The Journal of Physical Chemistry C最新文献

Reliable Element-Specific d-Band Analysis of Transition Metal Nanoparticles Using X-ray Absorption Spectroscopy 利用x射线吸收光谱可靠的过渡金属纳米颗粒元素特异性d波段分析

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-16 DOI: 10.1021/acs.jpcc.5c02020

Tyler Joe Ziehl, Peng Zhang

{"title":"Reliable Element-Specific d-Band Analysis of Transition Metal Nanoparticles Using X-ray Absorption Spectroscopy","authors":"Tyler Joe Ziehl, Peng Zhang","doi":"10.1021/acs.jpcc.5c02020","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c02020","url":null,"abstract":"Metallic nanoparticles (NPs) have been extensively studied as improved catalysts due to their unique atomic structures and electronic properties. A reliable strategy to characterize the electronic properties, specifically the d-band structure, of metal NPs is challenging. In this work, we present a general strategy for fitting the X-ray absorption near-edge spectroscopy (XANES) spectrum to accurately determine the electronic properties in metal NPs and deduce d-band parameters such as the d-band width and d-band center position. In conjunction with valence-band X-ray photoelectron spectroscopy (VBXPS), our fitting analysis reliably calibrates the XANES spectrum such that effects of instrumental and core-hole broadening are minimized and the d-band structure can be accurately determined. For a series of palladium (Pd) NPs, we use our XANES fitting analysis approach to characterize the Pd d-band and identify trends in the electronic properties consistent with prior literature reports. In closing, we propose a mechanism in which the Pd d-band changes due to size and surface effects based on our element-specific XANES fitting analysis within the framework of the popular Nørskov d-band model of transition metal surfaces. We anticipate that this experimental d-band analysis methodology will be useful for studying structure–property relationships and catalysis on monometallic and multimetallic NPs.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"91 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144296227","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

Preparation of the Amorphous SiO2-Coated Li4Ti5O12 Anode and Its High Cyclability 非晶二氧化硅包覆Li4Ti5O12阳极的制备及其高循环性能

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-15 DOI: 10.1021/acs.jpcc.5c01712

Ryota Nomura, Yoshinao Kobayashi, Shintaro Yasui

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Suppression of Auger Recombination and Promotion of Carrier Diffusion in Ag(I)-Doped CdSe Nanotetrapods Ag(I)掺杂CdSe纳米四足体对俄歇复合的抑制和载流子扩散的促进

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-14 DOI: 10.1021/acs.jpcc.5c02719

Priya Bhandari, Fariyad Ali, Anindya Datta

引用次数: 0

Design of Efficient Artificial Light-Harvesting Systems Using Cationic Porphyrin–Titania Nanosheet Assemblies: Insights into Excitation Energy Transfer and Deactivation Pathways 利用阳离子卟啉-二氧化钛纳米片组件设计高效人工光收集系统：激发能转移和失活途径的见解

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-14 DOI: 10.1021/acs.jpcc.5c02536

Masbooth Rasa Melechalil, Taichi Sawasaki, Tetsuya Shimada, Tamao Ishida, Shinsuke Takagi

{"title":"Design of Efficient Artificial Light-Harvesting Systems Using Cationic Porphyrin–Titania Nanosheet Assemblies: Insights into Excitation Energy Transfer and Deactivation Pathways","authors":"Masbooth Rasa Melechalil, Taichi Sawasaki, Tetsuya Shimada, Tamao Ishida, Shinsuke Takagi","doi":"10.1021/acs.jpcc.5c02536","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c02536","url":null,"abstract":"The remarkable efficiency of natural photosynthetic systems arises from the precise and highly ordered arrangement of dye molecules, enabling complex photofunctionalities. Replicating such systems, however, remains a significant challenge. To address this, we have developed cationic porphyrin/TNS (titania nanosheet) complexes with high-density adsorption, achieved through the “size-matching effect”, which prevents molecular aggregation and enhances light-harvesting capabilities. Tetracationic o-TMPyP (tetrakis (1-methylpyridinium-2-yl) porphyrin) and m-TMPyP (tetrakis (1-methylpyridinium-3-yl) porphyrin) were employed as energy donor and acceptor molecules, respectively, coadsorbed on the TNS surface in a 1:1 ratio. This arrangement facilitated efficient energy transfer from o-TMPyP to m-TMPyP, achieving an efficiency of nearly 95%. This high performance was realized by suppressing the molecular aggregation and mitigating self-fluorescence quenching. In this study, we provide a comprehensive analysis of deactivation pathways, forward and reverse energy transfer mechanisms, energy losses due to quenching, as well as adsorption behavior and density. By leveraging the systematic molecular arrangement and the size-matching effect, our findings contribute to the design of advanced artificial photosynthetic models on semiconducting nanosheets.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"9 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144290099","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

Durable Tape-Cast Trilayer La0.8Sr0.2Ga0.8Mg0.2O3-δ Electrolyte with Infiltrated Electrodes for Intermediate Temperature Solid Oxide Fuel Cells 带铸三层La0.8Sr0.2Ga0.8Mg0.2O3-δ渗透电极中温固体氧化物燃料电池电解质

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-13 DOI: 10.1021/acs.jpcc.5c01421

Daniel Sikstrom, Venkataraman Thangadurai

{"title":"Durable Tape-Cast Trilayer La0.8Sr0.2Ga0.8Mg0.2O3-δ Electrolyte with Infiltrated Electrodes for Intermediate Temperature Solid Oxide Fuel Cells","authors":"Daniel Sikstrom, Venkataraman Thangadurai","doi":"10.1021/acs.jpcc.5c01421","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01421","url":null,"abstract":"As global energy demands shift toward a sustainable alternative, hydrogen-powdered solid oxide fuel cells (SOFCs) offer a high-efficiency, low-emission solution for electrical energy conversion. However, performance limitations at intermediate temperatures (600–800 °C) necessitate advancements in electrolyte and electrode design. The present work presents the fabrication of a trilayer (porous/dense/porous) La0.8Sr0.2Ga0.8Mg0.2O3-δ electrolyte using a tape casting method, yielding a sintered structure with ∼55 μm thick, porous layers (∼55% porosity) and a ∼20 μm dense electrolyte supported by La0.8Sr0.2Ga0.8Mg0.2O3-δ rings. The porous La0.8Sr0.2Ga0.8Mg0.2O3-δ backbone is infiltrated with nominal chemical composition NdBaCoFeO5+δ (NBCF) and a Ni–Gd-doped-Ce (Ni-GDC) anode. Electrochemical impedance spectroscopy, distribution functions of relaxation times, and equivalent circuit modeling identified an optimal NBCF loading of 1.58 mg/cm2, which minimizes charge transfer and diffusion resistance, reducing the area-specific resistance to 0.025 Ω cm2 at 800 °C. Full cell testing under SOFC conditions achieves a peak powder density of 400 mW/cm2 at 750 °C with low ohmic (0.11 Ω cm2) and polarization (0.33 Ω cm2) resistances.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"26 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278916","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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Fluorophore-Induced Plasmonic Current from Copper and Silver Mixed-Metal Films 铜和银混合金属薄膜的荧光团诱导等离子体电流

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-13 DOI: 10.1021/acs.jpcc.5c01887

Daniel R. Pierce, Clifton Cunningham, Sean Avryl Villaver, Abdullah Bajwah, Samuel Oluwarotimi, Chris D. Geddes

{"title":"Fluorophore-Induced Plasmonic Current from Copper and Silver Mixed-Metal Films","authors":"Daniel R. Pierce, Clifton Cunningham, Sean Avryl Villaver, Abdullah Bajwah, Samuel Oluwarotimi, Chris D. Geddes","doi":"10.1021/acs.jpcc.5c01887","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01887","url":null,"abstract":"In recent years, our laboratory has demonstrated that excited-state fluorophores can nonradiatively couple through space to noble metal nanoparticles. If the noble metal nanoparticles are isolated, both highly photostable and enhanced fluorescence can be observed, a phenomenon known as metal-enhanced fluorescence (MEF). However, if the nanoparticles are spaced relatively much closer together, the coupled quanta can now “hop” between the nanoparticles, ultimately producing a current across the nanoparticle film. The magnitude of this fluorophore-induced plasmonic current (FIPC) is a function of how far apart both the donor (fluorophore) and acceptor (nanoparticle) are spaced; the excitation polarization and, importantly, the degree of overlap between the fluorophores’ emission spectrum with that of the nanoparticles plasmon absorption. All of the work to date on FIPC has paired the plasmon absorption wavelengths with those of the emission of an appropriate fluorophore, which ultimately leads to nanoparticle films that can produce current over narrow wavelength ranges. In this paper, we demonstrate that mixed-metal substrates composed of both Cu and Ag nanoparticles can significantly broaden the wavelength range over which multiple fluorophores from the ultraviolet (UV) to the red part of the visible spectrum can both couple and induce plasmonic current.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"32 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144290100","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

Lattice Phonon-Mediated Exciton-Surface Plasmon Polariton Scattering in Monolayer MoS2–Gold Hybrid Nanostructure 晶格声子介导激子-表面等离子体极化子在单层mos2 -金杂化纳米结构中的散射

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-13 DOI: 10.1021/acs.jpcc.5c01547

Sushant Sharma, Arjun Upadhyay, Parinda Vasa

{"title":"Lattice Phonon-Mediated Exciton-Surface Plasmon Polariton Scattering in Monolayer MoS2–Gold Hybrid Nanostructure","authors":"Sushant Sharma, Arjun Upadhyay, Parinda Vasa","doi":"10.1021/acs.jpcc.5c01547","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01547","url":null,"abstract":"We investigate lattice phonon-mediated scattering in the presence of strong light-matter interaction between excitons in monolayer MoS2 and propagating surface plasmon polaritons (SPPs) at the gold–MoS2 interface at room temperature. The strong radiative exciton–SPP interaction results in characteristic anticrossing in dispersion relation of the hybrid nanostructure at both A and B excitons of monolayer MoS2. The exciton–SPP polariton formation is probed by angle-resolved coherent scattering as well as photoluminescence spectroscopy of the hybrid nanostructure in the Kretschmann configuration and rationalized within the coupled oscillator framework. The phonon-mediated polariton scattering is explored by angle-resolved Raman spectroscopy under resonant excitation conditions. The exciton–SPP polariton Raman spectrum reveals considerable enhancement and broadening, particularly in two-phonon modes involving intervalley scattering accompanied by blue shift of the E2 mode. The pronounced changes are suggestive of higher polariton–phonon interaction cross sections and induced strain. The nonradiative relaxation of the hybrid polariton modes results in hot-electron transfer to monolayer MoS2 that induces compressive strain due to its piezoelectric nature. Our experimental results shed light on the relationship between exciton–SPP interaction, charge transfer, and mechanical strain in metal–semiconductor hybrid nanostructures and demonstrate an innovative all-optical approach to engineer the optical, electronic, and mechanical properties of 2D semiconductors.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"27 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278918","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

In Situ Second Harmonic Generation and Extinction Spectroscopy for Studying Colloidal Gold–Silver–Gold Core–Shell–Shell Nanoparticle Growth Dynamics 研究胶体金-银-金核-壳-壳纳米颗粒生长动力学的原位二次谐波产生和消光光谱

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-13 DOI: 10.1021/acs.jpcc.5c02596

Stena C. Peterson, Daniel A. Babayode, Christopher P. Reso, Louis H. Haber

{"title":"In Situ Second Harmonic Generation and Extinction Spectroscopy for Studying Colloidal Gold–Silver–Gold Core–Shell–Shell Nanoparticle Growth Dynamics","authors":"Stena C. Peterson, Daniel A. Babayode, Christopher P. Reso, Louis H. Haber","doi":"10.1021/acs.jpcc.5c02596","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c02596","url":null,"abstract":"Time-dependent in situ second harmonic generation (SHG) spectroscopy coupled with extinction spectroscopy is used to monitor the growth dynamics involved in the synthesis of colloidal gold–silver–gold core–shell–shell (Au–Ag–Au CSS) nanoparticles in real time. A stepwise seed-mediated method is applied to grow an outer gold shell onto gold–silver core–shell nanoparticles in aqueous solution, using four sequential additions of chloroauric acid and reducing agents. The first addition results in Au–Ag–Au CSS nanoparticles with a bumpy, urchin-like morphology. With each subsequent addition, the outer gold shell thickness increases, while the nanoparticle surface morphology becomes smoother and more uniform. Transmission electron microscopy (TEM) is also utilized to determine the nanoparticle size distribution and surface morphology after each addition. As the size and surface smoothness of the CSS nanoparticles increase, the plasmon extinction spectra blue shift with spectral narrowing and increasing extinction intensity. Comparison with corresponding Mie theory extinction spectra calculations shows general agreement after the fourth addition, demonstrating a spherical concentric nanoarchitecture with a smooth nanoparticle surface. The surface-sensitive SHG signal increases dramatically during the first addition, corresponding to the urchin-like surface morphology, and then decreases as the surface becomes smoother with each subsequent addition. In situ monitoring of the two-photon fluorescence (TPF) signal provides complementary information for comparison to the extinction and SHG results. This combined approach of in situ SHG and extinction spectroscopy with Mie theory simulations and TEM imaging provides a detailed analysis of the synthesis of Au–Ag–Au CSS nanoparticles for investigating complex colloidal nanoparticle growth dynamics occurring at the nanoscale.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"42 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278933","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

Thione–Thiol Tautomerization Induced by Hydrogen Atoms in Amorphous Solids 非晶固体中氢原子诱导的硫-硫醇互变异构

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-13 DOI: 10.1021/acs.jpcc.5c01534

Sándor Góbi, Igor Reva, Barbara Keresztes, Anita Schneiker, György Tarczay

{"title":"Thione–Thiol Tautomerization Induced by Hydrogen Atoms in Amorphous Solids","authors":"Sándor Góbi, Igor Reva, Barbara Keresztes, Anita Schneiker, György Tarczay","doi":"10.1021/acs.jpcc.5c01534","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01534","url":null,"abstract":"Low-temperature neat amorphous ices of thiourea (TU) and N-methyl thiourea (NMTU) were exposed to hydrogen (H) atoms during deposition, generated by an H atom beam source. New spectral features emerged, at positions close to the ones observed in similar experiments, recently reported for the related compound, thioacetamide. These new features appearing upon H atom bombardment were assigned to higher-energy thiol tautomeric forms of TU and NMTU. The mid-infrared (MIR) spectra of unprocessed amorphous TU and NMTU ices are also reported here for the first time. Both compounds, either in amorphous state or in crystals, adopt exclusively the thione form in neat ices. The spectra undergo irreversible changes when the ices are heated up to the crystallization temperature. The MIR spectra of crystalline samples show great similarity with the ones in microcrystalline state dispersed in KBr pellets reported in the literature. The simulated IR spectra provided by quantum-chemical computational methods are in good agreement with the experimental ones; the theoretical data also enabled us to perform the vibrational analysis of the samples. Based on the MIR spectra of the crystalline samples, those of the amorphous ices could also be interpreted. The appearance of the new thiol bands, upon H atom bombardment of the thione precursors, points to the universal nature of thione → thiol tautomerization of thioamides in the presence of H atoms, most probably taking place on the ice surface. Furthermore, we provide a mechanistic explanation of the experimental observations, initiated by the generally facile manner of H atom addition to the sulfur of the thione group.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"4 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278917","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

Photoelectrochemical Hydrogen Generation by Ni-Coated Gallium Arsenide Epilayers on Silicon 硅上镀镍砷化镓薄膜的光电化学制氢

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2025-06-13 DOI: 10.1021/acs.jpcc.5c01840

Fatima Merhi, Bienvenu Boulingui Koumba, Rozenn Bernard, Antoine Létoublon, Paul Huillery, Yoan Léger, Nicolas Bertru, Charles Cornet, Patrick Garrigue, Bruno Fabre, Gabriel Loget

{"title":"Photoelectrochemical Hydrogen Generation by Ni-Coated Gallium Arsenide Epilayers on Silicon","authors":"Fatima Merhi, Bienvenu Boulingui Koumba, Rozenn Bernard, Antoine Létoublon, Paul Huillery, Yoan Léger, Nicolas Bertru, Charles Cornet, Patrick Garrigue, Bruno Fabre, Gabriel Loget","doi":"10.1021/acs.jpcc.5c01840","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01840","url":null,"abstract":"Green hydrogen (H2) can play a pivotal role in reducing global carbon emissions. This renewable fuel can be produced by water-splitting photoelectrochemical (PEC) devices that require a photoanode and a photocathode to serve as solar light absorbers and energy converters. So far, the use of III–V semiconductor materials as photoelectrodes has resulted in the best performance for PEC water splitting. However, the cost of these materials still prohibits their spread. Instead of employing bulk III–V wafers as photoelectrode substrates, using III–V thin film layers on inexpensive substrates to manufacture photoelectrodes appears to be, thus, a promising solution to solve this problem. Herein, we present the preparation and the study of photocathodes consisting of a thin film of GaAs grown by molecular beam epitaxy (MBE) on a p-doped Si (Si:p) substrate, which are subsequently modified by photoelectrodeposition of Ni catalyst. These Ni/GaAs/Si:p photocathodes are used for the solar-driven H2 evolution reaction (HER) in alkaline medium. We show that these photocathodes are stable in operation for several hours under illumination with a 100% Faradaic efficiency for H2. This constitutes the first example of the use of Ni as a catalyst on GaAs photocathodes. While these results support the fact that MBE-grown III–V thin films can afford HER in alkaline media when modified with an inexpensive catalyst, the effect of the GaAs thickness on incident-photon-to-electron conversion efficiency (IPCE) data shows that the III–V layer hinders the overall HER activity of the photoelectrode. Therefore, further material engineering strategies are required to improve the HER performance of these promising photocathodes.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"11 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278931","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