{"title":"银纳米粒子核心电子结合能的测量及其与银簇电子传播计算的模型建立","authors":"","doi":"10.1016/j.ica.2024.122338","DOIUrl":null,"url":null,"abstract":"<div><p>Silver nanoparticles were synthesized by ionic exchange with zeolites and further reduction with hydrogen flux. Core electron binding energies were determined by X-ray photoelectron spectroscopy at different times of the reduction process. Electron propagator calculations of core electron binding energies were performed including scalar relativistic effects using effective core potentials and zero order regular approximation. Theoretical results were compared to the experiment to get insight into the origin of the experimental signals for carbon, oxygen, silicon, aluminum and silver. Small model molecules and zeolite fragments were used for the calculation of core electron binding energies. It is evidenced that although binding energies tend to converge, fluctuations of more than 1 eV are found for non-symmetric structures in neutral and cationic silver clusters. Detailed analysis shows that these fluctuations originate on the different coordination numbers of ionized silver atoms and charge fluctuations.</p></div>","PeriodicalId":13599,"journal":{"name":"Inorganica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Measurement of core electron binding energies of silver nanoparticles and their modeling with electron propagator calculations of silver clusters\",\"authors\":\"\",\"doi\":\"10.1016/j.ica.2024.122338\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Silver nanoparticles were synthesized by ionic exchange with zeolites and further reduction with hydrogen flux. Core electron binding energies were determined by X-ray photoelectron spectroscopy at different times of the reduction process. Electron propagator calculations of core electron binding energies were performed including scalar relativistic effects using effective core potentials and zero order regular approximation. Theoretical results were compared to the experiment to get insight into the origin of the experimental signals for carbon, oxygen, silicon, aluminum and silver. Small model molecules and zeolite fragments were used for the calculation of core electron binding energies. It is evidenced that although binding energies tend to converge, fluctuations of more than 1 eV are found for non-symmetric structures in neutral and cationic silver clusters. Detailed analysis shows that these fluctuations originate on the different coordination numbers of ionized silver atoms and charge fluctuations.</p></div>\",\"PeriodicalId\":13599,\"journal\":{\"name\":\"Inorganica Chimica Acta\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2024-08-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganica Chimica Acta\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0020169324004298\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganica Chimica Acta","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0020169324004298","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0
摘要
银纳米粒子是通过与沸石进行离子交换并进一步用氢气通量还原而合成的。通过 X 射线光电子能谱测定了还原过程中不同时间的核心电子结合能。利用有效核心势和零阶正则近似对核心电子结合能进行了电子传播计算,其中包括标量相对论效应。将理论结果与实验结果进行比较,以深入了解碳、氧、硅、铝和银实验信号的来源。计算核心电子结合能时使用了小模型分子和沸石碎片。结果表明,虽然结合能趋于收敛,但在中性和阳离子银簇的非对称结构中发现了超过 1 eV 的波动。详细分析表明,这些波动源于电离银原子的不同配位数和电荷波动。
Measurement of core electron binding energies of silver nanoparticles and their modeling with electron propagator calculations of silver clusters
Silver nanoparticles were synthesized by ionic exchange with zeolites and further reduction with hydrogen flux. Core electron binding energies were determined by X-ray photoelectron spectroscopy at different times of the reduction process. Electron propagator calculations of core electron binding energies were performed including scalar relativistic effects using effective core potentials and zero order regular approximation. Theoretical results were compared to the experiment to get insight into the origin of the experimental signals for carbon, oxygen, silicon, aluminum and silver. Small model molecules and zeolite fragments were used for the calculation of core electron binding energies. It is evidenced that although binding energies tend to converge, fluctuations of more than 1 eV are found for non-symmetric structures in neutral and cationic silver clusters. Detailed analysis shows that these fluctuations originate on the different coordination numbers of ionized silver atoms and charge fluctuations.
期刊介绍:
Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews.
Topics covered include:
• chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies;
• synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs);
• reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models;
• applications of inorganic compounds, metallodrugs and molecule-based materials.
Papers composed primarily of structural reports will typically not be considered for publication.