Two new Gd Ⅲ complexes with nitrilotriacetic acid(nta) and trans-1,2-cyclohexanediaminetetraacetic acid(Cydta) ligands were synthesized. Their crystal structures were determined by single-crystal X-ray structure anal...Two new Gd Ⅲ complexes with nitrilotriacetic acid(nta) and trans-1,2-cyclohexanediaminetetraacetic acid(Cydta) ligands were synthesized. Their crystal structures were determined by single-crystal X-ray structure analyses. The crystal data are as follows: K 3[Gd Ⅲ(nta) 2·(H 2O)]·6H 2O, monoclinic system, C2/c space group, a=1.534 81(15) nm, b=1.292 05(12) nm, c=2.610 8(3) nm, β=96.244(2)°, V=5.146 7(9) nm 3, Z=8, M=776.87, D c=2.005 g/cm 3, μ= 3.149 mm -1 and \{F(000)=\}3 080, R=0.024 5, wR=0.064 3 for 4 455 unique reflections and R= 0.028 9, wR=0.067 2 for all 10 305 reflections. The Gd ⅢN 2O 7 part in the [Gd Ⅲ(nta) 2(H 2O)] 3- anion is a pseudo-monocapped square antiprismatic nine-coordination structure.(NH 4)[Gd Ⅲ(Cydta)(H 2O) 2]·5H 2O, triclinic system, P1 space group, a=0.866 2(3) nm, b=1.006 7(3) nm, c= 1.444 8(5) nm, α= 88.282(5)°, β=75\^190(5)°, γ=88.317(4)°, V=1.217 2(7) nm 3, Z=2, M=643.69, D c=1.756 g/cm 3, μ=2.798 mm -1 and F(000)=650, R=0.030 3, wR=0.080 9 for 4 273 unique reflections and R=0.033 2, wR=0.082 5 for all 5 062 reflections. The Gd ⅢN 2O 6 part in the [Gd Ⅲ(Cydta)(H 2O) 2] - anion has a pseudo-square antiprismatic eight-coordination structure.展开更多
利用水热合成法合成了分子组成为(C6H11NH3)5H(P2Mo5O23)4H2O的杂多化合物, 用单晶X-ray衍射方法测定了它的结构,该晶体属于单斜晶系,空间群P21/c, a = 12.830(3), b = 14.848(3), c = 25.258(5) ? b = 92.95(3), Mr = 1483.62, V = 48...利用水热合成法合成了分子组成为(C6H11NH3)5H(P2Mo5O23)4H2O的杂多化合物, 用单晶X-ray衍射方法测定了它的结构,该晶体属于单斜晶系,空间群P21/c, a = 12.830(3), b = 14.848(3), c = 25.258(5) ? b = 92.95(3), Mr = 1483.62, V = 4805.1(17) 3, Z = 4, Dc = 2.051 g/cm3, m = 1.431 mm-1, F(000) = 3000, I >2s(I) 的可观察衍射点4426个, 最终结构偏差因子R = 0.0464, wR = 0.0801, S = 0.731。在[P2Mo5O23]6-杂多阴离子中5个MoO6八面体通过共边和共角相连, 形成1个近似的五角平面骨架, 2个PO4四面体加在五角平面的两侧。热性质研究表明杂多阴离子骨架在547.4 ℃左右分解。展开更多
Shape-selective methylation of 2-methylnaphthalene (2-MN) was carried out over NH 4 F and Pt modified HZSM-5 (SiO 2 /Al 2 O 3 = 83) catalysts in a fixed-bed down-flow reactor using methanol as methylating agent and 1,...Shape-selective methylation of 2-methylnaphthalene (2-MN) was carried out over NH 4 F and Pt modified HZSM-5 (SiO 2 /Al 2 O 3 = 83) catalysts in a fixed-bed down-flow reactor using methanol as methylating agent and 1,3,5-trimethylbenzene (1,3,5-TMB) as a solvent. Pt promoted HZSM-5 catalysts showed low concentration of coke-like polycondensed aromatics, NH 4 F modification decreased non-shape-selective acid sites. After Pt and NH 4 F co-modification, both conversion of 2-MN and selectivity to 2,6-DMN were improved. 6%NH 4 F/0.5%Pt/HZSM-5 catalyst exhibited 13.8% of 2-MN conversion with 6.2% of 2,6-DMN yield after 7 h time on stream (TOS), and 2,6-/2,7-DMN ratio of 1.7 after 10 h of TOS.展开更多
文摘Two new Gd Ⅲ complexes with nitrilotriacetic acid(nta) and trans-1,2-cyclohexanediaminetetraacetic acid(Cydta) ligands were synthesized. Their crystal structures were determined by single-crystal X-ray structure analyses. The crystal data are as follows: K 3[Gd Ⅲ(nta) 2·(H 2O)]·6H 2O, monoclinic system, C2/c space group, a=1.534 81(15) nm, b=1.292 05(12) nm, c=2.610 8(3) nm, β=96.244(2)°, V=5.146 7(9) nm 3, Z=8, M=776.87, D c=2.005 g/cm 3, μ= 3.149 mm -1 and \{F(000)=\}3 080, R=0.024 5, wR=0.064 3 for 4 455 unique reflections and R= 0.028 9, wR=0.067 2 for all 10 305 reflections. The Gd ⅢN 2O 7 part in the [Gd Ⅲ(nta) 2(H 2O)] 3- anion is a pseudo-monocapped square antiprismatic nine-coordination structure.(NH 4)[Gd Ⅲ(Cydta)(H 2O) 2]·5H 2O, triclinic system, P1 space group, a=0.866 2(3) nm, b=1.006 7(3) nm, c= 1.444 8(5) nm, α= 88.282(5)°, β=75\^190(5)°, γ=88.317(4)°, V=1.217 2(7) nm 3, Z=2, M=643.69, D c=1.756 g/cm 3, μ=2.798 mm -1 and F(000)=650, R=0.030 3, wR=0.080 9 for 4 273 unique reflections and R=0.033 2, wR=0.082 5 for all 5 062 reflections. The Gd ⅢN 2O 6 part in the [Gd Ⅲ(Cydta)(H 2O) 2] - anion has a pseudo-square antiprismatic eight-coordination structure.
基金Supported by the Program for New Century Excellent Talents in University (NCET-04-0268)the Expertise-Introduction Project for Disciplinary Innovation of Universities
文摘Shape-selective methylation of 2-methylnaphthalene (2-MN) was carried out over NH 4 F and Pt modified HZSM-5 (SiO 2 /Al 2 O 3 = 83) catalysts in a fixed-bed down-flow reactor using methanol as methylating agent and 1,3,5-trimethylbenzene (1,3,5-TMB) as a solvent. Pt promoted HZSM-5 catalysts showed low concentration of coke-like polycondensed aromatics, NH 4 F modification decreased non-shape-selective acid sites. After Pt and NH 4 F co-modification, both conversion of 2-MN and selectivity to 2,6-DMN were improved. 6%NH 4 F/0.5%Pt/HZSM-5 catalyst exhibited 13.8% of 2-MN conversion with 6.2% of 2,6-DMN yield after 7 h time on stream (TOS), and 2,6-/2,7-DMN ratio of 1.7 after 10 h of TOS.
