Due to the highly sensitive electrochemiluminescence (ECL), tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy)32+) is often used in the field of bioarrays with the help of co-reactants. However, the generally used co-reacta...Due to the highly sensitive electrochemiluminescence (ECL), tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy)32+) is often used in the field of bioarrays with the help of co-reactants. However, the generally used co-reactant, tripropylamine (TPA), is toxic, corrosive and volatile. Therefore, the search for safe, sensitive and economical co-reactants is critical. Herein, three aminocarboxylic acids, ethylenediamine-tetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and 2-hydroxyethylethylene diaminetriacetic acid (HEDTA), have been investigated as potential co-reactants for promoting Ru(bpy)32+ ECL behaviour. A possible ECL mechanism is also presented. The experimental results suggested that the co-reactants have a different ECL behaviour compared to TPA, such as different pH- and surfactant-responses. The detection limits of Ru(bpy)32+ using NTA, EDTA and HEDTA as co-reactants are 1, 60 and 680 fmol·L-1, respectively. The results indicate that NTA has a much higher efficiency than TPA to excite Ru(bpy)3 2+ ECL under their own optimal conditions. NTA could be widely used in many fields because it is less toxic, corrosive and volatile than TPA. Moreover, using Ru(bpy)3 2+ ECL, a sensitive method for the detection of aminocarboxylic acids is also developed. An improvement of four orders of magnitude in detection limits is obtained for EDTA compared to the known Ru(bpy) 3 2+ chemiluminescent methods.展开更多
HfTiN film was deposited by co-reactive sputtering and then was annealed in dif-ferent gas ambients at temperature of 650 ℃ for 2 min to form HfTiON film. Capacitance-voltage and gate-leakage characteristics were inv...HfTiN film was deposited by co-reactive sputtering and then was annealed in dif-ferent gas ambients at temperature of 650 ℃ for 2 min to form HfTiON film. Capacitance-voltage and gate-leakage characteristics were investigated. The N2O-annealed sample exhibited small inter-face-state and oxide-charge densities, and enhanced reliability, which was attributed to the fact that nitridation could create strong Si≡N bonds to passivate dangling Si bonds and replaced strained Si-O bonds, thus forming a hardened dielectric/Si interface with high reliability. As a result, it is possible to prepare high-quality HfTiON gate dielectric of small-scaling CMOS devices in the industry-preferred N2O environment.展开更多
A co-reaction of methane with methanol over zeolite catalysts has emerged as a new approach to the long-standing challenge of methane transformation.However,the effect of catalyst acid properties on the co-reaction ha...A co-reaction of methane with methanol over zeolite catalysts has emerged as a new approach to the long-standing challenge of methane transformation.However,the effect of catalyst acid properties on the co-reaction has been rarely studied.In this study,a series of HZSM-5 zeolites with comparable diffusion abilities and various acidities were synthesized directly through steaming with 100%water vapor at 693 K.The co-reaction of methane and methanol was subsequently evaluated.Br?nsted acidity at 0.262 mmol/g was detected to reach the maximum methane conversion of 5.42%at 673 K,which was also the odd point in the relationship between acid concentration and C4 hydrogen transfer index.Moreover,the influence of methanol feed was investigated over parent and steamed ZSM-5 catalyst,with results showing that excessive acid sites or methanol molecules reduce methane conversion.It is proposed that acid sites adsorbed with methanol molecules construct the methane activation sites.Hence,a proper design of zeolite acidity should be achieved to obtain higher methane conversion in the co-reaction process.展开更多
Acidity plays a vital role in methane conversion by co-feeding method,which is one of the best strategies to improve the utilization and gentle the reaction conditions of methane.In this work,Zn,Ni,Mo,La,Ga,Fe and Co-...Acidity plays a vital role in methane conversion by co-feeding method,which is one of the best strategies to improve the utilization and gentle the reaction conditions of methane.In this work,Zn,Ni,Mo,La,Ga,Fe and Co-impregnated ZSM-5 zeolites have been prepared with the same substitutions to variate the acidities and tested in co-aromatization of methanol with methane.It is demonstrated that the new medium-strong acid sites formed by metal and strong acid sites are the key role to activate methane in co-reaction.Zn-modified ZSM-5 catalyst is preferred to exhibit the best methane conversion of 12%,whose aromatic selectivity increases from 27.2%to 52.2%compared with that of HZSM-5.Besides,the addition of methane further improves the production of high-valued aromatics compared with methanol to aromatics(MTA)reaction.展开更多
基金Supported by the National Natural Science Foundation of China (Grant No. 90717104)the Program for New Century Excellent Talents in University (Grant No. NCET-06-0214), Ministry of Education of China
文摘Due to the highly sensitive electrochemiluminescence (ECL), tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy)32+) is often used in the field of bioarrays with the help of co-reactants. However, the generally used co-reactant, tripropylamine (TPA), is toxic, corrosive and volatile. Therefore, the search for safe, sensitive and economical co-reactants is critical. Herein, three aminocarboxylic acids, ethylenediamine-tetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and 2-hydroxyethylethylene diaminetriacetic acid (HEDTA), have been investigated as potential co-reactants for promoting Ru(bpy)32+ ECL behaviour. A possible ECL mechanism is also presented. The experimental results suggested that the co-reactants have a different ECL behaviour compared to TPA, such as different pH- and surfactant-responses. The detection limits of Ru(bpy)32+ using NTA, EDTA and HEDTA as co-reactants are 1, 60 and 680 fmol·L-1, respectively. The results indicate that NTA has a much higher efficiency than TPA to excite Ru(bpy)3 2+ ECL under their own optimal conditions. NTA could be widely used in many fields because it is less toxic, corrosive and volatile than TPA. Moreover, using Ru(bpy)3 2+ ECL, a sensitive method for the detection of aminocarboxylic acids is also developed. An improvement of four orders of magnitude in detection limits is obtained for EDTA compared to the known Ru(bpy) 3 2+ chemiluminescent methods.
基金Funded by the National Natural Science Foundation of China (NSFC, No. 60376019)
文摘HfTiN film was deposited by co-reactive sputtering and then was annealed in dif-ferent gas ambients at temperature of 650 ℃ for 2 min to form HfTiON film. Capacitance-voltage and gate-leakage characteristics were investigated. The N2O-annealed sample exhibited small inter-face-state and oxide-charge densities, and enhanced reliability, which was attributed to the fact that nitridation could create strong Si≡N bonds to passivate dangling Si bonds and replaced strained Si-O bonds, thus forming a hardened dielectric/Si interface with high reliability. As a result, it is possible to prepare high-quality HfTiON gate dielectric of small-scaling CMOS devices in the industry-preferred N2O environment.
基金Project supported by the National Natural Science Foundation of China(No.U1663222)。
文摘A co-reaction of methane with methanol over zeolite catalysts has emerged as a new approach to the long-standing challenge of methane transformation.However,the effect of catalyst acid properties on the co-reaction has been rarely studied.In this study,a series of HZSM-5 zeolites with comparable diffusion abilities and various acidities were synthesized directly through steaming with 100%water vapor at 693 K.The co-reaction of methane and methanol was subsequently evaluated.Br?nsted acidity at 0.262 mmol/g was detected to reach the maximum methane conversion of 5.42%at 673 K,which was also the odd point in the relationship between acid concentration and C4 hydrogen transfer index.Moreover,the influence of methanol feed was investigated over parent and steamed ZSM-5 catalyst,with results showing that excessive acid sites or methanol molecules reduce methane conversion.It is proposed that acid sites adsorbed with methanol molecules construct the methane activation sites.Hence,a proper design of zeolite acidity should be achieved to obtain higher methane conversion in the co-reaction process.
基金supported by the National Natural Science Foundation of China(No.U1663222).
文摘Acidity plays a vital role in methane conversion by co-feeding method,which is one of the best strategies to improve the utilization and gentle the reaction conditions of methane.In this work,Zn,Ni,Mo,La,Ga,Fe and Co-impregnated ZSM-5 zeolites have been prepared with the same substitutions to variate the acidities and tested in co-aromatization of methanol with methane.It is demonstrated that the new medium-strong acid sites formed by metal and strong acid sites are the key role to activate methane in co-reaction.Zn-modified ZSM-5 catalyst is preferred to exhibit the best methane conversion of 12%,whose aromatic selectivity increases from 27.2%to 52.2%compared with that of HZSM-5.Besides,the addition of methane further improves the production of high-valued aromatics compared with methanol to aromatics(MTA)reaction.
