Surface Science最新文献

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Physical processes in coadsorption of oxygen and carbon on the W(100) surface: influence of atomic carbon dissolved in the bulk 氧和碳在W（100）表面共吸附的物理过程：溶解在体中的原子碳的影响

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-15 DOI: 10.1016/j.susc.2025.122837

E.V. Rut’kov, E.Y. Afanas’eva, N.R. Gall

Interaction between atomic oxygen and carbon on the W(100) surface is being considered in the wide range of temperatures (300 - 2000 K) and concentrations of both adsorbates. Oxygen atoms do not dissolve in the substrate bulk and leave the surface in the form of CO molecules. In the case of initially pure tungsten bulk and at oxygen and carbon coverage ϑ ≈ 0.5 these atoms peacefully coexist on the surface without forming CO molecules up to T ∼ 1050 K; at higher temperatures C atoms are displaced from the surface into the bulk, in the dissolved state. At T > 1400 K, the dissolved carbon atoms come to the surface, forming CO molecules with adsorbed oxygen which are desorbed. Complete purification of the surface is achieved at 1600 K. Carbon atoms predissolved in the tungsten bulk significantly influence the processes of CO molecules formation. In the presence of C atoms preliminary dissolved in the tungsten bulk, the reaction of CO formation with subsequent desorption starts at 800 K, and complete oxygen removal is observed at 1200 K.

在W（100）表面原子氧和碳之间的相互作用被考虑在很宽的温度范围内（300 - 2000 K）和两种吸附剂的浓度。氧原子不溶解在基体中，而是以CO分子的形式离开表面。在最初纯钨体的情况下，在氧和碳覆盖度（≈0.5）时，这些原子在表面和平共存，不形成CO分子，直至T ~ 1050 K；在较高的温度下，C原子从表面转移到体中，处于溶解状态。在1400k时，溶解的碳原子来到表面，与吸附的氧形成CO分子，并被解吸。在1600k的温度下可以完全净化表面。预溶在钨体中的碳原子显著影响CO分子的形成过程。在C原子初步溶解于钨体的情况下，在800 K时开始CO生成和随后的脱附反应，在1200 K时观察到完全脱氧。

引用次数: 0

Density functional theory study of adsorption of dissolved gas in transformer oil on Nb -doped SnS2 monolayer 掺铌SnS2单层吸附变压器油中溶解气体的密度泛函理论研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-15 DOI: 10.1016/j.susc.2025.122836

Chunlu Wan , Junhua Wang , Xia Deng , Miao Wang , Xiaolan Yang

Based on the density functional theory (DFT), It was found that the adsorption capacity of C₂H₂, CO and H₂ on intrinsic SnS₂ was weak, and CH₄ on intrinsic SnS₂ was strong. Meanwhile, the adsorption energies of these five gas molecules on their surfaces are increased to different degrees. Among them, the adsorption capacity of C₂H₂ on Nb/SnS₂ is stronger, with an adsorption energy of -1.365 eV. From the point of view of the recovery time after adsorption of the gases, at a temperature equal to 498 K, the recovery time of C₂H₂ gas molecules on Nb/SnS₂ is 64.5 s, which makes it a promising gas-sensitive sensor for C₂H₂. The results show that the replacement of S atoms by Nb atoms in the doping of SnS₂ improves the gas adsorption performance of the SnS₂ material, and at the same time, its preparation method is close to the reality, and it can be considered to be used as a material for making gas sensors.

基于密度泛函理论（DFT），发现C2H2、CO和H2在本征SnS2上的吸附能力较弱，CH4在本征SnS2上的吸附能力较强。同时，这五种气体分子在其表面的吸附能都有不同程度的提高。其中，C2H2对Nb/SnS2的吸附能力较强，吸附能为-1.365 eV。从气体吸附后的回收时间来看，在498 K的温度下，C2H2气体分子在Nb/SnS2上的回收时间为64.5 s，是一种很有前途的C2H2气敏传感器。结果表明，SnS2掺杂中以Nb原子取代S原子提高了SnS2材料的气体吸附性能，同时其制备方法接近实际，可以考虑作为制作气体传感器的材料。

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引用次数: 0

Effect of biaxial tensile strain on the photovoltaic properties of O-doped monolayer SnSe2: a first-principles study 双轴拉伸应变对o掺杂单层SnSe2光电性能影响的第一性原理研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-13 DOI: 10.1016/j.susc.2025.122829

Xinning Li, Lu Yang, Hangqing Wu, Liqun Wu, Ruiyuan Li

In this study, we investigate the synergistic modulation mechanism of non-metallic element O doping and biaxial tensile strain on the electronic structure and optical properties of monolayer SnSe₂ materials based on DFT. In particular, oxygen doping can transform SnSe₂ from an indirect bandgap to a direct bandgap, thus improving its photoelectric conversion efficiency. After applying biaxial tensile strains (2 %-8 %), the bandgap of the O-doped system shows a nonlinear change, which increases to 0.458 eV at 4 % strain and maintains semiconducting properties. In terms of optical properties, O- doped with strain regime significantly improves static dielectric constant (up to 4.03 at 8 % strain) and the light absorption efficiency, and the reflectance in the UV region decrease to 0.13, indicating a significant enhancement of the photovoltaic conversion performance. It has been shown that the 2D Materials semiconductor SnSe₂ can significantly improve the carrier mobility and light absorption efficiency of the material in the doping and stretching regime, which lays the foundation for the development of high-efficiency optoelectronic devices.

在这项研究中，我们研究了非金属元素O掺杂和双轴拉伸应变对基于DFT的单层SnSe2材料的电子结构和光学性质的协同调制机制。特别是，氧掺杂可以将SnSe2从间接带隙转变为直接带隙，从而提高其光电转换效率。在施加双轴拉伸应变（2% ~ 8%）后，掺o体系的带隙呈现非线性变化，在4%应变下增加到0.458 eV，并保持半导体性能。光学性能方面，应变掺O显著提高了材料的静态介电常数（8%应变下可达4.03）和光吸收效率，紫外区反射率降至0.13，光伏转换性能显著增强。研究表明，在掺杂和拉伸状态下，2D Materials半导体SnSe2可以显著提高材料的载流子迁移率和光吸收效率，这为开发高效光电器件奠定了基础。

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引用次数: 0

Tunable electronic structures of two-dimensional ZnO bilayers with different stacking 不同堆叠方式的二维ZnO双分子层的可调谐电子结构

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-13 DOI: 10.1016/j.susc.2025.122833

Hongduo Hu , Zhihua Xiong , Juanli Zhao , Lanli Chen

Two-dimensional ZnO materials have recently attracted widespread research attention for their promising properties, chemical stability, and mechanical strength. These special properties make them not only imply a scientific interest but also indicate great technological applications in optoelectronics, photonics, and sensors. Herein, based on the first-principles calculations with the HSE06 potential, the atomic structures and electronic properties of ZnO bilayer with different stacking are investigated. The results demonstrate that AB-stacking is the most energetically favorable configuration among all those considered. The AB-stacking is mechanically and dynamically stable. The calculated band gap is 2.88 eV using the HSE06 potential and 1.45 eV using the PBE potential. Moreover, we found that it is possible to modulate the energy bandgap both by the type of bilayer stacking and by the effect of the biaxial strain and interfacial distance. The ability to tune the energy bandgap in ZnO bilayers by adjusting their geometric configuration or applying an external strain or changing the interfacial distance could inspire new applications in various technological fields.

近年来，二维氧化锌材料因其良好的性能、化学稳定性和机械强度而引起了广泛的研究关注。这些特殊的性质使它们不仅具有科学意义，而且在光电子学、光子学和传感器方面也有很大的技术应用。本文基于HSE06势第一性原理计算，研究了不同堆叠方式ZnO双分子层的原子结构和电子性能。结果表明，在所有考虑的构型中，ab层是能量最有利的构型。ab -堆垛是机械和动态稳定的。使用HSE06电势计算的带隙为2.88 eV，使用PBE电势计算的带隙为1.45 eV。此外，我们还发现可以通过双层堆积类型以及双轴应变和界面距离的影响来调节能带隙。通过调整ZnO双分子层的几何结构或施加外部应变或改变界面距离来调节ZnO双分子层的能带隙，可以在各种技术领域激发新的应用。

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引用次数: 0

A DFT study on the electrocatalytic water splitting performance of heterostructure Bi2S3/Ni3S2 异质结构Bi2S3/Ni3S2电催化水裂解性能的DFT研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-13 DOI: 10.1016/j.susc.2025.122832

Dan Yi , Xiao Chen , Wanfei Cai , Laicai Li

The global environmental pollution issue is becoming increasingly severe, making the design of efficient and cost-effective bifunctional electrocatalysts an important and highly valuable area of research. This paper investigates the electrocatalytic performance of the Bi₂S₃/Ni₃S₂ heterostructure for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) using density functional theory (DFT). The catalytic performance for HER is evaluated by the change in Gibbs free energy of hydrogen atom adsorption on the catalyst surface (|∆G* H|), while the overpotential (η) is used to assess the catalytic performance for OER. The calculations reveal that the Bi₂S₃/Ni₃S₂ heterostructure exhibits a low overpotential of -0.098/0.85 V, outperforming the electrocatalytic performance of Ni₃S₂, making it a promising bifunctional electrocatalyst. By analyzing its electronic structure and charge transfer behavior, it is demonstrated that the enhanced catalytic performance is primarily attributed to the Bi₂S₃/Ni₃S₂ heterostructure, which contributes to high conductivity, a high density of states near the valence band maximum, and more stable H₂O adsorption. Furthermore, the effect of impurity atoms on the catalytic performance of Bi₂S₃/Ni₃S₂ is examined. The results indicate that doping Co into Ni₃S₂ enhances the electrocatalytic performance of the Bi₂S₃/Ni₃S₂ heterostructure.

随着全球环境污染问题的日益严重，设计高效、经济的双功能电催化剂成为一个重要且极具价值的研究领域。利用密度泛函理论（DFT）研究了Bi2S3/Ni3S2异质结构对析氢反应（HER）和析氧反应（OER）的电催化性能。用催化剂表面氢原子吸附的吉布斯自由能变化量（|∆G* H|）评价HER的催化性能，用过电位（η）评价OER的催化性能。计算结果表明，Bi2S3/Ni3S2异质结构具有-0.098/0.85 V的过电位，优于Ni3S2的电催化性能，是一种很有前途的双功能电催化剂。通过对其电子结构和电荷转移行为的分析，表明催化性能的增强主要归功于Bi2S3/Ni3S2的异质结构，该异质结构具有较高的电导率，在价带最大值附近具有较高的态密度，并且对H2O的吸附更稳定。此外，还考察了杂质原子对Bi2S3/Ni3S2催化性能的影响。结果表明，在Ni3S2中掺杂Co提高了Bi2S3/Ni3S2异质结构的电催化性能。

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引用次数: 0

Temperature-dependent optical transmittance and gas sensing mechanism of MnSnO3 nanocrystalline thin-films through the nebulizer spray pyrolysis (NSP) technique 雾化器喷雾热解（NSP）技术制备二氧化锰纳米晶薄膜的温度依赖光学透过率和气敏机理

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-12 DOI: 10.1016/j.susc.2025.122828

P. Usha , Somoju Ramesh , G. Srinivas , P. Jayamurugan , R. Mariappan

In this work, nanocrystalline MnSnO₃ thin films were successfully synthesized using the nebulizer spray pyrolysis technique at substrate temperatures ranging from 300 °C to 600 °C. X-ray diffraction (XRD) analysis confirmed the polycrystalline rhombohedral structure, with crystallite size increasing from 25 nm at 300 °C to 42 nm at 600 °C. Scanning electron microscopy (SEM) revealed spherical grains at lower temperatures transitioning to larger, plate-like grains (∼110 nm) at 600 °C due to thermally activated grain growth. Energy-dispersive X-ray spectroscopy (EDAX) confirmed the elemental composition, and HRTEM-SAED analysis validated high crystalline quality. Optical studies showed that transmittance increased with temperature, and the optical band gap widened from 2.03 eV to 2.50 eV. Gas sensing experiments demonstrated that the films exhibited a maximum sensitivity of 6.7 at 250 ppm ammonia concentration, with impedance spectra indicating significant changes in electrical behavior upon gas exposure. These results highlight the potential of MnSnO₃ thin films for use in high-performance, cost-effective ammonia gas sensors.

在这项工作中，利用雾化器喷雾热解技术在300 ~ 600℃的衬底温度下成功地合成了纳米晶MnSnO₃薄膜。x射线衍射（XRD）分析证实了多晶菱面体结构，晶粒尺寸从300℃时的25 nm增加到600℃时的42 nm。扫描电镜（SEM）显示，由于热激活晶粒生长，低温下的球形晶粒在600℃时转变为较大的片状晶粒（~ 110 nm）。能量色散x射线光谱（EDAX）证实了元素组成，HRTEM-SAED分析证实了高晶体质量。光学研究表明，透射率随温度升高而增加，带隙从2.03 eV扩大到2.50 eV。气敏实验表明，在氨浓度为250 ppm时，膜的最大灵敏度为6.7，阻抗谱表明在气体暴露时电行为发生了显著变化。这些结果突出了MnSnO₃薄膜用于高性能、经济高效的氨气传感器的潜力。

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引用次数: 0

Adsorption of CO2 on N-doped carbon materials: the effect of the subsurface layer n掺杂碳材料对CO2的吸附：次表层的影响

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-08 DOI: 10.1016/j.susc.2025.122819

Kirill A. Dmitruk , Ignat A. Podolyako , Dmitry A. Shlyapin , Aleksandr A. Shubin , Olga V. Netskina

In this work, density functional theory (DFT) was employed to study CO₂ adsorption on graphite sheets with different types of nitrogen-containing adsorption sites: graphitic-N, pyrrolic-N, pyridinic-N. A periodic graphite model consisting of two layers was used in this study, and many-body dispersion (MBD) corrections were utilized to accurately account for the interactions between the graphite layers and the CO₂ molecule. For the first time, the effect of the subsurface graphite layer on the CO₂ adsorption properties of nitrogen-doped carbon materials was investigated. It was shown that the substitution of carbon atoms with nitrogen results in a redistribution of the electron density between the surface and the subsurface layer, especially in the presence of a carbon vacancy. The electron density redistribution on the graphite surface has a significant impact on CO₂ adsorption energy, the distance between the surface and the adsorbate molecule, and the geometry of CO₂ during its interaction with the graphite layer. CO₂ adsorption energy was found to increase in comparison to that on pristine graphite in the case of carbon materials containing one graphitic-N site or pyridinic-N sites with a varying (1–3) number of nitrogen atoms, allowing the regulation of adsorption properties.

本文采用密度泛函理论（DFT）研究了石墨片上不同含氮位点（石墨- n、吡咯- n、吡啶- n）对CO2的吸附。本研究采用了一个由两层组成的周期石墨模型，并利用多体色散（MBD）修正准确地解释了石墨层与CO2分子之间的相互作用。首次研究了亚表面石墨层对氮掺杂碳材料CO2吸附性能的影响。结果表明，氮原子取代碳原子会导致表面和亚表面层之间电子密度的重新分布，特别是在存在碳空位的情况下。石墨表面的电子密度重分布对CO2吸附能、表面与吸附物分子的距离以及CO2与石墨层相互作用时的几何形状有显著影响。与原始石墨相比，在含有一个石墨- n位点或含有不同（1-3）个氮原子数量的吡啶- n位点的碳材料中，二氧化碳吸附能增加，从而可以调节吸附性能。

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引用次数: 0

Cohesion strength and fracture toughness of V-Mo2C interfaces from first principles calculation 用第一性原理计算V-Mo2C界面的内聚强度和断裂韧性

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-07 DOI: 10.1016/j.susc.2025.122818

L.C. Liu , J.T. Zheng , Z.Y. Xu , S.F. Zhou

First principles calculations demonstrate that interface orientation critically governs cohesion properties in V-Mo₂C interfaces systems. Specifically, incorporating Mo₂C(100) or (111) onto V(110) enhances cohesive strength and fracture toughness, whereas Mo₂C(100) on V(100) reduces these properties. In addition, the V-Mo₂C interfaces formed by epitaxial Mo₂C growth on V substrates show superior cohesion compared to V on Mo₂C interfaces. The interface orientation critically determines interface properties of V-Mo₂C. These finding align with reported experimental observations in the literature, providing mechanistic insights into cohesion properties and fracture toughness of V-Mo₂C interfaces.

第一性原理计算表明，界面取向对V-Mo2C界面系统的内聚性能起关键作用。具体来说，在V（110）上掺入Mo2C（100）或（111）可以增强内聚强度和断裂韧性，而在V（100）上掺入Mo2C（100）则会降低这些性能。此外，在V衬底上外延生长Mo2C形成的V-Mo2C界面比V在Mo2C界面上的内聚力更强。界面取向决定了V-Mo2C的界面性能。这些发现与文献中报道的实验观察结果一致，为V-Mo2C界面的内聚性能和断裂韧性提供了机制见解。

引用次数: 0

The influence of alkali and alkaline earth substitution on the reduction of Fe2O3[001] by H2 – a DFT study 碱和碱土取代对H2 - a - DFT还原Fe2O3的影响[001]

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-05 DOI: 10.1016/j.susc.2025.122816

Saeid Khesali Azadi , Matti Alatalo , Marko Huttula , Timo Fabritius , Samuli Urpelainen

The reactivity of Fe₂O₃ oxygen carriers (OCs) in the presence of alkali and alkaline earth metal substitutions was investigated using density functional theory (DFT) to enhance their reduction behavior. Our calculations reveal that these substitutions preferentially occupy surface sites on Fe₂O₃[001], rather than the bulk. Compared to alkaline earth metals, the surface oxygen vacancy formation energy (E_vac), a measure of reducibility, is substantially lower near alkali substitutions, indicating more oxygen release. Additionally, we investigated H₂ oxidation and adsorption on pure and Na-substituted Fe₂O₃[001] surfaces that have an oxygen vacancy. Adsorption energies demonstrate that H₂ preferentially dissociates on O top and hollow sites rather than on Fe-related sites. The oxidation of H₂ is both thermodynamically and kinetically more advantageous on O sites, resulting in the production of H₂O via either direct adsorption or H atom migration pathways. Conversely, Fe sites demonstrate elevated steric hindrances and reduced reactivity. Finally, oxygen migration from the bulk to the surface was identified as a mechanism driven by high temperatures, which may influence oxygen availability during cycling. These findings offer essential understanding of the impact of substitutions on the redox behavior of Fe₂O₃ OCs, relevant to applications in chemical looping and sustainable hydrogen consumption.

采用密度泛函理论（DFT）研究了Fe2O3氧载体（OCs）在碱金属和碱土金属取代物存在下的反应性。我们的计算表明，这些取代优先占据Fe2O3的表面位置[001]，而不是大块。与碱土金属相比，表面氧空位形成能（Evac），一种还原性的度量，在碱取代附近明显较低，表明更多的氧释放。此外，我们还研究了H2在具有氧空位的纯Fe2O3和na取代Fe2O3[001]表面上的氧化和吸附。吸附能表明H2优先在O顶和空心位点而不是铁相关位点解离。H2在O位上的氧化在热力学和动力学上都更有利，从而通过直接吸附或H原子迁移途径生成H2O。相反，铁位表现出空间位阻升高和反应性降低。最后，氧从体向表面的迁移被确定为高温驱动的机制，这可能影响循环过程中的氧可用性。这些发现对取代对Fe2O3氧化还原行为的影响提供了重要的理解，与化学环和可持续氢消耗的应用有关。

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引用次数: 0

Theoretical investigation of transition metal-doped CrSe₂ monolayer as a high-performance gas sensor for CO, SO₂, NO, and NO₂ detection 过渡金属掺杂CrSe₂单层作为CO、SO₂、NO和NO₂检测的高性能气体传感器的理论研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-08-04 DOI: 10.1016/j.susc.2025.122814

Liujie Yang , Xiaolei Li , Tiantian Xu , Jiahao Yang , Tengfei Wang

This study investigates the adsorption and sensing properties of H-CrSe₂ monolayers doped with gold (Au) and silver (Ag) for detecting four toxic gases. First-principles calculations were performed to analyze the formation energy, structural changes, charge transfer, and density of states before and after gas adsorption. Meanwhile, molecular dynamics simulations at 300 K confirmed the stability of Ag/Au-CrSe₂ materials at room temperature. The results show that the adsorption energies of Ag/Au-CrSe₂ for these four gases range between 0.5 eV and 1.2 eV, indicating that the doping of Ag and Au atoms enhances the material's performance while preventing excessive adsorption that could lead to prolonged recovery times. Additionally, under 2 % biaxial tensile strain, the recovery times of Ag/Au-CrSe₂ for these four gases were significantly reduced to below 2 seconds. This study supports the application of H-CrSe₂ materials as gas sensors in environmental monitoring and industrial emission control.

本文研究了掺杂金（Au）和银（Ag）的H-CrSe₂单层膜对四种有毒气体的吸附和传感性能。利用第一性原理计算分析了气体吸附前后的地层能量、结构变化、电荷转移和态密度。同时，300 K下的分子动力学模拟证实了Ag/Au-CrSe 2材料在室温下的稳定性。结果表明，Ag/Au- crse 2对这四种气体的吸附能在0.5 eV ~ 1.2 eV之间，表明Ag和Au原子的掺杂提高了材料的性能，同时防止了过度吸附导致恢复时间延长。此外，在2%的双轴拉伸应变下，Ag/Au-CrSe 2对这四种气体的恢复时间显著缩短至2秒以下。本研究支持了H-CrSe₂材料作为气体传感器在环境监测和工业排放控制中的应用。

引用次数: 0

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