Faraday Discussions最新文献_第8页

Hydrogen ionic conductors and ammonia conversions 氢离子导体和氨转化

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-02-10 DOI: 10.1039/D3FD00012E

John T. S. Irvine, Stephy Wilson, Sujitra Amnuaypanich, Gavin J. Irvine, Maarten C. Verbraeken, Kamil Nowicki and George M. Carins

引用次数: 1

Structural modifications to platinum(ii) pincer complexes resulting in changes in their vapochromic and solvatochromic properties† 铂螯合物的结构修饰导致其气相变色和溶剂变色性质的变化

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-02-09 DOI: 10.1039/D3FD00025G

Mathew J. Bryant, Sara Fuertes, Lauren E. Hatcher, Lynne H. Thomas and Paul R. Raithby

{"title":"Structural modifications to platinum(ii) pincer complexes resulting in changes in their vapochromic and solvatochromic properties†","authors":"Mathew J. Bryant, Sara Fuertes, Lauren E. Hatcher, Lynne H. Thomas and Paul R. Raithby","doi":"10.1039/D3FD00025G","DOIUrl":"https://doi.org/10.1039/D3FD00025G","url":null,"abstract":"There is a need to develop rapidly responsive chemical sensors for the detection of low concentrations of volatile organic solvents (VOCs). Platinum pincer complexes have shown promise as sensors because of their colours and vapochromic and solvatochromic properties, that may be related to the non-covalent interactions between the pincer complexes and the guest VOCs. Here we report an investigation into a series of Pt(II) complexes based on the 1,3-di(pyridine)benzene tridentate (N⁁C⁁N) skeleton with the formula [Pt(N⁁C(R)⁁N)(CN)] (R = C(O)Me 2, C(O)OEt 3, C(O)OPh 4) with the fourth coordination site occupied by a cyanide ligand. Solid-state samples of the complexes have been tested with a range of volatiles including methanol, ethanol, acetone, dichloromethane and water, and while 2 displays thermochromism, 3 and 4 display rapidly reversible vapochromism and solvatochromism. These results are correlated with X-ray powder and single crystal X-ray structural data including an assessment of the crystal packing and the void space in the crystalline space. The cyanide ligand and the R substituents are involved in hydrogen bonding that creates the voids within the structures and interact with the solvent molecules that influence the Pt⋯Pt separation in the crystalline state.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"244 ","pages":" 411-433"},"PeriodicalIF":3.4,"publicationDate":"2023-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/fd/d3fd00025g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3936052","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

Electrochemical experiments define potentials associated with binding of substrates and inhibitors to nitrogenase MoFe protein† 电化学实验确定了底物和抑制剂与氮酶MoFe蛋白†结合的电位

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-02-06 DOI: 10.1039/D2FD00170E

Ting Chen, Philip A. Ash, Lance C. Seefeldt and Kylie A. Vincent

{"title":"Electrochemical experiments define potentials associated with binding of substrates and inhibitors to nitrogenase MoFe protein†","authors":"Ting Chen, Philip A. Ash, Lance C. Seefeldt and Kylie A. Vincent","doi":"10.1039/D2FD00170E","DOIUrl":"https://doi.org/10.1039/D2FD00170E","url":null,"abstract":"Nitrogenases catalyse the 6-electron reduction of dinitrogen to ammonia, passing through a series of redox and protonation levels during catalytic substrate reduction. The molybdenum–iron nitrogenase is the most well-studied, but redox potentials associated with proton-coupled transformations between the redox levels of the catalytic MoFe protein have proved difficult to pin down, in part due to a complex electron-transfer pathway from the partner Fe protein, linked to ATP-hydrolysis. Here, we apply electrochemical control to the MoFe protein of Azotobacter vinelandii nitrogenase, using europium(III/II)-ligand couples as low potential redox mediators. We combine insight from the electrochemical current response with data from gas chromatography and in situ infrared spectroscopy, in order to define potentials for the binding of a series of inhibitors (carbon monoxide, methyl isocyanide) to the metallo-catalytic site of the MoFe protein, and the onset of catalytic transformation of alternative substrates (protons and acetylene) by the enzyme. Thus, we associate potentials with the redox levels for inhibition and catalysis by nitrogenase, with relevance to the elusive mechanism of biological nitrogen fixation.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"243 ","pages":" 270-286"},"PeriodicalIF":3.4,"publicationDate":"2023-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/fd/d2fd00170e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3936039","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

Correction: In situ study of the evolution of FeNi nanocatalysts in reductive and oxidative environments upon thermal treatments 更正:原位研究FeNi纳米催化剂在还原和氧化环境下热处理的演变

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-31

引用次数: 0

Correction: Interplay between interdiffusion and shape transformations in nanoalloys evolving from core–shell to intermixed structures 更正:纳米合金从核-壳结构到混合结构的相互扩散和形状转变之间的相互作用

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-31

引用次数: 0

List of participants 参会人员名单

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-31

引用次数: 0

Poster list 海报列表

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-31

引用次数: 0

Catalytic templated length-controlled oligomerization 催化模板长度控制寡聚化

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-30 DOI: 10.1039/D3FD00002H

Bartosz Lewandowski, Rebecca J. B. Schäfer, Etienne Cotter, Dora Harangozo and Helma Wennemers

引用次数: 0

Recent advances in plasma-enabled ammonia synthesis: state-of-the-art, challenges, and outlook 等离子体氨合成的最新进展:现状、挑战和展望

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-30 DOI: 10.1039/D3FD00006K

Xin Zeng, Shuai Zhang, Xiucui Hu, Cheng Zhang, Kostya (Ken) Ostrikov and Tao Shao

{"title":"Recent advances in plasma-enabled ammonia synthesis: state-of-the-art, challenges, and outlook","authors":"Xin Zeng, Shuai Zhang, Xiucui Hu, Cheng Zhang, Kostya (Ken) Ostrikov and Tao Shao","doi":"10.1039/D3FD00006K","DOIUrl":"https://doi.org/10.1039/D3FD00006K","url":null,"abstract":"With the increase in the greenhouse effect and reduction of fossil fuel resources, it is urgent to find a feasible solution to directly convert power to chemicals using renewable energy and achieving zero carbon emissions targets. It is necessary to convert renewable energy (i.e., solar, wind, water, etc.) into electrical power replacing fossil-fuel-fired power. Therefore, the power-to-chemicals approach is gaining more and more attention. In the past two decades, non-thermal plasma, electro-catalysis, photo-catalysis, and their hybrid approaches have shown great potential for the power-to-chemicals solution. This paper introduces the application of plasma technology in energy conversion, focusing on three main routes for plasma-enabled ammonia synthesis, and analyses the state-of-the-art. Research results of ammonia synthesis based on plasma technology are discussed. The application of advanced in situ diagnostics evidences the importance of specific intermediate species and reaction pathways. Electrons, vibrationally-excited species, free radicals, and surface-adsorbed species play important roles in plasma-catalytic ammonia synthesis. Combined with experiments and simulations, the mechanisms of plasma-catalytic ammonia synthesis are examined. Vibrationally-excited species can effectively reduce the catalytic surface energy barrier. The techno-economics of the plasma-enabled ammonia synthesis technology is discussed in view of its competitive advantages. It is emphasized that the power-to-chemicals approach can be adapted for most chemical manufacturers, and these methods would play crucial roles in reducing carbon emissions and environmental pollution. Finally, suggestions are provided for the sustainable development of the power-to-chemicals industry in the future.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"243 ","pages":" 473-491"},"PeriodicalIF":3.4,"publicationDate":"2023-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3675838","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 influence of substrate binding on photocatalytic dehalogenation with a heteroleptic supramolecular [M4La2Lb2] square containing PDI photosensitizers as ligands† 用含PDI光敏剂的异亲超分子[M4La2Lb2]方阵探讨底物结合对光催化脱卤的影响

IF 3.4 3区化学

Faraday Discussions Pub Date : 2023-01-19 DOI: 10.1039/D2FD00179A

C. Jasslie Nielsen, Petrus C. M. Laan, Raoul Plessius, Joost N. H. Reek, Jarl Ivar van der Vlugt and Sonja Pullen

{"title":"Probing the influence of substrate binding on photocatalytic dehalogenation with a heteroleptic supramolecular [M4La2Lb2] square containing PDI photosensitizers as ligands†","authors":"C. Jasslie Nielsen, Petrus C. M. Laan, Raoul Plessius, Joost N. H. Reek, Jarl Ivar van der Vlugt and Sonja Pullen","doi":"10.1039/D2FD00179A","DOIUrl":"https://doi.org/10.1039/D2FD00179A","url":null,"abstract":"Photoredox catalysis is a valuable tool in a large variety of chemical reactions. Main challenges still to be overcome are photodegradation of photocatalysts and substrates, short lifetimes of reactive intermediates, and selectivity issues due to unwanted side reactions. A potential solution to these challenges is the pre-organization of the photosensitizer, substrate and (co)-catalyst in supramolecular self-assembled structures. In such architectures, (organic) dyes can be stabilized, and higher selectivity could potentially be achieved through pre-organizing desired reaction partners via non-covalent interactions. Perylene diimide (PDI) is an organic dye, which can be readily reduced to its mono- and dianion. Excitation of both anions leads to highly reducing excited states, which are able to reduce a variety of substrates via single electron transfer. The incorporation of PDI into a heteroleptic [M4La2Lb2] supramolecular square has been recently demonstrated. Herein we investigate its photophysical properties and demonstrate that incorporated PDI indeed features photocatalytic activity. Initial results suggest that the pre-organisation by binding positively affects the outcome.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"244 ","pages":" 199-209"},"PeriodicalIF":3.4,"publicationDate":"2023-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/fd/d2fd00179a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3693586","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