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1.
The removal of nitrogen oxides from exhaust gases has attracted great attention in recent years, and many approaches have been developed depending on the application. Methane. the main component of natural gas, has great potential as a NO reductant. In this paper, a number of catalysts previous reported for this catalytic reduction of NO have been reviewed, including a direct comparison of the relative activities and effective factors of the catalysts. Reaction mechanisnls have also been explored preliminarily.  相似文献   

2.
Nanocarbons incorporating non-hexagonal aromatic rings - such as five-, seven-, and eight-membered rings - have various intriguing physical properties such as curved structures, unique one-dimensional packing, and promising magnetic, optical, and conductivity properties. Herein, we report an efficient synthetic approach to polycyclic aromatics containing seven-membered rings via a palladium-catalyzed intramolecular Ar−H/Ar−Br coupling. In addition to all-hydrocarbon scaffolds, heteroatom-embedded heptagon-containing polyarenes can be efficiently constructed with this method. Rhodium- and palladium-catalyzed sequential six- and seven-membered ring formations also afford complex heptagon-containing molecular nanocarbons from readily available arylacetylenes and biphenyl boronic acids. Detailed mechanistic analysis by DFT calculations showed the feasibility of seven-membered ring formation by a concerted metalation-deprotonation mechanism. This reaction can serve as a template for the synthesis of a wide range of seven-membered ring-containing molecular nanocarbons.  相似文献   

3.
ATP-binding cassette (ABC) transporters shuttle diverse substrates across biological membranes. Transport is often achieved through a transition between an inward-facing (IF) and an outward-facing (OF) conformation of the transmembrane domains (TMDs). Asymmetric nucleotide-binding sites (NBSs) are present among several ABC subfamilies and their functional role remains elusive. Here we addressed this question using concomitant NO−NO, Mn2+−NO, and Mn2+−Mn2+ pulsed electron–electron double-resonance spectroscopy of TmrAB in a time-resolved manner. This type-IV ABC transporter undergoes a reversible transition in the presence of ATP with a significantly faster forward transition. The impaired degenerate NBS stably binds Mn2+−ATP, and Mn2+ is preferentially released at the active consensus NBS. ATP hydrolysis at the consensus NBS considerably accelerates the reverse transition. Both NBSs fully open during each conformational cycle and the degenerate NBS may regulate the kinetics of this process.  相似文献   

4.
Selective catalytic reduction (SCR) of nitric oxide with propane in excess oxygen was investigated on Ni-ZrO2 (NZ) and sulfated Ni-ZrO2 (SNZ), prepared by coprecipitation from a mixture of nickel nitrate-zirconium oxychloride followed by modifying with (NH4)2SO4. It was found that sulfated Ni-ZrO2 catalyst showed higher activity for the SCR of NO with propane than that of Ni-ZrO2. The structural and surface properties of catalysts were studied by XRD, BET, SEM and FT-IR of pyridine adsorption. The experimental results indicated that the modification of (NH4)2SO4 resulted in the generation of strong BrOnsted and Lewis acid sites and promoted the dispersion of the Ni species, which could lead to higher NO conversion and propane efficiency in NO reduction.  相似文献   

5.
《Analytical letters》2012,45(13):951-956
Abstract

A copolymer of 1-phenyl-2-diethylaminoethyl-p-aminobenzoate and polyvinyl-benzyl chloride was found to have a greater capacity for NO3 ? and NO2 ? than a previously reported nitron polymer but did not react as rapidly. The resin is readily regenerated with NH4OH or NH4Cl and is not affected by the pH of the water over the range of 4–10.

A copolymer of 1-(4′-nitrophenyl)-2-diethyl aminoethyl-p-nitrobenzoate and polyvinylbenzyl chloride was found to react nearly as fast as the nitron polymer and have a larger capacity for NO3 ? and NO2 ?.  相似文献   

6.
The concept of local aromaticity has been successfully utilized in understanding the stability of certain atomic clusters. However, all the skeleton atoms in these clusters are covered by at least one local aromatic feature, collectively making the multiple local aromaticities coexist globally. Herein we show the robustness of local aromaticity as a tool for the discovery of novel magic clusters: not all of the skeleton atoms need to be covered by an aromatic feature to make the cluster magic. In this study, the PtMg2,3H5 cluster anions are generated by a unique high-current pulsed discharge ion source and found to be magic numbers using mass spectrometry. Photoelectron spectroscopy and calculations confirm that only the PtH42− kernels in these clusters are locally aromatic. Based on these results, we propose that local aromaticity can be gainfully utilized as a new potential magic rule in the search for magic numbers.  相似文献   

7.
Zusammenfassung Es werden vier Methoden zur Analyse einer Gasmischung N2–NO–NO2–N2O4–N2O3–HNO2 besprochen und ihre Bedeutung für die Bestimmung der einzelnen Molekelarten kritisch auseinandergesetzt. Nach keiner der Methoden kann man den Gehalt an Salpetriger Säure und Salpetersäure neben den Oxyden des Stickstoffes auffinden. Aus diesem Grunde ist die Analyse der genannten Gasmischung nach den vier Methoden allgemein nicht genau durchführbar.Mit 1 Abbildung.Herrn Prof. Dr.A. Skrabal zum 75. Geburtstag gewidmet.  相似文献   

8.
The basic isotopic exchange reaction is responsible for the separation of15N in the Nitrox system that between gaseous nitrogen oxides and aqueous nitric acid with a single stage separation factor α=1.055 for 10M nitric acid, at 25°C and atmospheric pressure takes place. In order to know what happens in15N separation at higher pressure, when the isotopic transport between two phases is improved, a stainless steel laboratory experimental plant with a 1000 mm long × 18 mm i.d. column, packed with triangular wire springs 1.8×1.8×0.2 mm2, was utilised. At 1.5 atm (absolute), and 2.36 ml·cm−2·min−1 flow rate HETP was 7% smaller than at atmospheric pressure and 1.5 times smaller flow rate. HETP at 3.14 ml·cm−2·min−1 flow rate and 1.8 atm is practically equal with that obtained at atmospheric pressure and 2 times smaller flow rate. The operation of the15N separation plant at 1.8 atm (absolute), instead of atmospheric pressure, will permit doubling of the 10M nitric acid flow rate and of15N production of the given column.  相似文献   

9.
The polarographic catalytic wave of oxygen reduction caused by mefenamic acid (MA) with redox properties was reported in this paper. The electrochemical process of the catalytic wave was proposed that the superoxide anion O(?) was generated polarographically and the dismutation of the O(?) was catalyzed by MA to reproduce O_2 and H_2O_2. This explained chemically the scavenging of the O_2~- by MA im biomedical area. Based on the catalytic wave, a new method for the determination of MA by single-sweep polarography was developed.  相似文献   

10.
Recently ,muchattentionhasbeendirectedtotheselectivecatalyticreduction (SCR)ofNOwithmethaneasreductant[1,2 ] .Pd basedcatalystshavebeenfoundtobeactiveforthereaction[3~ 6 ] .Howev er,theperformanceofthePd basedcatalystsforthisreactiondependsstronglyonthenatureofthesup ports[3,4 ] .Sofar ,onlyacidiczeolites[3,4 ] andacidiczirconia[4~ 6 ] havebeenshowntobetheeffectivesup portsforthePd basedcatalysts .Incontrast,Pd/γ Al2 O3,whichisoneofthemostwidelyusedthree waycatalystsatpresent[7] ,exhibi…  相似文献   

11.
The perovskite type oxides (nominal formula LaTi0.5Mg0.5O3) with addition of Pd were prepared by annealing the ethanol solution of precursors in nitrogen flow at 1200°C and characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption of NO (NO-TPD). Their activity was evaluated for NO reduction by CO under stoichiometric and oxidizing conditions and for direct decomposition of NO. Pd substituted samples exhibited high NO reduction activity and selectivity towards N2. Nearly complete elimination of NO was achieved at 200°C. Two simultaneous reactions, NO reduction by CO and direct decomposition of NO as well as two forms of NO adsorption were observed on the surface of Pd substituted perovskite samples. The distribution of Pd in different catalytically active sites or complexes on at the catalyst surface may be responsible for the proceeding of two reactions: NO reduction with CO and direct NO decomposition.   相似文献   

12.
13.
14.
Two remarkable reducing agents NaBH_4 (or NaBD_4)/SnCl_2(orSnCl_4·2Et_2O) with chiral ligands are applied to the asymmetricreduction of carbonyl compounds with excellent chemical yieldsand enantioselective excesses.  相似文献   

15.
SCR of NO with NH3 is considered to be the most effective process for the treatment of stack gases from stationary sources1. The commercial catalysts for NH3-SCR are V2O5/TiO2 (anatase) promoted with either WO3 or MoO32-5. Although the vanadium- based cat…  相似文献   

16.
《Analytical letters》2012,45(1-2):79-87
Abstract

The electrochemical behaviour of 1, 2, 3, 4-thiatriazol-5-thiolate CS2N3 ? ion in acidic solutions has been investigated. A cathodic wave has been detected, (E1/2 =?1.05V versus S.C.E., M=1.0M (NaC104) and NaCS2N3 1.00 × 10?3M). The characteristics of this wave have been investigated by D.C., A.C. polarography and controlled potential electrolysis. A mechanism which involves the interaction of CS2N3 ? with mercury and cyclic regeneration of mercury has been proposed. The reduction of CS2N3 ? by amalgamated zinc has been also investigated and the results correlated with the pseudo-halide electrochemical reduction.  相似文献   

17.
Two-dimensional covalent organic frameworks (2D COFs) are often employed for electrocatalytic systems because of their structural diversity. However, the efficiency of atom utilization is still in need of improvement, because the catalytic centers are located in the basal layers and it is difficult for the electrolytes to access them. Herein, we demonstrate the use of 1D COFs for the 2e oxygen reduction reaction (ORR). The use of different four-connectivity blocks resulted in the prepared 1D COFs displaying good crystallinity, high surface areas, and excellent chemical stability. The more exposed catalytic sites resulted in the 1D COFs showing large electrochemically active surface areas, 4.8-fold of that of a control 2D COF, and thus enabled catalysis of the ORR with a higher H2O2 selectivity of 85.8 % and activity, with a TOF value of 0.051 s−1 at 0.2 V, than a 2D COF (72.9 % and 0.032 s−1). This work paves the way for the development of COFs with low dimensions for electrocatalysis.  相似文献   

18.
In┐situInfraredStudyonSurfaceSpeciesinSelectiveCatalyticReductionofNOwithHydrocarbonoverCopperZSM┐5ZeoliteZHANGWen-xiang*,JIA...  相似文献   

19.
Two remarkable reducing agents NaBH4 (or NaBD4)/SnCl2(or SnCl4·2Et2O) with chiral ligands are applied to the asymmetric reduction of carbonyl compounds with excellent chemical yields and enantioselective excesses.  相似文献   

20.
To show the synthetic utility of the catalytic C−C activation of less strained substrates, described here are the collective and concise syntheses of the natural products (−)-microthecaline A, (−)-leubehanol, (+)-pseudopteroxazole, (+)-seco-pseudopteroxazole, pseudopterosin A–F and G—J aglycones, and (+)-heritonin. The key step in these syntheses involve a Rh-catalyzed C−C/C−H activation cascade of 3-arylcyclopentanones, which provides a rapid and enantioselective route to access the polysubstituted tetrahydronaphthalene cores presented in these natural products. Other important features include 1) the direct C−H amination of the tetralone substrate in the synthesis of (−)-microthecaline A, 2) the use of phosphoric acid to enhance efficiency and regioselectivity for problematic cyclopentanone substrates in the C−C activation reactions, and 3) the direct conversion of serrulatane into amphilectane diterpenes by an allylic cyclodehydrogenation coupling.  相似文献   

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