Chemistry - A European Journal最新文献_第9页

Physicochemical Properties of New Ionic Liquids and Plastic Crystal Based on Huckel Anions.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202403681

Azra Sourjah, Agnieszka Mikus, Craig M Forsyth, Wladyslaw Wieczorek, Luke A O'Dell, Jennifer M Pringle

{"title":"Physicochemical Properties of New Ionic Liquids and Plastic Crystal Based on Huckel Anions.","authors":"Azra Sourjah, Agnieszka Mikus, Craig M Forsyth, Wladyslaw Wieczorek, Luke A O'Dell, Jennifer M Pringle","doi":"10.1002/chem.202403681","DOIUrl":"https://doi.org/10.1002/chem.202403681","url":null,"abstract":"There is increasing interest in ionic liquid electrolytes for battery applications due to their potential as safer alternatives to conventional liquid electrolytes. By carefully selecting cations and anions, the physicochemical properties of these salts can be optimised. However, investigation of new cations and anions is still required to achieve the desired electrolyte properties such as high conductivity, electrochemical stability and low corrosivity. Thus, here a new series of room temperature ionic liquids (RTILs) and an organic ionic plastic crystal (OIPC) were synthesized and characterized based on N-ethyl-N-methylpyrrolidinium ([C2mpyr]+) and N-ethyl-N-methyloxazolidinium ([C2moxa]+) cations, paired with 4,5-dicyano-2-(trifluoromethyl)imidazolide ([TDI]-) and 4,5-dicyano-2-(pentafluoroethyl)imidazolide ([PDI]-) anions, forming [C2mpyr][TDI] (OIPC), [C2mpyr][PDI] (IL), [C2moxa][TDI] (IL), and [C2moxa][PDI] (IL). Thermal properties were analysed using DSC and TGA. The plastic phase of the OIPC [C2mpyr][TDI] is wide and spans most electrolyte application temperatures, extending from -40 to 56 °C. All salts exhibit thermal stability above 200 °C. The temperature dependence of the transport properties (viscosity, ionic conductivity, self-diffusion coefficient) were measured and fitted by the Vogel-Fulcher-Tamman (VFT) equation, and the ionicity of the ILs is reported. The electrochemical stability windows of the salts were analysed by CV, and the [C2mpyr]+ cation-based ILs showed the widest window of ~5 V.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403681"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Unveiling Quantum Coherence Effects in Modulating Electron Transfer in Platinum (II) Donor-Acceptor-Donor Systems.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202404512

Juanjuan Li, Yuqing Shi, Can Cui, Yefan Li, Chenluwei Ruan, Tao Cheng

{"title":"Unveiling Quantum Coherence Effects in Modulating Electron Transfer in Platinum (II) Donor-Acceptor-Donor Systems.","authors":"Juanjuan Li, Yuqing Shi, Can Cui, Yefan Li, Chenluwei Ruan, Tao Cheng","doi":"10.1002/chem.202404512","DOIUrl":"10.1002/chem.202404512","url":null,"abstract":"Quantum coherence effects (QCEs), arising from the interference of wave-like amplitudes, are crucial in controlling the electron transfer function of molecular systems. Here, we report a coherence phenomenon associated with charge separation (CS) in a range of Pt (II) cis-acetylide donor-acceptor-donor (D-A-D) systems, where the photogenerated Pt (III) center acts as an acceptor connecting two (R)phenothiazine (R = H or tBu) donors. Femtosecond transient absorption spectroscopy revealed that CS rates in D-A-D systems with double CS paths were accelerated by 4-8 times compared to their donor-acceptor (D-A) counterparts with a single path. An enhancement factor of 2-3 in electronic coupling, within the context of interference between CS paths, is derived, providing a clear signature of QCEs. This enhancementin CS processes closely correlates with the strength of coupling between donors. This study highlights the significant impact of QCEs on the photophysical properties of molecular systems and offers insights into charge and energy transport mechanisms in both natural and artificial systems.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202404512"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Pyrrolation of Melem: A Facile Gateway into the Field of Monomeric s-Heptazine Chemistry. Melem 的吡咯烷化：进入单体 s-庚嗪化学领域的捷径。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202500271

Thaddäus J Koller, Kristian Witthaut, Florian Wolf, Johannes N Singer, Jakob Blahusch, Changyong Li, Vasiliki Valsamidou, Dirk Johrendt, Wolfgang Schnick

{"title":"Pyrrolation of Melem: A Facile Gateway into the Field of Monomeric s-Heptazine Chemistry.","authors":"Thaddäus J Koller, Kristian Witthaut, Florian Wolf, Johannes N Singer, Jakob Blahusch, Changyong Li, Vasiliki Valsamidou, Dirk Johrendt, Wolfgang Schnick","doi":"10.1002/chem.202500271","DOIUrl":"10.1002/chem.202500271","url":null,"abstract":"Monomeric s-heptazines are an intriguing class of compounds with many attractive properties for various areas of application such as photocatalysis or organic light-emitting diodes. However, research into these properties has so far been challenging, as only a few synthetic routes for the preparation of monomeric s-heptazines are known in the literature. Furthermore, these few reported synthetic pathways generally require the use of specialized equipment that may not be available to all laboratories interested in studying monomeric s-heptazines. For this reason, a more accessible synthetic route for the preparation of monomeric s-heptazines has been developed in the course of this work. The central compound of this new approach is 2,5,8-tri(1H-pyrrol-1-yl)-s-heptazine, which could be conveniently synthesized via an acid catalyzed pyrrolation of melem with bench-stable 2,5-dimethoxytetrahydrofuran in a simple one-pot synthesis in air. This compound was shown to be a potent starting material for the synthesis of numerous other monomeric s-heptazines by reaction with both nucleophiles and electrophiles. The monomeric s-heptazines thus accessible were analyzed for their crystal structures by single crystal X-ray diffraction and for their optical properties by ultraviolet/visible and photoluminescence spectroscopy.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202500271"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Optimization of Catalytic Soot Oxidation by 3DOM Perovskite-Type La_0.5-xK_xSr_0.5CoO_3-δ Catalysts: Structural Insights and K Substitution.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202404379

Jing Xiong, Xiaoxiao Yu, Peng Zhang, Yuanfeng Li, Yaxiao Ma, Linsheng Xu, Sicheng Zhang, Jie Gao, Jian Liu, Zhen Zhao, Yuechang Wei

{"title":"Optimization of Catalytic Soot Oxidation by 3DOM Perovskite-Type La0.5-xKxSr0.5CoO3-δ Catalysts: Structural Insights and K Substitution.","authors":"Jing Xiong, Xiaoxiao Yu, Peng Zhang, Yuanfeng Li, Yaxiao Ma, Linsheng Xu, Sicheng Zhang, Jie Gao, Jian Liu, Zhen Zhao, Yuechang Wei","doi":"10.1002/chem.202404379","DOIUrl":"10.1002/chem.202404379","url":null,"abstract":"A series of 3DOM La0.5-xKxSr0.5CoO3-δ catalysts were synthesized using colloidal crystal templating and citric acid complexation methods. The substitution of K ions for A-site La ions was found to markedly enhance the catalysts' intrinsic activity, with the La0.4K0.1Sr0.5CoO3-δ catalyst showing exceptional performance comparable to commercial precious metal catalysts. The La0.4K0.1Sr0.5CoO3-δ catalyst demonstrated the highest catalytic activity, with T10, T50, and T90 values of 280 °C, 335 °C, and 387 °C, respectively. The enhancement in intrinsic activity is primarily attributed to the electron-donating effect of K ions which maintains charge conservation and consequently increases the concentration of surface oxygen vacancies, leading to the formation of abundant active oxygen species. Additionally, the catalysts exhibited a highly ordered macroporous structure with interconnected pores, facilitating the diffusion of soot particles and enhancing contact efficiency with active sites. These findings not only advance the understanding of the structure-performance relationship in perovskite catalysts but also pave the way for the development of cost-effective catalysts for low-temperature soot abatement.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202404379"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Aluminum Photosensitizers on Trial: Synthesis, Crystal Structures, Photophysical and Photobiological Properties of Tris(Dipyrrinato)Aluminum(III) Complexes with Long-Lived Triplet States.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202404777

Zoi Melissari, Brendan Twamley, Lígia C Gomes-da-Silva, John E O'Brien, Fábio A Schaberle, Christopher J Kingsbury, René M Williams, Mathias O Senge

{"title":"Aluminum Photosensitizers on Trial: Synthesis, Crystal Structures, Photophysical and Photobiological Properties of Tris(Dipyrrinato)Aluminum(III) Complexes with Long-Lived Triplet States.","authors":"Zoi Melissari, Brendan Twamley, Lígia C Gomes-da-Silva, John E O'Brien, Fábio A Schaberle, Christopher J Kingsbury, René M Williams, Mathias O Senge","doi":"10.1002/chem.202404777","DOIUrl":"10.1002/chem.202404777","url":null,"abstract":"Metal coordination compounds are currently a focus of research in developing new photosensitizers for materials and medicinal applications. As an abundant element in the earth's crust aluminum is a suitable target element. However, only limited studies are available on its use in photoactive systems. We now report the facile preparation of a library of homoleptic tris(dipyrrinato)aluminum(III) [AL(DIPY)3] complexes. The majority of complexes was characterized by single crystal X-ray analysis and their photophysical properties upon photoexcitation and their tendency to react with the molecular oxygen of the microenvironment and generate singlet oxygen - in polar and non-polar environment was investigated. These studies are complemented by density functional theory (DFT) calculations to assess the possible electronic distribution on the frontier molecular orbitals within the complexes. As a result of charge transfer states, long-lived triplet excited states were formed and allowed for singlet oxygen generation. An initial screening of the AL(DIPY)3 complexes via in vitro phototoxicity studies against a mouse colon carcinoma cell line (CT26) was promising as these complexes were able to trigger cell death upon irradiation at nanomolar and micromolar concentrations. The results highlight the potential of aluminum dipyrrin complexes as a broadly applicable class of photosensitizers.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202404777"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143381201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Spin Crossover Composite Film as Recyclable Catalyst for Acetalization Reaction.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202404700

Yongjian Lai, Romain Carrasco, Alejandro Enríquez-Cabrera, Lucie Routaboul, Azzedine Bousseksou

引用次数: 0

Embedding Coupled Pd/Fe Sites in Electrospun MOF-Derived Carbon Nanofibers Achieves Efficient and Durable Oxygen Reduction Catalysis.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202500053

Yun Liang, Junyu Shi, Dandan Wang, Qiaoxia Li, Qunjie Xu

{"title":"Embedding Coupled Pd/Fe Sites in Electrospun MOF-Derived Carbon Nanofibers Achieves Efficient and Durable Oxygen Reduction Catalysis.","authors":"Yun Liang, Junyu Shi, Dandan Wang, Qiaoxia Li, Qunjie Xu","doi":"10.1002/chem.202500053","DOIUrl":"10.1002/chem.202500053","url":null,"abstract":"High costs, poor durability of Pt electrocatalysts, and the low performance of non-precious metals hinder the large-scale commercialization of fuel cells. To address these challenges, a bimetallic, highly dispersed catalyst containing Pd and Fe uniformly distributed on porous nitrogen-doped carbon nanofibers was developed. This catalyst demonstrated remarkable oxygen reduction catalytic performance. The Pd-Fe-N-C catalyst exhibited catalytic activity 4.6 times higher than that of the JM 20 % Pt/C catalyst, despite containing only 0.62 wt. % Pd. Moreover, it achieved a half-wave potential (E1/2=0.953 V vs. RHE) that is 40 mV higher than the JM 20 % Pt/C catalyst (0.913 V vs. RHE). Significantly, with a total metal content of just 1.19 wt. %, the E1/2 of Pd-Fe-N-C catalyst decreased by only 1 mV after 10,000 cycles, highlighting its exceptional durability. Furthermore, a stability test revealed a current retention rate of 84.87 % after 50,000 s of operation, with no evidence of agglomeration. These results suggest that combining electrostatic spinning of MOFs with pyrolysis provides an effective and innovative method for synthesizing electrocatalysts with reduced reliance on precious metals.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202500053"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143381207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Poly(Ferrocenylene Iminoborane) and the Merging of 1,1'-Ferrocenylene with p-Phenylene Iminoborane Building Blocks into Alternating Copolymers, Oligomers, and Macrocycles.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-10 DOI: 10.1002/chem.202404533

Johannes S Schneider, Vivien Zeh, Jonas Klopf, Philipp M Schneider, Jonas Bachmann, Ivo Krummenacher, Holger Braunschweig, Holger Helten

{"title":"Poly(Ferrocenylene Iminoborane) and the Merging of 1,1'-Ferrocenylene with p-Phenylene Iminoborane Building Blocks into Alternating Copolymers, Oligomers, and Macrocycles.","authors":"Johannes S Schneider, Vivien Zeh, Jonas Klopf, Philipp M Schneider, Jonas Bachmann, Ivo Krummenacher, Holger Braunschweig, Holger Helten","doi":"10.1002/chem.202404533","DOIUrl":"10.1002/chem.202404533","url":null,"abstract":"The combination of redox-active ferrocene moieties, conjugated B=N units, and p-phenylene building blocks in linearly concatenated architectural arrangements has been explored. Oligo- and poly(ferrocenylene iminoborane)s have been successfully prepared, whereby in the latter case, the formation of linear polymers vs. discrete molecular macrocycles could be largely influenced by the polymerization conditions applied. In addition, a series of well-defined co-oligomers composed of ferrocenylene and p-phenylene moieties bridged by one or two B=N units in all possible combinations have been prepared, many of which have been structurally characterized using single-crystal X-ray diffraction. Pendent triisopropylphenyl groups on boron provide pronounced kinetic stabilization. Polycondensation of complementary monomers gave copolymers comprising alternating ferrocenylene and p-phenylene iminoborane building blocks, which were found to be cyclic in nature. UV-vis absorption spectroscopic and electrochemical studies provided highly valuable insights into the interaction of the different moieties over the B=N bonds, particularly, the electronic communication between the electroactive ferrocene units.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202404533"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389561","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Regio- and Redox Divergent Hydrated Ring Expansion of Butafulvenes.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-08 DOI: 10.1002/chem.202500245

Bo-Chao Zhou, Ting-Ting Song, Bing-Zhi Chen, Shan-Tong Xu, Yong Liu, Ding-Wei Ji, Boshun Wan, Qing-An Chen

引用次数: 0

Pt Nanoparticles Loaded on Bimetallic Porphyrinic MOF for Selective Hydrogenation Reactions.

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2025-02-07 DOI: 10.1002/chem.202500099

Meihua Zhao, Zhuo Li, Jianfa Chen, Danyu Guo, Zhongfen Nie, Ruiqi Fang, Yingwei Li

引用次数: 0