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Hydride Migration from a Triangular Face to a Tetrahedral Cavity in Tetranuclear Iron Carbonyl Clusters upon Coordination of [AuPPh3]+ Fragments 下载免费PDF全文
Dr. Marco Bortoluzzi Dr. Iacopo Ciabatti Dr. Cristina Femoni Dr. Mohammad Hayatifar Prof. Maria Carmela Iapalucci Prof. Giuliano Longoni Prof. Stefano Zacchini 《Angewandte Chemie (International ed. in English)》2014,53(28):7233-7237
Metal hydrides are of fundamental importance in chemistry, both as solid‐state materials and molecular compounds. The first low‐valent molecular metal cluster containing an interstitial four‐coordinate hydride in a tetrahedral site is decribed, which undergoes hydride migration from the surface to the tetrahedral cavity of the cluster upon coordination of a [AuPPh3]+ fragment. The [HFe4(CO)12(AuPPh3)2]? mono‐anion, which contains a surface μ3‐H, was obtained from the reaction of [HFe4(CO)12]3? with two equivalents of [Au(PPh3)Cl]. This is, in turn, transformed into the neutral [HFe4(CO)12(AuPPh3)3] upon addition of a third [AuPPh3]+ fragment, with concomitant migration of the unique hydride from the surface of the cluster to its tetrahedral cavity. All of these species have been fully characterized in solution by means of IR and multinuclear NMR spectroscopy, and in the solid state by single‐crystal X‐ray diffractometry. 相似文献
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Tunable Trimers: Using Temperature and Pressure to Control Luminescent Emission in Gold(I) Pyrazolate‐Based Trimers 下载免费PDF全文
Dr. Christopher H. Woodall Dr. Sara Fuertes Dr. Christine M. Beavers Lauren E. Hatcher Andrew Parlett Dr. Helena J. Shepherd Dr. Jeppe Christensen Dr. Simon J. Teat Mourad Intissar Dr. Alexandre Rodrigue‐Witchel Dr. Yan Suffren Prof. Christian Reber Christopher H. Hendon Dr. Davide Tiana Prof. Aron Walsh Prof. Paul R. Raithby 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(51):16933-16942
A systematic investigation into the relationship between the solid‐state luminescence and the intermolecular Au???Au interactions in a series of pyrazolate‐based gold(I) trimers; tris(μ2‐pyrazolato‐N,N′)‐tri‐gold(I) ( 1 ), tris(μ2‐3,4,5‐ trimethylpyrazolato‐N,N′)‐tri‐gold(I) ( 2 ), tris(μ2‐3‐methyl‐5‐phenylpyrazolato‐N,N′)‐tri‐gold(I) ( 3 ) and tris(μ2‐3,5‐diphenylpyrazolato‐N,N′)‐tri‐gold(I) ( 4 ) has been carried out using variable temperature and high pressure X‐ray crystallography, solid‐state emission spectroscopy, Raman spectroscopy and computational techniques. Single‐crystal X‐ray studies show that there is a significant reduction in the intertrimer Au???Au distances both with decreasing temperature and increasing pressure. In the four complexes, the reduction in temperature from 293 to 100 K is accompanied by a reduction in the shortest intermolecular Au???Au contacts of between 0.04 and 0.08 Å. The solid‐state luminescent emission spectra of 1 and 2 display a red shift with decreasing temperature or increasing pressure. Compound 3 does not emit under ambient conditions but displays increasingly red‐shifted luminescence upon cooling or compression. Compound 4 remains emissionless, consistent with the absence of intermolecular Au???Au interactions. The largest pressure induced shift in emission is observed in 2 with a red shift of approximately 630 cm?1 per GPa between ambient and 3.80 GPa. The shifts in all the complexes can be correlated with changes in Au???Au distance observed by diffraction. 相似文献
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Dr. Matthias Böge Prof.Dr. Jürgen Heck 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(20):6787-6792
Crystals of mixed‐valent Au complexes have been grown from solutions of cyclohexanecarbonitrile and a stoichiometric amount of gold(I) and gold(III) chloride. The purely obtained compound was characterized as bis(cyclohexanecarbonitrile)gold(I) tetrachloridoaurate(III). The crystal packing of the mixed valent Au(I/III) compound demonstrates a columnar arrangement of the gold(I) and gold(III) atoms. The new structure displays the shortest unsupported gold(I)–gold(III) interactions with the sub‐van der Waals distance of 324–325 pm, which is assumed as an aurophilic bonding interaction. 相似文献
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Alejandro Portugus Lydia Gonzlez Delia Bautista Juan Gil‐Rubio 《Angewandte Chemie (International ed. in English)》2020,59(35):15220-15225
The first binuclear AuI compounds containing bridging (CF2)n chains (n=4, 6, 8) and AuIII metallaperfluorocyclopentanes have been obtained by photoinitiated reactions of LAuMe (L=PPh3, PMe3, PCy3, or IPr) with α,ω‐diiodoperfluorocarbons. Complexes LAu(CF2)4AuL present an unusual looped structure stabilized by an aurophilic interaction for L=PMe3, PPh3, and PCy3. The study of their dynamic behaviour has provided new insights about the strength of aurophilic interactions in solution, allowing quantification of the energy of a single Au???Au interaction. 相似文献
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Weidner T Ballav N Zharnikov M Priebe A Long NJ Maurer J Winter R Rothenberger A Fenske D Rother D Bruhn C Fink H Siemeling U 《Chemistry (Weinheim an der Bergstrasse, Germany)》2008,14(14):4346-4360
1,1'-Difunctionalised ferrocene derivatives have been studied, which contain groups suitable for chemisorption on gold substrates, namely -NC, -PR(2) as well as a range of sulfur-containing units like -NCS, -SR, and thienyl. Thin films on gold have been fabricated from solution with most of these adsorbate species. Film thickness, composition and structure were investigated primarily by X-ray photoelectron and near-edge X-ray absorption fine-structure spectroscopy. The quality of self-assembled monolayers fabricated from 1,1'-diisocyanoferrocene (1) and 1,1'-diisothiocyanatoferrocene (2) turned out to be superior to that of films based on the other adsorbate species investigated. In addition to the surface coordination behaviour of 1 towards gold substrates, relevant aspects of the molecular coordination chemistry of 1 have also been addressed, including the synthesis and characterisation of [(mu-1){Cr(CO)(5)}(2)], [Ag(2)(mu-1)(2)](NO(3))(2) x H(2)O and [(mu-1)(AuCl)(2)]. The crystal structure of the gold complex is governed by aurophilic interactions and can be taken as a model for the arrangement of 1 in self-assembled monolayers on gold. 相似文献
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Yukie Takemura Hiroe Takenaka Takayuki Nakajima Prof. Tomoaki Tanase Prof. 《Angewandte Chemie (International ed. in English)》2009,48(12):2157-2161
A flexible building block : Flexible tetragold(I) chain complexes supported by a new single methylene‐bridged tetraphosphine ligand were synthesized and further transformed into discrete linear octagold(I) {Au8} and cyclic hexagold(I) {Au6} structures by reaction with KI and NaAuCl4, respectively (see picture, Au purple, Cl dark green, PF6 light green, I pink). The tetragold complexes are also luminescent at room temperature.
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Lefebvre J Callaghan F Katz MJ Sonier JE Leznoff DB 《Chemistry (Weinheim an der Bergstrasse, Germany)》2006,12(26):6748-6761
The structures of two cyanoaurate-based coordination polymers, M(mu-OH(2))(2)[Au(CN)(2)](2) (M=Cu, Ni), were determined by using a combination of powder and single-crystal X-ray diffraction techniques. The basic structural motif for both polymers contains rarely observed M(mu-OH(2))(2)M double aqua-bridges, which generate an infinite chain; two trans [Au(CN)(2)](-) units also dangle from each metal center. The chains form ribbons that interact three dimensionally through CNH hydrogen bonding. The magnetic properties of both compounds and of the dehydrated analogue Cu[Au(CN)(2)](2) were investigated by direct current (dc) and alternating current (ac) magnetometry; muon spin-relaxation data was also obtained to probe their magnetic properties in zero-field. In M(mu-OH(2))(2)[Au(CN)(2)](2), ferromagnetic chains of M(mu-OH(2))(2)M are present below 20 K. Interchain magnetic interactions mediated through hydrogen bonding, involving water and cyanoaurate units, yield a long-range magnetically ordered system in Cu(mu-OH(2))(2)[Au(CN)(2)](2) below 0.20 K, as indicated by precession in the muon spin polarization decay. Ni(mu-OH(2))(2)[Au(CN)(2)](2) undergoes a transition to a spin-glass state in zero-field at 3.6 K, as indicated by a combination of muon spin-relaxation and ac-susceptibility data. This transition is probably due to competing interactions that lead to spin frustration. A phase transition to a paramagnetic state is possible for Ni(mu-OH(2))(2)[Au(CN)(2)](2) upon application of an external field; the critical field was determined to be 700 Oe at 1.8 K. The dehydrated compound Cu[Au(CN)(2)](2) shows weak antiferromagnetic interactions at low temperatures. 相似文献