Dalton Transactions最新文献

Mechanistic insights into nitric oxide generation from nitrite via O-atom transfer in the unsymmetrical ꞵ-diketiminato copper(II) nitrite complex 亚硝酸铜（II）不对称ꞵ-二酮体亚硝酸铜（II）络合物中通过 O 原子转移从亚硝酸盐生成一氧化氮的机理探究

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt02359e

Yi-Rong Hsiang, Naorem Jemes Meitei, Gifta Evangeline Henry, Sodio C. N. Hsu, Ya-Fan Lin

{"title":"Mechanistic insights into nitric oxide generation from nitrite via O-atom transfer in the unsymmetrical ꞵ-diketiminato copper(II) nitrite complex","authors":"Yi-Rong Hsiang, Naorem Jemes Meitei, Gifta Evangeline Henry, Sodio C. N. Hsu, Ya-Fan Lin","doi":"10.1039/d4dt02359e","DOIUrl":"https://doi.org/10.1039/d4dt02359e","url":null,"abstract":"In this study, we employed DFT calculations to elucidate the mechanism of NO generation from nitrite via PPh3-induced oxygen atom transfer (OAT) in the unsymmetrical ß-diketiminato copper(II), LCuIIONO. We discovered that the OAT process involves the cooperation of the two PPh3 and follows the mechanism distinct from that of the symmetrical ß-diketiminato analogue. The ΔG‡ value, calculated to be 34.8 kcal/mol, closely matches experimental data. The finding is further supported by analyzing the OAT product yields with varying equivalents of PPh3. The penta-coordinated species 5a, with PPh3 occupying the axial site, forms in the final stage of the OAT process. The isomerization of 5a and the decoordination of the hemilabile pyridyl arm synergistically reduce Cu(II) to Cu(I), facilitating NO-releasing from the Cu(I) centre. These computational results provide valuable insights for the ligand design of PPh3-induced OAT reactions to produce NO in Cu(II) nitrite systems.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452516","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

DFT-based 11B solid state NMR calculations for guiding fine local structure identification and phase-property modulation in ZnxY1-xBO3-0.5x borate oxide ion conductors 基于 DFT 的 11B 固态核磁共振计算用于指导 ZnxY1-xBO3-0.5x 硼酸盐氧化物离子导体中的精细局部结构识别和相特性调制

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt02339k

Yuan Gou, Xiaohui Li, Xiaoge Wang, Mengjia Zhang, Jinxiao Zhang, Qiang Li, Xianran Xing, Xiaojun Kuang

{"title":"DFT-based 11B solid state NMR calculations for guiding fine local structure identification and phase-property modulation in ZnxY1-xBO3-0.5x borate oxide ion conductors","authors":"Yuan Gou, Xiaohui Li, Xiaoge Wang, Mengjia Zhang, Jinxiao Zhang, Qiang Li, Xianran Xing, Xiaojun Kuang","doi":"10.1039/d4dt02339k","DOIUrl":"https://doi.org/10.1039/d4dt02339k","url":null,"abstract":"Solid-state nuclear magnetic resonance (NMR) spectroscopy serves as a powerful technique for probing local structures. However, the interpretation of NMR signals mainly based on empirical knowledge could lead to unprecise local structural determinations. To address this, density functional theory (DFT)-based theoretical NMR calculations, aided by the experimental three-dimensional continuous rotation electronic diffraction (3D cRED) technique, were performed for ZnxY1-xBO3-0.5x borate oxide ion conductors and provided a fine local structure identification for the experimental 11B NMR spectra of ZnxY1-xBO3-0.5x, acquiring rich information on the multiple experimental 11B NMR signals to the complex boron oxide anions associated with bridging oxygen vacancies and the coexistence of the monoclinic phase (C2/c), hexagonal (P63/m), and trigonal (R32) phases in ZnxY1-xBO3-0.5x. Thanks to the advantages of solid-state NMR in identifying close phases exceeding X-ray/neutron diffraction technique, and the advanced 3D cRED technique that allows for rapid phase identification and structure determination, we provide a fine local structure identification and a more inclusive insight into the coexistence of multiple phases in borate with the same composition, and more importantly, in turn provides guidance for phase and property modulation. The phase modulation in ZnxY1-xBO3-0.5x was carried out in thermodynamic and kinetic, respectively, and eventually realized the modulation of the local structures and the resultant oxide ion conductivity of ZnxY1-xBO3-0.5x. This work provides a theoretical and experimental platform to access the flexible structural assignment of boron oxide anions and therefore offer new guidance and insights into the defect structures and the phase-property modulation of inorganic solid functional materials not only in the borate oxide ion conductors.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452517","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

Monolayers of a Thiacalix[3]pyridine-Supported Molybdenum(0) Tricarbonyl Complex on Au(111): Characterisation with Surface Spectroscopy and Scanning Tunneling Microscopy 金(111)上的硫杂[3]吡啶支持的三羰基钼(0)络合物单层：利用表面光谱和扫描隧道显微镜进行表征

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt02521k

Kai Uwe Clausen, Xiangzhi Meng, Katrin Reisig, Christian Nather, Thomas Strunskus, Richard Berndt, Felix Tuczek

{"title":"Monolayers of a Thiacalix[3]pyridine-Supported Molybdenum(0) Tricarbonyl Complex on Au(111): Characterisation with Surface Spectroscopy and Scanning Tunneling Microscopy","authors":"Kai Uwe Clausen, Xiangzhi Meng, Katrin Reisig, Christian Nather, Thomas Strunskus, Richard Berndt, Felix Tuczek","doi":"10.1039/d4dt02521k","DOIUrl":"https://doi.org/10.1039/d4dt02521k","url":null,"abstract":"Deposition of dome-shaped metal-organic complexes on metallic surfaces to produce well-defined single site catalysts is a novel approach combining aspects of homogeneous and heterogeneous catalysis. In order to investigate the bonding of small molecules to such systems, a molybdenum(0) tricarbonyl complex supported by a thiacalix[3]pyridine is synthesized and deposited on Au(111) and Ag(111) surfaces by vacuum evaporation. The resulting mono- and submonolayers are investigated with surface spectroscopy and STM. All of these methods indicate a parallel orientation of the molybdenum complex with respect to the surface. The vibrational properties and frequency shifts of the adsorbed complexes with respect to the bulk are evaluated with the help of conventional IR and IRRA spectroscopy, coupled to DFT calculations. Compared to a similar Mo(0) tricarbonyl complex supported by an azacalixpyridine ligand, the title complex exhibits a higher stability in the bulk and adsorbed to surfaces which goes along with a lower reactivity towards oxygen.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452513","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

Enhancing CO2 Reduction Efficiency through Electrolyte Immersion in Hierarchical Bismuth-Nickel Catalysts 通过电解质浸入分层铋镍催化剂提高二氧化碳还原效率

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt02441a

Yongsu An, Yongju Lee, Yujing Ji, Young Dok Kim, Hyun Ook Seo, Duk-Young Jung

{"title":"Enhancing CO2 Reduction Efficiency through Electrolyte Immersion in Hierarchical Bismuth-Nickel Catalysts","authors":"Yongsu An, Yongju Lee, Yujing Ji, Young Dok Kim, Hyun Ook Seo, Duk-Young Jung","doi":"10.1039/d4dt02441a","DOIUrl":"https://doi.org/10.1039/d4dt02441a","url":null,"abstract":"Nanostructures are critical to improve contact area with an electrolyte and catalytic efficiency for the CO2 reduction reaction (CO2RR). However, their hydrophobicity conflicts with the intended increase in contact area and complicates determination of active contact area. Here, bismuth-nickel (BiNi) micro-nano hierarchical catalysts for CO2RR were studied to understand the effects of electrolyte-catalyst contact area variation with immersion duration in an aqueous electrolyte. The immersed BiNi samples showed about 13.4-fold higher formate production compared to the pristine BiNi sample. The 2-day pre-immersed BiNi sample exhibited Faradaic efficiencies (FE%) of ~80.1% for formate and ~10% for H2 with a current density of 10.2 mA cm-2 at -1.5 V vs. Ag/AgCl. In contrast, the pristine BiNi catalysts exhibited an FE% of ~12.9% for formate and ~76.3% for H2 with a current density of 5.38 mA cm-2. Our experimental results reveal that improved contact between the electrolyte and catalyst surface through pre-immersion can lead to enhanced CO2RR efficiency of formate production in hierarchical BiNi catalysts.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452515","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

Introduce 1D rGO nanoribbons as spacers between 2D MXene for high performance electrode of supercapacitor 引入一维 rGO 纳米带作为二维 MXene 之间的间隔，用于制造高性能超级电容器电极

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt02127d

Xiaolong Lu, Yan Zhou, Cancan Li, Qi Wang, Bijun Fang, Yi Shi, Ningyi Yuan, Jian Ning Ding

{"title":"Introduce 1D rGO nanoribbons as spacers between 2D MXene for high performance electrode of supercapacitor","authors":"Xiaolong Lu, Yan Zhou, Cancan Li, Qi Wang, Bijun Fang, Yi Shi, Ningyi Yuan, Jian Ning Ding","doi":"10.1039/d4dt02127d","DOIUrl":"https://doi.org/10.1039/d4dt02127d","url":null,"abstract":"Two-dimension (2D) transition metal carbide Ti3C2TX (MXene) possesses good electrical conductivity, high specific surface areas and metal oxide-like surfaces, which make it ideal for application in supercapacitors with both high energy density and power density. However, similar to other 2D materials, the issue of self-stacking leads to narrower ion transport channels, along with a drastic reduction of active sites, severe limiting the performance of MXene-based electrodes. To address this problem, this work proposes to introduce one-dimension (1D) reduced graphene oxide (rGO) nanoribbons as spacers between MXene nanosheets to construct composite structure for inhibiting the self-stacking. As expected, thanks to the steric effect and high aspect ratio of rGO nanoribbons, the fabricated MXene/rGO hybrid electrode with addition of 5 wt% graphene oxide (GO) exhibits a greatly improved specific capacitance (397.4 F g−1 at 5 mV s−1) and an unparalleled rate capability (with a capacitance retention of 52.9% at 2000 mV s−1). This work significantly shed light to develop MXene-based materials for advanced energy storage devices.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452514","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

Modulating Magnetic Anisotropy in Linear Tetranuclear Dysprosium(III) Complexes via Coordinated Anions 通过配位阴离子调节线性四核镝(III)配合物的磁各向异性

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt01949k

Guan-Lin Lu, Shih-Ting Chiu, Po-Heng Lin, Jérôme Long

引用次数: 0

Light Switchable Ir(III)-Based Photosensitizers: A Dual-State System for Non-Invasive, Reversible ROS Control in Tumor Therapy 光可转换铱(III)基光敏剂：在肿瘤治疗中实现非侵入性、可逆 ROS 控制的双态系统

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-22 DOI: 10.1039/d4dt02673j

Zhi-Tong Chu, Na Xu, Yan Su, Hongbao Fang, Zhi Su

{"title":"Light Switchable Ir(III)-Based Photosensitizers: A Dual-State System for Non-Invasive, Reversible ROS Control in Tumor Therapy","authors":"Zhi-Tong Chu, Na Xu, Yan Su, Hongbao Fang, Zhi Su","doi":"10.1039/d4dt02673j","DOIUrl":"https://doi.org/10.1039/d4dt02673j","url":null,"abstract":"Photodynamic therapy (PDT), a powerful anticancer approach converting oxygen to ROS for tumor ablation, encounters hurdles like limited spatio-temporal selectivity, and the consequent unnecessary damage to normal tissues. Addressing these challenges, developing controllable Ir(III)-based photosensitizers (PSs) emerges as a promising solution, offering enhanced efficacy and precision in cancer therapy, while propelling the clinical progression of metal-based PSs. Herein, we proposed a series of light-controlled PSs, integrating Ir(III)-based moiety with a light-responsive module, enabling non-invasive \"off-on\" control of ROS production via efficient energy transfer. The open form (OF) in this dual-state system has better lipid solubility and cellular uptake compared to the closed form (CF), which facilitates targeted delivery of metal drugs. Comprehensive intracellular experiments demonstrated the OF complex's superior cytotoxicity under light irradiation, with the CF complex achieving comparable toxicity post-conversion. Notably, the PSs inhibited 3D tumor growth and modulated intracellular ROS production. These findings underscore the potential of Ir(III)-based dual-state photoswitchable complexes as a platform for non-invasive, reversible ROS control, offering broad prospects in tumor therapy and beyond.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452310","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 acidity-triggered aggregation nanoplatform based on degradable mesoporous organosilica nanoparticles for precise drug delivery and phototherapy of focal bacterial infection 基于可降解介孔有机硅纳米颗粒的酸性触发聚合纳米平台，用于精确给药和病灶细菌感染的光疗

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-21 DOI: 10.1039/d4dt02111h

Yunhan Huang, Wei Guo, Xinyu Wang, Jingrui Chang, Bo Lu

引用次数: 0

High-performance electromagnetic wave absorption in FeS2/SnS2@multi-walled carbon nanotube composites with honeycomb-shaped structure 具有蜂窝状结构的 FeS2/SnS2@ 多壁碳纳米管复合材料的高性能电磁波吸收能力

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-21 DOI: 10.1039/d4dt02335h

Weiao Kong, Xianhan Lin, Chuanhe Wang, Gen Li, Zhiqiang Xue, Shoubing Wang, Yani Zhang, Zhidong Liu, Huanian Zhang, Min Zhang, Wei Ding, Liping Guo, Shugang Tan

引用次数: 0

Construction of a homologous bimetallic oxide Bi2Fe4O9@Bi25FeO40 heterostructure to boost supercapacitor performance 构建同源双金属氧化物 Bi2Fe4O9@Bi25FeO40 异质结构以提高超级电容器性能

IF 4 3区化学

Dalton Transactions Pub Date : 2024-10-21 DOI: 10.1039/d4dt02585g

Bingjie Cheng, Xiaoqiang Li, Ruqu Han, Jun Xiang, Yamei Zhang

{"title":"Construction of a homologous bimetallic oxide Bi2Fe4O9@Bi25FeO40 heterostructure to boost supercapacitor performance","authors":"Bingjie Cheng, Xiaoqiang Li, Ruqu Han, Jun Xiang, Yamei Zhang","doi":"10.1039/d4dt02585g","DOIUrl":"https://doi.org/10.1039/d4dt02585g","url":null,"abstract":"Herein, a Bi2Fe4O9@Bi25FeO40 heterostructure with a high specific surface area of 30.07 m2 g−1 and abundant heterogeneous interfaces was successfully fabricated and applied to supercapacitors for the first time. The Bi2Fe4O9@Bi25FeO40 electrode exhibits a high specific capacity (550.8 F g−1 at 1.0 A g−1) and good cycling stability (75% capacitance retention and 92.3% coulombic efficiency after 3000 cycles at 5.0 A g−1), significantly outperforming the pure Bi2Fe4O9 or Bi25FeO40 electrode. This work proposes an effective interfacial engineering strategy to enhance supercapacitor performance.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":4.0,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452348","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