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A Computational Outlook on Ascertaining the Reactivity of Transition Metal-Based Olefin Metathesis Catalysts 确定过渡金属基烯烃复分解催化剂反应活性的计算展望
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-28 Epub Date: 2026-09-07 DOI: 10.1021/acs.organomet.6c00210
Rama Padavettan, Arun Ramamurthy, Vikiho Wotsa, Deepa Masilamani, Chinnappan Sivasankar
{"title":"A Computational Outlook on Ascertaining the Reactivity of Transition Metal-Based Olefin Metathesis Catalysts","authors":"Rama Padavettan,&nbsp;Arun Ramamurthy,&nbsp;Vikiho Wotsa,&nbsp;Deepa Masilamani,&nbsp;Chinnappan Sivasankar","doi":"10.1021/acs.organomet.6c00210","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00210","url":null,"abstract":"<p>Densityfunctional theory (DFT) calculations were performed toevaluate the relative efficiencies of Nb-, Mo-, and W-based Schrock-typealkylidene complexes (<strong>1</strong>–<strong>11</strong>) in olefinmetathesis. The study reveals that catalytic efficiency is stronglygoverned by the electrostatic nature of the M–C bond. A largerelectrostatic contribution imparts greater ionic and polarizable characterto the metal–carbene interaction, facilitating electron redistributionduring olefin coordination and promoting efficient metallacyclobutaneformation in the Chauvin mechanism. W-based complexes, particularly(<strong>7</strong>), (<strong>9</strong>), and (<strong>11</strong>), exhibitshorter M–C bonds, higher ν(M–C) frequencies,larger WBIs, and stronger orbital stabilization, indicating highlystabilized and more covalent metal–carbene interactions. Incontrast, Mo complex (<strong>1</strong>) shows a larger electrostaticcontribution, longer M–C bond distance, smaller charge separation,lower WBI, and lower steric congestion, indicating a more ionic andreadily polarizable Mo–C interaction favorable for catalyticturnover. EDA, %VBur, and mechanistic analyses further demonstratethat although W complex (<strong>11</strong>) is thermodynamically morestable, its greater covalent stabilization and steric congestion reducecatalytic efficiency, whereas Mo complex (<strong>1</strong>) exhibitsmore favorable energetics for four-membered TS formation and is themost catalytically efficient system among the complexes studied herein,in accordance with experimental reports.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 18","pages":"2209–2228"},"PeriodicalIF":2.4,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067504","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
Flash Communication: Exploring the Coordination of π-Acids and Redox-Active Diatomics to a High-Spin and Highly Fluorinated Ferrous Compound 闪光通讯：探索π-酸与氧化还原活性双原子在高自旋高氟亚铁化合物中的配位
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-28 Epub Date: 2026-09-08 DOI: 10.1021/acs.organomet.6c00262
Morgan Hern, Christopher D. Hastings, Justin Q. Hao, William W. Brennessel, Brandon R. Barnett
{"title":"Flash Communication: Exploring the Coordination of π-Acids and Redox-Active Diatomics to a High-Spin and Highly Fluorinated Ferrous Compound","authors":"Morgan Hern,&nbsp;Christopher D. Hastings,&nbsp;Justin Q. Hao,&nbsp;William W. Brennessel,&nbsp;Brandon R. Barnett","doi":"10.1021/acs.organomet.6c00262","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00262","url":null,"abstract":"<p>A new trigonallysymmetric ligand scaffold is reported from thereaction of tris(2-aminoethyl)amine (TREN) and methyl trifluoroacetate.Deprotonation and metalation with iron(II) yields a trigonal monopyramidalferrate that bears an open coordination site surrounded by C–Fmotifs. The weak-field ligand environment promoted by the fluorinatedamidate donors leads to distinctive behaviors that are apparent inreactions with π-acids such as CO and <em>tert</em>-butylisocyanide.As shown by structural, spectroscopic, and computational studies,the trifluoromethyl substituents lead to an attenuation of π-backbondingcapabilities, while also labilizing the Fe–N<sub>amidate</sub> bonds. While no tractable reactivity with O<sub>2</sub> occurs,the ferrate irreversibly coordinates NO to yield a high-spin {FeNO}<sup>7</sup> complex.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 18","pages":"2190–2194"},"PeriodicalIF":2.4,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067562","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
Hydroboration of Alkynes Catalyzed by Fe(II) PCP Pincer Complexes Fe(II) PCP钳形配合物催化炔的硼氢化反应
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-28 Epub Date: 2026-09-14 DOI: 10.1021/acs.organomet.6c00268
Matthias Käfer, Luis F. Veiros, Karl Kirchner
{"title":"Hydroboration of Alkynes Catalyzed by Fe(II) PCP Pincer Complexes","authors":"Matthias Käfer,&nbsp;Luis F. Veiros,&nbsp;Karl Kirchner","doi":"10.1021/acs.organomet.6c00268","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00268","url":null,"abstract":"<p>A stereo- and regioselective Fe(II)-catalyzed hydroborationofboth terminal and internal alkynes with pinacolborane (HBpin) is described.The hydroboration reaction is in all cases highly <em>syn</em>-selective. The reaction requires no additives and proceeds witha catalyst loading of 1–2 mol % at 45–55 °C. Anactive pre-catalyst is the bench-stable alkyl Fe(II) complex [Fe(PCP<sup>CH2</sup>-<em>i</em>Pr)(CH<sub>2</sub>CH<sub>2</sub>CH<sub>3</sub>)(CO)<sub>2</sub>]. This complex reacts with an excess ofHBpin to form the Fe(II) pinacolborane complex [Fe(PCP<sup>CH2</sup>-<em>i</em>Pr)(κ<sup>2</sup>-H<sub>2</sub>BPin)(CO)],which is an equally active pre-catalyst but more difficult to handle,as it decomposes in the absence of substrates. Both pre-catalystsafford the highly reactive hydride catalyst [Fe(PCP<sup>CH2</sup>-<em>i</em>Pr)(H)(CO)] under catalytic conditions. A broad varietyof aromatic and aliphatic alkynes were efficiently and selectivelyborylated. Mechanistic insights are provided based on experimentaldata and DFT calculations.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 18","pages":"2195–2198"},"PeriodicalIF":2.4,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067616","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
Flash Communication: Siloxides Promote the Iron-Catalyzed Borylation of Aryl Chlorides 闪光通讯：硅氧化物促进铁催化芳基氯化物的硼化反应
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 Epub Date: 2026-08-14 DOI: 10.1021/acs.organomet.6c00235
Patrick Daly-Dee, Luke Davies, Graham J. Tizzard, Simon J. Coles, Sebastien Monfette, Robin B. Bedford
{"title":"Flash Communication: Siloxides Promote the Iron-Catalyzed Borylation of Aryl Chlorides","authors":"Patrick Daly-Dee,&nbsp;Luke Davies,&nbsp;Graham J. Tizzard,&nbsp;Simon J. Coles,&nbsp;Sebastien Monfette,&nbsp;Robin B. Bedford","doi":"10.1021/acs.organomet.6c00235","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00235","url":null,"abstract":"<p>In contrast to alkoxidesalts, siloxide salts MOSiR<sub>3</sub> (M = Na, Li) can be used togood effect as activators for B<sub>2</sub>pin<sub>2</sub> in theiron-catalyzed borylation of aryl chloridesubstrates, in many cases giving results comparable to or better thanthose obtained previously with highly pyrophoric <em><sup>t</sup></em>BuLi acting as an activator. Preliminary mechanistic investigationsreveal a protracted induction period, most likely associated withprecatalyst reduction, and these also suggest that the NaOSi<em><sup>t</sup></em>BuMe-activated B<sub>2</sub>pin<sub>2</sub> isnot as reducing as the equivalent <em><sup>t</sup></em>BuLi-activatedspecies.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2083–2087"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958051","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 and Characterization of Spirofluorene Xanthene-Functionalized Platinum(II) Complexes with Bispyrazolyl Borate Ligands 含双吡唑硼酸酯配体的螺芴杂蒽功能化铂（II）配合物的合成与表征
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 Epub Date: 2026-08-26 DOI: 10.1021/acs.organomet.6c00211
Tim Riesebeck, Róbert Gyepes, Thomas Strassner
{"title":"Synthesis and Characterization of Spirofluorene Xanthene-Functionalized Platinum(II) Complexes with Bispyrazolyl Borate Ligands","authors":"Tim Riesebeck,&nbsp;Róbert Gyepes,&nbsp;Thomas Strassner","doi":"10.1021/acs.organomet.6c00211","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00211","url":null,"abstract":"<p>We report the synthesis and photophysical characterizationof twospirofluorene xanthene-functionalized benzimidazolylidene platinum(II)complexes with bis(3-methylpyrazolyl)borate and bis(3-trifluoromethylpyrazolyl)borateauxiliary ligands. Both complexes were synthesized from a μ-chloro-bridgedbimetallic intermediate in 40% and 72% yields. Photophysical investigationsrevealed green-blue emission with CIE coordinates of (0.16; 0.23)and (0.17; 0.27), and photoluminescence quantum yields of 63% and58%.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2159–2164"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958071","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
Revisiting the Bench Stability of B2pin2 重新审视B2pin2的台架稳定性
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 Epub Date: 2026-07-16 DOI: 10.1021/acs.organomet.6c00167
Wesley D. Hatcher, Vanaparthi Satheesh, Michael C. Young, Erik A. Romero
{"title":"Revisiting the Bench Stability of B2pin2","authors":"Wesley D. Hatcher,&nbsp;Vanaparthi Satheesh,&nbsp;Michael C. Young,&nbsp;Erik A. Romero","doi":"10.1021/acs.organomet.6c00167","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00167","url":null,"abstract":"<p>Bis(pinacolato)diboron (B<sub>2</sub>pin<sub>2</sub>)is a widelyused diboron reagent for the installation of modular boryl groupsand is generally regarded as bench stable. Here we show that traceimpurities can initiate an autocatalytic process that promotes oxidativedecomposition of B<sub>2</sub>pin<sub>2</sub> in the solid state.Once initiated, this process renders B<sub>2</sub>pin<sub>2</sub> susceptibleto reaction with molecular oxygen and HO–Bpin, leading to degradationof bulk material. Notably, decomposition propagates under closed containerconditions but is suppressed in loosely capped containers, consistentwith the involvement of volatile components in the degradation process.These findings reveal an unexpected vulnerability in a widely usedboron reagent and establish practical guidelines for its storage andhandling.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2069–2073"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958068","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
Flash Communication: Addition of Acid Anhydrides to Monomeric Stibine Oxides 闪光通讯：酸性酸酐加入到单体锑氧化物中
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 Epub Date: 2026-08-19 DOI: 10.1021/acs.organomet.6c00231
Madhu Ayyer, Addis Getahun, Timothy C. Johnstone
{"title":"Flash Communication: Addition of Acid Anhydrides to Monomeric Stibine Oxides","authors":"Madhu Ayyer,&nbsp;Addis Getahun,&nbsp;Timothy C. Johnstone","doi":"10.1021/acs.organomet.6c00231","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00231","url":null,"abstract":"<p>The polarized andunsaturated Sb–O bond of stibine oxidesexhibits a combination of electrophilicity at the antimony atom andnucleophilicity at the oxygen atom. Here, we explore the consequentability of Mes<sub>3</sub>SbO compounds to undergo 1,2-addition chemistrywith carboxylic, sulfonic, and phosphinic acid anhydrides to affordstiboranes of the type Mes<sub>3</sub>SbX<sub>2</sub>. With the bulkierstibine oxide Dipp<sub>3</sub>SbO, reaction with triflic anhydridepermits in situ preparation of Dipp<sub>3</sub>Sb(OTf)<sub>2</sub>, which crystallized as the stibonium triflate salt. This reactivityalso enables the disaggregation of the polymeric stibine oxide (Ph<sub>3</sub>SbO)<sub>n</sub> under mild conditions, providing an alternativesynthetic route to Ph<sub>3</sub>SbX<sub>2</sub> products.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2074–2077"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958040","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
Pioneers and Influencers in Organometallic Chemistry: Prof. Jennifer C. Green, Determining the Electronic Structures of Organometallic Complexes Using a Combination of Experiments and Theory 有机金属化学的先驱和影响者：Jennifer C. Green教授，用实验和理论的结合来确定有机金属配合物的电子结构
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 DOI: 10.1021/acs.organomet.6c00172
Natalie Fey, Nilay Hazari
{"title":"Pioneers and Influencers in Organometallic Chemistry: Prof. Jennifer C. Green, Determining the Electronic Structures of Organometallic Complexes Using a Combination of Experiments and Theory","authors":"Natalie Fey,&nbsp;Nilay Hazari","doi":"10.1021/acs.organomet.6c00172","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00172","url":null,"abstract":"","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2061–2068"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958020","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
Flash Communication: Challenges in the Characterization of a Bisphosphine Nickel Fluoride Complex 闪光通信：表征二膦氟化镍配合物的挑战
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 Epub Date: 2026-09-01 DOI: 10.1021/acs.organomet.6c00218
Josie B. Rojo, Aurora F. Wilson, David A. Vicic
{"title":"Flash Communication: Challenges in the Characterization of a Bisphosphine Nickel Fluoride Complex","authors":"Josie B. Rojo,&nbsp;Aurora F. Wilson,&nbsp;David A. Vicic","doi":"10.1021/acs.organomet.6c00218","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00218","url":null,"abstract":"<p>A prior report (<em>Inorg. Chim. Acta</em> <strong>2011</strong>, 376, 118–122)detailed the use of “[Ni(THF)<sub>6</sub>][(BF<sub>4</sub>)<sub>2</sub>]” to prepare [(dtbe)Ni(μ-F)]<sub>2</sub>[BF<sub>4</sub>]<sub>2</sub> (dtbe = 1,2-bis(di-<em>tert</em>-butylphosphino)ethane)using a DCM/THF (1:1) solvent system. Herewe describe a procedure that affords [Ni(THF)<sub>4</sub>(BF<sub>4</sub>)<sub>2</sub>] in the solid-state, and note that reaction of [Ni(THF)<sub>4</sub>(BF<sub>4</sub>)<sub>2</sub>] with the similar phosphine dcpe(dcpe = 1,2-bis(dicyclohexylphosphino)ethane) only produces [(dcpe)Ni(μ-F)]<sub>2</sub>[BF<sub>4</sub>]<sub>2</sub> when run in thoroughly driedTHF solvent. If a 1:1 mixture of DCM/THF solvents is used as previouslydescribed, the bridging chloride derivative [(dcpe)Ni(μ-Cl)]<sub>2</sub>[BF<sub>4</sub>]<sub>2</sub> is formed. Moreover, we showthat bridging fluorides of [(dcpe)Ni(μ-F)]<sub>2</sub>[BF<sub>4</sub>]<sub>2</sub> can be short-lived in solution, reacting withthe medium to produce unexpected products.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2088–2090"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958055","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
Silent Neighbors? Dissecting Borane–Carbonyl Interactions at Nickel–Oxirane Models 沉默的邻居?在镍-氧环模型中解剖硼烷-羰基相互作用
IF 2.4 3区 化学
Organometallics Pub Date : 2026-09-14 Epub Date: 2026-08-19 DOI: 10.1021/acs.organomet.6c00225
Brady J. H. Austen, A. Dina Dilinaer, Marcus W. Drover
{"title":"Silent Neighbors? Dissecting Borane–Carbonyl Interactions at Nickel–Oxirane Models","authors":"Brady J. H. Austen,&nbsp;A. Dina Dilinaer,&nbsp;Marcus W. Drover","doi":"10.1021/acs.organomet.6c00225","DOIUrl":"https://doi.org/10.1021/acs.organomet.6c00225","url":null,"abstract":"<p>Metalloxiranes are mechanistically relevant intermediatesin carbonylfunctionalization by metals. Herein, we investigate carbonyl activationusing a nickel complex supported by a diphosphine ligand bearing apendent Lewis-acidic monoborane. Reaction of this ambiphilic systemwith a series of carbonyl substrates affords nickeloxiranes whoseisomeric distributions and relative energies were examined experimentallyand computationally through density functional theory. Despite theproximity of borane functionality, the nickeloxiranes derived frombenzophenone and acetophenone exhibited no definitive evidence forintra- or intermolecular O→B interactions. In contrast, thebenzaldehyde analogue displayed a well-defined noncovalent O→Binteraction in both the solution and solid states. These findingsprovide insights into the factors governing carbonyl activation byambiphilic nickel systems.</p>","PeriodicalId":56,"journal":{"name":"Organometallics","volume":"45 17","pages":"2170–2176"},"PeriodicalIF":2.4,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958016","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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