Computational and Theoretical Chemistry最新文献

{"title":"Rational design and DFT-based study of non-fullerene acceptors for high-performance organic solar cells: End-cap and Core modifications for enhanced charge transfer","authors":"Adeel Mubarik,&nbsp;Faiza Shafiq,&nbsp;Xue-Hai Ju","doi":"10.1016/j.comptc.2025.115209","DOIUrl":"10.1016/j.comptc.2025.115209","url":null,"abstract":"<div><div>In this article, we reported the 64 newly designed non-fullerene acceptors (NFAs) using density functional theory (DFT) approaches combined with both central core and end-cap modification. We screened out five promising molecules among 64 molecules using four specific criteria and their structural as well as optoelectronic attributes were calculated. Using DFT techniques, we thoroughly examined the optical, electrical, and excited state characteristics such as energy gap, maximum absorption, excitation energy (<em>E</em>_<em>x</em>), and oscillator strength to evaluate the effects of various end-cap groups on different core architectures. Furthermore, we paired the most promising NFAs with the P3HT polymer donor to generate donor-acceptor interfaces, and we examined the open circuit voltage (<em>V</em>_<em>oc</em>) and rate of charge transfer (CT) at these interfaces. The conclusions offer insightful advice and useful design guidelines for high-performance NFAs that have the potential to greatly increase solar devices' efficiency.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115209"},"PeriodicalIF":3.0,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143726216","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}

{"title":"First-principles study on single-layer electronic structure of Fe-doped MoS2 and the reduction of NO on the doped surface","authors":"Xiangzhen Xiao ,&nbsp;Yinli Cao ,&nbsp;Linfeng Hu","doi":"10.1016/j.comptc.2025.115172","DOIUrl":"10.1016/j.comptc.2025.115172","url":null,"abstract":"<div><div>Electrocatalytic reduction represents an effective approach for the conversion of the harmful gas nitric oxide (NO) into ammonia (NH₃), a vital chemical precursor in industrial production. However, the large-scale practical application of NO electrocatalytic reduction remains a significant challenge, particularly in the identification of efficient, low-cost, and stable catalysts. In this study, we investigate the electronic structure, magnetic properties, and stability of the Fe-MoS₂ doping system using first-principles calculations. We explore the activation mechanism of NO molecules by Fe-MoS₂ and assess its potential as an electrocatalyst for NO reduction by examining the electronic structure of the adsorbed states. Our results show that Fe doping effectively modulates the electronic structure of MoS₂, significantly enhancing its capacity to adsorb NO compared to pristine molybdenum disulfide surfaces. Analysis of charge transfer and electronic properties during NO adsorption reveals a charge transfer of 0.32e between the substrate and the adsorbed NO molecule. Furthermore, the 2p<span><math><msub><mrow></mrow><mrow><mi>y</mi></mrow></msub></math></span> and 2p<span><math><msub><mrow></mrow><mrow><mi>x</mi></mrow></msub></math></span> orbitals of the nitrogen atom exhibit partial overlap with the 3d<span><math><msub><mrow></mrow><mrow><mi>xy</mi></mrow></msub></math></span>, 3d<span><math><msub><mrow></mrow><mrow><mi>yz</mi></mrow></msub></math></span>, and 3d<span><math><msub><mrow></mrow><mrow><mi>xz</mi></mrow></msub></math></span> orbitals of the Fe atom near the Fermi level, indicating strong interactions that facilitate NO activation. The hydrogenation process of NO to ammonia was further investigated using two different approaches. The results demonstrated the exceptional electrocatalytic reduction activity of Fe-doped S vacancy towards NO. This study not only provides a concise depiction of the Fe-MoS₂ electrocatalyst but also verifies the feasibility of utilizing Fe-MoS₂ for the electrocatalytic synthesis of ammonia from NO.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115172"},"PeriodicalIF":3.0,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143705491","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}

{"title":"Theoretical study of catalytic performance of X-γ-Graphyne as cathodes for lithium-air batteries","authors":"Armando Vera-Garcia ,&nbsp;J.H. Pacheco-Sanchez ,&nbsp;Frank J. Isidro-Ortega ,&nbsp;Abraham González-Ruíz ,&nbsp;J.S. Arellano","doi":"10.1016/j.comptc.2025.115197","DOIUrl":"10.1016/j.comptc.2025.115197","url":null,"abstract":"<div><div>Lithium-air batteries (Li<img>O₂) are considered one of the most promising energy storage and conversion device candidates for future mobility applications, such as electric vehicles, due to their ultrahigh theoretical energy density (up to ∼3600 Wh kg^‐1). The main goal in this work is to study an electrochemical catalytic model for a cathode in Li<img>O₂ batteries to simulate the OER during the discharging process. Density Functional Theory (DFT) calculations were performed to investigate γ-Graphyne and N-γ-Graphyne (N-Doped γ-Graphyne) as the potential cathode catalyst for Li<img>O₂ batteries. γ-Graphyne and N-γ-Graphyne surfaces exhibit high stability according to calculations, the pristine surface exhibits a slight improvement in the formation energy of Li_xO₂, moreover, the N-Doped surface can reduce the significant formation energy of Li_xO₂ in the OER. Calculations explain the catalytic mechanism and identify the active sites to perform N-doping on pristine γ-Graphyne. This study demonstrates a feasible approach to achieve designed γ-Graphyne and N-γ-Graphyne as cathode catalysts for Li air batteries, which is promising for cost reduction in mass production of Li-air batteries.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115197"},"PeriodicalIF":3.0,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143726219","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}

{"title":"Theoretical calculations of thermal functions of diatomic molecules using shifted Deng-Fan potential","authors":"Ahmad Ghanbari","doi":"10.1016/j.comptc.2025.115186","DOIUrl":"10.1016/j.comptc.2025.115186","url":null,"abstract":"<div><div>We have theoretically investigated the thermodynamic properties of diatomic molecules using shifted Deng-Fan potential. To this end, we have solved the Schrödinger eq. (SE) with the oscillator potential applying the Nikiforov-Uvarov method and have obtained energy eigenvalues. Using calculated eigenvalues, we have determined partition function and thermodynamic properties of diatomic molecules such as H₂, HCl and LiH. We have obtained the properties like mean energy, specific heat in constant volume, entropy and free energy. Also, we have calculated specific heat in constant pressure, enthalpy and Gibbs free energy of the molecules and compared our calculated data with experimental data. Our results show that there is a good agreement between them. We have determined average deviations of our results and experimental data.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115186"},"PeriodicalIF":3.0,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143734517","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}

{"title":"Theoretical investigation on the reaction kinetics of H with furfural","authors":"Qiongxuan Zhu ,&nbsp;Lili Xing ,&nbsp;Liuchao Lian ,&nbsp;Jing Zhu ,&nbsp;Xuetao Wang","doi":"10.1016/j.comptc.2025.115190","DOIUrl":"10.1016/j.comptc.2025.115190","url":null,"abstract":"<div><div>The reaction between furfural and H plays a crucial role in its thermal decomposition, but its specific kinetic data are not yet available. We used a high-level quantum chemistry method to model the potential energy surface of the furfural + H system. According to the potential energy surface, H-addition to the C_ε site has the highest energy barrier, while H-addition to the C_δ position has the lowest energy barrier. In the low-temperature range of 298-600 K, H-abstraction is faster than preliminary H-addition reaction. However, the H-addition reaction dominates when T&gt;600K. Subsequent reaction pathways of the formed intermediates were also analyzed. The temperature and pressure dependence of rate constants were studied and discussed. This study reveals distinct behaviors in the rate constants for intermediates and bimolecular products across different temperature ranges. These findings could aid in developing more accurate kinetic models.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115190"},"PeriodicalIF":3.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143715742","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}

{"title":"Isomorphic graphene-like building unit","authors":"Fernando Alvarez-Ramírez ,&nbsp;Ariel A. Valladares","doi":"10.1016/j.comptc.2025.115195","DOIUrl":"10.1016/j.comptc.2025.115195","url":null,"abstract":"<div><div>A novel structural unit is proposed for constructing crystalline materials and molecular systems by mimicking the morphologies of carbon in its sp² allotropic forms. The new family of layered graphene-like crystals in 2D lattices exhibit crown ether-like cycles. The proposed structures are not limited to a single chemical element, carbon, and have the potential to modulate electronic properties based on their composition. Nine combinations of atomic elements of the structural unit are presented, which give rise to structures whose electronic gaps can vary from zero to 2.597 eV for a B-N-S-Si combination of the basic unit. Depending on the atomic composition, this structural unit may give rise to unstable or stable structures. The elastic constant analysis shows that three of the proposed structures are mechanically stable, while only the N-C-O-Ni configuration is both mechanically and dynamically stable, which is confirmed by the absence of negative frequencies in the dispersion calculations.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115195"},"PeriodicalIF":3.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682226","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}

{"title":"What drives enhanced chloride recognition of squaramide-based receptors over urea and thiourea? A computational exploration in the gas-phase and various solvents","authors":"Yasin Gholiee","doi":"10.1016/j.comptc.2025.115191","DOIUrl":"10.1016/j.comptc.2025.115191","url":null,"abstract":"<div><div>Significant progress in anion recognition has been achieved through the development of synthetic receptors. Urea-, thiourea-, and squaramide-based molecules, known for hydrogen-bonding capabilities, have gained prominence in supramolecular chemistry. The superior anion recognition of squaramide-based receptors, compared to urea- and thiourea-based ones, is repeatedly attributed to the crucial involvement of C<img>H fragments. This study computationally investigates chloride recognition by nine symmetric urea-, thiourea-, and squaramide-based receptors, focusing on solvent effects, interactions, and intrinsic affinity. The findings suggest that while C<img>H fragments aid anion recognition in squaramide-based receptors, the absence of steric repulsion and the presence of attractive forces between amide NH groups in squaramide, unlike in urea and thiourea receptors, significantly enhances anion-binding ability. Although solvation energy becomes less favorable from urea to squaramide, negative gas-phase Gibbs free energy drives complex formation. The accuracy of computational results is validated by excellent correlation between experimental and calculated formation constants.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115191"},"PeriodicalIF":3.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682225","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}

{"title":"Examining the power of BiXO3 (X = Cr, Cu) oxide-perovskites: A first-principles study for next-generation solar cells","authors":"Hadia Khalil ,&nbsp;Misbah Tabassum ,&nbsp;Jalil Ur Rehman ,&nbsp;Syed Mansoor Ali ,&nbsp;Rajeh Alotaibi","doi":"10.1016/j.comptc.2025.115194","DOIUrl":"10.1016/j.comptc.2025.115194","url":null,"abstract":"<div><div>The current study investigates the structural, electronic, optical, and mechanical aspects of Bi-based oxide-perovskites BiXO₃ (X = Cr, Cu) while using first-principles simulations. BiCrO₃ and BiCuO₃ have lattice parameters of 3.85 and 3.87 Å, respectively. Both the materials have semiconducting properties with a direct band gap as indicated by the band structure and density of states. The computed energy band gap for BiCrO₃ and BiCuO₃ is found 1.68 and 1.36 eV, respectively. To describe how light interacts with the material, the optical characteristics of both materials are examined for photon energies between 0 and 12 eV. Based on their mechanical properties, it is found that both materials are mechanically stable, hard, and incompressible. According to Cauchy pressure and Pugh's ratio, both the compounds show a ductile behavior. The overall investigation shows that both materials are appropriate for next generation solar cells.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115194"},"PeriodicalIF":3.0,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682227","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}

{"title":"Substitution and coordination effects of boron in FeC and FeNC single-atom catalysts for ORR: A DFT study","authors":"L.L. Sun ,&nbsp;Z.Y. Wang ,&nbsp;Y.H. Wang ,&nbsp;Y. Wang ,&nbsp;Y.C. Li","doi":"10.1016/j.comptc.2025.115192","DOIUrl":"10.1016/j.comptc.2025.115192","url":null,"abstract":"<div><div>The development of durable and cost-effective cathode catalysts is critical to improving the oxygen reduction reaction (ORR) of fuel cells. The B-substituted Fe-based graphene single atom catalysts (SACs) were systematically analyzed using density functional theory (DFT). After analysis of the computational formation energy, 12 stable configurations are identified from 49 candidates. B-substituted in the first coordination sphere layer resulted in excessively strong adsorption of oxygen-containing intermediates, thereby increasing the overpotential. In contrast, the FeN₄B_<del>4</del> and FeN₄B₅ catalysts, with B substitution in the second coordination sphere, exhibited low overpotentials of 0.32 V and 0.36 V, respectively. This enhancement is attributed to the B-atom-induced reconfiguration of the electronic structure and modulation of chemical bonding properties.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115192"},"PeriodicalIF":3.0,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682224","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}

{"title":"Two bond-exchange modes in sodium silicate liquids: Slide and oscillation modes","authors":"Fumiya Noritake","doi":"10.1016/j.comptc.2025.115196","DOIUrl":"10.1016/j.comptc.2025.115196","url":null,"abstract":"<div><div>The network structure of polymerized silicate liquids suppresses the diffusion mechanism of silicon and oxygen atoms. Several diffusion model for these network forming elements have been presented based on nuclear magnetic resonance spectroscopy and molecular dynamics simulations. The authors' previous study introduced the concept of bond-breaking/forming particle, that can analyze quantitatively the certain bond exchange event from pair correlation functions of those particles. In this study, the angular part of the pair-correlation function of bond-breaking/forming particles was introduced, and an atomistic description of the two different bond exchange modes, that found in the author's previous study, was revealed. The first peak represent exchange of Si<img>O bonds in a sliding manner, whereas the second peak correspond to exchange in an oscillating manner. The inner product of vectors correspond to broken and newly formed bond is zero to positive in former mode, negative in latter mode.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1248 ","pages":"Article 115196"},"PeriodicalIF":3.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682223","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}