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Pt/SnO2/Sb2O4 nanoparticle catalyst embedded in Multi-walled carbon nanotubes as active material for electrochemical hydrogen storage inquiries
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-21 DOI: 10.1039/d5dt00336a
Raziyeh Akbarzadeh
{"title":"Pt/SnO2/Sb2O4 nanoparticle catalyst embedded in Multi-walled carbon nanotubes as active material for electrochemical hydrogen storage inquiries","authors":"Raziyeh Akbarzadeh","doi":"10.1039/d5dt00336a","DOIUrl":"https://doi.org/10.1039/d5dt00336a","url":null,"abstract":"Hydrogen storage and safe transport are the most important issues for hydrogen energy applications. Hydrogen has the necessary potential to provide clean fuel for heating and transportation because its only product of this combustion is pure water. Hydrogen is identified as one of the most renewable energy sources by supplying an efficient storage method. The electrochemical method with high energy conversion efficiency, through absorbtion/desorbtion mechanisms, is considered an appropriate strategy to achieve hydrogen storage. Hence, we propose a hydrogen energy storage system based on efficient electrode materials and electrochemical method. Due to obtaining high efficiency hydrogen storage, the Pt/SnO2/Sb2O4 nanoparticle catalyst embedded in multi-walled carbon nanotubes (MWCNTs) is synthesized via a facile polyol method, as active material. The sample structure was characterized by different techniques to determine its crystal structure, surface morphology, elements and porosity. Further, the electrochemical hydrogen storage abilities and the specific capacitance values of the as-prepared nanocomposite were assessed in alkaline media by chronopotentiometry analysis. The XRD studies exhibit that the average crystallite size of the Pt/SnO2/Sb2O4 nanoparticle catalyst is estimated to be around 7.5 nm. Also, the BET measurement shows a specific surface area, pore volume and pore diameter of 137.89 m2g-1, 0.3379 cm3g-1 and 9.8 nm for Pt/SnO2/Sb2O4/MWCNTs nanocomposite, respectively. The electrochemical consequences indicate that the incorporation of Pt/SnO2/Sb2O4 nanoparticle catalyst with MWCNTs showed excellent cycle stability and a high degree of electrochemical reversibility as an optimistic active candidate for use in electrochemical hydrogen storage. The maximum discharge capacity of Pt/ SnO2/Sb2O4 /MWCNTs nanocomposite was obtained to be 3480 mAhg-1 after 12 cycles. The higher and excellent discharge capacity of nanocomposite can partially be ascribed to its higher porosity, large specific surface area and the small size of Pt/SnO2/Sb2O4 nanoparticle catalyst.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"41 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666740","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
Metal Ion-Modulated Synthesis of γ-MnO2 Nanosheet for Catalytic Oxidative Degradation of Clomiprazole
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-21 DOI: 10.1039/d5dt00058k
Jinlian Zhang, Yu Xie, Xinli Zhang, Yuanhong Zhong, Ming Sun, Lin Yu
{"title":"Metal Ion-Modulated Synthesis of γ-MnO2 Nanosheet for Catalytic Oxidative Degradation of Clomiprazole","authors":"Jinlian Zhang, Yu Xie, Xinli Zhang, Yuanhong Zhong, Ming Sun, Lin Yu","doi":"10.1039/d5dt00058k","DOIUrl":"https://doi.org/10.1039/d5dt00058k","url":null,"abstract":"Two-dimensional non-layered oxide nanosheets exhibit exceptional catalytic properties, offering significant potential for environmental applications. In this study, we report the development of a novel Fe-doped γ-MnO₂ material with a hierarchical microsphere morphology, achieved through a metal ion regulation strategy. Unlike conventional sea urchin-like γ-MnO₂, Fe doping induced a transformation to a two-dimensional non-layered structure composed of nanosheets, significantly increasing the specific surface area and exposing more active sites. The Fe-doped γ-MnO₂ catalysts were evaluated for the degradation of chlorimiprazole (CBZ), a persistent pollutant, using a sulfate radical-based advanced oxidation process. Among the synthesized catalysts, NF-0.25Fe exhibited superior performance, achieving 93% CBZ removal within 16 min under near-neutral conditions. This exceptional activity was attributed to the optimized morphology, higher low-valence Mn content, and enhanced surface-active oxygen species. Systematic investigations revealed that the catalyst dosage, PMS concentration, and pH critically influenced the catalytic efficiency. This work demonstrates the potential of metal ion modulation in tailoring the structural and catalytic properties of transition metal oxides. The insights gained here provide a robust foundation for designing advanced nanomaterials for environmental remediation and other catalytic applications.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"61 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666741","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
Dual Emissive Ytterbium (III) Complexes with π-Conjugated BODIPY-Bipyridine Ligands
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-21 DOI: 10.1039/d5dt00354g
Priyangika P. Senevirathne, Hongshan He, Kraig Wheeler, Radu F Semeniuc
{"title":"Dual Emissive Ytterbium (III) Complexes with π-Conjugated BODIPY-Bipyridine Ligands","authors":"Priyangika P. Senevirathne, Hongshan He, Kraig Wheeler, Radu F Semeniuc","doi":"10.1039/d5dt00354g","DOIUrl":"https://doi.org/10.1039/d5dt00354g","url":null,"abstract":"Four BODIPY-functionalized bipyridine ligands (B1, B2, B3 and B4) were synthesized for sensitizing the near-infrared emission of Yb (III) ions. In these ligands, a BODIPY moiety was conjugated to 2,2′-bipyridine through an acetylene spacer at its C2 position, whereas its C6 position was substituted by H (B1), iodine (B2), 4-carboxylphenylacetylene (B3) or 4-thiocyanophenylacetylene (B4). The ligands exhibit strong absorption in the visible region and readily form stable complexes with ytterbium (III) trishexafluoroacetylacetonate (hfac-) hydrate in dichloromethane. Single-crystal X-ray diffraction analysis for Yb-B2 showed that the BODIPY unit almost falls into the bipyridine plane with Yb (III) being coordinated by six O from hfac<small><sup>-</sup></small> and two N atoms from bipyridine. All complexes exhibit strong absorption between 530 and 570 nm and can sensitize the ytterbium (III) for its emission at 980 nm under the UV-VIS light illumination. Interestingly, the visible emission from the complex increased when excited at 375 nm, making the complexes dual emissive, which is due to the increased absorption of the complex at 375 nm and inefficient energy transfer from BODIPY moiety to the Yb(III) ion.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"183 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666639","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
Correction: Dicopper(i) complexes of a binucleating, dianionic, naphthyridine bis(amide) ligand 更正:双核、二阴离子、萘啶双(酰胺)配体的二氯化铜(I)配合物
IF 3.5 3区 化学
Dalton Transactions Pub Date : 2025-03-21 DOI: 10.1039/D5DT90059J
Laurent Sévery, T. Alexander Wheeler, Amelie Nicolay, Simon J. Teat and T. Don Tilley
{"title":"Correction: Dicopper(i) complexes of a binucleating, dianionic, naphthyridine bis(amide) ligand","authors":"Laurent Sévery, T. Alexander Wheeler, Amelie Nicolay, Simon J. Teat and T. Don Tilley","doi":"10.1039/D5DT90059J","DOIUrl":"10.1039/D5DT90059J","url":null,"abstract":"<p >Correction for ‘Dicopper(<small>I</small>) complexes of a binucleating, dianionic, naphthyridine bis(amide) ligand’ by Laurent Sévery <em>et al.</em>, <em>Dalton Trans.</em>, 2025, https://doi.org/10.1039/d5dt00034c.</p>","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":" 14","pages":" 5954-5954"},"PeriodicalIF":3.5,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/dt/d5dt90059j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672572","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 difunctional Dy(III)-complex exhibiting single-molecule magnet behaviour and fluorescent cellular-imaging
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-21 DOI: 10.1039/d5dt00559k
Xuelian Wang, Zhaopeng Zeng, Mengyuan Li, Shuman Zhang, Xuhui Qin, Peipei Cen, Runmei Ding, Danian Tian, Xiangyu Liu
{"title":"A difunctional Dy(III)-complex exhibiting single-molecule magnet behaviour and fluorescent cellular-imaging","authors":"Xuelian Wang, Zhaopeng Zeng, Mengyuan Li, Shuman Zhang, Xuhui Qin, Peipei Cen, Runmei Ding, Danian Tian, Xiangyu Liu","doi":"10.1039/d5dt00559k","DOIUrl":"https://doi.org/10.1039/d5dt00559k","url":null,"abstract":"A mononuclear Dy(III) complex, with formula [Dy(Dicnq)(TFNB)3] (1), is synthesized through a self-assembly with 4,4,4-trifluoro-1-(2-naphthyl)-1,3-butanedione (TFNB) and 6,7-dicyanodipyrido [2,2-d:2′,3′-f] quinoxaline (Dicnq) ligands. Single-crystal structure determination reveals that Dy(III) ion in complex 1 features an N2O6 octacoordinated environment with distorted square-antiprism D4d geometry. Magnetic data analysis shows that 1 behaves as a single-molecule magnet, with an energy barrier of 192 K under zero dc field. With an external field of 1200 Oe, the quantum tunneling of magnetization is suppressed in 1, resulting in an enhanced energy barrier of 261 K. Additionally, 1 displays a room-temperature photoluminescence. Leveraging the optical properties coupled with minimal cytotoxic effects of 1, we assess its suitability for cellular imaging applications. Subsequent laser confocal microscopy analysis reveals that 1 is capable of efficiently traversing the plasma membrane and nuclear membrane of HeLa cells, an observation that is not commonly reported in dysprosium-based complexes.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"14 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666654","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
Isothiourea-based burial interface modification for high-efficiency and stable perovskite solar cells
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-20 DOI: 10.1039/d4dt03269a
Zipeng Tang, Chunlong Wang, Chunying Ma, Wenzhen Zou, Chao Wei, Xuanshuo Shanguan, Lu Zhou, Xiaoyu Li, Yongchun Ye, Liguo Gao, Yusran Sulaiman, Tingli Ma, Chu Zhang
{"title":"Isothiourea-based burial interface modification for high-efficiency and stable perovskite solar cells","authors":"Zipeng Tang, Chunlong Wang, Chunying Ma, Wenzhen Zou, Chao Wei, Xuanshuo Shanguan, Lu Zhou, Xiaoyu Li, Yongchun Ye, Liguo Gao, Yusran Sulaiman, Tingli Ma, Chu Zhang","doi":"10.1039/d4dt03269a","DOIUrl":"https://doi.org/10.1039/d4dt03269a","url":null,"abstract":"Abstract: Senior oxygen-related defects including O vacancies and dangling O-H bonds in the SnO2 ETL result in non-radiative carrier recombination, which directly affect the efficiency performance and stability of perovskite solar cells. Meanwhile, undercoordinated Pb2+ can also induce non-radiative recombination of photogenerated carriers and provide a pathway for ion migration, leading to further degradation of solar cell performance. To tackle such issues, interface modification with multi-functional small molecules is usually considered a convenient way to inhibit non-radiative recombination and improving carrier transportation. Here, we employ two isothiourea group-based bridge molecule CESC (S-carboxyethyl isothiourea hydrochloride) together with DASC (S-[2-(Dimethylamino) ethyl] isothiourea Dihydrochloride) to passivate the burial interface between SnO2 and perovskite, realizing the dual functional passivation towards both filling O2- vacancy in SnO2 lattice and binding the uncoordinated ions. Perovskite solar cells fabricated with this method shows well-improved optoelectronic performance as well as resistance against ambient moisture. Compared with the control device (17.20%), the efficiency of the devices modified by DASC and CESC increased to 18.75% and 19.04%, respectively. The unpackaged solar cells treated with CESC and DASC maintained 91.2% and 89.5% of their initial efficiency, respectively, after aging for 1000 hours in a high humidity environment.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"76 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660769","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 Bioactivity of Diorganotin(IV) Schiff Base Complexes as Potential Antimalarial and Antioxidant Agents: Insight through Cytotoxicity and Molecular Docking
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-20 DOI: 10.1039/d5dt00274e
Jai Devi, Bharti Taxak, Binesh Kumar, swati rani
{"title":"Synthesis, Characterization and Bioactivity of Diorganotin(IV) Schiff Base Complexes as Potential Antimalarial and Antioxidant Agents: Insight through Cytotoxicity and Molecular Docking","authors":"Jai Devi, Bharti Taxak, Binesh Kumar, swati rani","doi":"10.1039/d5dt00274e","DOIUrl":"https://doi.org/10.1039/d5dt00274e","url":null,"abstract":"The infectious ailments are raising on rapid scale globally causing a high rate of mortality and morbidity. In pursuit of new and effective anti-infectious agents, this research presents the synthesis of eight diorganotin(IV) complexes (3–10), derived from 1-naphthyl thiourea and ketone derivatives. Comprehensive structural analysis, employing FT-IR, NMR (¹H, ¹³C, and ¹¹⁹Sn), SEM-EDAX, TGA, P-XRD and mass spectrometry, demonstrate that the ligands chelated with diorganotin(IV) ion through O-, S- and N- donor sites, adopting an pentacoordinated geometry. Biological assays states that the complexes have enhanced bio-efficacy relative to their corresponding ligands, with activity ranked as Ph₂SnL1-2 &gt; Bu₂SnL1-2 &gt; Et₂SnL1-2 &gt; Me₂SnL1-2. Notably, complexes 6 (Ph2SnL1) and 10 (Ph2SnL2) exhibited highest malaria and oxidant controlling properties, with IC50 values ranging from 0.83 ± 0.08 - 0.95 ± 0.15 µM and 2.82 ± 0.03 - 3.09 ± 0.01 µM, correspondingly, comparable to their standard agents. The cytotoxicity evaluation against Vero cells also states that the complex 6 (Ph2SnL1) has lowest toxicity (21.96 ± 0.09 %) at 3.12 µg/mL concentration. Moreover, molecular docking study also reveals lowest binding score of -9.7 kcal/mol and significant hydrophobic interactions with key residues against 1U5A protein, demonstrating its highest bio-efficacy compared to ligand 1(H2L1). Theoretical and computational studies, along with ADMET Lab 2.0 evaluation, highlight the bioactivity of complex 6 (Ph2SnL1), suggesting its potential application in the medicinal sector due to its compliance with Lipinski's Rule of Five and strong pharmacokinetic properties, including oral bioavailability, permeability, and clearance comparable to standard drugs.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"70 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660771","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 novel ratiometric fluorescent probe for the detection of co-existing Fe3+ and Ag+ ions: characterization and mechanism exploration
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-20 DOI: 10.1039/d5dt00012b
Qi Wu, Qianwei Wang, Jinhu Guo, Mengxuan Fang, Xinyu Yang, Yichong Cheng, Dalai Jin, Longcheng Wang
{"title":"A novel ratiometric fluorescent probe for the detection of co-existing Fe3+ and Ag+ ions: characterization and mechanism exploration","authors":"Qi Wu, Qianwei Wang, Jinhu Guo, Mengxuan Fang, Xinyu Yang, Yichong Cheng, Dalai Jin, Longcheng Wang","doi":"10.1039/d5dt00012b","DOIUrl":"https://doi.org/10.1039/d5dt00012b","url":null,"abstract":"A novel white-light-emitting Ln-MOF composite, g-C₃N₄@TbEu(cpioa), was developed as a ratiometric fluorescent probe for the qualitative and quantitative analysis of metal ions. Among the tested ions, only Fe³⁺ and Ag⁺ exhibited distinct quenching behaviors. Mechanistic studies revealed that Fe³⁺ and Ag⁺ quench luminescence via dynamic and static processes, respectively, involving energy competitive absorption (ECA), photoinduced electron transfer (PET), Förster resonance energy transfer (FRET), and intramolecular weak interactions. The probe demonstrated high sensitivity with limits of detection (LOD) of 0.117 μM for Fe³⁺ and 0.383 μM for Ag⁺. Notably, the observable chromaticity variations enabled differentiation of co-existing Fe³⁺ and Ag⁺ in solutions—a first-reported achievement. Empirical equations derived from orthogonal experiments and multiple regression analysis validated the probe’s capability for dual-ion detection. This work pioneers the application of Ln-MOF-based probes in analyzing mixed analytes, offering significant potential for environmental monitoring, clinical diagnostics, and industrial applications.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"26 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660772","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
Alkylamido Lutetium Complexes as Prospective Lutetium Imido Precursors: Synthesis, Characterization and Ligand Design
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-20 DOI: 10.1039/d5dt00338e
Jackson P. Knott, Shou-Jen Hsiang, Paul G. Hayes
{"title":"Alkylamido Lutetium Complexes as Prospective Lutetium Imido Precursors: Synthesis, Characterization and Ligand Design","authors":"Jackson P. Knott, Shou-Jen Hsiang, Paul G. Hayes","doi":"10.1039/d5dt00338e","DOIUrl":"https://doi.org/10.1039/d5dt00338e","url":null,"abstract":"Mixed alkyl-amido lutetium complexes, L&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt;Lu(CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;SiMe&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;)(NHCPh&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;) (&lt;strong&gt;7&lt;/strong&gt;&lt;strong&gt;&lt;small&gt;&lt;sub&gt;CPh3&lt;/sub&gt;&lt;/small&gt;&lt;/strong&gt;) and L&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt;Lu(CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;SiMe&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;)(NHDipp) (&lt;strong&gt;7&lt;/strong&gt;&lt;strong&gt;&lt;small&gt;&lt;sub&gt;Dipp&lt;/sub&gt;&lt;/small&gt;&lt;/strong&gt;) (L&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt; = 2,5-[&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;Pr&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;P=N(4-&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;PrC&lt;small&gt;&lt;sub&gt;6&lt;/sub&gt;&lt;/small&gt;H&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt;)]&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;C&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt;H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;N&lt;small&gt;&lt;sup&gt;–&lt;/sup&gt;&lt;/small&gt;), were synthesized by addition of a bulky primary amine, NH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;R (R = CPh&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;, Dipp) (Dipp = 2,6-&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;Pr&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;C&lt;small&gt;&lt;sub&gt;6&lt;/sub&gt;&lt;/small&gt;H&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;) to the dialkyl complex L&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt;Lu(CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;SiMe&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;)&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; (&lt;strong&gt;6&lt;/strong&gt;). Unlike complexes supported by the related pincer ligand L&lt;small&gt;&lt;sup&gt;Ph&lt;/sup&gt;&lt;/small&gt; (L&lt;small&gt;&lt;sup&gt;Ph&lt;/sup&gt;&lt;/small&gt; = 2,5-[Ph&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;P=N(4-&lt;small&gt;&lt;sup&gt;&lt;em&gt;i&lt;/em&gt;&lt;/sup&gt;&lt;/small&gt;PrC&lt;small&gt;&lt;sub&gt;6&lt;/sub&gt;&lt;/small&gt;H&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt;)]&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;C&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt;H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;N&lt;small&gt;&lt;sup&gt;–&lt;/sup&gt;&lt;/small&gt;) these species proved resistant to C–H cyclometalative processes. Attempts to access lutetium imdes via addition of 4-dimethylaminopyridine (DMAP) to &lt;strong&gt;7&lt;/strong&gt;&lt;strong&gt;&lt;small&gt;&lt;sub&gt;CPh3&lt;/sub&gt;&lt;/small&gt;&lt;/strong&gt; and &lt;strong&gt;7&lt;/strong&gt;&lt;strong&gt;&lt;small&gt;&lt;sub&gt;Dipp&lt;/sub&gt;&lt;/small&gt;&lt;/strong&gt; promoted disproportionation, affording 0.5 equivalents of the corresponding bisamide complexes L&lt;em&gt;&lt;small&gt;&lt;sup&gt;i&lt;/sup&gt;&lt;/small&gt;&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt;Lu(NHCPh&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;)&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; (&lt;strong&gt;8&lt;/strong&gt;&lt;strong&gt;&lt;small&gt;&lt;sub&gt;CPh3&lt;/sub&gt;&lt;/small&gt;&lt;/strong&gt;) and L&lt;em&gt;&lt;small&gt;&lt;sup&gt;i&lt;/sup&gt;&lt;/small&gt;&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt;Lu(NHDipp)&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; (&lt;strong&gt;8&lt;/strong&gt;&lt;strong&gt;&lt;small&gt;&lt;sub&gt;Dipp&lt;/sub&gt;&lt;/small&gt;&lt;/strong&gt;), respectively, as well as 0.5 equivalents of L&lt;em&gt;&lt;small&gt;&lt;sup&gt;i&lt;/sup&gt;&lt;/small&gt;&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt;Lu(CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;SiMe&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;)&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;, which decomposed in the presence of DMAP. Incorporation of internal Lewis bases was accomplished by replacing the N-aryl substituents in L&lt;em&gt;&lt;small&gt;&lt;sup&gt;i&lt;/sup&gt;&lt;/small&gt;&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Pr&lt;/sup&gt;&lt;/small&gt; with 4,6-dimethylpyrimidine groups (L&lt;small&gt;&lt;sup&gt;Pm&lt;/sup&gt;&lt;/small&gt;, &lt;strong&gt;11&lt;/strong&gt;). The corresponding dialkyl lutetium complex L&lt;small&gt;&lt;sup&gt;Pm&lt;/sup&gt;&lt;/small&gt;Lu(CH&lt;small&gt;","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"56 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660732","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
Influence of imidazole functionalization on the properties of small molecule models of the LPMO active site
IF 4 3区 化学
Dalton Transactions Pub Date : 2025-03-20 DOI: 10.1039/d4dt03424d
Ugo Gilbert, Xiao Mu, Sarah Lam, Gaël De Leener, Martin Schoenauen, Maëlle Bottin, Koen Robeyns, Michel Luhmer, Raphaël Robiette, Michael L Singleton
{"title":"Influence of imidazole functionalization on the properties of small molecule models of the LPMO active site","authors":"Ugo Gilbert, Xiao Mu, Sarah Lam, Gaël De Leener, Martin Schoenauen, Maëlle Bottin, Koen Robeyns, Michel Luhmer, Raphaël Robiette, Michael L Singleton","doi":"10.1039/d4dt03424d","DOIUrl":"https://doi.org/10.1039/d4dt03424d","url":null,"abstract":"A series of small molecule Cu(II) complexes based on tridentate N3 ligands relevant to the histidine brace of the active site of lytic polysaccharide monooxygenase were synthesized and characterized by X-ray crystallography and spectroscopic studies. In order to better understand the role of different structural features and to help bridge the differences between previously reported models, the methylation patterns, imidazole connectivity, linker nature, and type of heterocycle were systematically varied across the series. These modifications lead to important differences in the electrochemical properties of the complexes and their reactivity towards the oxidation of a model substrate.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":"20 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660768","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
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