Computational and Theoretical Chemistry最新文献_第7页

Intrinsic reactivity of stoichiometric IrO2(1 1 0) surface toward oxidative coupling of methane 定量IrO2(1 1 0)表面对甲烷氧化偶联的内在反应性

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-20 DOI: 10.1016/j.comptc.2024.114922

Jungwon Yun , Seongjun Lee , Dasol Bae , Minkyu Kim

{"title":"Intrinsic reactivity of stoichiometric IrO2(1 1 0) surface toward oxidative coupling of methane","authors":"Jungwon Yun , Seongjun Lee , Dasol Bae , Minkyu Kim","doi":"10.1016/j.comptc.2024.114922","DOIUrl":"10.1016/j.comptc.2024.114922","url":null,"abstract":"<div><div>This study investigates the oxidative coupling of methane on the IrO<sub>2</sub>(110) surface using TPRS simulations informed by DFT-derived data. We discover that the efficiency of the IrO<sub>2</sub>(110) surface in generating ethylene is strongly influenced by methane surface coverage. Our simulations reveal that the presence of surface hydroxyl group enhances the yield of C<sub>2</sub>+ species from methane oxidation, but this effect is counteracted at high methane coverages due to the accelerated formation of CH<sub>2</sub>OH. In addition, the study reveals that slight modifications in energy barriers at the branching point (C<sub>2</sub>H<sub>4</sub> formation vs. CH<sub>2</sub>OH formation) significantly affect C<sub>2</sub>H<sub>4</sub>(g) production from the simulation, underscoring the importance of precise energetic data for accurate catalytic reaction predictions. The results have broader implications for reactions and catalysts where branching point selectivity determines high-value product yields. Thus, combining surface science with computational analysis is crucial for accurately determining energy profiles of key steps at the branching points.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114922"},"PeriodicalIF":3.0,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529106","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

Mechanistic studies on phosphine-catalyzed [4 + 3] annulation of β′-acetoxy allenoate with 1C,3N-dinucleophile 膦催化 β′-乙酰氧基异烯酸酯与 1C,3N-二核亲和剂的 [4 + 3] 环化机理研究

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-19 DOI: 10.1016/j.comptc.2024.114924

Kui Yuan, Hao-Ran Yang, Yang Wang

{"title":"Mechanistic studies on phosphine-catalyzed [4 + 3] annulation of β′-acetoxy allenoate with 1C,3N-dinucleophile","authors":"Kui Yuan, Hao-Ran Yang, Yang Wang","doi":"10.1016/j.comptc.2024.114924","DOIUrl":"10.1016/j.comptc.2024.114924","url":null,"abstract":"<div><div>The mechanism and role of catalyst on the PPh<sub>3</sub>-catalyzed [4 + 3] annulation reaction have been systematically investigated using density functional theory (DFT) method. Based on the calculations, the possible mechanism contains six steps: nucleophilic addition of PPh<sub>3</sub> to allenoate to give Z-configured intermediate, cleavage of C<img>O bond for forming phosphonium diene, nucleophilic addition of phosphonium diene with anionic 1C,3N-dinucleophile, intramolecular <span><span>[1]</span></span>, <span><span>[5]</span></span>-proton shift, ring-closure, and dissociation of catalyst. Non-covalent interaction (NCI) analysis shows that the O<strong>⋯</strong>P interaction would be the key for leading to the Z-configured pathway more favorable and electron localization function (ELF) analysis indicates that the implication of PPh<sub>3</sub> can significantly lower the energy barrier involved in C<img>O cleavage process, which mainly because the addition of PPh<sub>3</sub> reduces the electron density of C<img>O bond and thus facilities the cleavage of C<img>O bond. This theoretical study would provide some clues for understanding the role of catalyst in a catalytic reaction.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114924"},"PeriodicalIF":3.0,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529113","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

A comprehensive DFT Study of the electronic structure and optical properties of Iodine-based halide double perovskites for photovoltaic applications 用于光伏应用的碘基卤化物双包晶石的电子结构和光学特性的 DFT 综合研究

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-18 DOI: 10.1016/j.comptc.2024.114916

B. Mouhib , S. Dahbi , N. Baaalla , N. Tahiri , O. El Bounagui , A. El Mansouri , H. Ez-Zahraouy

{"title":"A comprehensive DFT Study of the electronic structure and optical properties of Iodine-based halide double perovskites for photovoltaic applications","authors":"B. Mouhib , S. Dahbi , N. Baaalla , N. Tahiri , O. El Bounagui , A. El Mansouri , H. Ez-Zahraouy","doi":"10.1016/j.comptc.2024.114916","DOIUrl":"10.1016/j.comptc.2024.114916","url":null,"abstract":"<div><div>This study aims to explore the electronic structure, thermodynamic, mechanical stability, and optical response of Iodine-based ordered vacancy double halide perovskite compounds through the application of density functional theory. The two compounds Cs<sub>2</sub>ZrI<sub>6</sub> and Rb<sub>2</sub>ZrI<sub>6</sub> exhibit thermodynamic stability, with displaying particularly notable. Moreover, analysis of the calculated coefficients of elastic stiffness confirms the mechanical stability of all materials under ambient pressure conditions. By using the Density Functional Theory with Spin-Orbit Coupling (SOC), it was observed that Cs2TeI6 and Rb2TeI6 possess an indirect band gap located between the X and L high-symmetry points, this show that Cs<sub>2</sub>TeI<sub>6</sub>, Rb<sub>2</sub>ZrI<sub>6</sub>, Cs<sub>2</sub>HfI<sub>6</sub>, and Rb<sub>2</sub>HfI<sub>6</sub> are identified as direct semiconductor compounds. Moreover, the band gap values of X<sub>2</sub>YI<sub>6</sub> (where X = Cs, Rb, and Y = Te, Zr, and Hf) exhibit an increasing trend as we progress along the alkali and transition metal elements in the periodic table, ranging from 1.422 eV for Cs<sub>2</sub>TeI<sub>6</sub> to 2.465 eV for Rb<sub>2</sub>TeI<sub>6</sub>. Besides, the optical behavior of the visible light show that X<sub>2</sub>YI<sub>6</sub> compounds have a high absorption of about 70%, reflectance of 30%, and a low transmittance. Thanks to their advantageous bandgap, enduring stabilities, and effective absorption of visible light, Cs<sub>2</sub>TeI<sub>6</sub> and Rb<sub>2</sub>TeI<sub>6</sub> hold significant promise for a wide range of electronic and optoelectronic applications, particularly in photovoltaics.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114916"},"PeriodicalIF":3.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529107","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

TM@MoSSe (TM = Ni, Fe) as novel electrocatalysts for reduction of CO2 to CO: A DFT study TM@MoSSe（TM = Ni、Fe）作为将 CO2 还原成 CO 的新型电催化剂：DFT 研究

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-18 DOI: 10.1016/j.comptc.2024.114929

Yu-Pu He , Tian-Hao Guo , Shao-Yi Wu , Shi-Yu Zuo , Jun-Chao Fu , Xiao-Yu Li

{"title":"TM@MoSSe (TM = Ni, Fe) as novel electrocatalysts for reduction of CO2 to CO: A DFT study","authors":"Yu-Pu He , Tian-Hao Guo , Shao-Yi Wu , Shi-Yu Zuo , Jun-Chao Fu , Xiao-Yu Li","doi":"10.1016/j.comptc.2024.114929","DOIUrl":"10.1016/j.comptc.2024.114929","url":null,"abstract":"<div><div>It is crucial to develop highly efficient, selective and low-overpotential electrocatalysts for CO<sub>2</sub> reduction. This paper proposes an efficient iron and nickel single-atom catalyst using Janus MoSSe as the substrate to reduce CO<sub>2</sub> to CO by using DFT calculations. The adsorption of a single TM atom like Fe, Co, Ni, Ru, Rh, Pd, Os, Ir and Pt on Janus MoSSe monolayer results in a decrease in band gap, which may accelerate the catalytic CO<sub>2</sub> reduction. The excellent catalytic activity of Fe@MoSSe and Ni@MoSSe is owing to the high <em>d</em>-band center and hence the strong TM-CO<sub>2</sub> bonding. The asymmetric structure of Janus MoSSe creates the local built-in electric field, which further increases by about 8% or 0.8% after the adsorption of single Ni or Fe atom so as to afford the better electrocatalytic performances for reduction of CO<sub>2</sub> to CO in both TM modified systems. So, this work proposes the catalysts Fe@MoSSe and Ni@MoSSe with good selectivity and activity for CO<sub>2</sub> reduction by revealing their underlying mechanisms, and Janus MoSSe may be used as a potential substrate material for CO<sub>2</sub> reduction catalysts.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114929"},"PeriodicalIF":3.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529116","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

Atomic-scale mechanistic study of oxygen reduction mechanism for B-site doped Pr(Ba,Sr)Co2O5+δ by density functional theory calculations 通过密度泛函理论计算对 B 位掺杂 Pr(Ba,Sr)Co2O5+δ的氧还原机制进行原子尺度的机理研究

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-18 DOI: 10.1016/j.comptc.2024.114930

Lin Li , Xiaolu Xiong , Jian-Qiang Wang

{"title":"Atomic-scale mechanistic study of oxygen reduction mechanism for B-site doped Pr(Ba,Sr)Co2O5+δ by density functional theory calculations","authors":"Lin Li , Xiaolu Xiong , Jian-Qiang Wang","doi":"10.1016/j.comptc.2024.114930","DOIUrl":"10.1016/j.comptc.2024.114930","url":null,"abstract":"<div><div>Pr(Ba,Sr)Co<sub>2</sub>O<sub>5+δ</sub> is a promising cathode material for solid oxide fuel cell (SOFC) due to its high oxygen ion transport capability and oxygen reduction activity. Density functional theory (DFT) calculations were performed to elucidate the oxygen reduction mechanism of B-site doped Pr(Ba,Sr)(Co,M)<sub>2</sub>O<sub>5+δ</sub> (M = Fe, Ni, Cu, and Zn) materials. First, we investigated the formation of O vacancies. The results indicate that Cu and Zn doping facilitate O vacancy formation, resulting in lower O vacancy formation energies. Furthermore, the interaction between oxygen and the (0 0 1) surfaces of B-site doped Pr(Ba,Sr)(Co,M)<sub>2</sub>O<sub>5+δ</sub> has been comprehensively discussed, involving both perfect and defective surfaces. The results demonstrate that the presence of O vacancies enhances the catalytic activity for oxygen reduction, by reducing the energy required for O<sub>2</sub> dissociation. Zn-doped Pr(Ba,Sr)(Co,M)<sub>2</sub>O<sub>5+δ</sub> exhibits a low O vacancy formation energy, resulting in a stable adsorption configuration upon oxygen dissociation, indicating its potential as a cathode material for SOFC.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114930"},"PeriodicalIF":3.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529103","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

A theoretical approach on the removal of elemental Cu and Cu (I) ions applying the g-C3N4S, g-C3N4O, g-C3N4N, and g-C3N4 nanosheets 利用 g-C3N4S、g-C3N4O、g-C3N4N 和 g-C3N4 纳米片去除元素铜和铜 (I) 离子的理论方法

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-18 DOI: 10.1016/j.comptc.2024.114917

Farag M.A. Altalbawy , Safaa Mustafa Hameed , M.M. Rekha , Anurag Mishra , Shilpa Sharma , G.V. Siva Prasad , Iman Samir Alalaq , Ayadh Al-khalidi , Ahmed Ali Mtasher , Fadeel F. Seed

{"title":"A theoretical approach on the removal of elemental Cu and Cu (I) ions applying the g-C3N4S, g-C3N4O, g-C3N4N, and g-C3N4 nanosheets","authors":"Farag M.A. Altalbawy , Safaa Mustafa Hameed , M.M. Rekha , Anurag Mishra , Shilpa Sharma , G.V. Siva Prasad , Iman Samir Alalaq , Ayadh Al-khalidi , Ahmed Ali Mtasher , Fadeel F. Seed","doi":"10.1016/j.comptc.2024.114917","DOIUrl":"10.1016/j.comptc.2024.114917","url":null,"abstract":"<div><div>In this project, the possibility of removal of copper (elemental Cu (0) and Cu (I) ion) from the environment by applying some heteroatom decorated graphitic carbonitride (g-C<sub>3</sub>N<sub>4</sub>) nanosheets has been investigated. Due to the recent reports about the toxicity of Cu overload and its intervention in a wide range of health problems such as Wilson’s disease (Cu overload), elimination of this element from the environment is important (in view of medicinal chemistry and health science). Thus, this research has focused on the investigations that are related to the possibility of removal of Cu ions from the environment (applying the g-C<sub>3</sub>N<sub>4</sub> nanosheet and its derivatives). The results have shown that the g-C<sub>3</sub>N<sub>4</sub>N is the strongest nanosheet for adsorption and removal of both Cu (0) atom, and Cu (I) ion. In addition, in view of sensing abilities, the results have indicated that the best sensor (having the ability of recognition of Cu (0) atom from Cu (I) ion, is C<sub>3</sub>N<sub>4</sub>O.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114917"},"PeriodicalIF":3.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529110","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

Theoretical computation of thermodynamic functions of sodium dimer with modified shifted Morse potential 用修正的移位莫尔斯势理论计算钠二聚体的热力学函数

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-18 DOI: 10.1016/j.comptc.2024.114925

U.S. Okorie, G.J. Rampho

引用次数: 0

Novel topological reverse indices and entropies of armchair versus zigzag polyhex carbon nanotubes with spectroscopic applications 臂形与人字形聚己碳纳米管的新型拓扑反向指数和熵及其光谱应用

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-17 DOI: 10.1016/j.comptc.2024.114921

Medha Itagi Huilgol , P.H. Shobha , Krishnan Balasubramanian

引用次数: 0

Molecular design and characterization of the PANI/yttrium oxide multifunctional nanocomposite material PANI/yttium oxide 多功能纳米复合材料的分子设计与表征

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-16 DOI: 10.1016/j.comptc.2024.114904

Regina M. Burganova, Sadegh Kaviani, Irina I. Piyanzina, Oleg V. Nedopekin

引用次数: 0

Machine learning prediction of hydrogen adsorption energy on platinum nanoclusters: A comparative study of SOAP descriptors 铂纳米团簇氢吸附能的机器学习预测：SOAP 描述子比较研究

IF 3 3区化学

Computational and Theoretical Chemistry Pub Date : 2024-10-15 DOI: 10.1016/j.comptc.2024.114923

Zhiheng Yu , Yanli Li , Yanwei Wen , Bin Shan , Jiaqiang Yang

{"title":"Machine learning prediction of hydrogen adsorption energy on platinum nanoclusters: A comparative study of SOAP descriptors","authors":"Zhiheng Yu , Yanli Li , Yanwei Wen , Bin Shan , Jiaqiang Yang","doi":"10.1016/j.comptc.2024.114923","DOIUrl":"10.1016/j.comptc.2024.114923","url":null,"abstract":"<div><div>Hydrogen binding energy in metal materials is of high significance in the hydrogen storage as well as the hydrogen evolution reaction of electrocatalysis. In this work, the datasets (more than 9000 data) of hydrogen adsorbed on Pt nanoclusters with different sizes are obtained by first-principles calculations. Data analysis shows that the binding strength of hydrogen with Pt is closely relevant to the local structures of the adsorption sites. The local features of the distance between the platinum and hydrogen and the size of the nanoclusters are supplemented to the Smooth Overlap of Atomic Positions descriptors to fit and predict the adsorption energies of hydrogen on different Pt nano-structures by performing the machine learning method. Gaussian Process Regression (GPR) and Random Forest Regressor (RFR) are used to construct the prediction model of hydrogen binding energies and it is found the R<sup>2</sup> of test set is improved from 0.63 to 0.78 with modified descriptors. By applying it into other nanoclusters, the MAE of the prediction model is 0.08 eV, which exhibits high accuracy of the hydrogen adsorption energy. Our model can be easily extended to the prediction of hydrogen adsorption energy of other materials with affordable computational cost and accuracy, which would be helpful for the structural design of high-performance catalysts.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1241 ","pages":"Article 114923"},"PeriodicalIF":3.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142529642","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