ChemPlusChem最新文献_第4页

Applying Machine Learning to Predict Electron Transfer Kinetics from Voltammetry Experiments.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-05 DOI: 10.1002/cplu.202400720

Austen C Adams, Melodee O Seifi, Ashan P Wettasinghe, Jason D Slinker

{"title":"Applying Machine Learning to Predict Electron Transfer Kinetics from Voltammetry Experiments.","authors":"Austen C Adams, Melodee O Seifi, Ashan P Wettasinghe, Jason D Slinker","doi":"10.1002/cplu.202400720","DOIUrl":"https://doi.org/10.1002/cplu.202400720","url":null,"abstract":"Electrochemistry enables precise measurements for sensors, electronics, and biochemical devices. Nonetheless, modeling the electron transfer kinetics of electrochemistry experiments is time-consuming to perform and account for nonideality. We utilize multiple machine learning (ML) approaches to create adaptive and predictive models to rapidly determine the parameters of electron transfer kinetics from heterogeneous experimental square wave voltammograms from surface-bound electrochemistry. Our models include Gaussian process regressions (GPRs), randomized forests of decision trees, and ML ensemble techniques. Whereas conventional approaches with manual background subtraction and analytic modeling took ~10 hours, ML approaches were trained in 0.2-120 minutes and implemented in a fraction of a second. The GPR method ardExponential performed most accurately but exhibited the longest training time. Randomized forests produced respectable estimates with the shortest training times, while ensembles balanced accuracy and time. Adding one to three kinetic parameters improved the training of these ML models with each parameter added. Overall, this shows that ML can efficiently predict kinetic parameters for surface-bound electrochemistry experiments with heterogeneous voltammograms, enabling rapid automated determination of electron transfer kinetics.","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400720"},"PeriodicalIF":3.0,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143555450","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

Machine Learning Clustering of Water-Water Interactions in the Cambridge Structural Database.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-04 DOI: 10.1002/cplu.202400764

Jelena Živković, Milan Milovanović, Marina Andrić

引用次数: 0

Urea-based carbon quantum dots for recognition of Fe3+ by fluorescence quenching and Pb2+ by fluorescence enhancement.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-04 DOI: 10.1002/cplu.202400715

Shruti Sharma, Papia Chowdhury

引用次数: 0

Zinc-Containing BEA Zeolites for the Propane Dehydrogenation Reaction: Influence of Adding Yttrium on the Catalytic Properties.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-04 DOI: 10.1002/cplu.202400723

Svitlana M Orlyk, Nina V Vlasenko, Valeriy I Chedryk, Yurii M Nychiporuk, Frederic Averseng, Yannick Millot, Laetitia Valentin, Jacek Gurgul, Stanislaw Dzwigaj

{"title":"Zinc-Containing BEA Zeolites for the Propane Dehydrogenation Reaction: Influence of Adding Yttrium on the Catalytic Properties.","authors":"Svitlana M Orlyk, Nina V Vlasenko, Valeriy I Chedryk, Yurii M Nychiporuk, Frederic Averseng, Yannick Millot, Laetitia Valentin, Jacek Gurgul, Stanislaw Dzwigaj","doi":"10.1002/cplu.202400723","DOIUrl":"https://doi.org/10.1002/cplu.202400723","url":null,"abstract":"Research results about the structure, acid-base, redox, and adsorption characteristics of zinc(yttrium)-containing dealuminated BEA zeolites (Si/Al=1000), Zn(Y)SiBEA and their catalytic properties in the propane dehydrogenation with CO2 (CO2-PDH) are presented. The catalysts were prepared through a two-step procedure involving complete dealumination of the BEA zeolite followed by the introduction of Zn2+ and Y3+ cations into vacant T-atom sites, by impregnation. The samples obtained were characterized using XRD, XPS, 29Si DP MAS NMR, low-temperature N2 ad/desorption, TPR-H2, C3H8/C3H6 (CO2, NH3)-TPD, and FTIR-Py techniques. The influence of zinc content and yttrium on the functional properties of Zn(Y)SiBEA surface and activity/selectivity of the catalysts (Zn1.0-, Zn2.0-, and Zn2.0Y2.0SiBEA) in the CO2-PDH process are analyzed. The balanced acid-base characteristics of the Zn(Y)SiBEA catalysts determine their activity/selectivity in the CO2-mediated propane dehydrogenation to propene. Propane conversion and propene selectivity/yield over Zn(Y)SiBEA catalysts are higher in the CO2-PDH process compared to direct propane dehydrogenation (without CO2).","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400723"},"PeriodicalIF":3.0,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539633","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

Mechanistic Insight into the Thermochromic Emission of One-Dimensional Platinum(II) and Palladium(II) Complex Crystals.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-03 DOI: 10.1002/cplu.202400743

Masaki Yoshida, Masako Kato

引用次数: 0

Phosphoric acid vs biogenic mineralization of carbonate apatite and hydroxyapatite in relation to infection-induced urinary stones: physical, chemical and microbiological aspects.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-03 DOI: 10.1002/cplu.202400712

Jolanta Prywer, Ewa Mielniczek-Brzóska, Agnieszka Torzewska

引用次数: 0

Dibenzofuran[a]-Fused BODIPYs: Synthesis, Photophysical Properties, and N₂O₂-Boron-Chelation Towards NIR Materials for Application in Organic Photodetectors.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-03 DOI: 10.1002/cplu.202500021

Airi Suzuki, Risa Yamamoto, Masato Ito, Yuji Kubo

{"title":"Dibenzofuran[a]-Fused BODIPYs: Synthesis, Photophysical Properties, and N2O2-Boron-Chelation Towards NIR Materials for Application in Organic Photodetectors.","authors":"Airi Suzuki, Risa Yamamoto, Masato Ito, Yuji Kubo","doi":"10.1002/cplu.202500021","DOIUrl":"10.1002/cplu.202500021","url":null,"abstract":"Highly annulated boron-dipyrromethenes (BODIPYs) were synthesized with the objective to develop a near-infrared (NIR)-absorbing photodetector. Post-functionalization of the dibenzoBODIPY scaffold enabled it to fuse with the dibenzofuran heterocycle at the a-bond of the pyrrole unit to give the related dyes 1 and 2, which absorb far-red light in tetrahydrofuran. Further structural modification by intramolecular B,O-chelation of 2 yielded the benzo[1,3,2]oxazaborinine-containing dye 14 having an intense absorption band with a λmax value of 812 nm (ϵ=1.3×105 M-1 cm-1), as rationalized by time dependent density functional theory (TD-DFT)/DFT calculations. Dye 14 exhibited unique emission properties, wherein irradiation at 375 nm led to a dual emission at 822 nm (Φ=5.1 %) and 470 nm (Φ=7.8 %), which could be attributed to the electronic non-adiabatic coupling due to the large energy difference between the S2 and S1 states, according to the anti-Kasha rule. Using a resistance-heating-type vacuum-deposition method, the rigid π-conjugated structure of 14 enabled its application as an NIR photodetector in a single-component device (indium tin oxide/14/Al). Current-voltage (J-V) measurements under photoirradiation at 870 nm (120 μW cm-2) produced a photocurrent of 6.05×10-7 A cm-2 at a bias potential of 0.1 V.","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202500021"},"PeriodicalIF":3.0,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539620","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

Shape-Persistent Anthracene-Based Macrocycles Prepared by Reversible Boronic Ester Formation: Crystallization and Structural Analysis.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-03-02 DOI: 10.1002/cplu.202500014

Shoma Kasahara, Hironobu Hayashi, Takayuki Okumura, Michio Matsumoto, Mitsuaki Yamauchi, Yoshiyuki Mizuhata, Naoki Aratani, Hiroko Yamada

{"title":"Shape-Persistent Anthracene-Based Macrocycles Prepared by Reversible Boronic Ester Formation: Crystallization and Structural Analysis.","authors":"Shoma Kasahara, Hironobu Hayashi, Takayuki Okumura, Michio Matsumoto, Mitsuaki Yamauchi, Yoshiyuki Mizuhata, Naoki Aratani, Hiroko Yamada","doi":"10.1002/cplu.202500014","DOIUrl":"10.1002/cplu.202500014","url":null,"abstract":"Shape-persistent macrocycles with confined inner spaces have gained significant interest due to their unique properties and potential applications in gas/molecular recognition, nanoscale templates, and nanoelectronics. In this study, we present an efficient synthesis of macrocycles containing anthracene units through reversible boronic ester formation between 1,2-diols and boronic acids. These template-free macrocycles exhibited diverse internal cavities ranging from 11 Å to 20 Å and readily crystallized in solution and on solid substrates. Powder X-ray diffraction analysis revealed that the crystallinity remained after solvent removal. Single crystal X-ray analysis provided detailed insights into the molecular geometry and packing structure. Notably, a macrocycle with phenyl linkers resembles a pseudo-nanocapsule, as the bulky substituents on both sides of the macrocycles prevented the cavity filling by neighbouring molecules. Consequently, the crystalline powders of the macrocycle with phenyl linkers maintained its crystallinity even after annealing, likely resulting in the highest N2 gas adsorption properties among synthesized macrocycles. This work highlights a robust synthesis strategy for macrocycles, broadening their potential for advanced applications and enabling self-assembled nanoarchitectures.","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202500014"},"PeriodicalIF":3.0,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143536279","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

Enzymatic Synthesis of Functional PEGylated Adipate Copolymers. 功能性 PEG 化己二酸酯共聚物的酶法合成。

IF 3 4区化学

ChemPlusChem Pub Date : 2025-02-28 DOI: 10.1002/cplu.202400668

Eleni Axioti, Emily G Dixon, Thomas Jepras, Fen Tin He, Peter J V Hartman, Bradley Hopkins, Vincenzo Di Bari, Jiraphong Suksiriworapong, Valentina Cuzzucoli Crucitti, Luciano Galantini, Iolanda Francolini, Robert J Cavanagh, Vincenzo Taresco

{"title":"Enzymatic Synthesis of Functional PEGylated Adipate Copolymers.","authors":"Eleni Axioti, Emily G Dixon, Thomas Jepras, Fen Tin He, Peter J V Hartman, Bradley Hopkins, Vincenzo Di Bari, Jiraphong Suksiriworapong, Valentina Cuzzucoli Crucitti, Luciano Galantini, Iolanda Francolini, Robert J Cavanagh, Vincenzo Taresco","doi":"10.1002/cplu.202400668","DOIUrl":"10.1002/cplu.202400668","url":null,"abstract":"Many new active pharmaceutical ingredients (APIs) demonstrate high hydrophobicity and low water-solubility issues. In this regard, polymeric nanoparticles (NPs) have been extensively used as drug delivery carriers for the encapsulation of such APIs. One commonly used polymer is polyethylene glycol (PEG), owing to its biocompatibility, high water solubility, and capacity to prolong the drug residence time. However, concerns have arisen regarding PEG's immunogenicity and limited biodegradability. In addition, inherent limitations, including limited chemical handles can restrict PEG's effectiveness in physiological conditions. For this reason, in the present study, we combine the advantages offered by PEG with the use of an enzymatic synthetic route to produce novel PEGylated polyesters. Furthermore, it has been proven that incorporation of hydrophobic diols into the PEGylated backbone influences NPs formation, stability, and drug encapsulation, despite high chemical similarity. As a preliminary result, samples containing PEG and 1,6-hexanediol in a 50 : 50 ratio (PEGA-Hex 50 %) and PEG and 2-hydroxyethyl disulfide in a 50 : 50 ratio (PEGA-SS 50 %) have proved to be the most promising candidates in this small library analysed. Both samples exhibited sufficient NPs stability, biocompatibility, and superior encapsulation efficiency compared to the other variants.","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400668"},"PeriodicalIF":3.0,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143522161","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

Catalytic Performance of Highly Dispersed Bimetallic Catalysts for CO Hydrogenation to DME.

IF 3 4区化学

ChemPlusChem Pub Date : 2025-02-28 DOI: 10.1002/cplu.202500010

Chunqiu Zhao, Qiang Chang, Fu Yin, Guowei Niu, Chenghua Zhang, Dan Liu, Bhekie B Mamba, Alex T Kuvarega

{"title":"Catalytic Performance of Highly Dispersed Bimetallic Catalysts for CO Hydrogenation to DME.","authors":"Chunqiu Zhao, Qiang Chang, Fu Yin, Guowei Niu, Chenghua Zhang, Dan Liu, Bhekie B Mamba, Alex T Kuvarega","doi":"10.1002/cplu.202500010","DOIUrl":"10.1002/cplu.202500010","url":null,"abstract":"Highly dispersed bimetallic atomic-scale catalysts have garnered significant attention in syngas conversion filed due to the synergistic effects of the precisely structured bimetallic site, which facilitate the effective activation of CO. Despite their potential, synthesizing these catalysts to meet the specific application requirements remains challenging. Herein, various bimetallic catalysts were synthesized through the pyrolysis of the bimetallic ZIF precursors which were prepared by in situ doping of different metals (Mn, Fe, Co, Ni and Cu) into the ZIF-8 structure. In the presence of a highly dispersed and highly loaded Zn, the doping content in the ultimate second metallic catalysts varied between 0.15-1.20 wt % for different metals. The catalysts were systematically characterized using XRD, BET, TEM, XPS, Raman, ICP, and H2-TPD techniques. Among them, the Zn-NC regulated with Cu or Ni exhibited superior catalytic performance. Notably, the Cu-Zn-NC catalyst showed the highest activity, achieving a CO conversion of 32.8 % and optimal DME selectivity approaching 95.2 % in CO hydrogenation reactions. These enhanced performance metrics were attributed to the synergetic effects of bimetallic components. The incorporation of Cu not only preserved the original Zn-N structure but also preserved the catalytic performance unchanged. This preparation strategy is expected to filter out new research targets to use in diverse catalytic applications.","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202500010"},"PeriodicalIF":3.0,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143522164","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