidation state of Ru but slightly inhibits its evaporation from the surface. It is also demonstrated that Ru in the Ru/CeO2 catalyst exists predominantly in the Run+ (n > 4) oxidation states at typical VOC oxidation temperatures rather than the expected Ru4+ state.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"43 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975577","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}

引用次数: 0

Prediction of the TiS2 Bilayer with Self-Intercalation: Robust Ferromagnetic Semiconductor with a High Curie Temperature 具有自插层的TiS2双分子层的预测：高居里温度的稳健铁磁半导体

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-01-14 DOI: 10.1021/acs.jpcc.4c06216

Fangyu Zhang, Linhui Lv, Zihao Xu, Diancong Qi, Weiyi Wang, Xingxing Li, Ya Su, Yanyan Jiang, Zhaoyong Guan

{"title":"Prediction of the TiS2 Bilayer with Self-Intercalation: Robust Ferromagnetic Semiconductor with a High Curie Temperature","authors":"Fangyu Zhang, Linhui Lv, Zihao Xu, Diancong Qi, Weiyi Wang, Xingxing Li, Ya Su, Yanyan Jiang, Zhaoyong Guan","doi":"10.1021/acs.jpcc.4c06216","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c06216","url":null,"abstract":"The search for new two-dimensional magnetic materials has been a hot topic since the discovery of graphene in 2004 as these materials play a crucial role in fields such as spintronics. In this study, we systematically investigated the 2H-TiS2 bilayer with self-intercalation (SI) of the Ti atom, revealing that SI can introduce magnetism to a nonmagnetic 2H-TiS2. Taking Ti19S36-AB stacking as an example, we find that 2H–SI–TiS2 exhibits a ferromagnetic order with a Curie temperature of 377 K. Ti19S36 shows perpendicular magnetic anisotropy, with a magnetic anisotropy energy (MAE) of 7.43 × 10–2 meV. Additionally, the MAE increases as the self-intercalated Ti’s (TiSI) concentration (x) decreases, attributed to the enhanced hybridization interaction between the dx2–y2 and dxy orbitals of Ti atoms. Ti19S36-AB stacking is identified as a bipolar magnetic semiconductor (BMS) with an indirect band gap of 0.53 eV. As x increases, TimSn transitions from BMS to half-semiconductor (HSC) and metal and then back to HSC, demonstrating a rich phase. TimSn shows good dynamic and thermodynamic stabilities at 300 and 500 K, respectively. Furthermore, the formation energy (εf) of TimSn increases monotonically with rising x. Moreover, TimSn can be easily synthesized under higher μTi. The migration barrier of TiSI between adjacent coordination sites is 0.740 eV, further confirming the stability of the self-intercalated structure. These findings imply the potential of 2H-TiS2 and nonmagnetic transition metal dichalcogenides in spintronics.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"2 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981714","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}

引用次数: 0