Structural Chemistry最新文献_第6页

Zwitterionic energetic materials containing an oxatriazole explosophore: an exploration of structure and performance 含恶三唑炸药的两性离子高能材料：结构和性能的探索

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-23 DOI: 10.1007/s11224-025-02456-z

Congming Ma, Zhihui Gu, Jiani Xu, Peng Ma, Bo Wu

{"title":"Zwitterionic energetic materials containing an oxatriazole explosophore: an exploration of structure and performance","authors":"Congming Ma, Zhihui Gu, Jiani Xu, Peng Ma, Bo Wu","doi":"10.1007/s11224-025-02456-z","DOIUrl":"10.1007/s11224-025-02456-z","url":null,"abstract":"<div>Inspired by high nitrogen and oxygen content and a unique internal onium salt structure, twenty-seven zwitterionic molecules containing an oxatriazole explosophore were designed and further explored. Their electronic structures, heats of formation (HOF), detonation properties, thermal stabilities, thermodynamic properties, and electrostatic potential were systematically investigated by density functional theory. The calculation results indicate that after ionization of the oxatriazole ring, the bond length shows an average trend, providing impetus for the formation of energetic oxatriazole cationic salts. And energetic materials with diazo substituted structures are more extensive, which is consistent with the results of electronic structure. Interaction region indicator studies have shown that the more places and wider the range of van der Waals forces exist in similar energetic inner salts, the higher the calculated density of the substance. It has been proved that the atomization method is superior for calculating heat of formation of energetic inner salts. When the carbon atom of the triazole ring is replaced with a nitrogen atom, detonation velocity increases by 8–12%, and detonation pressure increases by 20–28%. This work could provide interesting inspiration for the hunting of novel zwitterionic energetic materials.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1339 - 1353"},"PeriodicalIF":2.2,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145167953","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

Re3(C6O6)2 monolayer: a promising metal–organic framework-based electro-catalyst for N2 reduction reaction Re3(C6O6)2单层：一种很有前途的用于N2还原反应的金属-有机骨架电催化剂

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-22 DOI: 10.1007/s11224-025-02449-y

Honglan Li, Lei Yang, Xinglin Yang

{"title":"Re3(C6O6)2 monolayer: a promising metal–organic framework-based electro-catalyst for N2 reduction reaction","authors":"Honglan Li, Lei Yang, Xinglin Yang","doi":"10.1007/s11224-025-02449-y","DOIUrl":"10.1007/s11224-025-02449-y","url":null,"abstract":"<div>Electro-catalytic nitrogen (N2) reduction reaction (NRR) is a highly efficient approach for synthesizing ammonia (NH3). Herein, we have designed a series of transition metal atom-based single-layer organic frameworks (TM3(C6O6)2) using density functional theory (DFT) calculations to systematically investigate their electro-catalytic performance for NRR. Our studies indicate that two-dimensional (2D) Re3(C6O6)2 exhibits the most moderate N2 activation and lowest limiting potential of − 0.31 V among the 24 TM3(C6O6)2 candidates. Also, Re3(C6O6)2 can severely mitigate the competitive process of hydrogen evolution reaction (HER), which suggests remarkable performance regarding efficiency and selectivity of NRR. More interestingly, a feasible self-assembly strategy is proposed due to its suitable lattice matching compared with Cu(111) bulk, further contributing to its successful synthesis. This work may provide solid theoretical support for the rational design of outstanding electro-catalysts toward sustainable NH3 synthesis.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1331 - 1338"},"PeriodicalIF":2.2,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145168186","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

Conformational analysis of soticlestat, an inhibitor of CYP46A1 (CH24H), and its derivatives by variable-temperature nmr and computational methods CYP46A1 （CH24H）抑制剂soticlestat及其衍生物的变温核磁共振和计算分析

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-22 DOI: 10.1007/s11224-025-02459-w

Wenqian Huang, Xinwei Hu, Xiaotong Lin, Maaz Khan, Chunli Qian, Jiang Wu, Fancui Meng, Guilong Zhao

引用次数: 0

Quantum chemical study of the structure and structural transformations of hydrated forms of tin dioxide 水合二氧化锡结构和结构转化的量子化学研究

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-21 DOI: 10.1007/s11224-025-02460-3

O. V. Filonenko, A. G. Grebenyuk, V. V. Lobanov

{"title":"Quantum chemical study of the structure and structural transformations of hydrated forms of tin dioxide","authors":"O. V. Filonenko, A. G. Grebenyuk, V. V. Lobanov","doi":"10.1007/s11224-025-02460-3","DOIUrl":"10.1007/s11224-025-02460-3","url":null,"abstract":"<div>A systematic quantum chemical study on the spatial structure and energy characteristics of the cluster models for nanoparticles of hydrated forms of tin dioxide (SnO2)x⋅yH2O has been carried out by the second-order Möller-Plesset perturbation theory with the SBKJC valence-only basis set expanded by polarization d and p functions and with respective effective core potential, and the formation mechanisms of the simplest nanostructures from the initial forms of tin hydroxide have been elucidated. It has been shown that the formation of the dimer (SnO2)2⋅4H2O due to association of two Sn(OH)4 molecules is energetically most advantageous, and a possible mechanism of its formation is proposed. Various forms for trimeric and tetrameric structures of tin hydroxide have been considered. The most energetically profitable isomers are characterized by double oxygen bridges. Besides, some of them are additionally strengthened by intermolecular hydrogen bonds. Further transformations of the nanoparticles lead to an increase in their size, dehydration, and the formation of denser structures that have crystallinity features inherent in solid-phase SnO2.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1295 - 1304"},"PeriodicalIF":2.2,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145166958","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

Computational study on the mechanisms and kinetics of the CH2XO2 + I (X = F、Cl、Br and I) reactions in the atmosphere 大气中CH2XO2 + I （X = F, Cl， Br和I）反应机理和动力学的计算研究

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-20 DOI: 10.1007/s11224-025-02453-2

Jikang Gao, Meilian Zhao, Junchao Liao, Yaru Wang, Yunju Zhang

{"title":"Computational study on the mechanisms and kinetics of the CH2XO2 + I (X = F、Cl、Br and I) reactions in the atmosphere","authors":"Jikang Gao, Meilian Zhao, Junchao Liao, Yaru Wang, Yunju Zhang","doi":"10.1007/s11224-025-02453-2","DOIUrl":"10.1007/s11224-025-02453-2","url":null,"abstract":"<div>The mechanisms, kinetics and ecotoxicity valuation of the gas-phase CH2XO2 (X = F、Cl、Br and I) with I reactions were investigated by using quantum chemical methods. The calculated results indicate that the title reactions could ocure on either the singlet or triplet potential energy surfaces (PES). Addition/elimination, SN2 displacement and H-abstraction mechanisms were found on the singlet PES, and only SN2 displacement mechanism was located on the triplet PES. The dominant reaction takes place on the singlet PES, and the primary pathway is CH2XO2 + I → IM1 (CH2XOOI) → P1 (CHXO + HIO). Owing to high energy barriers and unstable products, other products generation channels could be neglected. RRKM theory was used to calculate rate constants, and the rate constant at 298 K of the CH2IO2 + I reaction is consistent with the experimental data. Time-dependent density functional theory (TDDFT) calaulations revealed that the primary intermediates CH2XOOI could undergo photolysis under sunlight. CH2XOOI and primary products CHXO (X = F, Cl, Br and I) were regard as toxic substance with potential significant hazards to three aquatic organisms.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1281 - 1294"},"PeriodicalIF":2.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145167441","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

Theoretical studies on the effects of solvents on the mechanisms of configuration transformation of ε-CL-20 溶剂对ε-CL-20构型转变机理影响的理论研究

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-18 DOI: 10.1007/s11224-025-02452-3

Jincheng Ji, Hui Li, Weihua Zhu

{"title":"Theoretical studies on the effects of solvents on the mechanisms of configuration transformation of ε-CL-20","authors":"Jincheng Ji, Hui Li, Weihua Zhu","doi":"10.1007/s11224-025-02452-3","DOIUrl":"10.1007/s11224-025-02452-3","url":null,"abstract":"<div>Density functional theory tight binding molecular dynamics (DFTB-MD) and density functional theory (DFT) are used to study the mechanisms of configuration transformation of ε-2,4,6,8,10,12-hexanitro-2,4,6,6,8,10,12-hexaazaisowurtzitane (ε-CL-20) molecule under the effects of toluene and acetone. DFTB-MD results show that a series of configuration transformations occur to ε-CL-20 molecule in ε-CL-20/toluene solution, which is transformed to γ-CL-20 firstly, then to ζ-CL-20, and finally to ω-CL-20, while ε-CL-20 is transformed to α-CL-20, and finally to ω-CL-20 in ε-CL-20/acetone solution. The DFT calculation results indicate that the ε → γ(α) → ζ → ω transformation of ε-CL-20 molecule is thermodynamically feasible. Because γ(α)-CL-20 molecule is thermodynamically the most stable during γ(α)-, ζ-, and ω-CL-20 molecules, only transformation of ε-CL-20 molecule from configuration ε- to γ(α)- has occurred in experiments. Both Bader’s atoms in molecules (AIM) and independent gradient model (IGM) analyses indicate that the C-H···O type hydrogen bond is the main intermolecular interaction in the CL-20/solvent dimer and plays a major role in the formation of the dimer. This work reveals the configuration transformation mechanism of energetic molecules affected by solvent at the micro level, providing theoretical guidance for the preparation of pure form energetic crystals.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1269 - 1279"},"PeriodicalIF":2.2,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145166791","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

Density functional theory calculations on the electronic and optical properties of 2,7,12,17-tetrakis(pinacolatoboryl) porphyrin and its derivatives 2,7,12,17-四酰基卟啉及其衍生物的电子和光学性质的密度泛函理论计算

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-18 DOI: 10.1007/s11224-025-02458-x

Shu-qi Yang, Zhi Li

{"title":"Density functional theory calculations on the electronic and optical properties of 2,7,12,17-tetrakis(pinacolatoboryl) porphyrin and its derivatives","authors":"Shu-qi Yang, Zhi Li","doi":"10.1007/s11224-025-02458-x","DOIUrl":"10.1007/s11224-025-02458-x","url":null,"abstract":"<div>In order to explore novel porphyrins with excellent conductivity and selective light absorption, the influence of metal atom embedding and functional group attachment on the electronic and optical characteristics of porphyrins has been concerned. In this study, the structures, electronic, and optical properties of the 2,7,12,17-tetrakis(pinacolatoboryl) porphyrin and its derivatives have been investigated using density functional theory (DFT). The N–Ni–N bond angles of the derivatives are mostly close to 90.00°, with the exception of the N6-Ni5-N9 bond angle (45.09°) for the Ar and Br co-attached porphyrins (5 porphyrins). Additionally, the calculated ruffling displacements (druf) for the 2, 3, 5, and 6 porphyrins are 1.2691 Å, 1.1427 Å, − 1.2561 Å, and 0.5139 Å, respectively. The lowest frequency out-of-plane (oop) normal deformation of the 4 porphyrins is a waving motion with a displacement of 0.0532 Å. The energy gaps for the 1–6 porphyrins are similar, ranging from 4.44 to 4.80 eV. The presence of Br atoms promotes the Hirshfeld charge transfer between the C atoms within the macro-cycle of the Ar and Br co-attached porphyrins and the Ar functional groups. Furthermore, the Ar attached porphyrins exhibit a 20-nm red-shift compared to the Bpin-attached porphyrins. The addition of Br leads to an additional about 6-nm red-shift compared to the Ar-attached porphyrins. This is advantageous for expanding the application of porphyrins in industrial fields such as sensors and photocatalysts.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1257 - 1268"},"PeriodicalIF":2.2,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145166784","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

Correction to: Determination of dissociation constants of cephalosporin antibiotics by cellmetry method 修正：用细胞法测定头孢菌素类抗生素解离常数

IF 2.1 4区化学

Structural Chemistry Pub Date : 2025-01-17 DOI: 10.1007/s11224-025-02451-4

Malek Sadatsharifi, Mihály Purgel

引用次数: 0

The structure-photovoltaic property relationship of arylamine-modified ruthenium polypyridyl sensitizers in dye-sensitized solar cell: probed by DFT and TD-DFT 用DFT和TD-DFT研究了芳胺改性钌多吡啶敏化剂在染料敏化太阳能电池中的结构-光电性能关系

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-16 DOI: 10.1007/s11224-024-02447-6

Teng-Fei Lu, Kun Wang, Xiaoming Han, Yan Cui, Hualong Tao, Ming He, Zhihua Zhang, Bin He

{"title":"The structure-photovoltaic property relationship of arylamine-modified ruthenium polypyridyl sensitizers in dye-sensitized solar cell: probed by DFT and TD-DFT","authors":"Teng-Fei Lu, Kun Wang, Xiaoming Han, Yan Cui, Hualong Tao, Ming He, Zhihua Zhang, Bin He","doi":"10.1007/s11224-024-02447-6","DOIUrl":"10.1007/s11224-024-02447-6","url":null,"abstract":"<div>Dyes play multiple roles in dye-sensitized solar cells (DSSCs); however, the rational design of efficient dyes is highly challenging due to the sophisticated optoelectronics physics and electrochemistry phenomena. In this work, Ru (II) complexes modified by arylamine groups were used to study the structure-performance relationship. Density functional theory (DFT) and time-dependent DFT methods were employed to calculate the geometries, electronic structures, and optical properties of dyes, while quantum dynamic simulation was conducted to study the interfacial electron transfer (IET) in dye/TiO2 combined systems. The calculated results suggest that dyes with electron-donating N,N-dibenzyl-aniline and piperidine-modified arylamine groups induce effective intermolecular charge transfer, quickening the IET rate and elevating the TiO2 conduction band (CB) edge, thus augmenting short-circuit current (Jsc) and open-circuit voltage (Voc). The N-phenylcarbazol ligand is not suitable for modifying dyes due to weak interfacial electron coupling and invalid IET rate. The simulation highlights the potential of structurally modified Ru-dyes with N,N-dibenzyl-aniline and piperidine ligands, and provides a method for designing and screening high-performance DSSC dyes.</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1241 - 1255"},"PeriodicalIF":2.2,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145166052","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

Computational analysis of chalcogen-enhanced triphenylamine–based D-π-A sensitizers for DSSCs: a DFT study 硫增强三苯胺基D-π-A致敏剂对DSSCs的计算分析：DFT研究

IF 2.2 4区化学

Structural Chemistry Pub Date : 2025-01-14 DOI: 10.1007/s11224-024-02446-7

Alberto Baez-Castro, Carlos A. Peñuelas, Rody Soto-Rojo, Samuel Soto-Acosta, Tomas Delgado-Montiel, Manuel Luque-Román, María Edith Ruelas-Ávila, Daniel Glossman-Mitnik, Jesús Baldenebro-López

{"title":"Computational analysis of chalcogen-enhanced triphenylamine–based D-π-A sensitizers for DSSCs: a DFT study","authors":"Alberto Baez-Castro, Carlos A. Peñuelas, Rody Soto-Rojo, Samuel Soto-Acosta, Tomas Delgado-Montiel, Manuel Luque-Román, María Edith Ruelas-Ávila, Daniel Glossman-Mitnik, Jesús Baldenebro-López","doi":"10.1007/s11224-024-02446-7","DOIUrl":"10.1007/s11224-024-02446-7","url":null,"abstract":"<div>Computational analysis of nine designs of triphenylamine-based sensitizers with donator-π-bridge-acceptor (D-π-A) structure for dye-sensitized solar cells (DSSC) was carried out via density functional theory (DFT). The purpose of this work was the modification of dye CP-II to improve the properties in DSSC with a series of changes using halogens like fluorine and chlorine in the donor group and chalcogens in the π-bridge. M06/6-31G(d) and M06/6-31G(d) + DZVP levels of calculation were utilized to determine ground state geometry optimization, frontier molecular orbitals, and their energy levels. The LUMO levels ranged from − 2.402 to − 2.568 eV, making them suitable for electron injection into the TiO₂ conduction band. Chemical reactivity parameters such as chemical hardness (η), electrophilicity index (ω), electroaccepting power (ω+), and electrodonating power (ω−) were studied. After their analysis, these values proved suitable for use as sensitizers. The free energy of electron injection (∆Ginject) was calculated with values between 1.203 and 1.683 eV, indicating a sufficient driving force for electron injection. Light-harvesting efficiency (LHE) and excited-state lifetime (τ) were estimated and analyzed. Time-dependent density functional theory (TD-DFT) with M06-2X/6-31G(d) and M06-2X/6-31G(d) + DZVP levels of calculation were used to determine the absorption wavelengths, oscillator strengths, and electron transitions. The incorporation of tellurium and selenium in the π-bridge reduced the HOMO–LUMO gap, enhanced charge transfer, and increased chemical stability. The best-performing sensitizer, MeTTe, exhibited a HOMO–LUMO gap of 2.715 eV, a high electrophilicity index (3.51 eV), and a long excited-state lifetime (9.73 ns).</div>","PeriodicalId":780,"journal":{"name":"Structural Chemistry","volume":"36 4","pages":"1229 - 1240"},"PeriodicalIF":2.2,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145165025","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