Chemical Physics Letters最新文献

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Transition metal anchored Lindqvist hexavanadate cluster, [(V6O19)]8− based single atom catalysts (TM@POV) for water splitting (HER/OER), and ORR: A computational evaluation 过渡金属锚定Lindqvist六氰酸酯簇，[(V6O19)]8−基单原子催化剂（TM@POV）对水裂解（HER/OER）和ORR的计算评价

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-16 DOI: 10.1016/j.cplett.2025.142607

Faheem Abbas , Ayed M. Binzowaimil , Asma Hassan , Saleem Nawaz Khan , Muhammad Salman Khan , Mohannad Al-Hmoud , Siti Maisarah Aziz

Polyoxometalate-based single-atom catalysts (POM–SACs) offer precise control over the structural and electronic environment of anchored transition metals (TMs) and their supports. In this study, we explored the catalytic performance of TMs anchored on a Lindqvist-type hexavanadate cluster, [(V₆O₁₉)]⁸⁻, forming TM@POV catalysts for the hydrogen evolution (HER), oxygen evolution (OER), and oxygen reduction (ORR) reactions. Using density functional theory (DFT), we evaluated their thermodynamic, structural, and thermal stability at the most favorable three-hollow (3H) sites of the POV framework. The complete HER mechanism was investigated via the Volmer, Volmer–Heyrovsky, and Volmer–Tafel pathways. The lowest HER overpotentials were observed for Sc@POV (ΔG_H⁎ = −0.03 eV) and Ni@POV (ΔG_H⁎ = 0.03 eV) through the Volmer–Tafel pathway. Electronic descriptors including the d-band center (ε_d), Bader charge (q/e), projected density of states (PDOS), and charge density difference (CDD) revealed efficient charge redistribution between metal centers and hydrogenated/oxygenated intermediates. For OER, Co@POV exhibited the lowest overpotential (η^OER = 0.43 V) at the second step (OH^⁎ → O^⁎), while Ni@POV achieved the best ORR performance (η^ORR = 0.65 V) at the final step (OH^⁎ → H₂O). Incorporating solvation effects through the VASPsol model further enhanced catalytic activity. The explicit solvation model with one water molecule achieved the lowest overpotentials (η^OER/η^ORR = 0.32/0.44 V), demonstrating improved charge transfer and proton coupling. Overall, these findings provide fundamental insights into designing low-cost, thermally stable, and highly efficient TM@POV-based multifunctional electrocatalysts for hydrogen production (H₂) and sustainable energy conversion.

基于多金属氧酸盐的单原子催化剂（POM-SACs）可以精确控制锚定过渡金属（tm）及其支架的结构和电子环境。在这项研究中，我们探索了锚定在lindqvist型六维酸盐簇[（V₆O₁₉）]8−上的TMs的催化性能，形成了TM@POV催化剂，用于出氢（HER）、出氧（OER）和氧还原（ORR）反应。利用密度泛函理论（DFT），我们评估了它们在POV框架最有利的三空心（3H）位点的热力学、结构和热稳定性。通过Volmer、Volmer - heyrovsky和Volmer - tafel通路研究了HER的完整机制。通过Volmer-Tafel通路，观察到Sc@POV （ΔGH = - 0.03 eV）和Ni@POV （ΔGH = 0.03 eV）的过电位最低。包括d带中心（εd）、Bader电荷（q/e）、投射态密度（PDOS）和电荷密度差（CDD）在内的电子描述符揭示了金属中心和氢化/氧化中间体之间有效的电荷再分配。对于OER， Co@POV在第二步（OH→O）表现出最低的过电位（ηOER = 0.43 V），而Ni@POV在最后一步（OH→H₂）表现出最好的过电位（ηORR = 0.65 V）。通过VASPsol模型加入溶剂化效应进一步提高了催化活性。单水分子的显式溶剂化模型获得了最低的过电位（ηOER/ηORR = 0.32/0.44 V），表明电荷转移和质子耦合得到了改善。总的来说，这些发现为设计低成本、热稳定和高效的TM@POV-based多功能电催化剂用于制氢（H2）和可持续的能量转换提供了基础见解。

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引用次数: 0

Electronic structure calculations and theoretical absorption spectra of I3− and I5− I3−和I5−的电子结构计算和理论吸收光谱

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-16 DOI: 10.1016/j.cplett.2025.142608

Megumi Takahashi , Erik Lötstedt , Kaoru Yamanouchi

We perform electronic structure calculations of an iodine atom, I₃⁻, and I₅⁻ by including the spin-orbit interaction. After confirming the accuracy of the calculations by critical comparison with the available spectroscopic data of I and I₃⁻, we predict the absorption spectrum of I₅⁻ in the visible-UV region by the SA-CASSCF (state-averaged complete active space self-consistent field) method with the aug-cc-pwCVDZ-pp basis set and estimate that the spectrum in aqueous solution can exhibit double peaks separated by ∼7000 cm⁻¹.

我们通过包含自旋轨道相互作用来计算碘原子I3−和I5−的电子结构。在与现有的I和I3 -光谱数据进行了临界比较，确认了计算的准确性后，我们用SA-CASSCF（状态平均完全主动空间自一致场）方法，以aug-cc-pwCVDZ-pp基集预测了I5 -在可见-紫外区的吸收光谱，并估计水溶液中的光谱可以出现双峰，间隔为~ 7000 cm−1。

引用次数: 0

Coverage effects on the interaction between Mg and ZnO surface 覆盖效应对Mg和ZnO表面相互作用的影响

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-15 DOI: 10.1016/j.cplett.2025.142584

Shenghua Feng , Yao Zou , Xin Huang , Ying Zhao , Weihua Zhu

The coverage-dependent deposition of Mg on ZnO(000

\bar{1}

) surface was investigated using density functional theory and ab initio molecular dynamics simulations. At low coverage, Mg stably adsorbs at FCC/HCP sites, with multiple Mg atoms cooperatively extracting surface oxygen atoms. As coverage increases, electron transfer from Mg exceeds the substrate capacity, reducing average charge transfer and adsorption stability while inducing site shifts, Mg repulsion, and cluster formation. At full coverage, Mg forms a uniform Top-site monolayer, each atom binding to one oxygen. These findings clarify Mg/ZnO interfacial formation mechanisms and provide atomic-level insights into thin-film morphology.

利用密度泛函理论和从头算分子动力学模拟研究了Mg在ZnO（0001¯）表面的覆盖依赖性沉积。在低覆盖率下，Mg稳定吸附在FCC/HCP位点，多个Mg原子协同萃取表面氧原子。随着覆盖率的增加，来自Mg的电子转移超过了衬底容量，降低了平均电荷转移和吸附稳定性，同时诱导了位位移、Mg排斥和簇形成。在完全覆盖的情况下，Mg形成一个均匀的顶部单分子层，每个原子与一个氧结合。这些发现阐明了Mg/ZnO界面的形成机制，并为薄膜形态提供了原子水平的见解。

引用次数: 0

Flash fabrication of Ti-doped Na3V2(PO4)3 single-crystals with boosted sodium storage and low-temperature performance 具有提高钠储存和低温性能的掺钛Na3V2(PO4)3单晶的闪蒸制备

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-15 DOI: 10.1016/j.cplett.2025.142604

Mingju Wang , Liying Hao , Xuqing Guo , Penghao Zhao , Yong Li , Yun Zhao

A novel Ti-doped Na₃V₂(PO₄)₃ single-crystal material (F-NVTP/C-0.7) is fabricated through an ultrafast flash Joule heating sintering at 1000 °C for 90 s. Compared to the counterpart that is fabricated via conventional furnace sintering, F-NVTP/C-0.7 exhibits much diminished particle size, thinner carbon coating and elevated electrical conductivity. The F-NVTP/C-0.7 electrode demonstrates prominently enhanced sodium storage performance, especially the superior long-term cycling stability upon 5000 cycles and low-temperature performance at −20 °C. The kinetics analyses and in-situ XRD characterization reveal that the accelerated charge/ion transportation rate, more pseudocapacitive behaviors and alleviated volume effect are responsible to the elevation of electrochemical performance.

采用超快闪烁焦耳加热烧结技术，在1000℃下烧结90 s制备了新型掺钛Na3V2(PO4)3单晶材料（F-NVTP/C-0.7）。与传统炉烧结法相比，F-NVTP/C-0.7的颗粒尺寸更小，碳涂层更薄，电导率更高。F-NVTP/C-0.7电极表现出显著增强的钠存储性能，特别是在5000次循环的长期稳定性和- 20°C的低温性能。动力学分析和原位XRD表征表明，加速的电荷/离子传输速率、更多的假电容行为和减轻的体积效应是电化学性能提高的原因。

引用次数: 0

1H polarization above 60 % at room temperature by triplet dynamic nuclear polarization 三态动态核极化，室温下1H极化60%以上

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-15 DOI: 10.1016/j.cplett.2025.142606

Kenichiro Tateishi , Shuji Otsuka , Akihiro Yamaji , Shunsuke Kurosawa , Tomohiro Uesaka

We achieved 61 % ¹H polarization at room temperature and in 0.64 T via Dynamic Nuclear Polarization using photoexcited triplet electrons (Triplet-DNP). Dibenz[a, h]anthracene was introduced as a new host for pentacene-d₁₄, providing a long spin-lattice relaxation time (T₁) exceeding 2 h. Single crystals doped with 0.05 mol% pentacene-d₁₄ were grown by the Bridgman method and cut to ∼1 mg for experiments. The ¹H polarization buildup and relaxation measurements indicated that paramagnetic relaxation dominates over spin-lattice relaxation. Finally, potential applications of room-temperature hyperpolarization, i.e., nuclear ordering and radiation-tolerant polarized targets, were discussed.

我们利用光激发三重态电子（triplet - dnp）在室温和0.64 T下实现了61% 1H的动态核极化。引入双苯并[a， h]蒽作为并五苯-d14的新载体，提供超过2小时的长自旋-晶格弛豫时间（T1）。通过Bridgman方法生长掺杂0.05 mol%的并五苯-d14的单晶，并切割至~ 1 mg用于实验。1H极化积累和弛豫测量表明，顺磁弛豫优于自旋晶格弛豫。最后，讨论了室温超极化的潜在应用，即核有序和耐辐射极化靶。

引用次数: 0

Densification processes of crystalline purine: Negative linear compressibility and pressure-induced phase transition 结晶嘌呤的致密化过程：负线性压缩和压力诱导相变

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-11 DOI: 10.1016/j.cplett.2025.142600

Hiroki Kobayashi, Kazuki Komatsu, Hiroyuki Kagi

We investigated the densification mechanisms of crystalline purine at room temperature using powder and single-crystal x-ray diffraction under quasi-hydrostatic pressure. The ambient orthorhombic phase exhibits negative linear compressibility until it transforms at 0.7–1.1 GPa into a newly reported high-pressure polymorph. This phase transition can be explained by flipping and translation of hydrogen-bonded molecular arrays. Judging from interatomic distances, intermolecular N–H…N hydrogen bonds in the high-pressure phase are weakened but doubled, leading to an efficient densification.

在准静水压力下，利用粉末和单晶x射线衍射研究了室温下结晶嘌呤的致密化机理。环境正交相表现为负线性压缩，直到它在0.7-1.1 GPa转变为新报道的高压多晶。这种相变可以用氢键分子阵列的翻转和平移来解释。从原子间距离来看，分子间的N - h…N氢键在高压相中被削弱但加倍，导致了有效的致密化。

引用次数: 0

The competition between ortho and ipso attacks in the reactions of O(3P) with functionalized monocyclic aromatic compounds O（3P）与功能化单环芳香族化合物反应中邻位和对位攻击的竞争

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-10 DOI: 10.1016/j.cplett.2025.142592

Dario Campisi , Nadia Balucani , Marzio Rosi

We present a density functional theory characterization of the adiabatic triplet potential energy surfaces for the reactions of atomic oxygen with seven functionalized arenes (aniline, phenol, 1,3-diphenylpropane, diphenyl ether, propylbenzene, formanilide, and benzonitrile) to characterize the competition between ortho and ipso additions. Ortho and ipso additions give rise to O/H or O/R exchange channels, respectively, where R represents the functional groups of the substituted arenes. Our results show that the ortho position is favored in all cases, except for phenol, where ortho competes with ipso. The study provides a useful guide for future experimental investigations.

我们提出了原子氧与七个功能化芳烃（苯胺、苯酚、1,3-二苯基丙烷、二苯基醚、丙苯、酰胺和苯腈）反应的绝热三重态势能表面的密度泛函理论表征，以表征邻位和对羟基加成物之间的竞争。邻位加成和对位加成分别生成O/H和O/R交换通道，其中R表示取代芳烃的官能团。我们的结果表明，在所有情况下，邻位都是有利的，除了苯酚，在邻位与异位竞争。该研究为今后的实验研究提供了有益的指导。

引用次数: 0

Charge transfer at the Magnéli-phase Ti4O7 surface with a self-passivated oxide layer 具有自钝化氧化层的magnacli相Ti4O7表面的电荷转移

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-08 DOI: 10.1016/j.cplett.2025.142585

Zhihao Cheng , Jianbang Ge , Biwu Cai , Yang Gao , Shun Cao , Zheng Fang , Fei Zhu , Handong Jiao , Dongbai Sun , Shuqiang Jiao

Magnéli-phase Ti₄O₇ is widely utilized as an electrode material or conductive support in electrochemical systems due to its outstanding conductivity and stability. However, this material typically exhibits sluggish electrode kinetics during electrochemical tests. Herein, we reveal that a self-passivated oxide layer forms on the Ti₄O₇ surface, severely impeding the electrode process. A pristine Ti₄O₇ electrode initially demonstrates significant electrochemical reactivity, which gradually diminishes as the surface becomes passivated via TiO₂ formation in both acidic and alkaline solutions. Using a kinetic-thickness model, the TiO₂ layer thickness is estimated to be ∼3 nm in alkaline solutions and ∼ 12 nm in acidic solutions.

由于其优异的导电性和稳定性，magnli相Ti4O7被广泛应用于电化学系统中作为电极材料或导电载体。然而，在电化学测试中，这种材料通常表现出缓慢的电极动力学。在此，我们发现在Ti4O7表面形成了一层自钝化的氧化层，严重阻碍了电极过程。原始的Ti4O7电极最初表现出显著的电化学反应性，随着表面在酸性和碱性溶液中通过TiO2的形成而钝化，反应性逐渐减弱。使用动力学厚度模型，估计在碱性溶液中TiO2层厚度为~ 3 nm，在酸性溶液中为~ 12 nm。

引用次数: 0

Characterization of the structural and dynamic properties of two polymorphs of leflunomide by solid-state NMR 固态核磁共振表征来氟米特两种多晶型物的结构和动力学性质

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-07 DOI: 10.1016/j.cplett.2025.142596

Arianna Ghelardi , Elisa Carignani , Elionai C. de L. Gomes , Marco Geppi

Solid-state Nuclear Magnetic Resonance (ssNMR) spectroscopy is a powerful tool for the structural and dynamic characterization of polymorphs, whose pharmaceutical properties can differ in terms of solubility, stability, and bioavailability. In this study, we present the first ssNMR characterization of the two polymorphs α and β of leflunomide, a Disease Modifying Anti-Rheumatic Drug. A multinuclear (¹H, ¹⁹F, ¹³C, ¹⁵N) NMR approach using spectral and relaxation data confirmed distinct structural and dynamic differences between the two polymorphs. In particular, the reorientational motions of the methyl, phenyl, and trifluoromethyl groups are at least two orders of magnitude faster in the β form.

固态核磁共振（ssNMR）光谱是一种强大的工具，用于结构和动态表征多晶型，其药物性质可以在溶解度，稳定性和生物利用度方面有所不同。在这项研究中，我们首次提出了来氟米特（一种疾病修饰抗风湿药物）的两个多态性α和β的ssmr表征。多核（1H, 19F, 13C, 15N） NMR方法利用光谱和弛豫数据证实了两种多晶态之间明显的结构和动态差异。特别是，甲基、苯基和三氟甲基的重定向运动在β形式中至少快两个数量级。

引用次数: 0

Designing dual-atom catalysts for CO2 reduction reactions: Synergistic effects of Ni-Fe in the NiFeN5P/C60 设计CO2还原反应的双原子催化剂：Ni-Fe在NiFeN5P/C60中的协同作用

IF 3.1 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters

Pub Date : 2025-12-05 DOI: 10.1016/j.cplett.2025.142599

Qamar Abuhassan , Ahmed Aldulaimi , Omayma Salim Waleed , G. PadmaPriya , Subhashree Ray , Y. Sasikumar , Renu Sharma , Saodatkhon Ibragimova , Rafiqjon Kazakov , Zukhra Atamuratova , Aseel Smerat

We employ density functional theory (DFT) calculations to explore CO₂ reduction on Fe₂N₅P/C₆₀ and its heteronuclear variants, CoFeN₅P/C₆₀ and NiFeN₅P/C₆₀. Fe₂N₅P/C₆₀ shows a high ΔG*H (>0.61 eV), favoring CO₂RR over HER. Phosphorus enhances intermediate stabilization and Fe site activity. NiFeN₅P/C₆₀ exhibits superior synergy due to its electronic structure and reduced Fe charge, achieving a low limiting potential (−0.27 V) and overpotential (0.16 V). These results highlight the catalytic promise of Fe₂N₅P-based DACs and the role of transition metal pairing in optimizing CO₂RR performance.

我们利用密度泛函理论（DFT）计算了Fe2N5P/C60及其异核变体CoFeN5P/C60和NiFeN5P/C60对CO2的还原作用。Fe2N5P/C60表现出较高的ΔG*H (>0.61 eV)，有利于CO2RR而不是HER。磷增强中间稳定性和铁位点活性。NiFeN5P/C60由于具有良好的电子结构和较低的Fe电荷，具有较低的极限电位（- 0.27 V）和过电位（0.16 V）。这些结果突出了fe2n5p基dac的催化前景以及过渡金属配对在优化CO2RR性能中的作用。

引用次数: 0

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