Chemphyschem最新文献_第10页

Cover Feature: Deciphering Mg-Surface Interactions with Unsaturated Hydrocarbons: An Integrated Experimental-Theoretical Study (ChemPhysChem 7/2025) 封面专题：破译mg -表面与不饱和烃的相互作用：一个综合的实验-理论研究（chemphysichem 7/2025）

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-04-02 DOI: 10.1002/cphc.202580702

Sourav Ghoshal, Nathaniel Carnegie, Chidozie Ezeakunne, Beni B. Dangi, Shyam Kattel

引用次数: 0

First-Principles Investigation of 2D o-Al2C2 Monolayer: A High-Performance Anode for Li/Na–Ion Batteries 二维o-Al2C2单层：高性能锂/钠离子电池负极的第一性原理研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-28 DOI: 10.1002/cphc.202500025

Mohamed Agouri, Ayoub Benaddi, Nabil Khossossi, Said El Filali, Abderrahman Abbassi, Abdellatif Hasnaoui, Souad Taj, Bouzid Manaut

{"title":"First-Principles Investigation of 2D o-Al2C2 Monolayer: A High-Performance Anode for Li/Na–Ion Batteries","authors":"Mohamed Agouri, Ayoub Benaddi, Nabil Khossossi, Said El Filali, Abderrahman Abbassi, Abdellatif Hasnaoui, Souad Taj, Bouzid Manaut","doi":"10.1002/cphc.202500025","DOIUrl":"10.1002/cphc.202500025","url":null,"abstract":"The development of novel anode materials with superior electrochemical performance is imperative for advancing next-generation high-performance rechargeable batteries beyond current limitations. In this study, it presents a 2D o-Al2C2 monolayer as a promising lightweight candidate for lithium and sodium–ion battery systems, based on the density functional theory investigations and ab initio molecular dynamics (AIMD) simulations. Our comprehensive investigation demonstrates that the o-Al2C2 monolayer exhibits remarkable stability with a cohesive energy of −5.30 eV atom−1 and maintains its structural integrity at room temperature during extended AIMD simulations. The o-Al2C2 monolayer demonstrates exceptional electrochemical characteristics for Li and Na storage: theoretical specific capacities of 3780.42 and 3436.75 mA h g−1, optimal average open circuit voltages of 0.81 and 0.67 V, and favorable diffusion barriers of 0.62 eV and 0.31 eV, respectively. These performance metrics significantly surpass those of conventional graphite (372 mA h g−1) and other recently reported 2D anode materials, establishing o-Al2C2 as an exceptionally promising candidate for next-generation energy storage applications. Hence, this current theoretical investigation suggests that the o-Al2C2 monolayer holds significant potential for future experimental studies in lithium and sodium storage applications for LIB and NIB systems.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143729067","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

Suppressing Halide Segregation in Wide-Bandgap Perovskite Absorbers by Transamination of Formamidinium. 甲酰胺转氨化抑制宽带隙钙钛矿吸收剂中的卤化物偏析。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-27 DOI: 10.1002/cphc.202500022

Georgios Loukeris, Clemens Baretzky, Dmitry Bogachuk, Audrey Elizabeth Gillen, Bowen Yang, Jiajia Suo, Waldemar Kaiser, Edoardo Mosconi, Filippo De Angelis, Gerrit Boschloo, Andreas Walter Bett, Uli Würfel, Markus Kohlstädt

{"title":"Suppressing Halide Segregation in Wide-Bandgap Perovskite Absorbers by Transamination of Formamidinium.","authors":"Georgios Loukeris, Clemens Baretzky, Dmitry Bogachuk, Audrey Elizabeth Gillen, Bowen Yang, Jiajia Suo, Waldemar Kaiser, Edoardo Mosconi, Filippo De Angelis, Gerrit Boschloo, Andreas Walter Bett, Uli Würfel, Markus Kohlstädt","doi":"10.1002/cphc.202500022","DOIUrl":"10.1002/cphc.202500022","url":null,"abstract":"All-perovskite tandem solar cells are emerging at a fast rate because of their potential to exceed efficiencies of Si-perovskite tandems, in combination with faster manufacturing, lower cost, and the ability to be processed on flexible substrates. Mixing halides is a key to achieve wide-bandgap absorbers, which however suffer from halide segregation under illumination, resulting in lowering of the bandgap. To tackle this problem, butylamine (BA) has been added to the perovskite precursor solution and is found to react with the formamidinium (FA) cation, producing N-butylformamidinium (BuFA+), which accumulates at the perovskite surface and grain boundaries. The creation of the BuFA cation results in suppressed halide segregation and improved crystallization. Density functional theory calculations propose the reduction of halide defect formation upon the addition of BA, being a key to stabilize mixed-halide perovskites. Lastly, we observe a more stable performance of single junction p-i-n perovskite solar cells with the addition of BA under constant illumination at 65 °C.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e2500022"},"PeriodicalIF":2.3,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143718111","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

N-Heterocyclic Carbenes: A Benchmark Study on their Singlet–Triplet Energy Gap as a Critical Molecular Descriptor n -杂环碳烯：Βenchmark单重态-三重态能隙作为关键分子描述符的研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-27 DOI: 10.1002/cphc.202500012

Konstantinos P. Zois, Andreas A. Danopoulos, Demeter Tzeli

{"title":"N-Heterocyclic Carbenes: A Benchmark Study on their Singlet–Triplet Energy Gap as a Critical Molecular Descriptor","authors":"Konstantinos P. Zois, Andreas A. Danopoulos, Demeter Tzeli","doi":"10.1002/cphc.202500012","DOIUrl":"10.1002/cphc.202500012","url":null,"abstract":"N-heterocyclic carbenes (NHCs) are used extensively in modern chemistry and materials science. The in-depth understanding of their electronic structure and their metal complexes remains an important topic of research and of experimental and theoretical interest. Herein, the adiabatic singlet–triplet gap as a superior, quantifiable critical descriptor, sensitive to the nature and the structural diversity of the NHCs, for a successful rationalization of experimental observations and computationally extracted trends is established. The choice is supported by a benchmark study on the electronic structures of NHCs, using high-level ab initio methods, that is, complete active space self-consistent field, n-electron valence second-order perturbation theory, multireference configuration interaction + singles + doubles, and domain-based local pair natural orbital-coupled cluster method with single-, double-, and perturbative triple excitations along with density functional theory methods such as BP86, M06, and M06-L, B3LYP, PBE0, TPSSh, CAM-B3LYP, and B2PLYP. In contrast to the adiabatic singlet–triplet (S–T) gap preferred as descriptor, the highest occupied molecular orbital-lowest unoccupied molecular orbital gap or the S–T vertical gap that has been used in the past occasionally leads to controversial results; some of these are critically discussed below. Extrapolation of these ideas to a group of copper–NHC complexes is also described.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cphc.202500012","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143718109","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

Exploring Quality Criteria for the Computational Modeling of Heterogeneous Catalysts 探索多相催化剂计算模型的质量标准。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-26 DOI: 10.1002/cphc.202401123

Florian Göltl

引用次数: 0

Computational Evaluation of Redox Potentials of Metal Complexes for Aqueous Flow Batteries 水液流电池金属配合物氧化还原电位的计算评价。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-26 DOI: 10.1002/cphc.202500046

Aliyeh Mehranfar, Jenna Hannonen, Ali Tuna, Maryam Jafarishiadeh, Anniina Kiesilä, Petri Pihko, Pekka Peljo, Kari Laasonen

{"title":"Computational Evaluation of Redox Potentials of Metal Complexes for Aqueous Flow Batteries","authors":"Aliyeh Mehranfar, Jenna Hannonen, Ali Tuna, Maryam Jafarishiadeh, Anniina Kiesilä, Petri Pihko, Pekka Peljo, Kari Laasonen","doi":"10.1002/cphc.202500046","DOIUrl":"10.1002/cphc.202500046","url":null,"abstract":"Flow batteries are a promising option for large-scale stationary energy storage, but better redox active materials are required. Computational density functional theory (DFT) approach to materials screening can identify the most promising avenues and accelerate the development of the technology. In this work, metal complexes with functionalized organic ligands are focused on. The right redox potential, good chemical stability, and high solubility are the main characters in designing a high-performance aqueous electrolyte. Here, Fe, Ti, Mn, and Ni are studied as central metals of the complexes with two ligand classes containing N- and O- groups. The accuracy of the DFT redox potentials is compared to experiments whenever available. In addition, some cyclic voltammetry measurements are performed for Fe-bipyridine, phenanthroline, and terpyridine complexes. The computational redox potentials for ≈180 different metal–ligand combinations are evaluated. Overall, this work presents a new insight into the design of new electrolytes for aqueous flow batteries.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cphc.202500046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143708867","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

A Direct Measurement of the Absolute Energies of Protonated Gly-Pro-Gly-Gly Conformations Using Ion Mobility Spectrometry and Guided Ion Beam Tandem Mass Spectrometry 离子迁移谱法和引导离子束串联质谱法直接测量质子化Gly-Pro-Gly-Gly构象的绝对能量。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-26 DOI: 10.1002/cphc.202500080

Brandon C. Stevenson, Shannon A. Raab, David E. Clemmer, Peter B. Armentrout

{"title":"A Direct Measurement of the Absolute Energies of Protonated Gly-Pro-Gly-Gly Conformations Using Ion Mobility Spectrometry and Guided Ion Beam Tandem Mass Spectrometry","authors":"Brandon C. Stevenson, Shannon A. Raab, David E. Clemmer, Peter B. Armentrout","doi":"10.1002/cphc.202500080","DOIUrl":"10.1002/cphc.202500080","url":null,"abstract":"Threshold collision-induced dissociation of conformations selected by ion mobility spectrometry is described as a method to determine their absolute relative energies. Here, the method is demonstrated with the cis and trans conformers of the protonated tetrapeptide, Gly-Pro-Gly-Gly, which differ in the orientation of the peptide bond at the proline residue. The trans conformation was found to be more stable than the cis conformation by 4.5 ± 2.5 kJ mol−1 at 0 K. Heating the molecule anneals it to the cis conformer, indicating it has a lower Gibbs energy at higher temperatures. These results are compared to theoretical values calculated here and from the literature. This experimental analysis is the first quantitative measurement of the relative stability of the conformers of a protonated peptide in the gas phase, which has far-reaching impacts on the selection of theoretical methods to describe the energetics of these systems.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cphc.202500080","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143729061","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

The Interaction of Ether-Based Functionalized Ionic Liquids in Lithium–Sulfur Batteries: A First-Principles Study 醚基功能化离子液体在锂硫电池中的相互作用：第一性原理研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-25 DOI: 10.1002/cphc.202400848

Chengren Li, Nan Zhou, Jiaxin Tang, Chen Wang, Rongde Sun, Baifeng Yang, Zhigao Chen, Xiaohan Lu, Zhen Chang, Shaoze Zhang, Changjun Peng, Honglai Liu

{"title":"The Interaction of Ether-Based Functionalized Ionic Liquids in Lithium–Sulfur Batteries: A First-Principles Study","authors":"Chengren Li, Nan Zhou, Jiaxin Tang, Chen Wang, Rongde Sun, Baifeng Yang, Zhigao Chen, Xiaohan Lu, Zhen Chang, Shaoze Zhang, Changjun Peng, Honglai Liu","doi":"10.1002/cphc.202400848","DOIUrl":"10.1002/cphc.202400848","url":null,"abstract":"Ionic liquids (ILs) as electrolytes in lithium-sulfur (Li-S) batteries effectively mitigate the shuttle effect. Solvated cationic ether-based ILs, comprising [Li(G1)2]+, [Li(G2)2]+, [LiG3]+, [LiG4]+, or [LiG6]+ paired with bis(trifluoromethyllsulfonyl)imide ([TFSA]–) anions, are evaluated for their ability to suppress short-chain lithium polysulfide (LiPS: Li2S1, Li2S2, Li2S4) adsorption on lithium metal. The chelating capacity of solvated cations governs interactions with LiPSs and anions. Solvation via Li+ chelation prevents free Li+ fusion with LiPSs, reducing shuttle effects. Remarkably, the cyclic [LiG6]+ cation exhibits superior Li+ chelation, stability, and minimized LiPS adsorption compared to linear cations. Ab initio molecular dynamics simulations confirm ether-based ILs stabilize anions and lower LiPS-lithium surface reactivity. These findings highlight solvated cation ILs as tailored electrolytes to control interfacial LiPS behavior, advancing high-performance LiS battery design.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143708871","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

High-Performance Mo-CoS2 Nanoplates Derived from Metal-Organic Frameworks for Asymmetric Supercapacitor Applications 非对称超级电容器用金属有机框架制备的高性能Mo-CoS2纳米板。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-25 DOI: 10.1002/cphc.202400910

Yu-Xuan Lai, Ri-Yu Li, Christine Young

{"title":"High-Performance Mo-CoS2 Nanoplates Derived from Metal-Organic Frameworks for Asymmetric Supercapacitor Applications","authors":"Yu-Xuan Lai, Ri-Yu Li, Christine Young","doi":"10.1002/cphc.202400910","DOIUrl":"10.1002/cphc.202400910","url":null,"abstract":"As global energy and environmental challenges intensify, advancing renewable energy storage technologies is critical. Supercapacitors, known for their rapid charge-discharge rates and exceptional cycling stability, are a promising solution; however, they are constrained by their comparatively low energy density. This study addresses this limitation by developing high-performance Mo-CoS2 nanoplates derived from metal-organic frameworks for asymmetric supercapacitor applications. Using ZIF-67 nanoplates as precursors, Mo-CoS2 hybrids were synthesized through a two-step process that included carbonization followed by sulfurization. The Mo-CoS2 hybrids maintained its plate-like morphology with plentiful active sites, which are crucial for superior electrochemical performance. The Mo-CoS2 electrode delivers a specific capacitance of 1382.6 F g−1 at 0.5 A g−1, significantly surpassing that of CoS2 and MoS2 alone. An asymmetric supercapacitor incorporating Mo-CoS2 and ZIF-67-derived carbon electrodes demonstrate a remarkable energy density of 49.4 Wh kg−1 at a power density of 703 W kg−1, while retaining 72.09% of their initial performance after 10 000 cycles. The findings underscore the potential of materials derived from metal-organic frameworks (MOFs) in enhancing supercapacitor technology, as they offer a combination of high capacitance and long-term stability.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143708869","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

Synthesis, Characterization, and Cytotoxicity of Photochromic Molybdenum Oxide-Doped Tungsten Oxide Polymeric Nanohybrid Films for Biomedical Applications 生物医学用光致变色氧化钼掺杂氧化钨聚合物纳米杂化膜的合成、表征及细胞毒性研究。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-03-24 DOI: 10.1002/cphc.202400987

Shephrah Olubusola Ogungbesan, Chao Zhou, Mulenga Kalulu, Oluwaseun Hannah Anselm, Adeyemi Lawrence Ogunneye, Rosemary Anwuli Adedokun, David Díaz Díaz, Guodong Fu

{"title":"Synthesis, Characterization, and Cytotoxicity of Photochromic Molybdenum Oxide-Doped Tungsten Oxide Polymeric Nanohybrid Films for Biomedical Applications","authors":"Shephrah Olubusola Ogungbesan, Chao Zhou, Mulenga Kalulu, Oluwaseun Hannah Anselm, Adeyemi Lawrence Ogunneye, Rosemary Anwuli Adedokun, David Díaz Díaz, Guodong Fu","doi":"10.1002/cphc.202400987","DOIUrl":"10.1002/cphc.202400987","url":null,"abstract":"Despite the known nontoxicity, stability, and efficiency of WO3 and MoO3 against microbes as a result of their catalytic activities, these oxides are not effective photocatalysts because the O2 absorbed cannot be reduced by the photogenerated electrons in their conduction band, which leads to the rebinding of electrons and holes on the surface. The doping of these two n-type semiconductor metal oxides and incorporation of a biocompatible, biodegradable, and bioavailable polymer (such as chitosan) to form a film, to a large extent, affects the surface area interaction and multipurpose applicability of the film as a therapeutic, controlled delivery, and dual sensitive material. The WO3-NP and WO3MoO3 nanocomposites are synthesized via a deep eutectic solvent-assisted hydrothermal-based method, which afford fine-sized nanoparticles and nanocomposites, which are further incorporated into a chitosan matrix to form nanohybrid films via the solvent casting method. The structural, optical, and morphological characterization of the materials is carried out via X-ray diffraction (XRD), Fourier transform infrared (FT-IR), UV, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, and dynamic light scattering. XRD and FT-IR analyses reveal that WO3MoO3 nanocomposites are successfully formed and incorporated into the chitosan matrix. The nanohybrid film shows antimicrobial activity with a minimum inhibitory concentration of 100 μg mL−1. Furthermore, the nanohybrid film shows no significant toxicity.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 12","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cphc.202400987","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143691008","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