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Stabilization of Catalytically Active Cu+ Surface Sites on Titanium–Copper Mixed‐Oxide Films
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Dr. Ashleigh E. Baber Dr. Xiaofang Yang Dr. Hyun You Kim Dr. Kumudu Mudiyanselage Markus Soldemo Dr. Jonas Weissenrieder Dr. Sanjaya D. Senanayake Dr. Abdullah Al‐Mahboob Dr. Jerzy T. Sadowski Dr. Jaime Evans Dr. José A. Rodriguez Dr. Ping Liu Dr. Friedrich M. Hoffmann Dr. Jingguang G. Chen Dr. Darío J. Stacchiola 《Angewandte Chemie (International ed. in English)》2014,53(21):5336-5340
The oxidation of CO is the archetypal heterogeneous catalytic reaction and plays a central role in the advancement of fundamental studies, the control of automobile emissions, and industrial oxidation reactions. Copper‐based catalysts were the first catalysts that were reported to enable the oxidation of CO at room temperature, but a lack of stability at the elevated reaction temperatures that are used in automobile catalytic converters, in particular the loss of the most reactive Cu+ cations, leads to their deactivation. Using a combined experimental and theoretical approach, it is shown how the incorporation of titanium cations in a Cu2O film leads to the formation of a stable mixed‐metal oxide with a Cu+ terminated surface that is highly active for CO oxidation. 相似文献
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Chemical investigation of n-butanol extract from the methanol extract of leaves of Grewia damine furnished lupeol, sitosterol beta-D-glucoside, flavone C-glycosides vitexin, isovitexin where as the same extracts from the leaves of Filicium decipiens furnished sitosterol beta-D-glucoside, 3-O-beta-D-glucopyranosyl kaempferol, 3-O-beta-D-glucopyranosylquercetin and 3-O-alpha-L-rhamnopyranosyl(1--> 2)-beta-D-glucopyranosylkaempferol. 相似文献
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Rigumula Wu Aruni P. K. K. Karunanayake Mudiyanselage Fatemeh Shafiei Bin Zhao Yousef Bagheri Qikun Yu Kathleen McAuliffe Kewei Ren Mingxu You 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(50):18439-18443
Precisely determining the intracellular concentrations of metabolites and signaling molecules is critical in studying cell biology. Fluorogenic RNA‐based sensors have emerged to detect various targets in living cells. However, it is still challenging to apply these genetically encoded sensors to quantify the cellular concentrations and distributions of targets. Herein, using a pair of orthogonal fluorogenic RNA aptamers, DNB and Broccoli, we engineered a modular sensor system to apply the DNB‐to‐Broccoli fluorescence ratio to quantify the cell‐to‐cell variations of target concentrations. These ratiometric sensors can be broadly applied for live‐cell imaging and quantification of metabolites, signaling molecules, and other synthetic compounds. 相似文献
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Chemical investigation of methanol extract of the fruits of Diploclisia glaucescens furnished 3-O-beta-D-glucopyranosyl-20-hydroxyecdysone, 3-O-[beta-D-glucopyranosyl-(1-->2)-beta-D-glucopyranosyl]serjanic acid 28-O-beta-D-glucopyranosyl ester and 3-O-[beta-xylopyranosyl(1-->2)-beta-D-glucopyranosyl-(1-->2)-beta-D-glucopyranosyl]serjanic acid 28-O-beta-D-glucopyranosyl ester. The latter saponin was found to be a new natural product while the other two are reported for the first time from the family Menispermaceae. 相似文献
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Dr. Kumudu Mudiyanselage Dr. Sanjaya D. Senanayake Dr. Leticia Feria Dr. Shankhamala Kundu Dr. Ashleigh E. Baber Dr. Jesús Graciani Dr. Alba B. Vidal Dr. Stefano Agnoli Prof. Jaime Evans Dr. Rui Chang Dr. Stephanus Axnanda Dr. Zhi Liu Prof. Javier F. Sanz Dr. Ping Liu Dr. José A. Rodriguez Dr. Darío J. Stacchiola 《Angewandte Chemie (International ed. in English)》2013,52(19):5101-5105
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Xiaofang Yang Shyam Kattel Ke Xiong Kumudu Mudiyanselage Sergei Rykov Sanjaya D. Senanayake Jos A. Rodriguez Ping Liu Dario J. Stacchiola Jingguang G. Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2015,127(41):12114-12119
Direct propylene epoxidation by O2 is a challenging reaction because of the strong tendency for complete combustion. Results from the current study demonstrate that by generating highly dispersed and stabilized Cu+ active sites in a TiCuOx mixed oxide the epoxidation selectivity can be tuned. The TiCuOx surface anchors the key surface intermediate, an oxametallacycle, leading to higher selectivity for epoxidation of propylene. 相似文献
8.
The adsorption and reaction of NO(2) on BaO (<1, ~3, and >20 monolayer equivalent (MLE))/Pt(111) model systems were studied with temperature programmed desorption (TPD), X-ray photoelectron spectroscopy (XPS), and infrared reflection absorption spectroscopy (IRAS) under ultra-high vacuum (UHV) as well as elevated pressure conditions. NO(2) reacts with sub-monolayer BaO (<1 MLE) to form nitrites only, whereas the reaction of NO(2) with BaO (~3 MLE)/Pt(111) produces mainly nitrites and a small amount of nitrates under UHV conditions (P(NO(2))≈ 1.0 × 10(-9) Torr) at 300 K. In contrast, a thick BaO (>20 MLE) layer on Pt(111) reacts with NO(2) to form nitrite-nitrate ion pairs under the same conditions. At elevated NO(2) pressures (≥1.0 × 10(-5) Torr), however, BaO layers at all these three coverages convert to amorphous barium nitrates at 300 K. Upon annealing to 500 K, these amorphous barium nitrate layers transform into crystalline phases. The thermal decomposition of the thus-formed Ba(NO(x))(2) species is also influenced by the coverage of BaO on the Pt(111) substrate: at low BaO coverages, these species decompose at significantly lower temperatures in comparison with those formed on thick BaO films due to the presence of a Ba(NO(x))(2)/Pt interface where the decomposition can proceed at lower temperatures. However, the thermal decomposition of the thick Ba(NO(3))(2) films follows that of bulk nitrates. Results obtained from these BaO/Pt(111) model systems under UHV and elevated pressure conditions clearly demonstrate that both the BaO film thickness and the applied NO(2) pressure are critical in the Ba(NO(x))(2) formation and subsequent thermal decomposition processes. 相似文献
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The formation and dissociation chemistry of the NH species on Pt(111) was characterized with reflection absorption infrared spectroscopy and temperature programmed desorption. Irradiation of a chemisorbed bilayer of ammonia with a 100 eV electron beam at 85 K leads to a mixture of NH, N, and H on the surface. Annealing to temperatures in the range of 200-300 K leads to reaction of N and H to form additional NH. The NH species has an intense and narrow NH stretch peak at 3320 cm(-1), while no peak due to the PtNH bend is observed above 800 cm(-1). The NH species is stable up to a temperature of approximately 400 K. The surface N atoms produced from NH dissociation are readily hydrogenated back to NH by exposure of the surface to H2. However, NH cannot be further hydrogenated to generate adsorbed NH2 or to NH3 under the conditions used here. Exposure of the NH/Pt(111) surface to D2 at 380 K produces the ND species. Comparison with the results of density functional theory calculations based on small Pt clusters indicates that NH occupies three-fold hollow sites with the molecular axis perpendicular to the surface. 相似文献
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Erandimala U. Kulawardana Thilini Kuruwita‐Mudiyanselage Douglas C. Neckers 《Journal of polymer science. Part A, Polymer chemistry》2009,47(13):3318-3325
Stimuli responsive hydrogels (PNIPAAm‐MSp) with a thermoresponsive backbone and photochromic pendant groups were synthesized via free radical polymerization using N‐isopropylacrylamide, modified spironaphthoxazines with a polymerizable double bond (MSp) as photochromic monomer, the crosslinker N,N′‐methylenebis(acrylamide) and the initiator 2,2′‐azobis(isobutyronitrile) in dimethylsulfoxide. The polymers are dual responsive, in that poly(N‐isopropylacrylamide) (PNIPAAm) responds to temperature changes whereas the pendant spironaphthoxazines respond to light. Irradiation enhanced the water absorption of the polymers while increases in temperature decreased it. The irradiated PNIPAAm‐MSp showed best water absorption at 0 °C (Q = 3.25) while water desorbed at higher temperatures (35 °C; Q = 0.30); where Q is the amount of water absorbed by a gram of dry polymer. © 2009 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 47: 3318–3325, 2009 相似文献