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Báo cáo hóa học: Supported quantum clusters of silver as enhanced catalysts for reduction
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Tuyển tập báo cáo các nghiên cứu khoa học quốc tế ngành hóa học dành cho các bạn yêu hóa học tham khảo đề tài: Supported quantum clusters of silver as enhanced catalysts for reduction
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Báo cáo hóa học: " Supported quantum clusters of silver as enhanced catalysts for reduction"Leelavathi et al. Nanoscale Research Letters 2011, 6:123http://www.nanoscalereslett.com/content/6/1/123 NANO EXPRESS Open AccessSupported quantum clusters of silver asenhanced catalysts for reductionAnnamalai Leelavathi, Thumu Udaya Bhaskara Rao, Thalappil Pradeep* Abstract Quantum clusters (QCs) of silver such as Ag7(H2MSA)7, Ag8(H2MSA)8 (H2MSA, mercaptosuccinic acid) were synthesized by the interfacial etching of Ag nanoparticle precursors and were loaded on metal oxide supports to prepare active catalysts. The supported clusters were characterized using high resolution transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and laser desorption ionization mass spectrometry. We used the conversion of nitro group to amino group as a model reaction to study the catalytic reduction activity of the QCs. Various aromatic nitro compounds, namely, 3-nitrophenol (3-np), 4-nitrophenol (4-np), 3-nitroaniline (3-na), and 4-nitroaniline (4-na) were used as substrates. Products were confirmed using UV-visible spectroscopy and electrospray ionization mass spectrometry. The supported QCs remained active and were reused several times after separation. The rate constant suggested that the reaction followed pseudo-first-order kinetics. The turn-over frequency was 1.87 s-1 per cluster for the reduction of 4-np at 35°C. Among the substrates investigated, the kinetics followed the order, SiO2 > TiO2 > Fe2O3 > Al2O3.Introduction noble metals has caused great excitement after theMonolayer-protected quantum clusters (QCs) composed initial report of Haruta [12]. It is known that reductionof a few atoms show unique properties due to their potential of silver nanoparticles change with size andnovel atomic and electronic structure. Their discrete shifts to more negative values with decrease in size,electronic states produce well-defined luminescence in which are in good agreement with previous predictionsclusters, such as Au25, Au23, Au22, Au8, etc. [1-7]. They [13]. QCs have very high negative reduction potential in comparison to bulk, and this makes them useful for thehave attracted the attention of various fields such as catalysis of electron transfer reactions. Silver is lesssensors, biolabels, live cell-targeted imaging [4], single expensive than other noble metals, and it was reportedmolecule electroluminescence [8], opto-electronics [9], as an efficient catalyst for several reactions. For example,and catalysis [10]. In the case of Au25, single crystal X- silver on alumina is a promising catalyst for selectiveray analysis has shown that it has an Au 13 core pro- catalytic reduction of NO by hydrocarbons from auto-tected with six [Au(SR)2] units in a core-shell-like pat- mobile exhausts [14]. It has been reported that Agtern. The icosahedral Au13 core has 20 triangular faces. nanoparticles on hydroxyapatite in the presence ofHowever, only 12 facets are face-capped by the exterior water catalyze the selective oxidation of various phenyl-12 Au atoms which keep eight facets open [1]. These“hole” sites may be useful as active sites [11] which may silanes into phenylsilanols [15] and also that the same system was found to be a highly efficient catalyst for theparticipate in catalytic processes. Although the single selective hydration of nitriles to amides [16]. It has beencrystal structures of the most of the clusters are yet to reported that chloroanilines wer ...
Nội dung trích xuất từ tài liệu:
Báo cáo hóa học: " Supported quantum clusters of silver as enhanced catalysts for reduction"Leelavathi et al. Nanoscale Research Letters 2011, 6:123http://www.nanoscalereslett.com/content/6/1/123 NANO EXPRESS Open AccessSupported quantum clusters of silver asenhanced catalysts for reductionAnnamalai Leelavathi, Thumu Udaya Bhaskara Rao, Thalappil Pradeep* Abstract Quantum clusters (QCs) of silver such as Ag7(H2MSA)7, Ag8(H2MSA)8 (H2MSA, mercaptosuccinic acid) were synthesized by the interfacial etching of Ag nanoparticle precursors and were loaded on metal oxide supports to prepare active catalysts. The supported clusters were characterized using high resolution transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and laser desorption ionization mass spectrometry. We used the conversion of nitro group to amino group as a model reaction to study the catalytic reduction activity of the QCs. Various aromatic nitro compounds, namely, 3-nitrophenol (3-np), 4-nitrophenol (4-np), 3-nitroaniline (3-na), and 4-nitroaniline (4-na) were used as substrates. Products were confirmed using UV-visible spectroscopy and electrospray ionization mass spectrometry. The supported QCs remained active and were reused several times after separation. The rate constant suggested that the reaction followed pseudo-first-order kinetics. The turn-over frequency was 1.87 s-1 per cluster for the reduction of 4-np at 35°C. Among the substrates investigated, the kinetics followed the order, SiO2 > TiO2 > Fe2O3 > Al2O3.Introduction noble metals has caused great excitement after theMonolayer-protected quantum clusters (QCs) composed initial report of Haruta [12]. It is known that reductionof a few atoms show unique properties due to their potential of silver nanoparticles change with size andnovel atomic and electronic structure. Their discrete shifts to more negative values with decrease in size,electronic states produce well-defined luminescence in which are in good agreement with previous predictionsclusters, such as Au25, Au23, Au22, Au8, etc. [1-7]. They [13]. QCs have very high negative reduction potential in comparison to bulk, and this makes them useful for thehave attracted the attention of various fields such as catalysis of electron transfer reactions. Silver is lesssensors, biolabels, live cell-targeted imaging [4], single expensive than other noble metals, and it was reportedmolecule electroluminescence [8], opto-electronics [9], as an efficient catalyst for several reactions. For example,and catalysis [10]. In the case of Au25, single crystal X- silver on alumina is a promising catalyst for selectiveray analysis has shown that it has an Au 13 core pro- catalytic reduction of NO by hydrocarbons from auto-tected with six [Au(SR)2] units in a core-shell-like pat- mobile exhausts [14]. It has been reported that Agtern. The icosahedral Au13 core has 20 triangular faces. nanoparticles on hydroxyapatite in the presence ofHowever, only 12 facets are face-capped by the exterior water catalyze the selective oxidation of various phenyl-12 Au atoms which keep eight facets open [1]. These“hole” sites may be useful as active sites [11] which may silanes into phenylsilanols [15] and also that the same system was found to be a highly efficient catalyst for theparticipate in catalytic processes. Although the single selective hydration of nitriles to amides [16]. It has beencrystal structures of the most of the clusters are yet to reported that chloroanilines wer ...
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