The Journal of Physical Chemistry C最新文献_第7页

Computational Investigation of the Effect of Nitrogen Dopants and Oxygen Vacancies on the Energetics of Lithium Lanthanum Titanates 氮掺杂和氧空位对钛酸镧锂能量学影响的计算研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-09 DOI: 10.1021/acs.jpcc.5c04703

Jiacheng Wang, Nianqiang Wu, Peng Bai

{"title":"Computational Investigation of the Effect of Nitrogen Dopants and Oxygen Vacancies on the Energetics of Lithium Lanthanum Titanates","authors":"Jiacheng Wang, Nianqiang Wu, Peng Bai","doi":"10.1021/acs.jpcc.5c04703","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c04703","url":null,"abstract":"Doping is a powerful strategy for improving the ionic conductivity of ceramic-type solid-state ion conductors. Compared to cation doping, anion doping is much less studied but has been shown to improve Li-ion transport in perovskite lithium lanthanum titanates (LLTOs). In this work, the structure and energetics of nitrogen-doped LLTOs were studied by using first-principles density functional theory calculations. The calculations found a high energy cost for nitrogen doping, which decreases with the introduction of oxygen vacancies or with the formation of nitrogen–nitrogen and nitrogen–oxygen dimers. Dimer formation reflects potentially significant structural distortions. Six machine learning models, including four descriptor-based models (multiple linear regression, random forest, support vector machine, and XGBoost) and two graph-based neural network models (CGCNN and MEGNet), were evaluated for predicting the energy of both unoptimized and DFT-optimized LLTO structures. XGBoost and MEGNet were found to be the best-performing models from the two categories, both exhibiting correlation coefficients larger than 0.99. SHAP analysis shows that oxygen vacancies prefer to form near La3+ ions, while the close proximity of Li+ and vacancies has a destabilizing effect. The latter suggests that thermodynamically Li+ may be repelled from the oxygen vacancy centers and thus be unable to directly benefit from the potential advantages of vacancies for Li+-ion transport. These results offer detailed insights into the stability of various anion-doped LLTOs and the interplay of various structural motifs in impacting ion conduction.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"1 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247383","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}

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Growth and Surface Characterization of a Type-II ZnO/ZnS Heterostructure ii型ZnO/ZnS异质结构的生长和表面表征

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-09 DOI: 10.1021/acs.jpcc.5c05124

P. R. A. de Oliveira, I. Coelho, G. Felix, P. Venezuela, F. Stavale

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Biotemplate-Guided Self-Assembly of Gold Nanoparticles with Plasmonic Circular Dichroism 具有等离子体圆二色性的金纳米颗粒的生物模板引导自组装

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-09 DOI: 10.1021/acs.jpcc.5c03459

B. Emre Aydemir, Matthew Smith, Teruo Hashimoto, Ahu G. Dumanli

{"title":"Biotemplate-Guided Self-Assembly of Gold Nanoparticles with Plasmonic Circular Dichroism","authors":"B. Emre Aydemir, Matthew Smith, Teruo Hashimoto, Ahu G. Dumanli","doi":"10.1021/acs.jpcc.5c03459","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c03459","url":null,"abstract":"Cholesteric assembly of plasmonic nanoparticles promotes applications in optics and sensing due to their inherent chiro-optical responses and strong interaction with light. Template-assisted colloidal assembly is a promising route to achieve such structures, yet it often suffers from difficulties in maintaining template integrity and attaining the required particle concentration. In this proof-of-concept work, we report the plasmonic activity of gold nanoparticles (AuNPs) coupled with circular dichroism, achieved through in situ cyclic deposition onto cholesteric biotemplates derived from prawn shells. Upon aging, the samples exhibited clear circular dichroism in both reflection and transmission under left- and right-circularly polarized light. These optical signatures confirm macroscopic coupling between the cholesteric periodicity of the biotemplate and the localized surface plasmon resonance (LSPR) of the AuNPs. High-resolution imaging further revealed handed arrangements of the nanoparticles within the membrane structure. Together, these findings offer a scalable and effective route for engineering chiral plasmonic materials using cholesteric templates.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"115 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261336","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}

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A Two-Dimensional Electron Gas at the Sulfurized SrTiO3 Interface 硫化SrTiO3界面上的二维电子气体

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-09 DOI: 10.1021/acs.jpcc.5c04680

Jiacheng Huang, Linhao Cheng, Jianjie Li, Ting Lin, Tianlin Zhou, Jing Chen, Yuchen Zhao, Minghang Li, Wenxiao Shi, Qinghua Zhang, Jie Su, Yunzhong Chen

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Dynamics of Volatile Products in the Electro-oxidation of Ethanol on Pt/C and PtSn/C Catalysts Pt/C和PtSn/C催化剂上乙醇电氧化挥发性产物的动力学研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-09 DOI: 10.1021/acs.jpcc.5c04854

N. Vilas-Bôas, G. N. Tessaro, L. Hostert, A. G. S. de Oliveira-Filho, J. Perez, H. Varela

{"title":"Dynamics of Volatile Products in the Electro-oxidation of Ethanol on Pt/C and PtSn/C Catalysts","authors":"N. Vilas-Bôas, G. N. Tessaro, L. Hostert, A. G. S. de Oliveira-Filho, J. Perez, H. Varela","doi":"10.1021/acs.jpcc.5c04854","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c04854","url":null,"abstract":"Ethanol electro-oxidation reaction (EEOR) is a strategically important reaction for the development of fuel cells and low-temperature electrolysis technologies, although its application is hindered by slow kinetics and poor selectivity toward the C1 pathway (CO2 formation) on platinum-based catalysts. In this study, the dynamic formation of volatile products (acetaldehyde, acetic acid, and CO2) was investigated during the EEOR on Pt/C and PtSn/C electrodes in acidic media, with particular emphasis on oscillatory conditions using online electrochemical mass spectrometry (OLEMS). PtSn/C catalysts were synthesized via chemical reduction and characterized by XRD, TEM, and XPS, revealing smaller particle sizes, a higher proportion of oxidized Pt species, and the presence of Sn4+ as SnO2. OLEMS experiments showed earlier onset for acetaldehyde, CO2, and acetic acid products for PtSn/C. Despite the low volatility of acetic acid, its production was confirmed and quantified by high-performance liquid chromatography (HPLC), reaching up to 965.2 ppm at 0.5 V, which is 97 times higher than that of Pt/C. Multivariate linear regression (MLR) analysis revealed a greater contribution of acetic acid and CO2 to the faradaic current for PtSn/C, indicating a substantial shift in the reaction pathway. Under oscillatory conditions, PtSn/C exhibited greater robustness, lower potential amplitude, and reduced susceptibility to surface poisoning. These results highlight the role of Sn in enhancing surface regeneration and promoting deeper oxidation pathways, demonstrating the importance of catalyst design in tuning the selectivity and efficiency of the EEOR.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"88 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261339","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}

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Computational Analysis of the Energetic Stability of High-Entropy Structures of a Prototypical Lanthanide-Based Metal–Organic Framework 典型镧系金属-有机骨架高熵结构能量稳定性的计算分析

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-09 DOI: 10.1021/acs.jpcc.5c04892

Surbhi K. A. Kumar, Dorina F. Sava Gallis, David S. Sholl

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Cations Enhance Hydride Transfer to Noncatalytic Metals in Concentrated Alkaline Electrolytes 在浓碱性电解质中，阳离子促进氢化物向非催化金属的转移

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-08 DOI: 10.1021/acs.jpcc.5c05397

Louka J. Moutarlier, Benjamin Cato, Casey S. Mezerkor, J. David Bazak, Paul A. Kempler

{"title":"Cations Enhance Hydride Transfer to Noncatalytic Metals in Concentrated Alkaline Electrolytes","authors":"Louka J. Moutarlier, Benjamin Cato, Casey S. Mezerkor, J. David Bazak, Paul A. Kempler","doi":"10.1021/acs.jpcc.5c05397","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c05397","url":null,"abstract":"Alkali metal cations are known to influence the kinetics of the hydrogen evolution reaction (HER), acting as either promoters or inhibitors to the rate-determining step depending on the metal surface, local pH, and cation concentration. Despite the importance of concentrated electrolytes for commercial electrochemical cells, the impact of cations on the HER in concentrated alkaline environments (>1 M) and in mixed cation systems remains poorly understood. This study quantifies the HER kinetics at polycrystalline metal surfaces (Pt, Au, Cu, and Fe) and the equilibrium solvation environment in pure and mixed alkali metal hydroxide electrolytes at concentrations up to 3.0 M. Kinetic analyses of Au, Cu, and Fe revealed a positive cation-concentration-effect that was primarily driven by changes to the charge transfer coefficient. Multinuclear NMR spectroscopy examined the solvation of H2O/OH– species and the alkali cations as a function of (mixed) alkali cation concentration(s), and demonstrated rapid exchange between solvent, hydroxide, and solvated cations. Together, these findings support models where HER kinetics on noncatalytic metal surfaces in strongly alkaline conditions are primarily governed by the average polarization and polarizability of the metal/solution interface and that increasing cation activity continues to increase the transfer coefficient at metal-hydroxide concentrations up to 3.0 M. Electrolytes and additives which can outcompete weakly hydrated cations and disrupt the interfacial water structure are expected to suppress parasitic HER at electrodes for energy storage and electroplating.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"28 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241245","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}

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First-Principles Study of Polarons in Multiple Crystal Phases of Bismuth Vanadate 钒酸铋多晶相极化子的第一性原理研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-08 DOI: 10.1021/acs.jpcc.5c05875

Xiao Jiang, Xu Cheng, Zhanqi Liu, Liyun Ding, Weihua Han

{"title":"First-Principles Study of Polarons in Multiple Crystal Phases of Bismuth Vanadate","authors":"Xiao Jiang, Xu Cheng, Zhanqi Liu, Liyun Ding, Weihua Han","doi":"10.1021/acs.jpcc.5c05875","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c05875","url":null,"abstract":"Bismuth vanadate (BiVO4) is a promising photocatalyst existing in multiple crystal phases, whose performance is critically influenced by charge carrier (polaron) behavior. Although polarons in monoclinic BiVO4 have been extensively studied, a comparative understanding of polaron behavior in its main crystal phases, including monoclinic scheelite, tetragonal zircon type, and tetragonal scheelite, is essential for optimizing photocatalytic efficiency. This study systematically investigates electron and hole polarons in these three BiVO4 phases using ab initio calculations. We find distinct polaron characteristics: electron polarons are consistently identified as Holstein type, whereas hole polarons are of the Fröhlich type in all three crystal structures. Our analysis reveals that although holes in all phases are scattered by longitudinal optical phonons of approximately 30 meV, variations in scattering strength lead to differing hole mobilities. The microscopic origins of these mobility differences are elucidated through analysis of dielectric tensors and Born effective charges. This work uncovers the mechanism by which crystal structure modulates polaron properties, offering crucial theoretical guidance for designing high-efficiency BiVO4-based photofunctional materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"37 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247388","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}

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Benchmarking DFT Accuracy in Predicting O 1s Binding Energies on Metals 预测金属上o1s结合能的DFT精度基准

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-08 DOI: 10.1021/acs.jpcc.5c05986

Elizabeth E. Happel, E. Charles H. Sykes, Matthew M. Montemore

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Synergistic Effects of Phonon Anderson Localization and Resonance in Si/Ge Superlattice Nanowires: Toward Lower Thermal Conductivity 硅/锗超晶格纳米线中声子安德森局域化和共振的协同效应：迈向低导热性

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-10-08 DOI: 10.1021/acs.jpcc.5c04546

Weikang Li, Xiaoyu Huang, Yuxiang Ni

{"title":"Synergistic Effects of Phonon Anderson Localization and Resonance in Si/Ge Superlattice Nanowires: Toward Lower Thermal Conductivity","authors":"Weikang Li, Xiaoyu Huang, Yuxiang Ni","doi":"10.1021/acs.jpcc.5c04546","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c04546","url":null,"abstract":"Manipulating heat transfer in thermal functional materials is of great importance, with wide applications such as thermoelectrics, thermal management devices, thermal insulating materials, and thermal diodes. To influence the phonon propagation in nanostructures, Anderson localization and phonon resonance are commonly employed methods due to the wave nature of phonons. In this study, we investigate the thermal transport in Si/Ge superlattice nanowires incorporating aperiodic interfaces and resonance pillars, wherein Anderson localization and phonon resonance are simultaneously introduced. In superlattice nanowires with aperiodic interfaces, the thermal conductivity initially increases with size and then decreases, suggesting the occurrence of phonon Anderson localization when sufficient random interfaces are present. The reduction in the thermal conductivity caused by Anderson localization reaches 55.6% at a nanowire length of 109 nm. On the other hand, introducing phonon resonance via resonance pillars to the superlattice nanowires results in a reduction of 39.7% at the same nanowire length. The coexistence of Anderson localization and phonon resonance leads to a much more significant reduction of 62.6% in the thermal conductivity. Furthermore, we reveal that Anderson localization predominantly affects phonons in the medium-low frequency range (1.5–3.5 THz), while phonon resonance impacts phonons at low frequencies (0–2.2 THz). These two methods collaboratively impede phonons with different frequencies, thereby achieving exceptionally low thermal conductivity. Our findings provide new insights into regulating the thermal conductivity of materials through the wave nature of phonons.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"63 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247382","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}

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