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991.
A 1,10-phenanthroline based polymer named PPPhen(i.e., polymer from pyrene 1,10-phenanthrolin) was prepared by the Friedel-Crafts reaction of 1,10-phenanthroline and pyrene cross-linked with dimethoxymethane. The related Pd catalyst Pd@PPPhen was prepared by supporting Pd nanoparticles(NPs) on the PPPhen material. PPPhen and Pd@PPPhen were characterized by means of scanning electron microscopy(SEM), transmission electron microscopy, N2 adsorption-desorption, Fourier-transform infrared and X-ray photoelectron spectroscopy analyses. The results showed that PPPhen polymer was highly porous and that the phenanthroline group can enhance the stability of the Pd nanoparticles. Pd@PPPhen also exhibited good catalytic activity in the aerobic oxidation of alcohols to aldehydes and ketones, and Pd@PPPhen was recyclable with durable activity and retentive structures. 相似文献
992.
993.
Inês A. S. Matias Ana P. C. Ribeiro Luísa M. D. R. S. Martins 《Molecules (Basel, Switzerland)》2020,25(23)
The direct, one-pot oxidation of ethane to acetic acid was, for the first time, performed using a C-scorpionate complex anchored onto a magnetic core-shell support, the Fe3O4/TiO2/[FeCl2{κ3-HC(pz)3}] composite. This catalytic system, where the magnetic catalyst is easily recovered and reused, is highly selective to the acetic acid synthesis. The performed green metrics calculations highlight the “greeness” of the new ethane oxidation procedure. 相似文献
994.
Weinan Xing Shengming Yin Wenguang Tu Guanyu Liu Shuyang Wu Haojing Wang Markus Kraft Guangyu Wu Rong Xu 《Angewandte Chemie (International ed. in English)》2020,59(3):1171-1175
A simple solvent ligation effect was successfully used to disrupt the growth of a model compound, Fe[(OH)(O3P(CH2)2CO2H)]?H2O (MIL‐37), into an extended 2D structure by replacing water with dimethylformamide (DMF) as the solvent during the synthesis. Owing to the lack of ?OH group, which provides the corner‐sharing (binding) oxygen atoms for the octahedra, an amorphous and porous structure is formed. When Fe3+ is partially replaced by Ni2+, the amorphous structure remains and the resultant binary metal catalyst displays excellent photocatalytic oxygen evolution activity with almost 100 % yield achieved under visible light irradiation using [Ru(bpy)3]2+ as the photosensitizer. This study opens up new possibilities of using the simple solvent effect to synthesize high surface area metal phosphonates for catalytic and other applications. 相似文献
995.
Electrochemical Vicinal Difluorination of Alkenes: Scalable and Amenable to Electron‐Rich Substrates
Sayad Doobary Alexi T. Sedikides Henry P. Caldora Darren L. Poole Alastair J. J. Lennox 《Angewandte Chemie (International ed. in English)》2020,59(3):1155-1160
Fluorinated alkyl groups are important motifs in bioactive compounds, positively influencing pharmacokinetics, potency and conformation. The oxidative difluorination of alkenes represents an important strategy for their preparation, yet current methods are limited in their alkene‐types and tolerance of electron‐rich, readily oxidized functionalities, as well as in their safety and scalability. Herein, we report a method for the difluorination of a number of unactivated alkene‐types that is tolerant of electron‐rich functionality, giving products that are otherwise unattainable. Key to success is the electrochemical generation of a hypervalent iodine mediator using an “ex‐cell” approach, which avoids oxidative substrate decomposition. The more sustainable conditions give good to excellent yields in up to decagram scales. 相似文献
996.
Jilai Li Caiyun Geng Thomas Weiske Helmut Schwarz 《Angewandte Chemie (International ed. in English)》2020,59(30):12308-12314
[V2O]+ remains “invisible” in the thermal gas‐phase reaction of bare [V2]+ with CO2 giving rise to [V2O2]+; this is because the [V2O]+ intermediate is being consumed more than 230 times faster than it is generated. However, the fleeting existence of [V2O]+ and its involvement in the [V2]+ → [V2O2]+ chemistry are demonstrated by a cross‐over labeling experiment with a 1:1 mixture of C16O2/C18O2, generating the product ions [V216O2]+, [V216O18O]+, and [V218O2]+ in a 1:2:1 ratio. Density functional theory (DFT) calculations help to understand the remarkable and unexpected reactivity differences of [V2]+ versus [V2O]+ towards CO2. 相似文献
997.
Jin Su Takashi Hisatomi Tsutomu Minegishi Kazunari Domen 《Angewandte Chemie (International ed. in English)》2020,59(33):13800-13806
Most CdTe photoanodes and photocathodes show positive and negative photocurrent onset potentials for water oxidation and reduction, respectively, and are thus unable to drive photoelectrochemical (PEC) water splitting without external applied biases. Herein, the activity of a CdTe photoanode having an internal p‐n junction during PEC water oxidation was enhanced by applying a CdCl2 annealing treatment together with surface modifications. The resulting CdTe photoanode generated photocurrents of 1.8 and 5.4 mA cm?2 at 0.6 and 1.2 VRHE, respectively, with a photoanodic current onset potential of 0.22 VRHE under simulated sunlight (AM 1.5G). The CdCl2 annealing increased the grain sizes and lowered the density of grain boundaries, allowing more efficient charge separation. Consequently, a two‐electrode tandem PEC cell comprising a CdTe‐based photoanode and photocathode split water without any external bias at a solar‐to‐hydrogen conversion efficiency of 0.51 % at the beginning of the reaction. 相似文献
998.
Azadeh Kiani Ali Ghaffarinejad Seyed Abolfazl Seyedsadjadi Atiyeh Mansouri 《Electroanalysis》2020,32(2):281-290
In this study, an available and inexpensive graphite substrate, was easily modified with Ni/Cr nanoparticles via electrodeposition technique in a very short time (3 min) and used as an electrocatalyst for glucose oxidation in alkaline solution. Graphite electrode modified with Ni/Cr nanoparticles demonstrated an outstanding electrocatalytic performance to glucose oxidation in comparison to examined Ni‐based electrodes or even different materials in other reports. It is noteworthy to mention that adding a little Cr led to a synergistic effect with Ni; accordingly, the presence of Cr not only resulted in a greater adsorption of glucose molecules by chromium oxide but also boosted conductivity of the nickel oxide because of the enhancement of Ni(III) amount. The electrochemical studies were performed by cyclic voltammetry and electrochemical impedance spectroscopy (EIS). The morphology and structure of catalyst layer was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X‐ray diffraction (XRD) and energy dispersive x‐ray spectroscopy (EDS). The linear range of the electrode by cyclic voltammetry was between 2–31 mM with a high sensitivity of 2094 μA cm?2 mM?1. The repeatability and reproducibility of the proposed electrode was examined in glucose solution which were 0.3 % and 4.7 %, respectively. According to the low cost, ease and fast preparation, good repeatability and high sensitivity, this electrode can be a good candidate for nonenzymatic glucose oxidation. 相似文献
999.
Liliya Dubenska Olha Dushna Solomiya Pysarevska Mykola Blazheyevskiy 《Electroanalysis》2020,32(3):626-634
In present paper we described a new simple voltammetric method of determination of nefopam alkaloid and its metabolite – N‐oxide. N‐oxide of nefopam is reduced at the dropping mercury electrode (DME) and silver solid amalgam electrodes (AgSAE), which can effectively replace mercury and chemically modified electrodes. The reduction consists of two one‐electron stages each accompanied with one proton transfer. N‐oxide of nefopam can be obtained from nefopam substance by oxidation with potassium peroxymonosulfate. It was studied the effect of various factors on N‐oxide quantitative yield (pH, oxidation duration, reagents concentration) as well as on the reduction of N‐oxide at DME and p‐AgSAE (pH, the nature of background electrolyte, potential and time of accumulation). It was showed that the reduction current linearly increased with increasing of concentration of analgesic. Limit of quantiation is 10?6 mol L?1 at DME and 10?7 mol L?1 at p‐AgSAE. The developed method was applied for the analysis of commercial drug solution for injection “Nefopam” with recovery of 96.7 %, as well as for the spiked human urine samples. Excellent repeatability with a relative standard deviation below 5 % was achieved. 相似文献
1000.
Langli Luo Yao Nian Shuangbao Wang Zejian Dong Yang He You Han Chongmin Wang 《Angewandte Chemie (International ed. in English)》2020,59(6):2505-2509
By using in situ aberration‐corrected environmental transmission electron microscopy, for the first time at atomic level, the dynamic evolution of the Cu surface is captured during CO oxidation. Under reaction conditions, the Cu surface is activated, typically involving 2–3 atomic layers with the formation of a reversible metastable phase that only exists during catalytic reactions. The distinctive role of CO and O2 in the surface activation is revealed, which features CO exposure to lead to surface roughening and consequently formation of low‐coordinated Cu atoms, while O2 exposure induces a quasi‐crystalline CuOx phase. Supported by DFT calculations, it is shown that crystalline CuOx reversibly transforms into the amorphous phase, acting as an active species to facilitate the interaction of gas reactants and catalyzing CO oxidation. 相似文献