Isolated metal atoms and clusters for alkane activation: translating knowledge from enzymatic and homogeneous to heterogeneous systems

Chem ◽  
2021 ◽  
Author(s):  
Lichen Liu ◽  
Avelino Corma
2014 ◽  
Vol 43 (22) ◽  
pp. 7536-7547 ◽  
Author(s):  
Jason F. Weaver ◽  
Can Hakanoglu ◽  
Abbin Antony ◽  
Aravind Asthagiri

Late transition-metal oxide surfaces that expose coordinatively-unsaturated metal atoms promote the formation and bond activation of alkane σ-complexes.


Author(s):  
S. Ritchie ◽  
J. C. Bennett ◽  
A. Prodan ◽  
F.W. Boswell ◽  
J.M. Corbett

A continuous sequence of compounds having composition NbxTa1-xTe4; 0 ≤ x ≤ 1 have been studied by electron diffraction and microscopy. Previous studies have shown that the end members of the series, TaTε4 and NbTε4 possess a quasi-one-dimensional character and exhibit charge density wave (CDW) distortions. In these compounds, the subcell structure is tetragonal with axes (a × a × c) and consists of the metal atoms (Nb or Ta) centered within an extended antiprismatic cage of Te atoms. At room temperature, TaTε4 has a commensurate modulation structure with a 2a × 2a × 3c unit cell. In NbTε4, an incommensurate modulation with × ∼ 16c axes is observed. Preliminary studies of the mixed compounds NbxTα1-xTε4 showed a discontinuous jump of the modulation wave vector commensurate to incommensurate when the Nb dopant concentration x, exceeded x ≃ 0.3, In this paper, the nature of the compositional dependence of is studied in greater detail and evidence is presented for a stepwise variation of . This constitutes the first direct evidence for a Devil's staircase in CDW materials.


Author(s):  
Klaus-Ruediger Peters

Topographic ultra high resolution can now routinely be established on bulk samples in cold field emission scanning electron microscopy with a second generation of microscopes (FSEM) designed to provide 0.5 nm probe diameters. If such small probes are used for high magnification imaging, topographic contrast is so high that remarkably fine details can be imaged on 2DMSO/osmium-impregnated specimens at ribosome surfaces even without a metal coating. On TCH/osmium-impregnated specimens topographic resolution can be increased further if the SE-I imaging mode is applied. This requires that beam diameter and metal coating thickness be made smaller than the SE range of ~1 nm and background signal contributions be reduced. Subnanometer small probes can be obtained (only) at high accelerating voltages. Subnanometer thin continuous metal films can be produced under the following conditions: self-shadowing effect between metal atoms must be reduced through appropriate deposition techniques and surface mobility of metal atoms must be diminished through high energy sputtering and/or specimen cooling.


1998 ◽  
Vol 37 (04/05) ◽  
pp. 518-526 ◽  
Author(s):  
D. Sauquet ◽  
M.-C. Jaulent ◽  
E. Zapletal ◽  
M. Lavril ◽  
P. Degoulet

AbstractRapid development of community health information networks raises the issue of semantic interoperability between distributed and heterogeneous systems. Indeed, operational health information systems originate from heterogeneous teams of independent developers and have to cooperate in order to exchange data and services. A good cooperation is based on a good understanding of the messages exchanged between the systems. The main issue of semantic interoperability is to ensure that the exchange is not only possible but also meaningful. The main objective of this paper is to analyze semantic interoperability from a software engineering point of view. It describes the principles for the design of a semantic mediator (SM) in the framework of a distributed object manager (DOM). The mediator is itself a component that should allow the exchange of messages independently of languages and platforms. The functional architecture of such a SM is detailed. These principles have been partly applied in the context of the HEllOS object-oriented software engineering environment. The resulting service components are presented with their current state of achievement.


2000 ◽  
Vol 626 ◽  
Author(s):  
Antje Mrotzek ◽  
Kyoung-Shin Choi ◽  
Duck-Young Chung ◽  
Melissa A. Lane ◽  
John R. Ireland ◽  
...  

ABSTRACTWe present the structure and thermoelectric properties of the new quaternary selenides K1+xM4–2xBi7+xSe15 (M = Sn, Pb) and K1-xSn5-xBi11+xSe22. The compounds K1+xM4-2xBi7+xSe15 (M= Sn, Pb) crystallize isostructural to A1+xPb4-2xSb7+xSe15 with A = K, Rb, while K1-xSn5-xBi11+xSe22 reveals a new structure type. In both structure types fragments of the Bi2Te3-type and the NaCl-type are connected to a three-dimensional anionic framework with K+ ions filled tunnels. The two structures vary by the size of the NaCl-type rods and are closely related to β-K2Bi8Se13 and K2.5Bi8.5Se14. The thermoelectric properties of K1+xM4-2xBi7+xSe15 (M = Sn, Pb) and K1-xSn5-xBi11+xSe22 were explored on single crystal and ingot samples. These compounds are narrow gap semiconductors and show n-type behavior with moderate Seebeck coefficients. They have very low thermal conductivity due to an extensive disorder of the metal atoms and possible “rattling” K+ ions.


1970 ◽  
Author(s):  
N.V. Antonishin ◽  
S. S. Zabrodsky ◽  
L.E. Simchenko ◽  
V.V. Lushchikov

2020 ◽  
Author(s):  
Laurent Sévery ◽  
Jacek Szczerbiński ◽  
Mert Taskin ◽  
Isik Tuncay ◽  
Fernanda Brandalise Nunes ◽  
...  

The strategy of anchoring molecular catalysts on electrode surfaces combines the high selectivity and activity of molecular systems with the practicality of heterogeneous systems. The stability of molecular catalysts is, however, far less than that of traditional heterogeneous electrocatalysts, and therefore a method to easily replace anchored molecular catalysts that have degraded could make such electrosynthetic systems more attractive. Here, we apply a non-covalent “click” chemistry approach to reversibly bind molecular electrocatalysts to electrode surfaces via host-guest complexation with surface-anchored cyclodextrins. The host-guest interaction is remarkably strong and allows the flow of electrons between the electrode and the guest catalyst. Electrosynthesis in both organic and aqueous media was demonstrated on metal oxide electrodes, with stability on the order of hours. The catalytic surfaces can be recycled by controlled release of the guest from the host cavities and readsorption of fresh guest. This strategy represents a new approach to practical molecular-based catalytic systems.


2019 ◽  
Author(s):  
Mingguang Chen ◽  
Wangxiang Li ◽  
Anshuman Kumar ◽  
Guanghui Li ◽  
Mikhail Itkis ◽  
...  

<p>Interconnecting the surfaces of nanomaterials without compromising their outstanding mechanical, thermal, and electronic properties is critical in the design of advanced bulk structures that still preserve the novel properties of their nanoscale constituents. As such, bridging the p-conjugated carbon surfaces of single-walled carbon nanotubes (SWNTs) has special implications in next-generation electronics. This study presents a rational path towards improvement of the electrical transport in aligned semiconducting SWNT films by deposition of metal atoms. The formation of conducting Cr-mediated pathways between the parallel SWNTs increases the transverse (intertube) conductance, while having negligible effect on the parallel (intratube) transport. In contrast, doping with Li has a predominant effect on the intratube electrical transport of aligned SWNT films. Large-scale first-principles calculations of electrical transport on aligned SWNTs show good agreement with the experimental electrical measurements and provide insight into the changes that different metal atoms exert on the density of states near the Fermi level of the SWNTs and the formation of transport channels. </p>


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