The rules on regulating aromatic compounds production was investigated by aqueous cat- alytic reforming of sorbitol. It was found that aromatics, ketones, furans, organic acids were main compounds in organic phase. Th...The rules on regulating aromatic compounds production was investigated by aqueous cat- alytic reforming of sorbitol. It was found that aromatics, ketones, furans, organic acids were main compounds in organic phase. The obvious effect of metal content showed that the highest carbon selectivity of aromatics was 34.36% when 3wt% Ni content was loaded on HZSM-5 zeolite modified by MCM-41. However, it was decreased only to 4.82% when Ni content was improved to 20wt%. Meanwhile, different reaction parameters also displayed important impacts on carbon selectivity. It was improved with the increase of temperature, while it was decreased as liquid hourly space velocity and hydrogen pressure was increased. The results showed that appropriate higher temperature, longer contact time and lower hy- drogen pressure were in favor of aromatics information, which suggested a feasible process to solve energy crisis.展开更多
A dual-reactor, assembled with the on-line syngas conditioning and methanol synthesis, was successfully applied for high efficient conversion of rich CO2 bio-oil derived syngas to bio-methanol. In the forepart catalys...A dual-reactor, assembled with the on-line syngas conditioning and methanol synthesis, was successfully applied for high efficient conversion of rich CO2 bio-oil derived syngas to bio-methanol. In the forepart catalyst bed reactor, the catalytic conversion can effectively adjust the rich-CO2 crude bio-syngas into the CO-containing bio-syngas using the CuZnA1Zr catalyst. After the on-line syngas conditioning at 450℃, the CO2/CO ratio in the blo- syngas significantly decreased from 6.3 to 1.2. In the rearward catalyst bed reactor, the conversion of the conditioned bio-syngas to bio-methanol shows the maximum yield about 1.21 kg/（kgcatarh） MeOH with a methanol selectivity of 97.9% at 260 ~C and 5.05 MPa using conventional CuZnA1 catalyst, which is close to the level typically obtained in the conventional methanol synthesis process using natural gas. The influences of temperature, pressure and space velocity on the bio-methanol synthesis were also investigated in detail.展开更多
We studied the hydrogenation of 2‐ethylanthraquinone（eAQ） over Pd/SiO2/COR（COR = cordierite） monometallic and Pd‐M/SiO2/COR（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts, which were prepared by the c...We studied the hydrogenation of 2‐ethylanthraquinone（eAQ） over Pd/SiO2/COR（COR = cordierite） monometallic and Pd‐M/SiO2/COR（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts, which were prepared by the co‐impregnation method. Detailed investigations showed that the particle sizes and structures of the Pd‐M（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts were great‐ly affected by the second metal M and the mass ratio of Pd to the second metal M. By virtue of the small particle size and the strong interaction between Pd and Ni of Pd‐Ni alloy, Pd‐Ni bimetallic monolithic catalysts with the mass ratio of Pd/Ni = 2 achieved the highest H2O2 yield（7.5 g/L） and selectivity（95.3%）. Moreover, density functional theory calculations were performed for eAQ ad‐sorption to gain a better mechanistic understanding of the molecule‐surface interactions between eAQ and the Pd（1 1 1） or PdM（1 1 1）（M = Ni, Fe, Mn, and Cu） surfaces. It was found that the high activity of the bimetallic Pd‐Ni catalyst was a result of strong chemisorption between Pd3Ni1（1 1 1） and the carbonyl group of eAQ.展开更多
The kinetics of CO2 reforming of methane has been studied at 976－1033K on a commercial NiO/CaO/Al2O3 catalyst in a packed-bed continuous reactor. The reaction was carried out at atmospheric pressure and CO2/CH4 ratio...The kinetics of CO2 reforming of methane has been studied at 976－1033K on a commercial NiO/CaO/Al2O3 catalyst in a packed-bed continuous reactor. The reaction was carried out at atmospheric pressure and CO2/CH4 ratio ＞ 2. The Hougen-Watson rate models were fitted to experimental data assuming the disso ciative adsorption of methane as the rate-determining step. The reaction rate showed an effective reaction order of about unity for CH4. The apparent activity energy was found to be 104 kJ·mol-1. Therefore the kinetic reaction parameters were determined and a possible reaction mechanism was proposed.展开更多
The calcined magnesite was utilized as a kind of MgO bearing additive to produce MgO bearing pellets. The effects of MgO on densification and consolidation of pellets were investigated. The experimental results show t...The calcined magnesite was utilized as a kind of MgO bearing additive to produce MgO bearing pellets. The effects of MgO on densification and consolidation of pellets were investigated. The experimental results show that, at the same process parameters, the porosity and pore size distribution of green pellets have no evident relation with the MgO bearing additive, pore size of green pellets is between 15 μm and 35 μm and the porosity of green pellets is about 34%. There is a densification and consolidation phenomenon during the induration process; the pore size and porosity of product pellets decrease gradually; and the structure of product pellets becomes dense. MgO makes a negative effect on the densification and consolidation of product pellets, the densification ratio of pellets decreases from 46.3% to 28.6% with the addition of MgO bearing additive from 0 to 2.0 %. The porosity and the pore size of product pellets increase gradually with the increase of MgO content; When the mass fraction of MgO bearing additive increases from 0 to 2.0%, the pore size of product pellet increases and the pore size distributes in a large range. Also, the porosity increases from 18.61% to 24.06%.展开更多
In this work,hydrogen is produced from partial oxidation reforming of dimethyl ether （DME） by a plasma-catalyst hybrid reformer under atmospheric pressure.The plasma-catalyst hybrid reformer which includes both plas...In this work,hydrogen is produced from partial oxidation reforming of dimethyl ether （DME） by a plasma-catalyst hybrid reformer under atmospheric pressure.The plasma-catalyst hybrid reformer which includes both plasma and catalyst reactors is designed.A spark discharge is used as a non-equilibrium plasma source,and it is used to ionize the mixture of DME and air.The performances of the reformer are characterized experimentally in terms of gas concentrations,hydrogen yield,DME conversion ratio,and specific energy consumption.The effects of discharge frequency,reaction temperature,air-to-DME ratio and space velocity are investigated.The experimental results show that the plasma-catalyst hybrid reformer enhances hydrogen yield when reaction temperature drops below 620 ℃.At 450 ℃,hydrogen yield of hybrid reforming is almost three times that of catalyst reforming.When space velocity is 510 h-1,hydrogen yield is 67.7%,and specific energy consumption is 12.2 k J/L-H2.展开更多
Three series of novel anti-immunodeficiency virus 1 （HIV-1） dual （RT/1N） inhibitors were rationally designed by introducing a functioning diketo acid （DKA） into pyridin-2-one scaffold. To efficiently analyze inh...Three series of novel anti-immunodeficiency virus 1 （HIV-1） dual （RT/1N） inhibitors were rationally designed by introducing a functioning diketo acid （DKA） into pyridin-2-one scaffold. To efficiently analyze inhibitory activity, these compounds were screened against HIV-1 RT and IN respectively via surface plasmon resonance （SPR）, and active compounds were subsequently evaluated by enzyme assay. It was noteworthy that compound A2 exhibited moderate activity against both HIV-1 RT and IN. This result provided information for further development of pyridinone analogues as potent dual HIV-1 inhibitors.展开更多
Six triarylamine derivatives 1–6 with branched multi-pyridine substituents were prepared and characterized. These compounds are distinguished by the substituent on one of the phenyl group with NO2 for 1, CN for 2, Cl...Six triarylamine derivatives 1–6 with branched multi-pyridine substituents were prepared and characterized. These compounds are distinguished by the substituent on one of the phenyl group with NO2 for 1, CN for 2, Cl for 3, p-C6 H4 OMe for 4, OMe for 5,and NMe2 for 6, respectively. As revealed by single crystal X-ray analysis, these substituents play an important role in determining the configuration of the triarylamine framework and the crystal packing of 1–6. The emission properties of these compounds were examined in different solvents(toluene, CH2 Cl2, acetone, tetrahydrofuran(THF), and N,N-dimethylformamide(DMF)) and in solid states. Distinct dual emissions from the localized emissive state and the intramolecular charge transfer state were observed for compound 5 in CH2 Cl2. Compounds 1 and 6 show apparent aggregated enhanced emissions in acetone/H2 O.The emission properties of these compounds were further modulated by the addition of tris(pentafluorophenyl)borane. In addition, density functional theory(DFT) and time-dependent DFT(TDDFT) calculations have been performed on the ground and singlet excited states to complement the experimental findings.展开更多
文摘The rules on regulating aromatic compounds production was investigated by aqueous cat- alytic reforming of sorbitol. It was found that aromatics, ketones, furans, organic acids were main compounds in organic phase. The obvious effect of metal content showed that the highest carbon selectivity of aromatics was 34.36% when 3wt% Ni content was loaded on HZSM-5 zeolite modified by MCM-41. However, it was decreased only to 4.82% when Ni content was improved to 20wt%. Meanwhile, different reaction parameters also displayed important impacts on carbon selectivity. It was improved with the increase of temperature, while it was decreased as liquid hourly space velocity and hydrogen pressure was increased. The results showed that appropriate higher temperature, longer contact time and lower hy- drogen pressure were in favor of aromatics information, which suggested a feasible process to solve energy crisis.
基金This work was supported by the National High Tech Research and Development Program （No.2009AA05Z435）, the National Basic Research Program of Ministry of Science and Technology of China （No.2007CB210206）, and the National Natural Science Foundation of China （No.50772107）.
文摘A dual-reactor, assembled with the on-line syngas conditioning and methanol synthesis, was successfully applied for high efficient conversion of rich CO2 bio-oil derived syngas to bio-methanol. In the forepart catalyst bed reactor, the catalytic conversion can effectively adjust the rich-CO2 crude bio-syngas into the CO-containing bio-syngas using the CuZnA1Zr catalyst. After the on-line syngas conditioning at 450℃, the CO2/CO ratio in the blo- syngas significantly decreased from 6.3 to 1.2. In the rearward catalyst bed reactor, the conversion of the conditioned bio-syngas to bio-methanol shows the maximum yield about 1.21 kg/（kgcatarh） MeOH with a methanol selectivity of 97.9% at 260 ~C and 5.05 MPa using conventional CuZnA1 catalyst, which is close to the level typically obtained in the conventional methanol synthesis process using natural gas. The influences of temperature, pressure and space velocity on the bio-methanol synthesis were also investigated in detail.
基金supported by the National Natural Science Foundation of China (21476009, 21406007, U1462104)~~
文摘We studied the hydrogenation of 2‐ethylanthraquinone（eAQ） over Pd/SiO2/COR（COR = cordierite） monometallic and Pd‐M/SiO2/COR（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts, which were prepared by the co‐impregnation method. Detailed investigations showed that the particle sizes and structures of the Pd‐M（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts were great‐ly affected by the second metal M and the mass ratio of Pd to the second metal M. By virtue of the small particle size and the strong interaction between Pd and Ni of Pd‐Ni alloy, Pd‐Ni bimetallic monolithic catalysts with the mass ratio of Pd/Ni = 2 achieved the highest H2O2 yield（7.5 g/L） and selectivity（95.3%）. Moreover, density functional theory calculations were performed for eAQ ad‐sorption to gain a better mechanistic understanding of the molecule‐surface interactions between eAQ and the Pd（1 1 1） or PdM（1 1 1）（M = Ni, Fe, Mn, and Cu） surfaces. It was found that the high activity of the bimetallic Pd‐Ni catalyst was a result of strong chemisorption between Pd3Ni1（1 1 1） and the carbonyl group of eAQ.
基金the Consejo Nacional de Investigacions Cientificas y Tecnicas (CONICET).
文摘The kinetics of CO2 reforming of methane has been studied at 976－1033K on a commercial NiO/CaO/Al2O3 catalyst in a packed-bed continuous reactor. The reaction was carried out at atmospheric pressure and CO2/CH4 ratio ＞ 2. The Hougen-Watson rate models were fitted to experimental data assuming the disso ciative adsorption of methane as the rate-determining step. The reaction rate showed an effective reaction order of about unity for CH4. The apparent activity energy was found to be 104 kJ·mol-1. Therefore the kinetic reaction parameters were determined and a possible reaction mechanism was proposed.
基金Projects(51074206,51074040) supported by the National Natural Science Foundation of China
文摘The calcined magnesite was utilized as a kind of MgO bearing additive to produce MgO bearing pellets. The effects of MgO on densification and consolidation of pellets were investigated. The experimental results show that, at the same process parameters, the porosity and pore size distribution of green pellets have no evident relation with the MgO bearing additive, pore size of green pellets is between 15 μm and 35 μm and the porosity of green pellets is about 34%. There is a densification and consolidation phenomenon during the induration process; the pore size and porosity of product pellets decrease gradually; and the structure of product pellets becomes dense. MgO makes a negative effect on the densification and consolidation of product pellets, the densification ratio of pellets decreases from 46.3% to 28.6% with the addition of MgO bearing additive from 0 to 2.0 %. The porosity and the pore size of product pellets increase gradually with the increase of MgO content; When the mass fraction of MgO bearing additive increases from 0 to 2.0%, the pore size of product pellet increases and the pore size distributes in a large range. Also, the porosity increases from 18.61% to 24.06%.
基金Project(21106002)supported by the National Natural Science Foundation of ChinaProject(2010DFA72760)supported by Collaboration on Cutting-Edge Technology Development of Electric Vehicle,China
文摘In this work,hydrogen is produced from partial oxidation reforming of dimethyl ether （DME） by a plasma-catalyst hybrid reformer under atmospheric pressure.The plasma-catalyst hybrid reformer which includes both plasma and catalyst reactors is designed.A spark discharge is used as a non-equilibrium plasma source,and it is used to ionize the mixture of DME and air.The performances of the reformer are characterized experimentally in terms of gas concentrations,hydrogen yield,DME conversion ratio,and specific energy consumption.The effects of discharge frequency,reaction temperature,air-to-DME ratio and space velocity are investigated.The experimental results show that the plasma-catalyst hybrid reformer enhances hydrogen yield when reaction temperature drops below 620 ℃.At 450 ℃,hydrogen yield of hybrid reforming is almost three times that of catalyst reforming.When space velocity is 510 h-1,hydrogen yield is 67.7%,and specific energy consumption is 12.2 k J/L-H2.
基金National Natural Science Foundation of China(Grant No.21172014,812111023 and 81172733)grants from the Ministry of Science and Technology of China(Grant No.200 9ZX09301-010)
文摘Three series of novel anti-immunodeficiency virus 1 （HIV-1） dual （RT/1N） inhibitors were rationally designed by introducing a functioning diketo acid （DKA） into pyridin-2-one scaffold. To efficiently analyze inhibitory activity, these compounds were screened against HIV-1 RT and IN respectively via surface plasmon resonance （SPR）, and active compounds were subsequently evaluated by enzyme assay. It was noteworthy that compound A2 exhibited moderate activity against both HIV-1 RT and IN. This result provided information for further development of pyridinone analogues as potent dual HIV-1 inhibitors.
基金supported by the National Natural Science Foundation of China(91622120,21601194,21472196,21501183,21521062)the Ministry of Science and Technology of China(2012YQ120060)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB 12010400)Science and Technology Commission of Shanghai Municipality(16DZ1100300)
文摘Six triarylamine derivatives 1–6 with branched multi-pyridine substituents were prepared and characterized. These compounds are distinguished by the substituent on one of the phenyl group with NO2 for 1, CN for 2, Cl for 3, p-C6 H4 OMe for 4, OMe for 5,and NMe2 for 6, respectively. As revealed by single crystal X-ray analysis, these substituents play an important role in determining the configuration of the triarylamine framework and the crystal packing of 1–6. The emission properties of these compounds were examined in different solvents(toluene, CH2 Cl2, acetone, tetrahydrofuran(THF), and N,N-dimethylformamide(DMF)) and in solid states. Distinct dual emissions from the localized emissive state and the intramolecular charge transfer state were observed for compound 5 in CH2 Cl2. Compounds 1 and 6 show apparent aggregated enhanced emissions in acetone/H2 O.The emission properties of these compounds were further modulated by the addition of tris(pentafluorophenyl)borane. In addition, density functional theory(DFT) and time-dependent DFT(TDDFT) calculations have been performed on the ground and singlet excited states to complement the experimental findings.
