A series of Ru supported on CeO_2 and Ce_(0.7)Zr_(0.3)O_2(CeZrO) was prepared by incipient-wet impregnation method and investigated in the catalytic wet oxidation of N,N-dimethyl formamide(DMF) in batch reactor. The p...A series of Ru supported on CeO_2 and Ce_(0.7)Zr_(0.3)O_2(CeZrO) was prepared by incipient-wet impregnation method and investigated in the catalytic wet oxidation of N,N-dimethyl formamide(DMF) in batch reactor. The physicochemical property of the catalysts was characterized by Brunauer-Emmett-Teller(BET), X-ray diffraction(XRD), H_2 temperature-programmed reduction(H_2-TPR), X-ray photoelectron spectroscopy(XPS) and thermogravimetry(TG). Compared with 3%Ru/CeO_2, 3%Ru/Ce_(0.7)Zr_(0.3)O_2 catalyst exhibits much higher performance for DMF degradation due to the promotion of Ru dispersion and the transfer of active oxygen, and 99% DMF conversion and 97% COD elimination are obtained at 453 K,2.5 MPa oxygen pressure after 5 h. The reaction mechanism of DMF degradation was suggested. The carbonaceous species deposition and oxidation of Ru can be responsible for catalyst deactivation. And the catalyst activity can be recovered by air calcination and H_2 reduction.展开更多
Five new zwitterionic surfactants with long chain alkyl betaine structure incorporated with hydroxylpropyl group have been synthesized. Their structures were identified by elemental analysis, IR (HNMR)-H-1, and (CNMR)...Five new zwitterionic surfactants with long chain alkyl betaine structure incorporated with hydroxylpropyl group have been synthesized. Their structures were identified by elemental analysis, IR (HNMR)-H-1, and (CNMR)-C-13. Surface tension experiments showed that these surfactants have higher surface activity than those without hydroxypropyl group. The values of CMC and gamma(CMC) of these surfactants have been determined.展开更多
The redox behaviours of a donor-acceptor model compound. p-tricyano-ethenyl-N, N-dimethyl aniline was investigated by electrochemical and spectroelectrochemical methods. The results indicate that charge transfer betwe...The redox behaviours of a donor-acceptor model compound. p-tricyano-ethenyl-N, N-dimethyl aniline was investigated by electrochemical and spectroelectrochemical methods. The results indicate that charge transfer between the donor(amino) and the acceptor(cyanoethenyl) groups takes place in the process of oxidation of this compound.展开更多
The title compound 3-bromo-5-（4-chlorophenyl）-4-cyanopyrrole-N,N-dimethyl-2-amide（3） was synthesized with 4-bromo-2-（4-chlorophenyl）-5-（trifluoromethyl）-1H-pyrrole-3-carbonitrile（1） and N,N-dimethylformamide...The title compound 3-bromo-5-（4-chlorophenyl）-4-cyanopyrrole-N,N-dimethyl-2-amide（3） was synthesized with 4-bromo-2-（4-chlorophenyl）-5-（trifluoromethyl）-1H-pyrrole-3-carbonitrile（1） and N,N-dimethylformamide（2） by the α-C acylation reaction catalyzed by potassium t-butoxide, and characterized by IR, 1H-NMR and X-ray single-crystal diffraction. It crystallizes in monoclinic, space group P2（1/n）with a = 12.789（2）, b = 13.783（2）, c = 17.980（3） °, β = 109.230（3）°, V = 2992.5 A3, Mr = 352.62, Dc = 1.565 mg/m3, Z = 8, m = 2.924 mm-1, F（000） = 1408, the final R = 0.0424 and w R = 0.0973 for 3518 observed reflections with I 〉 2σ（I）. A total of 23559 reflections were collected, of which 6242 were independent（Rint = 0.0566）. The insecticidal, herbicidal and antibacterial activities of compound 3 were determined, and the experimental results showed that the mortality of 3 at the concentration of 100 ppm on the Fipronil against Linnaeus was 76.6%, the growth inhibition rate of 3 against Cynodon Dactylon under the condition of 100 ppm was 35.8% and the inhibitory activity of 3 at the concentration of 25 ppm against Fusarium graminearum reached 50.9%. Hence, the title compound has the value of further research and application prospect.展开更多
A 2D plane coordination compound [Ag_2（Dpya）_2.（NO_3）_2]n was synthesized and characterized by FT-IR,elemental analysis and TG analysis.The red crystal was obtained via solvent diffusion method at room temperature...A 2D plane coordination compound [Ag_2（Dpya）_2.（NO_3）_2]n was synthesized and characterized by FT-IR,elemental analysis and TG analysis.The red crystal was obtained via solvent diffusion method at room temperature and is slightly soluble in organic solvents.Its structure was determined by single-crystal X-ray diffraction analysis.It crystallizes in monoclinic,space group P1 with a = 10.7995（13）,b = 7.4748（8）,c = 18.364（2） A,β = 98.916（4）o,V = 1464.5（3） A^3,Z = 2,C_（26）H_（28）Ag_2N_（10）O_6,M_r = 792.32,Dc = 1.302 Mg/m^3,F（000） = 792,μ（Mo Ka） = 1.356 mm^-1,R = 0.0575 and w R = 0.0826.The compound [Ag_2（Dpya）_2.（NO_3）_2]_n is a two-dimensional structure and there are two kinds of coordination configurations about the Ag atoms in the compound.The Ag（1） center is tetrahedrally coordinated with two O atoms of NO_3^-and two N atoms from the ligand Dpya.Meanwhile,the Ag（2） is five-coordinated by five O atoms from three NO_3^-anions.The Ag centers（Ag（1） and Ag（2）） connect to themselves as well as with each other by the bridging NO_3^-anions.And the coordination compound shows photoluminescence with an emission peak at 530 nm（λex = 450 nm） as the ligand Dpya.展开更多
In this work,the 0.1-0.5 mol·L-1 N,N-dimethylhydroxylamine(DMHA) were irradiated to 5-25 kGy,and gaseous products of mainly hydrogen,methane,ethane and n-butane were measured by gas chromatography.The results sho...In this work,the 0.1-0.5 mol·L-1 N,N-dimethylhydroxylamine(DMHA) were irradiated to 5-25 kGy,and gaseous products of mainly hydrogen,methane,ethane and n-butane were measured by gas chromatography.The results show that the volume fraction of hydrogen and methane increases with the concentration of DMHA and dose,and the latter does not change markedly at high doses.展开更多
The extraction of uranyl nitrate by novel extractants of N,N-dimethyl-N',N'-dioctylsuccinylamide(DMDOSA)and N,N-dimethyl-N',N'-didecylsuccinylamide(DMDDSA) from aqueous nitric/nitrate solutions was inv...The extraction of uranyl nitrate by novel extractants of N,N-dimethyl-N',N'-dioctylsuccinylamide(DMDOSA)and N,N-dimethyl-N',N'-didecylsuccinylamide(DMDDSA) from aqueous nitric/nitrate solutions was investigated.It was found both the concentration of HNO_3 and extractants had an effect on the U(Ⅵ) extraction distribution.The extraction mechanism was established,and stoichiometry of the main extracted species was confirmed to be UO_2(NO_3)_2·2DMDOSA and UO_2(NO_3)_2·2DMDDSA,respectively.Both of the extraction reactions are exothermic.FTIR spectral study of the U(Ⅵ) extracted species was also made.展开更多
N,N-dimethyl-3-oxa-glutaramic acid was purified and characterized by 1H-NMR, Fourier transform in-frared spectroscopy (FT-IR) and elemental analysis. The thermal decomposition of the title compound was studied by mean...N,N-dimethyl-3-oxa-glutaramic acid was purified and characterized by 1H-NMR, Fourier transform in-frared spectroscopy (FT-IR) and elemental analysis. The thermal decomposition of the title compound was studied by means of thermogravimetry differential thermogravimetry (TG-DTG) and FT-IR. The ki-netic parameters of its second-stage decomposition reaction were calculated and the decomposition mechanism was discussed. The kinetic model function in a differential form, apparent activation energy and pre-exponential constant of the reaction are 3/2 [(1-α) 1/3-1]-1, 203.75 kJ-mol-1 and 1017.95s-1, respec-tively. The values of ΔS≠, ΔH≠ andΔG≠ of the reaction are 94.28 J-mol-1-K-1, 203.75 kJ-mol-1 and 155.75 kJ-mol-1, respectively.展开更多
The hydrolysis mechanisms of N,N-dimethyl-N′-(2′,3′-dideoxy-3′-thiacytidine)formamidine (FA-3TC) in the gas phase and in aqueous solution were studied by use of the density functional theory B3LYP/6-31+G(d, p) met...The hydrolysis mechanisms of N,N-dimethyl-N′-(2′,3′-dideoxy-3′-thiacytidine)formamidine (FA-3TC) in the gas phase and in aqueous solution were studied by use of the density functional theory B3LYP/6-31+G(d, p) method. Two possible reaction pathways in the title reaction were considered. In one pathway water attacks the C=N double bond first (path A) while in the other water attacks the C—N single bond first (path B). The calculated results indicate that the first step in both pathways is the rate-limiting process and path A is more favorable than path B in the gas phase. The effect of solvent water on the title reaction was assessed at the B3LYP/6-31+G(d, p) level of theory based on the po-larizable continuum model (CPCM). In water the first mechanism (path A) is also favored.展开更多
基金This project supported by the National Key Research and Development Program of China(2016YFC0204300)the National Natural Science Foundation of China(21171055,21333003,21571061)+1 种基金the"Shu Guang"Project of the Shanghai Municipal Education Commission(12SG29)the Commission of Science and Technology of Shanghai Municipality(15DZ1205305)
文摘A series of Ru supported on CeO_2 and Ce_(0.7)Zr_(0.3)O_2(CeZrO) was prepared by incipient-wet impregnation method and investigated in the catalytic wet oxidation of N,N-dimethyl formamide(DMF) in batch reactor. The physicochemical property of the catalysts was characterized by Brunauer-Emmett-Teller(BET), X-ray diffraction(XRD), H_2 temperature-programmed reduction(H_2-TPR), X-ray photoelectron spectroscopy(XPS) and thermogravimetry(TG). Compared with 3%Ru/CeO_2, 3%Ru/Ce_(0.7)Zr_(0.3)O_2 catalyst exhibits much higher performance for DMF degradation due to the promotion of Ru dispersion and the transfer of active oxygen, and 99% DMF conversion and 97% COD elimination are obtained at 453 K,2.5 MPa oxygen pressure after 5 h. The reaction mechanism of DMF degradation was suggested. The carbonaceous species deposition and oxidation of Ru can be responsible for catalyst deactivation. And the catalyst activity can be recovered by air calcination and H_2 reduction.
文摘Five new zwitterionic surfactants with long chain alkyl betaine structure incorporated with hydroxylpropyl group have been synthesized. Their structures were identified by elemental analysis, IR (HNMR)-H-1, and (CNMR)-C-13. Surface tension experiments showed that these surfactants have higher surface activity than those without hydroxypropyl group. The values of CMC and gamma(CMC) of these surfactants have been determined.
文摘The redox behaviours of a donor-acceptor model compound. p-tricyano-ethenyl-N, N-dimethyl aniline was investigated by electrochemical and spectroelectrochemical methods. The results indicate that charge transfer between the donor(amino) and the acceptor(cyanoethenyl) groups takes place in the process of oxidation of this compound.
基金supported by the National Natural Science Foundation of China(No.21272086)
文摘The title compound 3-bromo-5-（4-chlorophenyl）-4-cyanopyrrole-N,N-dimethyl-2-amide（3） was synthesized with 4-bromo-2-（4-chlorophenyl）-5-（trifluoromethyl）-1H-pyrrole-3-carbonitrile（1） and N,N-dimethylformamide（2） by the α-C acylation reaction catalyzed by potassium t-butoxide, and characterized by IR, 1H-NMR and X-ray single-crystal diffraction. It crystallizes in monoclinic, space group P2（1/n）with a = 12.789（2）, b = 13.783（2）, c = 17.980（3） °, β = 109.230（3）°, V = 2992.5 A3, Mr = 352.62, Dc = 1.565 mg/m3, Z = 8, m = 2.924 mm-1, F（000） = 1408, the final R = 0.0424 and w R = 0.0973 for 3518 observed reflections with I 〉 2σ（I）. A total of 23559 reflections were collected, of which 6242 were independent（Rint = 0.0566）. The insecticidal, herbicidal and antibacterial activities of compound 3 were determined, and the experimental results showed that the mortality of 3 at the concentration of 100 ppm on the Fipronil against Linnaeus was 76.6%, the growth inhibition rate of 3 against Cynodon Dactylon under the condition of 100 ppm was 35.8% and the inhibitory activity of 3 at the concentration of 25 ppm against Fusarium graminearum reached 50.9%. Hence, the title compound has the value of further research and application prospect.
基金the sponsorship and financial support from the Key Laboratory of Organic Synthesis of Jiangsu Province
文摘A 2D plane coordination compound [Ag_2（Dpya）_2.（NO_3）_2]n was synthesized and characterized by FT-IR,elemental analysis and TG analysis.The red crystal was obtained via solvent diffusion method at room temperature and is slightly soluble in organic solvents.Its structure was determined by single-crystal X-ray diffraction analysis.It crystallizes in monoclinic,space group P1 with a = 10.7995（13）,b = 7.4748（8）,c = 18.364（2） A,β = 98.916（4）o,V = 1464.5（3） A^3,Z = 2,C_（26）H_（28）Ag_2N_（10）O_6,M_r = 792.32,Dc = 1.302 Mg/m^3,F（000） = 792,μ（Mo Ka） = 1.356 mm^-1,R = 0.0575 and w R = 0.0826.The compound [Ag_2（Dpya）_2.（NO_3）_2]_n is a two-dimensional structure and there are two kinds of coordination configurations about the Ag atoms in the compound.The Ag（1） center is tetrahedrally coordinated with two O atoms of NO_3^-and two N atoms from the ligand Dpya.Meanwhile,the Ag（2） is five-coordinated by five O atoms from three NO_3^-anions.The Ag centers（Ag（1） and Ag（2）） connect to themselves as well as with each other by the bridging NO_3^-anions.And the coordination compound shows photoluminescence with an emission peak at 530 nm（λex = 450 nm） as the ligand Dpya.
基金Supported by Natural Science Foundation of China(Contract No.20771074)Shanghai Leading Academic Disciplines(Contract No.S30109)
文摘In this work,the 0.1-0.5 mol·L-1 N,N-dimethylhydroxylamine(DMHA) were irradiated to 5-25 kGy,and gaseous products of mainly hydrogen,methane,ethane and n-butane were measured by gas chromatography.The results show that the volume fraction of hydrogen and methane increases with the concentration of DMHA and dose,and the latter does not change markedly at high doses.
基金supported by the National Natural Science Foundation of China(Nos.21077044 and 21171069)
文摘The extraction of uranyl nitrate by novel extractants of N,N-dimethyl-N',N'-dioctylsuccinylamide(DMDOSA)and N,N-dimethyl-N',N'-didecylsuccinylamide(DMDDSA) from aqueous nitric/nitrate solutions was investigated.It was found both the concentration of HNO_3 and extractants had an effect on the U(Ⅵ) extraction distribution.The extraction mechanism was established,and stoichiometry of the main extracted species was confirmed to be UO_2(NO_3)_2·2DMDOSA and UO_2(NO_3)_2·2DMDDSA,respectively.Both of the extraction reactions are exothermic.FTIR spectral study of the U(Ⅵ) extracted species was also made.
基金the National Natural Science Foundation of China (Grant No. 20106009)
文摘N,N-dimethyl-3-oxa-glutaramic acid was purified and characterized by 1H-NMR, Fourier transform in-frared spectroscopy (FT-IR) and elemental analysis. The thermal decomposition of the title compound was studied by means of thermogravimetry differential thermogravimetry (TG-DTG) and FT-IR. The ki-netic parameters of its second-stage decomposition reaction were calculated and the decomposition mechanism was discussed. The kinetic model function in a differential form, apparent activation energy and pre-exponential constant of the reaction are 3/2 [(1-α) 1/3-1]-1, 203.75 kJ-mol-1 and 1017.95s-1, respec-tively. The values of ΔS≠, ΔH≠ andΔG≠ of the reaction are 94.28 J-mol-1-K-1, 203.75 kJ-mol-1 and 155.75 kJ-mol-1, respectively.
基金the National Natural Science Foundation of China (Grant Nos. 20473055 and 20773089)the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry (Grant No. 20071108-18-15)
文摘The hydrolysis mechanisms of N,N-dimethyl-N′-(2′,3′-dideoxy-3′-thiacytidine)formamidine (FA-3TC) in the gas phase and in aqueous solution were studied by use of the density functional theory B3LYP/6-31+G(d, p) method. Two possible reaction pathways in the title reaction were considered. In one pathway water attacks the C=N double bond first (path A) while in the other water attacks the C—N single bond first (path B). The calculated results indicate that the first step in both pathways is the rate-limiting process and path A is more favorable than path B in the gas phase. The effect of solvent water on the title reaction was assessed at the B3LYP/6-31+G(d, p) level of theory based on the po-larizable continuum model (CPCM). In water the first mechanism (path A) is also favored.
