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Reaction of N-methylformamide with dimethyl carbonate: a DFT study N 甲基甲酰胺与碳酸二甲酯的反应：DFT 研究
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-09-11 DOI: 10.1007/s00214-024-03144-7
Yakov D. Samuilov, Alexander Ya. Samuilov
{"title":"Reaction of N-methylformamide with dimethyl carbonate: a DFT study","authors":"Yakov D. Samuilov, Alexander Ya. Samuilov","doi":"10.1007/s00214-024-03144-7","DOIUrl":"https://doi.org/10.1007/s00214-024-03144-7","url":null,"abstract":"<p>The detailed analysis of the mechanism of metathesis of <i>N</i>-methylformamide with dimethyl carbonate leading to the formation of N, O-dimethylcarbamate was carried out using the B3LYP/6-311++G(df,p), B3LYP-D3(BJ)/6-311++G(df,p) and ωB97XD/6-311++G(df,p) density functional methods. The reactions proceed in three stages. The first step consists in the tautomeric conversion of <i>N</i>-methylformamide to iminol. The second stage, which is the rate-limiting step, involves the addition of dimethyl carbonate via the N=C π-bond of iminol. The third stage of the reaction is the cleavage of the methyl formate molecule from <i>N</i>-methyl-<i>N</i>-[(hydroxy)(methoxy)methyl]-O-methylcarbamate. This conversion results in the formation of <i>N</i>, O-dimethylcarbamate. All stages of the reactions are catalyzed by associates of alcohols, which lead to a strong decrease in activation enthalpies.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142201996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Chemical reactivity inside carbon cages: theoretical insights from a fullerene confinement 碳笼内部的化学反应性：富勒烯封闭的理论启示
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-08-17 DOI: 10.1007/s00214-024-03141-w
Christophe Morell, Yanis Abid Charef, Guillaume Hoffmann
{"title":"Chemical reactivity inside carbon cages: theoretical insights from a fullerene confinement","authors":"Christophe Morell, Yanis Abid Charef, Guillaume Hoffmann","doi":"10.1007/s00214-024-03141-w","DOIUrl":"https://doi.org/10.1007/s00214-024-03141-w","url":null,"abstract":"<p>In this paper, we investigate two model reactions (an electrocyclic ring closure and a tautomerism equilibrium) in different sized fullerene cages to explore the intricate details of the confinement effect in chemistry and in chemical reactivity. Fullerene cages offers, with their unique geometry and electronic properties, an ideal theoretical model to explore confinement-induced alterations in reaction pathways and energy barriers. Computational results demonstrate that the induced confinement may significantly influence the thermodynamics and kinetics of the chemical processes under study through a comparative investigation of reactions in various fullerene cage sizes and their occurrence in gas phase. This theoretical investigation intends to improve our knowledge of molecular confinement events, while also highlighting the potential use of fullerene cages as adjustable nanoreactors for regulating and improving chemical reactivity.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202002","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Machine learning for pyrimidine corrosion inhibitor small dataset 嘧啶腐蚀抑制剂小型数据集的机器学习
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-08-09 DOI: 10.1007/s00214-024-03140-x
Wise Herowati, Wahyu Aji Eko Prabowo, Muhamad Akrom, Noor Ageng Setiyanto, Achmad Wahid Kurniawan, Novianto Nur Hidayat, Totok Sutojo, Supriadi Rustad
{"title":"Machine learning for pyrimidine corrosion inhibitor small dataset","authors":"Wise Herowati, Wahyu Aji Eko Prabowo, Muhamad Akrom, Noor Ageng Setiyanto, Achmad Wahid Kurniawan, Novianto Nur Hidayat, Totok Sutojo, Supriadi Rustad","doi":"10.1007/s00214-024-03140-x","DOIUrl":"https://doi.org/10.1007/s00214-024-03140-x","url":null,"abstract":"<p>Machine learning (ML) approaches have been developed to predict materials’ corrosion inhibition efficiency, particularly pyrimidine compounds. Notably, the virtual sample generation (VSG) technique enhances prediction accuracy, a novel approach for handling small datasets in this context. The random forest model, the best-performing nonlinear algorithm, showed substantial accuracy improvement based on the increase in <i>R</i><sup>2</sup> value from 0.05 to 0.99 and the decrease in RMSE value from 5.60 to 0.42, after applying VSG. These results underscore the efficacy of the VSG technique in boosting the predictive performance of ML models, particularly in scenarios constrained by limited data availability.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141943359","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Electronic and optical properties of several cluster-assembled materials based on Zn12O12: a first-principles study 基于 Zn12O12 的几种团簇组装材料的电子和光学特性：第一原理研究
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-08-03 DOI: 10.1007/s00214-024-03139-4
Peixian Wang, Bin Song, Gaoling Zhao
{"title":"Electronic and optical properties of several cluster-assembled materials based on Zn12O12: a first-principles study","authors":"Peixian Wang, Bin Song, Gaoling Zhao","doi":"10.1007/s00214-024-03139-4","DOIUrl":"https://doi.org/10.1007/s00214-024-03139-4","url":null,"abstract":"<p>Based on the first-principles calculations, we systematically studied and fully characterized the electronic structure and optical properties of four novel ZnO phases assembled by Zn<sub>12</sub>O<sub>12</sub> clusters and compared them with the results of wurtzite (WZ) ZnO. The results show that the density of states of the four cluster-assembled materials is similar to that of WZ-ZnO, but the bandgap is larger than that of the latter. Among them, FAU-ZnO, LTA-ZnO, and SOD-ZnO are direct bandgap semiconductors. The calculation of the optical properties of SOD-ZnO is most similar to those of WZ-ZnO, but R-ZnO has higher static permittivity, reflection, and refraction coefficients. Considering that the presence of cage-like voids in cluster-assembled materials is more conducive to doping of various elements, cluster-assembled materials are more likely to change the bandgap and corresponding electronic structure through doping than WZ-ZnO. From this perspective, these two materials have great potential for photocatalytic and optoelectronic device applications.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141943360","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Exploring host–guest interactions of bis(4-nitrophenyl)squaramide with halide anions: a computational investigation in the gas-phase and solution 探索双（4-硝基苯基）方酰胺与卤化阴离子的主客体相互作用：气相和溶液中的计算研究
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-07-25 DOI: 10.1007/s00214-024-03137-6
Yasin Gholiee
{"title":"Exploring host–guest interactions of bis(4-nitrophenyl)squaramide with halide anions: a computational investigation in the gas-phase and solution","authors":"Yasin Gholiee","doi":"10.1007/s00214-024-03137-6","DOIUrl":"https://doi.org/10.1007/s00214-024-03137-6","url":null,"abstract":"<p>A computational study on the host–guest complexes of neutral bis(4-nitrophenyl)squaramide (SQ) and halide anions is reported. In the gas-phase, the calculated interaction and stabilization energies indicates a diminishing intrinsic affinity of SQ for anions from fluoride to iodide. The nature of interactions is investigated using Natural Bond Orbital (NBO), Quantum Theory of Atoms in Molecules (QTAIM) along with Energy Decomposition Analysis-Natural Orbitals for Chemical Valence (EDA-NOCV). While electrostatic interactions account for roughly 60% of the total, EDA-NOCV analysis demonstrated increasing contributions of orbital interactions from <span>(left[ {{text{SQ}} cdots {text{I}}} right]^{ - })</span> to <span>(left[ {{text{SQ}} cdots {text{F}}} right]^{ - })</span> complexes. In solution, thermodynamic cycle analyses and Gibbs free energy calculations reveal a propensity towards the formation of <span>(left[ {{text{SQ}} cdots {text{F}}} right]^{ - })</span>, taking into account the influence of solvation energies on the overall stability. The consistent trend observed in selectivity both in the gas phase and in solution suggests that changes in solvation energy do not significantly impact the stability of complexes. The findings were additionally supported by a significant correlation observed between the computed and experimental formation constants.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141772031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Substitution-induced band shifts and relative population of cis–trans azobenzene 顺反偶氮苯的取代诱导波段移动和相对数量
IF 1.6 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-07-15 DOI: 10.1007/s00214-024-03138-5
Anshul Aggarwal, Anubhav Rajyan, C. N. Ramachandran
{"title":"Substitution-induced band shifts and relative population of cis–trans azobenzene","authors":"Anshul Aggarwal, Anubhav Rajyan, C. N. Ramachandran","doi":"10.1007/s00214-024-03138-5","DOIUrl":"https://doi.org/10.1007/s00214-024-03138-5","url":null,"abstract":"","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141645297","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Product state-resolved reactive scattering calculations using stair shaped grids in hyperspherical coordinates for the quantum wave packet method 使用超球面坐标阶梯形网格进行量子波包法的积态分辨反应散射计算
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-07-12 DOI: 10.1007/s00214-024-03133-w
Umair Umer, Syed Muhammad Usama, Hailin Zhao, Zhigang Sun
{"title":"Product state-resolved reactive scattering calculations using stair shaped grids in hyperspherical coordinates for the quantum wave packet method","authors":"Umair Umer, Syed Muhammad Usama, Hailin Zhao, Zhigang Sun","doi":"10.1007/s00214-024-03133-w","DOIUrl":"https://doi.org/10.1007/s00214-024-03133-w","url":null,"abstract":"<p>Efficient calculations of the quantum product state-resolved differential cross sections play a crucial role in unraveling the dynamics of a chemical reaction. Using hyperspherical coordinates, a stair-shaped grid-based time-dependent quantum wave packet method is proposed for efficiently calculating the product quantum state-resolved reactive scattering information. As numerical examples, quantum product state-resolved reaction probabilities for the reactions of O + O<span>(_{2})</span> and Cl + H<span>(_{2})</span>(<span>(v_0)</span>=1) with <span>(J=0)</span> are computed, which involve long-time resonance states extending over long-range grids and are difficult for obtaining accurate results using the time-dependent method. The results through calculations are being compared to those obtained using the reactant coordinate-based (RCB) method and the interaction-asymptotic decomposition method (IARD).</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141611972","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Comparison of various core electron treatments for studying the properties of II-VI quantum dots and their bulk counterparts: a DFT study 比较用于研究 II-VI 量子点及其大块对应物特性的各种核心电子处理方法：一项 DFT 研究
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-07-04 DOI: 10.1007/s00214-024-03134-9
Rakhi Thareja, Jyoti Singh, Pragati Malik, Rita Kakkar
{"title":"Comparison of various core electron treatments for studying the properties of II-VI quantum dots and their bulk counterparts: a DFT study","authors":"Rakhi Thareja, Jyoti Singh, Pragati Malik, Rita Kakkar","doi":"10.1007/s00214-024-03134-9","DOIUrl":"https://doi.org/10.1007/s00214-024-03134-9","url":null,"abstract":"<p>Quantum dots (QDs) have attracted significant interest because of their tunable bandgaps, which enable numerous applications in fields such as photovoltaics, biomedicine, and materials science. This study explores various core electron treatments in the density functional theory (DFT) analysis of II-VI semiconductor quantum dots and their bulk counterparts. We compared All-electron (AE), Effective Core Potential (ECP), All-Electron Relativistic (AER), and DFT-Semicore pseudopotential (DSPP) treatments. Our findings indicate that the AE treatment aligns closely with the experimental results for smaller QDs, whereas the accuracy of DSPP increases with larger QDs. DSPP provides an optimal balance between computational efficiency and accuracy, making it suitable for studying II-VI QDs. Notably, the bandgap behavior varies, being direct for zinc and cadmium chalcogenides, whereas mercury chalcogenides are zero-gap semiconductors (semimetals). The inner bonds of the QDs exhibit an ionic character, whereas the terminal bonds display a covalent character. This study enhances our understanding of the structural and electronic properties of II-VI quantum QDs, aiding their application in various technologies.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141551647","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Properties of Ti2CO2 and Ti2CO2/G heterostructures as anodes of sodium-ion batteries by first-principles study 通过第一原理研究作为钠离子电池阳极的 Ti2CO2 和 Ti2CO2/G 异质结构的特性
IF 1.7 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-07-03 DOI: 10.1007/s00214-024-03136-7
Cui Liu, Yu Yang, Kui Tang, Feiyang Wu, Yuyang Liu, Zhi Yang, Yuxin Chai, Jianping Sun
{"title":"Properties of Ti2CO2 and Ti2CO2/G heterostructures as anodes of sodium-ion batteries by first-principles study","authors":"Cui Liu, Yu Yang, Kui Tang, Feiyang Wu, Yuyang Liu, Zhi Yang, Yuxin Chai, Jianping Sun","doi":"10.1007/s00214-024-03136-7","DOIUrl":"https://doi.org/10.1007/s00214-024-03136-7","url":null,"abstract":"<p>In this study, the geometric and electronic properties of Ti2CO2 and Ti2CO2/G heterostructures as anode materials for sodium-ion batteries were systematically investigated using first-principles calculations. The storage mechanism and properties of sodium atoms on Ti<sub>2</sub>CO<sub>2</sub> and Ti<sub>2</sub>CO<sub>2</sub>/G heterostructures were further studied. By comparing the adsorption energy (− 1.4 eV, − 1.26 eV), diffusion barrier (0.21 eV, 0.14 eV), storage capacity (478mAh/g, 528mAh/g), average open-circuit voltage (0.68 eV, 0.51 eV), and elastic modulus (161.40 N/m, 364.82 N/m) of sodium atoms on Ti<sub>2</sub>CO<sub>2</sub> and Ti<sub>2</sub>CO<sub>2</sub>/G heterostructures, we found that Ti<sub>2</sub>CO<sub>2</sub>/G heterostructure exhibits superior structural stability, better electronic conductivity, higher storage capacity, lower average open-circuit voltage, lower diffusion barrier, and superior mechanical performance. Through this study, we explore the potential of Ti<sub>2</sub>CO<sub>2</sub>/G as an anode material for sodium-ion batteries and its sodium storage mechanism.</p>","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.7,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141551646","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
Aminolysis of O-methyl-N-methylcarbamate as a model for the production of polyureas. a DFT study 以 O-甲基-N-甲基氨基甲酸酯的氨基分解为聚脲生产模型的 DFT 研究
IF 1.6 4区 化学
Theoretical Chemistry Accounts Pub Date : 2024-07-01 DOI: 10.1007/s00214-024-03135-8
Yakov D. Samuilov, A. Samuilov
{"title":"Aminolysis of O-methyl-N-methylcarbamate as a model for the production of polyureas. a DFT study","authors":"Yakov D. Samuilov, A. Samuilov","doi":"10.1007/s00214-024-03135-8","DOIUrl":"https://doi.org/10.1007/s00214-024-03135-8","url":null,"abstract":"","PeriodicalId":23045,"journal":{"name":"Theoretical Chemistry Accounts","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141697155","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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
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