Chemphyschem最新文献_第2页

Difluorinated Cyclohexanes: Energetics and Intra- and Intermolecular Interactions. 二氟化环己烷：能量学和分子内与分子间相互作用。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-10 DOI: 10.1002/cphc.202500648

Matheus P Freitas

引用次数: 0

High-Throughput Photocatalysis for Generating Reliable Datasets Analyzed by Machine Learning. 高通量光催化用于生成可靠的机器学习分析数据集。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-10 DOI: 10.1002/cphc.202500039

Mark Croxall, Reece Lawrence, Jiaqi Gong, M Cynthia Goh

{"title":"High-Throughput Photocatalysis for Generating Reliable Datasets Analyzed by Machine Learning.","authors":"Mark Croxall, Reece Lawrence, Jiaqi Gong, M Cynthia Goh","doi":"10.1002/cphc.202500039","DOIUrl":"https://doi.org/10.1002/cphc.202500039","url":null,"abstract":"Photocatalysis is an environmentally conscious tool for removing contaminants from water. Novel photocatalytic materials are often measured on ability to degrade a small number of analytes, which may not be indicative of broader applicability. In this work, an experimental method dubbed high-throughput photocatalysis (HTP) is introduced to assay photocatalytic materials against a range of analytes in a time effective manner. HTP is modular; experimental parameters, including matrix, can be changed to fit a proposed application. The photodegradation of each analyte is attained in a consistent manner such that machine learning (ML) models can be applied to the obtained datasets. Three out of the box ML models-linear regression, random forest (RF), and neural network (NN)-are tasked with estimating the percentage removal as a function of irradiation time and molecular structure, as represented by Morgan fingerprints. Leave-out sets demonstrated that RF and NN models did not overfit the training data and reasonably estimated the degradation of unknown molecules. SHapley additive exPlanations values are utilized to correlate molecular substructures to the parent molecule's susceptibility to photocatalytic degradation. These correlations are used to generate heatmaps of estimated reactivity within molecules that corroborate reports in which dye degradation pathways were studied in detail.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500039"},"PeriodicalIF":2.2,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145257599","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 Automatic Pathway Searching Strategy in Enzyme Catalysis: A Case Study of LmCpfC. 酶催化中的自动路径搜索策略：以LmCpfC为例。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-07 DOI: 10.1002/cphc.202500515

Yuhong Lin, Yong Shen

{"title":"An Automatic Pathway Searching Strategy in Enzyme Catalysis: A Case Study of LmCpfC.","authors":"Yuhong Lin, Yong Shen","doi":"10.1002/cphc.202500515","DOIUrl":"https://doi.org/10.1002/cphc.202500515","url":null,"abstract":"To mitigate the artificial intervention on the exploration of the enzyme reaction mechanisms, an automatic pathway searching strategy based on discrete path sampling(DPS) is firstly employed to explore the reaction pathway of enzyme catalysis. For instance, in the case of Listeria monocytogenes coproporphyrin ferrochelatase (LmCpfC) catalyzing the insertion of Fe(II) into the substrate coproporphyrin III (cpIII), which is the first computational research about detailed mechanism of the CpfC. By searching the reaction pathways for Fe(II) insertion from both sides of cpIII, it is found that Fe(II) inserting from the Tyr12 side exhibited advantages in both thermodynamics and kinetics, which is consistent with experimental observations. The enthalpy change is determined to be -42.24 kcal mol-1 and the barrier energy is 7.28 kcal mol-1. In contrast, the insertion from the Glu263, His182 side has an enthalpy change of +21.88 kcal mol-1 and a barrier energy of 34.64 kcal mol-1. Compared with potential energy surface scanning and nudged elastic band methods, where the barrier energies are 9.78, 17.50 kcal mol-1 from Tyr12 side and 85.09, 58.26 kcal mol-1 from Glu263, His182 side, respectively, the DPS strategy yields obviously lower barriers reaction pathways with less intervention.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500515"},"PeriodicalIF":2.2,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145243873","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: Accelerating the Structure Exploration of Diverse Bi–Pt Nanoclusters via Physics-Informed Machine Learning Potential and Particle Swarm Optimization (ChemPhysChem 19/2025) 封面：通过物理信息机器学习潜力和粒子群优化加速不同Bi-Pt纳米团簇的结构探索（chemphyscheme 19/2025）

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-07 DOI: 10.1002/cphc.70107

Raphaël Vangheluwe, Carine Clavaguéra, Minh-Tue Truong, Dominik Domin, Huy Cong Pham, Mihai-Cosmin Marinica, Nguyen-Thi Van-Oanh

引用次数: 0

Cover Feature: Evidence for Anion-Anion Interaction in Amino Acid Ionic Liquids Probed by Far-Infrared Spectroscopy (ChemPhysChem 19/2025) 封面专题：用远红外光谱探测氨基酸离子液体中阴离子-阴离子相互作用的证据（chemphychem 19/2025）

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-07 DOI: 10.1002/cphc.70108

David Kotwica, Ralf Ludwig

引用次数: 0

Exploring the Potential of Self-Supported Laser-Induced Graphene-Cobalt Oxide Electrodes for Alkaline Electrolysis. 探索自支撑激光诱导石墨烯-氧化钴电极用于碱性电解的潜力。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-07 DOI: 10.1002/cphc.202500469

Otávio A L Alves, Thiago A S Soares, Lara F Loguercio, Felipe L N Sousa, Anderson Thesing, Marcelo Navarro, Giovanna Machado

{"title":"Exploring the Potential of Self-Supported Laser-Induced Graphene-Cobalt Oxide Electrodes for Alkaline Electrolysis.","authors":"Otávio A L Alves, Thiago A S Soares, Lara F Loguercio, Felipe L N Sousa, Anderson Thesing, Marcelo Navarro, Giovanna Machado","doi":"10.1002/cphc.202500469","DOIUrl":"https://doi.org/10.1002/cphc.202500469","url":null,"abstract":"A simple, fast, and cost-effective strategy to fabricate self-supported electrodes based on laser-induced graphene (LIG) decorated with cobalt oxide (LIG-CoO) for oxygen evolution reaction (OER) in alkaline media is reported. The method involves a dual-ablation process directly on commercial Kapton tape, eliminating the need for binders, metal current collectors, or post-synthesis thermal/chemical treatments. Raman, scanning electron microscopy, X-ray photoelectron spectroscopy (XPS), and X-ray diffraction analyses confirm the formation of a graphitic and porous LIG network decorated with CoO nanostructures. At the optimal cobalt precursor concentration, the electrochemical evaluation reveals superior OER achieved with an overpotential of 388.0 mV at a current density of 10.0 mA cm-2 and a Tafel slope of 65.8 mV dec- 1. Electrochemical impedance spectroscopy reveals enhanced charge transfer and increased electrochemical surface area with CoO loading. Notably, synchrotron XPS analysis shows compositional gradients and oxidation states across the electrode depth, confirming Co2+ stabilization and surface oxygenation. The proposed fabrication route demonstrates significant potential for scalable production of integrated electrocatalytic materials, addressing the increasing demands for green energy solutions.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500469"},"PeriodicalIF":2.2,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145243853","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

Entanglement of CH₄ and CO₂ Chemistries in Plasma-Assisted Dry Reforming of Methane. 等离子体辅助甲烷干重整过程中CH4和CO2的化学纠缠。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-06 DOI: 10.1002/cphc.202500318

Nils Hansen, Emma C Litzer, Leonid Sheps, Oisin J Shiels, Haodong Chen, Bin Yang

{"title":"Entanglement of CH4 and CO2 Chemistries in Plasma-Assisted Dry Reforming of Methane.","authors":"Nils Hansen, Emma C Litzer, Leonid Sheps, Oisin J Shiels, Haodong Chen, Bin Yang","doi":"10.1002/cphc.202500318","DOIUrl":"https://doi.org/10.1002/cphc.202500318","url":null,"abstract":"Plasma-assisted dry reforming of methane converts methane (CH4) and carbon dioxide (CO2) into valuable chemicals. To gain further chemical kinetic insights into this process, laboratory-scale experiments is combined using isotopically labeled 13CO2 with detailed chemical modeling. In the experiments, an atmospheric-pressure coaxial dielectric barrier discharge plasma reactor attached to a molecular-beam mass spectrometer is used to detect reaction products from a feed mixture containing equal amounts of CH4 and CO2. The experiments confirm that the formation of the observed hydrocarbons is clearly related to the CH4 chemistry and that the detected double-oxygenated C2H4O2, C3H6O2, and C4H8O2 species can partially be traced back to the CO2 chemistry. To provide further insights, the chemistry mechanism from the earlier work (Proc. Combust. Inst., 2024, 40, 105404) is expanded to include the formation chemistry of these double-oxygenated products. The updated mechanism predicts the formation of both acids and esters, for example, acetic acid (CH3COOH) and methyl formate [HC(=O)OCH3] for the C2H4O2 species. According to the reaction path analysis, the products are formed through the COOH radical that itself stems from the CO+OH reaction, with the CO being partially formed from plasma-initiated CO2 dissociation.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500318"},"PeriodicalIF":2.2,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145238222","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

Probing the Hybrid σ/π-Holes in sp²-Hybridized Chalcogen Bond Donors and their Complexes with Ammonia. sp2杂化硫键给体及其与氨配合物中杂化σ/π空穴的探测。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-05 DOI: 10.1002/cphc.202500381

Kirk A French, Daniel P Devore, Thomas L Ellington, Kevin L Shuford

{"title":"Probing the Hybrid σ/π-Holes in sp2-Hybridized Chalcogen Bond Donors and their Complexes with Ammonia.","authors":"Kirk A French, Daniel P Devore, Thomas L Ellington, Kevin L Shuford","doi":"10.1002/cphc.202500381","DOIUrl":"https://doi.org/10.1002/cphc.202500381","url":null,"abstract":"sp- and <math> <semantics><mrow><mi>s</mi> <msup><mi>p</mi> <mn>2</mn></msup> </mrow> <annotation>$s p^{2}$</annotation></semantics> </math> -hybridized chalcogen bond (ChB) donor molecules, an ammonia acceptor molecule, and the corresponding 1:1 donor-acceptor complexes formed between them are computed with density functional theory. Adding an allelic carbon linker into the backbone of the donor moiety generally reduces the number of σ/π-hole regions from two to one. This compositional modification to the interactive region of ChB donors results in a strip-like area of localized electropositive potential along the extension of the carbon-chalcogen bond. The presence of these regions gives rise to a reduction in ChB directionality and, thus, relatively flat potential energy surfaces. Remedies to this behavior are provided through additional hydrogen bond interactions between the amino hydrogen atoms and the electron-accepting strips on the sides of the ChB donors. These highly tunable ChB donors, and by extension their donor-ammonia complexes, are interrogated to differentiate subtle differences in the chemicophysical properties with and without electron-withdrawing substituents. The structures, electronics, and energetics exhibited by the ChB donors before and after complexation are discussed and utilized to identify the rational design guidelines developed herein.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500381"},"PeriodicalIF":2.2,"publicationDate":"2025-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145231487","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

Nucleophilic Control of BODIPY Decay Pathways: A Quantum Mechanical Study. BODIPY衰变途径的亲核控制：量子力学研究。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-01 DOI: 10.1002/cphc.202500593

Peng Cui, Zichao Ling, Zhiwei Li

{"title":"Nucleophilic Control of BODIPY Decay Pathways: A Quantum Mechanical Study.","authors":"Peng Cui, Zichao Ling, Zhiwei Li","doi":"10.1002/cphc.202500593","DOIUrl":"https://doi.org/10.1002/cphc.202500593","url":null,"abstract":"This study employs density functional theory to investigate nucleophilic substitution effects on photophysical properties of 3,5-substituted meso-(4-bromophenyl) BODIPY derivatives. BODIPY compounds with chloride, methoxy, cyano, fluoro, ethoxy, hydroxy, and azido substituents are examined, focusing on radiative and nonradiative decay mechanisms. Calculations reveal modest variations in radiative decay rates (kr: 1.08 × 108 to 3.05 × 108 s-1) across derivatives, while nonradiative rates show significantly greater variation. Internal conversion (IC) rates span 2.76 × 107 to 3.25 × 108 s-1, whereas decay via the minimum energy conical intersection pathway is negligible due to high activation barriers (>0.44 eV). Electron-withdrawing groups enhance radiative decay, while electron-donating groups promote nonradiative pathways. Huang-Rhys factors (SM), internal reorganization energies (λl), and electronic coupling (V) critically determine IC rates, with λl and SM being most influential. Electronic coupling varies modestly (0.23-0.30 eV), with CN2-BrPh-BODIPY exhibiting the lowest coupling (0.23 eV) and nonradiative rate (2.76 × 107 s-1). These findings confirm IC as the dominant nonradiative channel and provide insights for optimizing BODIPY-based fluorescent probes for biological imaging and chemical sensing applications.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202500593"},"PeriodicalIF":2.2,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145205685","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

Silver and Polyvalent Cobalt Encapsulated in N-Doped Carbon Nanomaterials as an Efficient Bifunctional Electrocatalyst for Zn-Air Battery. 氮掺杂碳纳米材料包裹银和多价钴作为锌空气电池的高效双功能电催化剂。

IF 2.2 3区化学

Chemphyschem Pub Date : 2025-10-01 DOI: 10.1002/cphc.202500496

Tengfei Wang, Wenjing Zhang, Yun Wang, Xiaoxia Lv, Jinjun Cai, Hua Wang

引用次数: 0