Chemphyschem最新文献_第10页

Formation of Paraldehyde (C₆H₁₂O₃) in Interstellar Analog Ices of Acetaldehyde Exposed to Ionizing Radiation. 暴露于电离辐射的乙醛星际模拟冰中副醛 (C6H12O3) 的形成。

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-04 DOI: 10.1002/cphc.202400837

Jia Wang, Andrew M Turner, Joshua H Marks, Ryan C Fortenberry, Ralf I Kaiser

{"title":"Formation of Paraldehyde (C6H12O3) in Interstellar Analog Ices of Acetaldehyde Exposed to Ionizing Radiation.","authors":"Jia Wang, Andrew M Turner, Joshua H Marks, Ryan C Fortenberry, Ralf I Kaiser","doi":"10.1002/cphc.202400837","DOIUrl":"10.1002/cphc.202400837","url":null,"abstract":"Acetaldehyde (CH3CHO) plays a crucial role in the synthesis of prebiotic molecules such as amino acids, sugars, and sugar-related compounds, and in the progress of chain reaction polymerization in deep space. Here, we report the first formation of the cyclic acetaldehyde trimer - paraldehyde (C6H12O3) - in low-temperature interstellar analog ices exposed to energetic irradiation as proxies of galactic cosmic rays (GCRs). Utilizing vacuum ultraviolet photoionization reflectron time-of-flight mass spectrometry and isotopic substitution experiments, paraldehyde was identified in the gas phase during the temperature-programmed desorption of the irradiated acetaldehyde ices based on the calculated adiabatic ionization energies and isomer-specific dissociative fragmentation patterns upon photoionization. As acetaldehyde is ubiquitous throughout the interstellar medium and has been tentatively identified in interstellar ices, paraldehyde could have formed in acetaldehyde-containing ices in a cold molecular cloud and is an excellent candidate for gas-phase observation in star-forming regions via radio telescopes. The identification of paraldehyde in the gas phase from the processed acetaldehyde ices advances our understanding of how complex organic molecules can be synthesized through polymerization reactions in extraterrestrial ices exposed to GCRs.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142371103","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

Front Cover: Spectral Hole-Burning Studies of a Mononuclear Eu(III) Complex Reveal Narrow Optical Linewidths of the 5D0→7F0 Transition and Seconds Long Nuclear Spin Lifetimes (ChemPhysChem 19/2024) 封面：单核 Eu(III)配合物的空穴燃烧光谱研究揭示 5D0→7F0 转变的窄光学线宽和长达数秒的核自旋寿命（ChemPhysChem 19/2024）

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-02 DOI: 10.1002/cphc.202481901

Sören Schlittenhardt, Evgenij Vasilenko, Vishnu Unni C., Nicholas Jobbitt, Olaf Fuhr, David Hunger, Mario Ruben, Senthil Kumar Kuppusamy

{"title":"Front Cover: Spectral Hole-Burning Studies of a Mononuclear Eu(III) Complex Reveal Narrow Optical Linewidths of the 5D0→7F0 Transition and Seconds Long Nuclear Spin Lifetimes (ChemPhysChem 19/2024)","authors":"Sören Schlittenhardt, Evgenij Vasilenko, Vishnu Unni C., Nicholas Jobbitt, Olaf Fuhr, David Hunger, Mario Ruben, Senthil Kumar Kuppusamy","doi":"10.1002/cphc.202481901","DOIUrl":"https://doi.org/10.1002/cphc.202481901","url":null,"abstract":"The Front Cover shows how spectral-hole burning (SHB) studies reveal a 0.205 μs-long optical coherence lifetime (T2opt) and seconds-long nuclear spin lifetime (T1spin) associated with a charge-neutral EuIII complex, featuring a 5D0-to-7F0 transition. The results indicate the utility of molecular rare-earth ion (MREI) complexes as tuneable and scalable platforms for creating coherent light–matter interfaces for quantum information processing (QIP) applications. More information can be found in the Research Article by D. Hunger, M. Ruben, S. K. Kuppusamy and co-workers (DOI: 10.1002/cphc.202400280).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cphc.202481901","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142428963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cover Feature: Sensitivity Enhancement of Ultra-Wideline NMR by Progressive Saturation of the Proton Reservoir Under Magic-Angle Spinning (ChemPhysChem 19/2024) 封面专题：魔角旋转下质子储库的逐渐饱和提高了超边线 NMR 的灵敏度（ChemPhysChem 19/2024）

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-02 DOI: 10.1002/cphc.202481902

Tamar Wolf, Yuval Goobes, Lucio Frydman

引用次数: 0

Cover Feature: Deciphering Stereoselectivity in Hurd-Claisen Rearrangements: A Comprehensive Study of Electrostatic Interactions from Shubin's Energy Decomposition Analysis (ChemPhysChem 19/2024) 封面专题：解密赫德-克莱森重排中的立体选择性：从舒宾能量分解分析看静电相互作用的综合研究（ChemPhysChem 19/2024）

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-02 DOI: 10.1002/cphc.202481903

Ana Gabriela Coelho Oliveira, Mateus Rodrigues Barbosa, Pedro Henrique Ferreira Matias, Charlley Anchieta Lourenço Silva, Dr. Daniel Francisco Scalabrini Machado, Dr. Ângelo Henrique de Lira Machado, Dr. Heibbe Cristhian Benedito de Oliveira

{"title":"Cover Feature: Deciphering Stereoselectivity in Hurd-Claisen Rearrangements: A Comprehensive Study of Electrostatic Interactions from Shubin's Energy Decomposition Analysis (ChemPhysChem 19/2024)","authors":"Ana Gabriela Coelho Oliveira, Mateus Rodrigues Barbosa, Pedro Henrique Ferreira Matias, Charlley Anchieta Lourenço Silva, Dr. Daniel Francisco Scalabrini Machado, Dr. Ângelo Henrique de Lira Machado, Dr. Heibbe Cristhian Benedito de Oliveira","doi":"10.1002/cphc.202481903","DOIUrl":"https://doi.org/10.1002/cphc.202481903","url":null,"abstract":"The Cover Feature illustrates the Hurd–Claisen rearrangement involving nitrile-containing compounds, highlighting the high stereoselectivity favoring the Z isomer (>99:1). Using Shubin Liu′s method, we revealed the significant role of electrostatic contributions in determining stereoselectivity, contrasting with Basavaiah's model. The cover depicts this process, showing reagents following an industrial path with electrostatic forces guiding the transition states, while steric and quantum forces compete. More information can be found in the Research Article by Â. H. de Lira Machado, H. C. Benedito de Oliveira and co-workers (DOI: 10.1002/cphc.202400565).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cphc.202481903","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142428965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Impact of Fe³⁺/Polyphenol Ratio in Iron-gall Ink on Superoxide Formation: Rationalizing Historic Recipes from a Kinetic Study. 从古代到 19 世纪的铁球墨配方的合理化。动力学研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-02 DOI: 10.1002/cphc.202400859

Natércia Teixeira, João Avó, Hugo Cruz, Tânia Moniz, Maria Rangel, Victor de Freitas, João C Lima, Maria J Melo, Fernando Pina

引用次数: 0

Se-Doping on Co₄S₃ Cathode Based on Soft Anion Chemistry to Enhance Magnesium Storage Performance. 基于软阴离子化学的 Co4S3 阴极掺杂硒以提高镁的储存性能

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-01 DOI: 10.1002/cphc.202400821

Chenkai Hu, Haifeng Ying, Wenwei Zhang, Feiyang Chao, Dongyao Zhu, Shaohua Zhu, Qinyou An

引用次数: 0

Theoretical study on intramolecular hydrogen bonds of flavonoid cocrystals. 黄酮类化合物分子内氢键的理论研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-01 DOI: 10.1002/cphc.202400591

Lisha Zhang, Wei Gao, Li Su, Wenying He, Yize Wang, Minghui Hu, Zixi Liu, Yanling Liu, Huajie Feng

{"title":"Theoretical study on intramolecular hydrogen bonds of flavonoid cocrystals.","authors":"Lisha Zhang, Wei Gao, Li Su, Wenying He, Yize Wang, Minghui Hu, Zixi Liu, Yanling Liu, Huajie Feng","doi":"10.1002/cphc.202400591","DOIUrl":"https://doi.org/10.1002/cphc.202400591","url":null,"abstract":"This study investigates the role of intramolecular hydrogen bonds in the formation of cocrystals involving flavonoid molecules, focusing on three active pharmaceutical ingredients (APIs): chrysin (CHR), isoliquiritigenin (ISO), and kaempferol (KAE). These APIs form cocrystals with different cocrystal formers (CCFs) through intramolecular hydrogen bonding. We found that disruption of these intramolecular hydrogen bonds leads to decreased stability compared to molecules with intact bonds. The extrema of molecular electrostatic potential surfaces (MEPS) show that flavonoid molecules with disrupted intramolecular hydrogen bonds have stronger hydrogen bond donors and acceptors than those with intact bonds. Using the artificial bee colony algorithm, dimeric structures of these flavonoid molecules were explored, representing early-stage structures in cocrystal formation, including API-API, API-CCF, and CCF-CCF dimers. It was observed that the number and strength of dimeric interactions significantly increased, and the types of interactions changed when intramolecular hydrogen bonds were disrupted. These findings suggest that disrupting intramolecular hydrogen bonds generally hinders the formation of cocrystals. This theoretical study provides deeper insight into the role of intramolecular hydrogen bonds in the cocrystal formation of flavonoids.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142342514","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

Attraction versus Repulsion between Methyl and Related Groups: (CH₃NHCH₃)₂ and (CH₃SeBr₂CH₃)₂. 甲基和相关基团之间的吸引力与排斥力：(CH3NHCH3)2 和 (CH3SeBr2CH3)2。

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-01 DOI: 10.1002/cphc.202400495

Mariusz Michalczyk, Steve Scheiner, Wiktor Zierkiewicz

{"title":"Attraction versus Repulsion between Methyl and Related Groups: (CH3NHCH3)2 and (CH3SeBr2CH3)2.","authors":"Mariusz Michalczyk, Steve Scheiner, Wiktor Zierkiewicz","doi":"10.1002/cphc.202400495","DOIUrl":"10.1002/cphc.202400495","url":null,"abstract":"The starting point for this work was a set of crystal structures containing the motif of interaction between methyl groups in homodimers. Two structures were selected for which QTAIM, NCI and NBO analyses suggested an attractive interaction. However, the calculated interaction energy was negative for only one of these systems. The ability of methyl groups to interact with one another is then examined by DFT calculations. A series of (CH3PnHCH3)2 homodimers were allowed to interact with each other for a range of Pn atoms N, P, As, and Sb. Interaction energies of these C⋅⋅⋅C tetrel-bonded species were below 1 kcal/mol, but could be raised to nearly 3 kcal/mol if the C atom was changed to a heavier tetrel. A strengthening of the C⋅⋅⋅C intermethyl bonds can also be achieved by introducing an asymmetry via an electron-withdrawing substituent on one unit and a donor on the other. The attractions between the methyl and related groups occur in spite of a coulombic repulsion between σ-holes on the two groups. NBO, AIM, and NCI tools must be interpreted with caution as they can falsely suggest bonding when the potentials are repulsive.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142342507","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 density functional benchmark for dehydrogenation and dehalogenation reactions on coinage metal surfaces. 硬币金属表面脱氢和脱卤反应的密度泛函基准。

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-10-01 DOI: 10.1002/cphc.202400865

Lin Chen, Johanna Rosen, Jonas Björk

{"title":"A density functional benchmark for dehydrogenation and dehalogenation reactions on coinage metal surfaces.","authors":"Lin Chen, Johanna Rosen, Jonas Björk","doi":"10.1002/cphc.202400865","DOIUrl":"https://doi.org/10.1002/cphc.202400865","url":null,"abstract":"The on-surface synthesis of low-dimensional organic nanostructures has been extensively investigated through both experimental and theoretical methods, particularly by density functional theory (DFT). However, the complex mixture of interactions often poses challenges within the DFT framework, and there is a knowledge-gap regarding how the choice of DFT approach affects the computed results. Here, five different approaches including vdW interactions, i.e., PBE+D3, PBE+vdWsurf, rev-vdW-DF2, r2SCAN+rVV10 and BEEF-vdW, are employed to describe three prototypical on-surface reactions; dehydrogenation of benzene, debromination of bromobenzene, and deiodination of iodobenzene on the (111) facets of the coinage metals. Overall, rev-vdW-DF2 outperforms the other methods in describing benzene adsorption, whereas BEEF-vdW falls short. For dehydrogenation and debromination on Cu(111), all functionals except BEEF-vdW give reasonable activation energies compared to experiments. A similar trend is observed for Ag(111) and Au(111), with BEEF-vdW yielding significantly higher activation and reaction energies. For dehalogenation, all the five vdW approaches correctly capture the reactivity trend - Cu(111) > Ag(111) > Au(111) - and the expected hierarchy between bromobenzene desorption and carbon- bromine activation. Only BEEF-vdW fails to predict the faster kinetics of deiodination than the iodobenzene desorption. Our work forms a basis for evaluating density functionals in describing chemical reactions on surfaces.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142364576","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

An operando spectroscopic investigation of the Re2O7.2H2O adduct obtained by controlled hydration of Re2O7. 对 Re2O7 受控水合得到的 Re2O7.2H2O 加合物进行操作性光谱研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2024-09-30 DOI: 10.1002/cphc.202400432

Xavier Sécordel, Shreya Nandi, Asma Tougerti, Sylvain Cristol, Jean-François Paul, Valérie Briois, Camille La Fontaine, Elise Berrier

引用次数: 0