Faraday Discussions最新文献

{"title":"Poster list","authors":"","doi":"10.1039/d3fd90023a","DOIUrl":"https://doi.org/10.1039/d3fd90023a","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"10 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136079473","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}

{"title":"List of participants","authors":"","doi":"10.1039/d3fd90022c","DOIUrl":"https://doi.org/10.1039/d3fd90022c","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"293 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136079472","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}

{"title":"Poster list","authors":"","doi":"10.1039/d3fd90043f","DOIUrl":"https://doi.org/10.1039/d3fd90043f","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"87 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135594669","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}

{"title":"List of participants","authors":"","doi":"10.1039/d3fd90055j","DOIUrl":"https://doi.org/10.1039/d3fd90055j","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"70 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135312819","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}

{"title":"List of participants","authors":"","doi":"10.1039/d3fd90044d","DOIUrl":"https://doi.org/10.1039/d3fd90044d","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"24 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135594522","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}

{"title":"List of participants","authors":"","doi":"10.1039/d3fd90045b","DOIUrl":"https://doi.org/10.1039/d3fd90045b","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"96 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136259911","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}

{"title":"Electrochemical nitrogen reduction reaction over gallium – a computational and experimental study†","authors":"Vivek Sinha, Fateme Rezai, Nihat Ege Sahin, Jacopo Catalano, Espen Drath Bøjesen, Farnaz Sotoodeh and Emil Dražević","doi":"10.1039/D2FD00169A","DOIUrl":"https://doi.org/10.1039/D2FD00169A","url":null,"abstract":"<p >Ga was identified earlier as one of the “overlooked” metals for catalyzing the electrochemical nitrogen reduction reaction (ENRR). We investigate here the electrocatalytic activity of Ga towards the nitrogen reduction reaction. We used a combination of molecular modelling and simulations using periodic density functional theory calculations (DFT), and experimental ENRR measurements. The ENRR was found to proceed <em>via</em> an associative mechanism where the first PCET to dinitrogen forming the surface adsorbed N<small>₂</small>H* species is the overpotential limiting step. The bare Ga cathode has a high overpotential (&gt;2 V (SHE)) for the ENRR. We also investigated the effect of a water-in-salt electrolyte (WISE) on the rate of ammonia formation. The addition of an Li salt lowers the overpotential to 1.88 V (SHE). DFT calculations revealed that the H-adatom was more favorably bound than the N-adatom, and the hydrogen evolution reaction (HER) is expected to dominate at high cathodic potentials. Experimental ENRR tests corroborate our results wherein no significant NH<small>₃</small> formation was detected. The low electrochemical activity of Ga is attributed to poor binding and activation of N<small>₂</small> which originates from an electropositive surface charge distribution.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"243 ","pages":" 307-320"},"PeriodicalIF":3.4,"publicationDate":"2022-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/fd/d2fd00169a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3936047","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}

{"title":"Uncovering the role of non-covalent interactions in solid-state photoswitches by non-spherical structure refinements with NoSpherA2†","authors":"Lauren E. Hatcher, Lucy K. Saunders and Ben A. Coulson","doi":"10.1039/D2FD00158F","DOIUrl":"https://doi.org/10.1039/D2FD00158F","url":null,"abstract":"<p >We present a charge density study of two linkage isomer photoswitches, [Pd(Bu<small>₄</small>dien)(NO<small>₂</small>)]BPh<small>₄</small>·THF (<strong>1</strong>) and [Ni(Et<small>₄</small>dien)(NO<small>₂</small>)<small>₂</small>] (<strong>2</strong>) using Hirshfeld Atom Refinement (HAR) methods implemented <em>via</em> the NoSpherA2 interface in Olex2. HAR is used to explore the electron density distribution in the photoswitchable molecules of <strong>1</strong> and <strong>2</strong>, to gain an in-depth understanding of key bonding features and their influence on the single-crystal-to-single-crystal reaction. HAR analysis is also combined with <em>ab initio</em> calculations to explore the non-covalent interactions that influence physical properties of the photoswitches, such as the stability of the excited state nitrito-(<em>η</em><small>¹</small>-ONO) isomer. This insight can be fed back into the crystal engineering process to develop new and improved photoswitches that can be optimised towards specific applications.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"244 ","pages":" 370-390"},"PeriodicalIF":3.4,"publicationDate":"2022-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/fd/d2fd00158f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3694292","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}

{"title":"Nanoalloy magnetic and optical properties, applications and structures: general discussion","authors":"Christine M. Aikens, Damien Alloyeau, Vincenzo Amendola, Catherine Amiens, Pascal Andreazza, Joost M. Bakker, Francesca Baletto, Stephan Barcikowski, Noelia Barrabés, Michael Bowker, Fuyi Chen, Isaac T. Daniel, Wolfgang E. Ernst, Riccardo Ferrando, Piero Ferrari, Alessandro Fortunelli, Didier Grandjean, Hazar Guesmi, Graham J. Hutchings, Ewald Janssens, Robert M. Jones, Miguel Jose Yacaman, Christian Kuttner, Maria J. Lopez, Éric Marceau, Marcelo M. Mariscal, John McGrady, Christine Mottet, Jaysen Nelayah, Cameron J. Owen, Micha Polak, Jonathan Quinson, Cesare Roncaglia, Rolf Schäfer, Rasmus Svensson, Mona Treguer-Delapierre and Yufei Zhang","doi":"10.1039/D2FD90087D","DOIUrl":"https://doi.org/10.1039/D2FD90087D","url":null,"abstract":"","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"242 ","pages":" 389-417"},"PeriodicalIF":3.4,"publicationDate":"2022-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3693574","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}

{"title":"On the mechanism of intermolecular nitrogen-atom transfer from a lattice-isolated diruthenium nitride intermediate†","authors":"Mario N. Cosio, Waad S. Alharbi, Aishanee Sur, Chen-Hao Wang, Ahmad Najafian, Thomas R. Cundari and David C. Powers","doi":"10.1039/D2FD00167E","DOIUrl":"https://doi.org/10.1039/D2FD00167E","url":null,"abstract":"<p >Catalyst confinement within microporous media provides the opportunity to site isolate reactive intermediates, enforce intermolecular functionalization chemistry by co-localizing reactive intermediates and substrates in molecular-scale interstices, and harness non-covalent host–guest interactions to achieve selectivities that are complementary to those accessible in solution. As part of an ongoing program to develop synthetically useful nitrogen-atom transfer (NAT) catalysts, we have demonstrated intermolecular benzylic amination of toluene at a Ru<small>₂</small> nitride intermediate confined within the interstices of a Ru<small>₂</small>-based metal–organic framework (MOF), Ru<small>₃</small>(btc)<small>₂</small>X<small>₃</small> (btc = 1,3,5-benzenetricarboxylate, <em>i.e.</em>, Ru-HKUST-1 for X = Cl). Nitride confinement within the extended MOF lattice enabled intermolecular C–H functionalization of benzylic C–H bonds in preference to nitride dimerization, which was encountered with soluble molecular analogues. Detailed study of the kinetic isotope effects (KIEs, <em>i.e.</em>, <em>k</em><small>_H</small>/<em>k</em><small>_D</small>) of C–H amination, assayed both as intramolecular effects using partially labeled toluene and as intermolecular effects using a mixture of per-labeled and unlabeled toluene, provided evidence for restricted substrate mobility on the time scale of interstitial NAT. Analysis of these KIEs as a function of material mesoporosity provided approximate experimental values for functionalization in the absence of mass transport barriers. Here, we disclose a combined experimental and computational investigation of the mechanism of NAT from a Ru<small>₂</small> nitride to the C–H bond of toluene. Computed kinetic isotope effects for a H-atom abstraction (HAA)/radical rebound (RR) mechanism are in good agreement with experimental data obtained for C–H amination at the rapid diffusion limit. These results provide the first detailed analysis of the mechanism of intermolecular NAT to a C–H bond, bolster the use of KIEs as a probe of confinement effects on NAT within MOF lattices, and provide mechanistic insights unavailable by experiment because rate-determining mass transport obscured the underlying chemical kinetics.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":"244 ","pages":" 154-168"},"PeriodicalIF":3.4,"publicationDate":"2022-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3666725","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}