Surface Science最新文献

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Mechanistic insights into the oxygen reduction reaction on the Fe-N4/C single-atom catalysts: Spectator species and solvent as the key driving force Fe-N4/C单原子催化剂氧还原反应机理研究：旁观物质和溶剂为关键驱动力

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-11-01 DOI: 10.1016/j.susc.2025.122875

Chaofang Deng , Can Deng , Shiwen Hu , Yanrong Ren

Noble-metal-free catalysts, such as metal-nitrogen-carbon (M-N-C) materials, have attracted significant attention owing to their excellent electrocatalytic activity toward the oxygen reduction reaction (ORR). Among them, FeN₄ single-atom catalysts embedded in graphene have been extensively investigated as promising ORR catalysts. However, the reaction mechanism still remains controversial, and the predicted potential deviates from experimental observations. In this work, we employed DFT calculations to elucidate the ORR mechanism taking the solvation effect into consideration. The results reveal that the central Fe atom is covered by *O_2, which acts as a modifying ligand to optimize the adsorption of reaction intermediates, yielding a theoretical limiting potential of 0.61 V. When solvation is included, the limiting potential increases to 0.78 V (implicit solvent) and 0.71 V (explicit solvent), in good agreement with experimental values. The enhanced catalytic activity originated from solvent stabilization of the adsorbed ORR intermediates via hydrogen bonding, which facilitates the overall reaction process. The solvent effect is particularly pronounced for the *OH species, whose adsorption is significantly stabilized by explicit water molecules, thereby hindering further reduction of *OH/*OH and rendering the O₂-mediated mechanism is more favorable for FeN₄ in explicit solvent surroundings. Finally, by incorporating the applied potential through a constant-potential model, the limiting potential reaches approximately 0.8 V, consistent with the experimental findings. This work demonstrates the necessity of assessing the effect of solvent and would help design better ORR electrocatalysts.

无贵金属催化剂，如金属-氮-碳（M-N-C）材料，由于其对氧还原反应（ORR）的优异电催化活性而受到人们的广泛关注。其中，石墨烯包埋的FeN4单原子催化剂作为极具发展前景的ORR催化剂得到了广泛的研究。然而，反应机理仍存在争议，预测电位与实验观测值存在偏差。在这项工作中，我们采用DFT计算来阐明考虑溶剂化效应的ORR机理。结果表明，中心Fe原子被*O2覆盖，作为修饰配体优化了反应中间体的吸附，其理论极限电位为0.61 V。当考虑溶剂作用时，极限电位增加到0.78 V（隐式溶剂）和0.71 V（显式溶剂），与实验值吻合较好。催化活性的增强是由于吸附的ORR中间体通过氢键使溶剂稳定，从而促进了整个反应过程。溶剂效应对于*OH尤为明显，其吸附被外显水分子显著稳定，从而阻碍了*OH/*OH的进一步还原，使得在外显溶剂环境下o2介导的机制更有利于FeN4。最后，通过恒电位模型加入外加电位，得到极限电位约为0.8 V，与实验结果一致。这一工作证明了评估溶剂影响的必要性，并有助于设计更好的ORR电催化剂。

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引用次数: 0

Real-space imaging and X-ray photoelectron spectroscopy of nitrogen segregation structures on Fe(100) Fe（100）表面氮偏析结构的实空间成像和x射线光电子能谱

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-25 DOI: 10.1016/j.susc.2025.122874

Markus Soldemo, Jonas Weissenrieder

Surface nitrogen structures on Fe(100) obtained by bulk-to-surface nitrogen segregation are studied using a combination of high-resolution X-ray photoelectron spectroscopy (XPS) and real-space imaging using scanning tunneling microscopy (STM). The core-level XPS N 1s results show one sharp peak, suggesting that the N atoms are mainly located in one site. The binding energy is consistent with the literature value of the Fe(100)/c(2 × 2)-N structure, for which the nitrogen atoms reside in four-fold hollow sites. Furthermore, the STM-images show regions of well-ordered Fe(100)/c(2 × 2)-N structure and regions with a high density of anti-phase domain boundaries. Regions with narrow stripe-like, 3 N atoms wide, anti-phase c(2 × 2)-N domains were observed. The anti-phase domain boundaries between the stripe-shaped domains have higher N coverage than within large well-ordered Fe(100)/c(2 × 2)-N domains.

利用高分辨率x射线光电子能谱（XPS）和扫描隧道显微镜（STM）实空间成像相结合的方法，研究了通过体-表面氮偏析获得的Fe（100）表面氮的结构。核能级XPS N - 1s结果有一个尖峰，表明N原子主要集中在一个位置。结合能与Fe(100)/c(2 × 2)-N结构的文献值一致，其中氮原子位于四重空心位。此外，stm图像显示出有序的Fe(100)/c(2 × 2)-N结构区域和高密度的反相畴边界区域。观察到具有窄条纹状，宽3n原子，反相c(2 × 2)-N畴的区域。条形畴之间的反相畴边界比大的有序Fe(100)/c(2 × 2)-N畴具有更高的N覆盖率。

引用次数: 0

Site - specific chemisorption of H2 on the V2O5(010) surface: Unveiling active sites and configurational selectivity via first - principles DFT H2在V2O5（010）表面的位点特异性化学吸附：通过第一性原理DFT揭示活性位点和构型选择性

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-20 DOI: 10.1016/j.susc.2025.122872

Yi Wu , Qi Lai , Jianxun Cai , Jinliang Chen , Chuanhai Xiao , Xiguang Zhao

This study investigates the microscopic mechanism of the hydrogen reduction on orthorhombic vanadium pentoxide (α-V₂O₅, space group Pmmn) using density functional theory (DFT) with the Hubbard U correction method. A V₂O₅(010) surface model incorporating more than ten typical adsorption configurations was constructed. Through geometric optimization and energy convergence analysis, we clarified the differential adsorption behaviors of H₂ molecules induced by configurational variations and surface peaks/valleys revealing the correlation between the topological structure of the V₂O₅(010) surface and its catalytic activity. Our results show that only bridging oxygen sites on the V₂O₅(010) surface adsorption occurs exclusively at; however, due to the presence of surface peaks and valleys, two distinct adsorption types exist, and H₂ molecules with specific structural arrangements are more prone to adsorption.

本研究利用密度泛函理论（DFT）和Hubbard U校正方法研究了正交五氧化钒（α-V₂O₅，空间群Pmmn）氢还原的微观机理。建立了包含十多种典型吸附构型的V2O5（010）表面模型。通过几何优化和能量收敛分析，我们明确了构型变化和表面峰/谷诱导的H₂分子的差异吸附行为，揭示了V2O5（010）表面拓扑结构与其催化活性之间的相关性。我们的研究结果表明，只有桥接氧位在V2O5（010）表面的吸附只发生在；但由于表面峰谷的存在，存在两种不同的吸附类型，具有特定结构排列的H2分子更容易被吸附。

引用次数: 0

First-principles investigation of electrified monolayered MoS2/water interface 带电单层MoS2/水界面的第一性原理研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-17 DOI: 10.1016/j.susc.2025.122870

Fabien Mortier , Di Zhao , Minoru Otani , Samuel Bernard , Yun Wang , Assil Bouzid

We investigate electrochemical properties of electrified MoS

_{2}

/water interface under applied bias potential. We show that water molecules rearrange depending on whether the surface is positively or negatively charged. A positive charge pulls water’s oxygen atoms closer to the surface, while extra electrons make water flip so that hydrogen atoms get nearer the surface. Abrupt changes are observed in the double layer charge and in the capacitance evolution as a function of bias potential and are explained by semiconductor nature of the MoS

_{2}

material. Overall, our findings confirm earlier results on the water dynamics at electrified metal–water interfaces and highlight that using explicit and hybrid modeling approaches helps to capture the fine details of electrochemical processes at solid/liquid interfaces.

研究了在外加偏置电位作用下，电化二硫化钼/水界面的电化学性质。我们表明水分子的重新排列取决于表面是带正电荷还是带负电荷。正电荷使水的氧原子更靠近表面，而额外的电子使水翻转，使氢原子更靠近表面。观察到双层电荷和电容随偏置电位的突变，这可以用二硫化钼材料的半导体性质来解释。总的来说，我们的研究结果证实了之前关于带电金属-水界面水动力学的结果，并强调使用显式和混合建模方法有助于捕捉固体/液体界面电化学过程的细节。

引用次数: 0

SO2 oxidation with H2O on low surface coverage Pt(111): A density functional theory investigation 水在低表面覆盖率Pt（111）上氧化SO2：密度泛函理论研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-15 DOI: 10.1016/j.susc.2025.122869

Theunis Nel , Jean Isabelle du Toit , Hermanus Cornelius Moolman Vosloo , Cornelia Gertina Catharina Elizabeth van Sittert

Despite recent advances towards understanding SO₂ oxidation to H₂SO₄ and H₂ on Pt, uncertainties regarding the reaction mechanism and intermediates exist. In this paper, SO₂ oxidation with H₂O on Pt(111) was modelled with density functional theory. On low surface coverages, SO₂ oxidation to H₂SO₄ and H₂ followed an Eley-Rideal instead of a Langmuir-Hinshelwood mechanism. Eley-Rideal oxidation was favoured more when H₂O was adsorbed instead of SO₂, and in both the Eley-Rideal and Langmuir-Hinshelwood mechanisms, H₂SO₄ and H₂ formation were significantly influenced by reaction intermediates and their adsorption geometries. More energy was consumed by SO₂ oxidation to H₂SO₄ and H₂ upon reactant coadsorption, with molecular and dissociated sulphurous acid readily formed as oxidation intermediate.

尽管最近在了解SO2在Pt上氧化成H2SO4和H2方面取得了进展，但关于反应机制和中间体存在不确定性。本文用密度泛函理论模拟了Pt（111）上H2O氧化SO2的过程。在低表面覆盖率下，SO2氧化为H2SO4和H2遵循的是Eley-Rideal机制，而不是Langmuir-Hinshelwood机制。吸附H2O比吸附SO2更有利于Eley-Rideal氧化，并且在Eley-Rideal和Langmuir-Hinshelwood两种反应机制中，H2SO4和H2的生成均受反应中间体及其吸附几何形状的显著影响。反应物共吸附使SO2氧化生成H2SO4和H2消耗更多能量，容易形成分子和解离硫酸作为氧化中间体。

引用次数: 0

A promising direct Z-scheme GeC/PtSe2 van der Waals heterostructure as a high-efficiency photocatalyst for overall water splitting 一种有前途的直接z型GeC/PtSe2范德华异质结构作为全水分解的高效光催化剂

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-14 DOI: 10.1016/j.susc.2025.122871

Yan Zhang, Hui Qiao, Li Duan

The constructed Z-scheme heterostructure for photocatalytic water splitting is an available approach to overcome serious environmental and energy problems. Here, the monolayers GeC and PtSe₂ are used to constructe van der Waals (vdW) heterostructure, and the corresponding electronical structure, Bader charge transfer, work function, optical absorption and solar-to-hydrogen efficiency are calculated in detail based on density functional theory. It is found that the GeC/PtSe₂ vdW heterostructure has not only a direct Z-scheme photocatalytic mechanism but also an intrinsic type-II band alignment and a decent band edge position to fully induce the redox reactions of overall water splitting. The direct Z-scheme GeC/PtSe₂ vdW heterostructure has a built-in electric field with direction from GeC side to PtSe₂ side. This direct Z-scheme GeC/PtSe₂ vdW heterostructure also has outstanding optical absorption, high solar-to-hydrogen efficiency and excellent catalytic activity, suggesting its potential application as a photocatalyst for overall water splitting.

构建用于光催化水分解的z型异质结构是克服严重的环境和能源问题的有效途径。本文利用单层GeC和PtSe2构建了范德华（vdW）异质结构，并基于密度泛函理论详细计算了相应的电子结构、Bader电荷转移、功函数、光吸收和太阳能制氢效率。发现GeC/PtSe2 vdW异质结构不仅具有直接的Z-scheme光催化机制，而且具有固有的ii型能带对准和良好的能带边缘位置，可以充分诱导整体水裂解的氧化还原反应。直接z型GeC/PtSe2 vdW异质结构具有从GeC侧到PtSe2侧的内置电场。这种直接Z-scheme GeC/PtSe2 vdW异质结构还具有出色的光吸收、高太阳能制氢效率和优异的催化活性，表明其作为全水分解光催化剂的潜在应用前景。

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引用次数: 0

First-principles study on the effects of X (X = O, Se, P, Cl) Doping on the electronic structure and optical properties of defective monolayer WS2 X （X = O, Se， P, Cl）掺杂对缺陷单层WS2电子结构和光学性质影响的第一性原理研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-14 DOI: 10.1016/j.susc.2025.122873

JingEn Jia , Yi Ma , YaNing Niu , Ying Ma

Based on first-principles calculations, the structural stability, electronic structure, and optical properties of monolayer WS₂ doped with O, Se, P, and Cl atoms under defect conditions were systematically investigated. It is found that among the three defect types (one W vacancy, one S vacancy, and double S vacancies), the structure with one S vacancy has the lowest formation energy. The doping of X atoms (X = O, Se, P, Cl) significantly alters the band gap of the defect system. Compared with other doping systems, the O–Vs–WS₂ system exhibits the largest valley value of ε₁, which remains positive, whereas its peak value of ε₂ is the lowest among all doping systems. In contrast, the P–Vs–WS₂ and Cl–Vs–WS₂ systems exhibit higher ε₂ peak values. Furthermore, P atom doping significantly enhances the peak intensity of light absorption and reflection in the defective WS₂ system.

基于第一性原理计算，系统地研究了缺陷条件下掺杂O、Se、P和Cl原子的单层WS₂的结构稳定性、电子结构和光学性质。发现在三种缺陷类型（一个W空位、一个S空位和双S空位）中，具有一个S空位的结构具有最低的形成能。X原子（X = O, Se， P, Cl）的掺杂显著改变了缺陷体系的带隙。与其他掺杂体系相比，O-Vs-WS₂体系ε 1的波谷值最大，ε 2波峰值为正，ε 2波峰值在所有掺杂体系中最低。相比之下，P-Vs-WS 2和Cl-Vs-WS 2体系的ε 2峰值更高。此外，P原子掺杂显著增强了缺陷WS₂体系的光吸收和反射峰值强度。

引用次数: 0

DFT and KMC study of graphene as a benchmark material for Li-Ion battery applications 石墨烯作为锂离子电池应用基准材料的DFT和KMC研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-06 DOI: 10.1016/j.susc.2025.122862

Fatima El Hiri , Zouhir Mansouri , Abedellah El Kenz , Abdelilah Benyoussef , Omar Mounkachi

In recent years, many studies have explored modified or functionalized graphene, such as doped graphene or graphene composites, to enhance Li-ion battery performance. In contrast, our study focuses on pristine graphene to establish a fundamental understanding of its intrinsic properties, combining density functional theory (DFT) and kinetic Monte Carlo (KMC) simulations. This approach provides critical benchmarks for future material design. DFT reveals that lithium preferentially adsorbs at hollow site with a strong binding energy (−1.9 eV), inducing a semi-metal-to-metal transition. The material exhibits a high theoretical capacity (744 mAh/g), a moderate average voltage (0.78 V), and a low Li diffusion barrier (0.31 eV). KMC simulations further quantify the concentration and temperature dependent Li diffusivity, yielding the empirical relation

D_{L i}

(

C_{L i}

,T) for Li concentrations in the range [0.01–0.1]. At room temperature, the calculated

D_{L i}

values span 2 × 10⁻⁹ to 5 × 10⁻⁸ cm²/s, showing excellent agreement with experimental data.

近年来，许多研究探索了改性或功能化石墨烯，如掺杂石墨烯或石墨烯复合材料，以提高锂离子电池的性能。相比之下，我们的研究重点是原始石墨烯，结合密度泛函理论（DFT）和动力学蒙特卡罗（KMC）模拟，建立对其内在特性的基本理解。这种方法为未来的材料设计提供了关键的基准。DFT表明，锂优先吸附在具有强结合能（- 1.9 eV）的空心位点，诱导半金属到金属的转变。该材料具有较高的理论容量（744 mAh/g）、中等的平均电压（0.78 V）和低Li扩散势垒（0.31 eV）。KMC模拟进一步量化了浓度和温度对锂扩散率的依赖，得出了锂浓度在[0.01-0.1]范围内的经验关系DLi（CLi，T）。在室温下，计算得到的DLi值范围为2 × 10−9 ~ 5 × 10−8 cm²/s，与实验数据吻合良好。

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引用次数: 0

First-principles study of the dissociative adsorption of H2S on the Ni(111) surface pre-covered with S atoms by Cr atoms Cr原子预覆盖S原子的Ni（111）表面对H2S解离吸附的第一性原理研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-06 DOI: 10.1016/j.susc.2025.122861

Zuoyu Jiang , Bensheng Huang , Tianning Li , Wenli Chen , Jianneng Zheng , Yongyou Zhu

This article used first-principles methods to study the effects of Cr atom doping and S atom pre-coverage on the adsorption and dissociation of H₂S on the Ni(111) surface. Cr doping increased the adsorption strength of H₂S, which was also the case on surfaces pre-covered with S atoms. Additionally, on the clean Ni(111) surface, the introduction of Cr atoms promoted the dissociation of H₂S and led to the direct occurrence of the second-step dissociation reaction (E_a,2 = 0 eV). The pre-coverage of S atoms can facilitate the first-step dissociation of H₂S on the Ni(111) surface but inhibited the second-step dissociation. With the addition of Cr atoms, S atoms suppressed both steps of H₂S dissociation. This demonstrated that in an environment where S atoms were present, the addition of Cr atoms provided a certain degree of corrosion resistance.

本文采用第一性原理方法研究了Cr原子掺杂和S原子预覆盖对H2S在Ni（111）表面吸附解离的影响。Cr的掺杂增加了H2S的吸附强度，在预覆盖有S原子的表面上也是如此。此外，在干净的Ni（111）表面，Cr原子的引入促进了H2S的离解，导致了第二步离解反应的直接发生（Ea,2 = 0 eV）。S原子的预覆盖有利于H2S在Ni（111）表面的第一步解离，但抑制了第二步解离。随着Cr原子的加入，S原子抑制了H2S解离的两个步骤。这表明，在S原子存在的环境中，Cr原子的加入提供了一定程度的耐腐蚀性。

引用次数: 0

R-graphyne monolayers as anodic material for future K-ion batteries: A DFT study 用作未来k离子电池阳极材料的r -石墨烯单层膜：DFT研究

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science

Pub Date : 2025-10-04 DOI: 10.1016/j.susc.2025.122860

Narinderjit Singh Sawaran Singh , Shahad Muthana Qasim , Ahmed Aldulaimi , Jameel M.A. Sulaiman , Rafid Jihad Albadr , Waam Nohammed Taher , Mariem Alwan , Hiba Mushtaq , M.A. Diab , Heba A. El-Sabban , Aseel Smerat

In the search for sustainable energy options, finding new, affordable, and reliable anode materials for potassium-ion batteries (KIBs) has become a crucial focus of research. Present research paper presents a potential K anode material in the form of a two-dimensional R-graphyne (R-gyn) monolayer, investigated using first-principles calculations. Stability of R-gyn has been verified through molecular dynamics (MD) simulations, examining both its structure and thermodynamics. Furthermore, an analysis of its electronic structure reveals that the R-gyn monolayer exhibits semi metallic features. Particularly noteworthy is the exceptionally high theoretical specific capacity (TSC) for potassium ions shown by R-gyn, which can reach up to 476.32 mAhg⁻¹. The significant capacity is paired with relatively minor diffusion barriers (95 meV) and advantageous open-circuit voltages (OCVs) ranging between 1.61–0.29 V. These attributes of the suggested R-gyn material suggest its capability to enable high-capacity energy storage and enhance swift ionic diffusion within potassium-ion batteries.

在寻找可持续能源选择的过程中，为钾离子电池（kib）寻找新的、负担得起的、可靠的阳极材料已经成为研究的一个关键焦点。本研究论文提出了一种二维r -石墨炔（R-gyn）单层形式的潜在K阳极材料，并使用第一性原理计算进行了研究。通过分子动力学（MD）模拟验证了R-gyn的稳定性，考察了其结构和热力学。此外，对其电子结构的分析表明，R-gyn单层具有半金属特征。特别值得注意的是R-gyn对钾离子表现出极高的理论比容量（TSC），可达476.32 mAhg−1。显著的容量与相对较小的扩散势垒（95 meV）和有利的开路电压（ocv）在1.61-0.29 V之间配对。所建议的R-gyn材料的这些属性表明，它能够实现高容量的能量存储，并增强钾离子电池中的快速离子扩散。

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