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1.
在水热条件下，得到了2例新的配位聚合物[Co(L)0.5(1，3-bib)] (1)和[Ni2(L)(1，4-bib)3(H2O)2]·2H2O (2)，其中L=1，2，4，5-苯四酸，1，3-bib=1，3-双((1H-咪唑1-基)甲基)苯，1，4-bib=1，4-双((1H-咪唑1-基)甲基)苯。并利用元素分析、红外光谱、单晶X射线衍射等对其进行了结构表征。结果表明：1和2均为三维网状结构，完全去质子化的配体(L4-)在1和2中分别采取了μ4-к2∶к1∶к2∶к1和μ2-к1∶к0∶к1∶к0的配位方式。进一步的研究表明，配合物1在H2O2和可见光照射的条件下，在水溶液中对染料甲基橙(MO)和亚甲蓝(MB)有很好的降解效果：在180 min时，降解率分别达到83.2%和84.5%。配合物2在同样的条件下，在水溶液中对染料MB和罗丹明B(RhB)也有较好的降解作用：在180 min时，降解率分别为87.0%和77.4%。此外还详细探讨了1和2对染料光催化降解的机理。 相似文献
2.
Ten solid complexes of zinc nitrate with L-α-leucine(Leu)， L-α-valine(Val)， L-α-tryptophan(Try) and L-α-threonine(Thr) were prepared in water. The compositions of these complexes are determined by chemical analysis and elemental analysis， which are identified as Zn(Leu)(NO3)2·2H2O(A)， Zn(Leu)2(NO3)2·H2O(B)， Zn(Val)(NO3)2·2H2O(C)， Zn(Val)2(NO3)2·H2O(D)， Zn(Val)3(NO3)2·H2O(E)， Zn(Try)(NO3)2·2H2O(F)， Zn(Try)2(NO3)2·H2O(G)， Zn(Thr)(NO3)2·2H2O(H)， Zn(Thr)2(NO3)2·H2O(I) and Zn(Thr)3(NO3)·H2O(J). The constant-volume combustion energies of the complexes， ΔcU(complex)， were determined by a precise rotating bomb calorimeter at 298.15K. Standard enthalpies of combustion，ΔcHm?(complex， s， 298.15K)， and standard enthalpies of formation， ΔfHm?(complex，s，298.15K) for these complexes were calculated as (4523.22±2.08)， (7208.86±4.28)， (3442.21±1.85)， (5971.21±3.32)， (9007.26±4.24)， (5802.35±2.14)， (10891.58±3.01)， (2147.40±1.28)， (4120.83±0.99)， (6444.68±3.85)kJ·mol-1 and (615.67±2.27)， (1863.16±4.60)， (1017.34±2.00)， (1742.93±3.61)， (2245.70±4.73)， (1161.18±2.61)， (1829.71±4.20)， (1632.82±1.43)， (1885.55±1.50)， (2770.25±4.21)kJ·mol-1， respectively. 相似文献
3.
采用芳香族π共轭及含氮原子有机连接剂,合成同构铽、铕发光配位聚合物(CPs){[Eu(PLIA)1.5(H2O)2]·H2O}n (1)和{[Tb(PLIA)1.5(H2O)2]·H2O}n (2),其中H2PLIA=5-((吡啶-4-基甲基)氧基)苯-1,3-二甲酸。对合成的配合物进行了结构测定、表征和荧光痕量识别实验研究。2个同构配合物具有理想的三维框架结构,π…π堆积及氢键等弱相互作用增强了其化学稳定性;表征显示配位聚合物1和2具有良好的荧光性质、结晶性、热力学稳定性及结构完整性,可作为荧光传感的材料。1和2对水溶液中的Zr4+、Cr2O72-和Fe3+、HPO42-具有选择性好、灵敏度高的荧光识别能力,其检出限分别为0.139 μmol·L-1(1,Zr4+)、0.626 μmol·L-1(1,Cr2O72-)、0.430 μmol·L-1(2,Fe3+)、1.36 μmol·L-1(2,HPO42-)。探究了1和2作为探针的荧光猝灭机理。更有趣的是,1和2具有指纹识别性能,其荧光指纹纹路清晰连贯,细节明显,可被清晰观察。 相似文献
4.
水热条件下,以钴(Ⅲ)-胺配合物[Co(en)3]3+,[Co(dien)2]3+为模板,合成出了3例新的稀土草酸盐化合物{[Co(en)3]·[KLa2(C2O4)5(H2O)6]·H2O}n (HNU-9)、{[Co(dien)2][La2(C2O4)4(H2O)2]·xH2O}n (HNU-11)和{K3[Co(dien)2][La4(C2O4)9(H2O)2]·5H2O}n (HNU-12)。在这3个化合物中,不同的模板剂(Co(en)33+,Co(dien)23+,K++Co(dien)23+)以不同的方式存在于这些化合物中,从而构筑出不同拓扑结构的三维骨架结构。有意思的是,由于中心金属原子La的配位模式不同,HNU-11和HNU-12展现出未报道过的新颖的拓扑结构。可见,具有高配位数的中心稀土金属原子较易构筑出具有新颖拓扑结构的化合物。 相似文献
5.
2D氢键网状Mg(Ⅱ)配合物的合成和晶体结构 总被引：1，自引：0，他引：1
The title complex [Mg(H2O)6]·(L)·(H2O) [L=2-formyl-benzenesulfonate-hydrazine] was synthesized by the reaction of magnesium chloride hexahydrate with 2-formyl-benzenesulfonic acid sodium-hydrazine in the CH3CH2OH/H2O. It was characterized by elemental analysis, IR and X-ray single crystal structure analysis. The crystal of the title complex [Mg(H2O)6]·(C14H12N2O7S2)·(H2O) belongs to triclinic, space group P1 with a=0.781 09(12) nm, b=0.781 27(13) nm, c=0.995 68(19) nm, α=102.054(2)°, β=92.331 0(10)°, γ=105.500(2)°, V=0.569 59(17) nm3, Z=1, Dc=1.559 Mg·m-3, μ=0.334 mm-1, F(000)=280, and final R1=0.033 9, wR2=0.091 6. The complex comprises a six-coordinated magnesium(Ⅱ) center, with a O6 distorted octahedron coordination environment. The molecules are connected by hydrogen bonds to form two dimensional network structures. CCDC: 716601. 相似文献
6.
采用溶剂热法,以含氮四羧酸3,5-二(3′,5′-二羧苯)-1H-1,2,4-三唑(H4BDT)为配体,成功合成了4种同构镧系金属有机框架(Ln-MOFs)：{[La3(BDT)2(HCOO)(H2O)5]·0.5H2O·3DMF}n (1)、{[Ce3(BDT)2(HCOO)(H2O)5]·3DMF}n (2)、{[Pr3(BDT)2(HCOO)(H2O)5]·3DMF}n (3)和{[Nd3(BDT)2(HCOO)(H2O)5]·3DMF}n (4),并采用单晶X射线衍射、粉末X射线衍射、元素分析、热重、红外、N2吸附实验和荧光光谱对其进行表征。结果表明,这些Ln-MOFs均为单斜C2/m空间群晶体,是双核为无机建筑单元的三维介孔结构。其中2可选择性荧光检测Fe3+离子和盐酸环丙沙星药物分子,检测限分别为4.59和0.77 μmol·L-1。 相似文献
7.
分别以E-3-[4-(羧甲氧基)-苯基]丙烯酸(H2L1)和E-3-[4-(羧甲氧基)-苯基]丙烯酸(H2L2)为主配体,合成了3种钴(Ⅱ)配位聚合物：[Co(L1)(bpp)]n(1),{[Co(μ3-OH)2(L2)4(bpy)2(H2O)4]·12H2O}n(2)和[Co(L2)(bpy)]n(3)(bpp：1,3-二吡啶基丙烷,bpy：4,4-联吡啶)。通过元素分析、红外光谱、X射线粉末和单晶衍射对其进行了结构表征。结果表明钴(Ⅱ)离子在这3种配合物中具有不同的配位环境,导致3种配合物具有不同的晶体结构和磁性特征。 相似文献
8.
采用溶剂热法,以含氮四羧酸3,5-二(3'',5''-二羧苯)-1H-1,2,4-三唑(H4BDT)为配体,成功合成了4种同构镧系金属有机框架(Ln-MOFs)：{[La3(BDT)2(HCOO)(H2O)5]·0.5H2O·3DMF}n(1)、{[Ce3(BDT)2(HCOO)(H2O)5]·3DMF}n(2)、{[Pr3(BDT)2(HCOO)(H2O)5]·3DMF}n(3)和{[Nd3(BDT)2(HCOO)(H2O)5]·3DMF}n(4),并采用单晶X射线衍射、粉末X射线衍射、元素分析、热重、傅里叶换红外光谱、N2吸附实验和荧光光谱对其进行表征。结果表明,这些Ln-MOFs均为单斜C2/m空间群晶体,是双核为无机建筑单元的三维介孔结构。其中2可选择性荧光检测Fe3+离子和盐酸环丙沙星药物分子,检测限分别为4.59和0.77 μmol·L-1。 相似文献
9.
采用芳香族π共轭及含氮原子有机连接剂,合成同构铽、铕发光配位聚合物(CPs){[Eu (PLIA)1.5(H2O)2]·H2O}n (1)和{[Tb (PLIA)1.5(H2O)2]·H2O}n (2),其中H2PLIA=5-((吡啶-4-基甲基)氧基)苯-1,3-二甲酸。对合成的配合物进行了结构测定、表征和荧光痕量识别实验研究。2个同构配合物具有理想的三维框架结构,π…π堆积及氢键等弱相互作用增强了其化学稳定性;表征显示配位聚合物1和2具有良好的荧光性质、结晶性、热力学稳定性及结构完整性,可作为荧光传感的材料。1和2对水溶液中的Zr4+、Cr2O72-和Fe3+、HPO42-具有选择性好、灵敏度高的荧光识别能力,其检出限分别为0.139 μmol·L-1(1,Zr4+)、0.626 μmol·L-1(1,Cr2O72-)、0.430 μmol·L-1(2,Fe3+)、1.36 μmol·L-1(2,HPO42-)。探究了1和2作为探针的荧光猝灭机理。更有趣的是,1和2具有指纹识别性能,其荧光指纹纹路清晰连贯,细节明显,可被清晰观察。 相似文献
10.
Al3+掺杂对Li2FeSiO4结构和电化学性能影响的研究 总被引：2，自引：2，他引：0
以CH3COOLi·2H2O、C6H8O7·H2O、FeC6H5O7·5H2O、Al2(SO4)3·18H2O和C8H20O4Si为起始原料,采用水热辅助溶胶凝胶法及二次煅烧合成了Li2Fe1-xAlxSiO4/C(x=0.00、0.01、0.03、0.05)正极材料。用IR、XRD、FE-SEM、EDS等方法对材料的晶体结构进行了表征,用ZetaPAL粒度分析仪测量了其粒径分布范围,用SQUID(超导量子干涉仪)测定了样品的磁性,用恒流充/放电对其电化学性能进行了测试。结果表明：n乙酸锂∶n柠檬酸=4∶1、掺Al3+量为3%,80 ℃回流24 h,350 ℃恒温煅烧5 h,700 ℃恒温13 h,所得试样颗粒集中分布在150 nm左右且未出现团聚。在0.1C(16 mA·g-1)、0.2C、0.5C下的首次放电比容量为127 mAh·g-1、103.6 mAh·g-1和91 mAh·g-1,15次循环后无明显衰减,具有很好的循环稳定性。 相似文献
11.
本文报道了[Cu3(ppda)3(tib)2(H2O)4]·6H2O(Cu-MOF)的合成、结构、吸附和光催化降解性能。在Cu-MOF中,1,4-苯二乙酸(H2ppda)和1,3,5-三(1-咪唑基)苯(tib)配体交替连接Cu离子形成二维层,层与层之间通过trans-ppda2-相互穿插形成稳定的三维结构。Cu-MOF对亚甲蓝(MB)的催化效率为97%,最高反应速率常数为0.019 7 min-1。光催化降解机理：在光的激发下,催化剂表面的光生电子和空穴对发生分离,并与O2、H2O、H2O2反应生成活性物质,将染料降解为CO2和H2O。在MB溶液中加入NaCl(200 g·L-1)后,Cu-MOF的吸附量有所提升(87.23 mg·g 相似文献
12.
Hao Wang Xiao‐Dong Li Fei‐Yan Yi Wan‐Guo Tian Yun‐Hui Li Ying Gao Xiu‐Yun Yang Shuang Yao 《无机化学与普通化学杂志》2014,640(11):2247-2254
The layered CuII coordination polymer {[Cu(tib)2(H2O)2](NO3)2} ( 1 ) based on the rigid tripodal 1,3,5‐tris(1‐imidazolyl)benzene (tib) ligand was synthesized by hydrothermal methods. By introducing different polycarboxylate coligands from linear 4,4′‐biphthalic acid (H4L1) to V‐shaped thiophene‐2,5‐dicarboxylic acid (H2L2), two new copper(II) compounds were obtained, namely, {Cu(tib)(H2L1)(H2O) · 3H2O} ( 2 ) and {Cu(tib)(L2) · 3H2O} ( 3 ). X‐ray diffraction analyses reveal that compound 2 displays a hydrogen‐bonded three‐dimensional (3D) supramolecular structure, in which protonated {H2L1}2– ligands occupy some coordination sites around the metal atoms to form one‐dimensional (1D) chain by blocking the formation of two‐dimensional (2D) Cu‐tib layer as in compound 1 . Interestingly, compound 3 features a rare twofold interpenetrating binodal seh ‐3,5‐P43212 topological network by synergistic effect of V‐shaped carboxylate group and functionally complementary N‐donor ligand. These compounds were characterized by elemental analyses, thermogravinetric analyses, and photoluminescent spectroscopy. 相似文献
13.
通过碱性水热-离子交换法制备了Cu、N共掺杂TiO2纳米管(Cu/N-TNT),对其光催化重整甘油制备合成气性能进行了研究。结果表明,Cu/N-TNT具有富含氧空位(Ov)的管状结构,N以Ti-N形式取代部分O形成杂质能级,Cu以Cu2+形式掺杂在催化剂晶格间隙和表面,Cu、N共掺杂促进TiO2表面电荷有效分离,有利于其光催化重整甘油制备合成气活性和选择性的提高。紫外光照射8h时,掺Cu量为0.15%的Cu/N-TNT催化剂上CO和H2产量分别为7.3和8.5 mmol·g-1,是原始TiO2的9.1和70.8倍,nH2/nCO从0.52提高为1.18,nCO/nCO2从0.21提高至0.42。Cu/N-TNT表面N和OV为醛类脱羰和甲酸脱水生成CO提供反应活性位点,Cu作为浅势阱提... 相似文献
14.
通过碱性水热-离子交换法制备了Cu、N共掺杂TiO2纳米管(Cu/N-TNT),对其光催化重整甘油制备合成气性能进行了研究。结果表明,Cu/N-TNT具有富含氧空位(OV)的管状结构,N以Ti-N形式取代部分O形成杂质能级,Cu以Cu2+形式掺杂在催化剂晶格间隙和表面,Cu、N共掺杂促进TiO2表面电荷有效分离,有利于其光催化重整甘油制备合成气活性和选择性的提高。紫外光照射8 h时,掺Cu量为0.15%的Cu/N-TNT催化剂上CO和H2产量分别为7.3和8.5 mmol·g-1,是原始TiO2的9.1和70.8倍,nH2/nCO从0.52提高为1.18,nCO/nCO2从0.21提高至0.42。Cu/N-TNT表面N和OV为醛类脱羰和甲酸脱水生成CO提供反应活性位点,Cu作为浅势阱提高光生电子-空穴分离效率。光生空穴(h+)是光催化重整甘油制备合成气过程中的主要活性物种,大量羟基自由基(·OH)和超氧自由基(·O2-)会导致甘油过度氧化,使CO选择性降低。 相似文献
15.
The first organic–inorganic hybrid compound based on the Keggin polyoxometalate and alkali-N-heterocycle ligand [Na4(tib)2(H2O)2(α-HBW12O40)]·2H2O (1) (tib = 1,3,5-tris(1-imidazoly)benzene) was hydrothermally synthesized by utilizing a pH-dependent approach in the POM/Cu/tib reaction systems. X-ray structural analyses reveal that compound 1, formed in pH 5.2, possesses a (3,4,6)-connected 2D net with the (42·5)(46)(33·46·52·64) topology. In addition, electrochemical and electrocatalytic properties of compound 1 were studied by cyclic voltammograms. Compound 1 displayed electrocatalytic activities toward reduction of nitrite. 相似文献
16.
Polyoxometalates decorated with metal-organic moieties as new molecular photo- and electro-catalysts
《Journal of Coordination Chemistry》2012,65(16-18):2604-2621
AbstractThree new polyoxometalate-based organic-inorganic hybrid compounds (POIHCs), [Cu(PBI)2(H2O)][{Cu(PBI)(OH)(H2O)}{PW12O40}]·5H2O (1), [Cu(PBI)2(H2O)][{Cu(PBI)2(H2O)}{SiW12O40}]·4H2O (2) and [Cu4(HPO4)(PO4)(H2O)2(PBI)4][PMo12O40]·H2O (3) (PBI =2-(pyridin-2-yl)-1H-benzo[d]imidazole), have been synthesized under hydrothermal conditions. All three compounds were characterized by elemental analysis, IR spectroscopy, thermogravimetric analysis, powder X-ray diffraction and single-crystal X-ray diffraction. In 1 and 2, the Keggin-type polyoxometalate (POM) units are decorated by the {Cu/PBI} metal-organic fragments, together with additional {Cu/PBI} isolated cations, which further stack into 3-D supramolecular frameworks with porous structural features. Compound 3 consists of a rare cationic cluster [Cu4(HPO4)(PO4)(H2O)2(PBI)4]3+ and the Keggin-type POM anion, forming a 3-D supramolecular framework with limited interspaces for the entry of guest molecules. Comparable photocatalytic properties of 1–3 were investigated by the use of methylene blue (MB) and Rhodamine B (RhB) degradation under UV light. All compounds showed good catalytic activity for the degradation of MB in contrast to RhB. The possible catalytic mechanism was discussed based on the size of dye molecules, the low adsorption ability and crystal packing mode of the as-synthesized compounds. Additionally, the electrochemical properties of 1–3 have also been investigated, exhibiting good electrocatalytic performance for nitrite reduction. 相似文献
17.
A dinuclear copper(II) complex, [CuII2(L)2] is afforded by the reaction of CuCl2 · 2H2O with a triazenido ligand, 1-[(2-carboxymethyl) benzene]-3-[2-carboxybenzene] triazene (H2L). Structural investigation shows that the copper-copper distance [2.3985(7) Å] is significantly shorter than the sum of the van der Waals radii of Cu (1.40 Å), suggesting that there are metal-metal bonds in [CuII2(L)2]. In solid, there is a strong antiferromagnetic interaction between copper(II) ions (J = –135.6 cm–1). In homogeneous environment, [CuII2(L)2] shows electrocatalytic activities for hydrogen generation both from acetic acid with a turnover frequency (TOF) of 32 mol of hydrogen per mole of catalyst per hour [mol(H2) · mol–1(catalyst) · h–1] at an overpotential (OP) of 941.6 mV, and neutral buffer with a TOF of 512 mol(H2) · mol–1(catalyst) · h–1 at an OP of 836.7 mV. 相似文献
18.
Zhaozhi Wang 《无机化学与普通化学杂志》2014,640(11):2208-2211
The coordination polymers {[Zn2(HIDC)2(tib)] · H2O}n ( 1 ) and {[Cd(HIDC)(tib)] · H2O}n ( 2 ) [H3IDC = 1H‐imidazole‐4, 5‐dicarboxylic acid, tib = 1, 3,5,‐tris(1‐imidazolyl) benzene] were obtained under hydrothermal conditions. Their structures were determined by single‐crystal X‐ray diffraction analysis and further characterized by elemental analysis and IR spectroscopy. Complex 1 exhibits a two‐dimensional layer structure with a 63‐hcb topology. Complex 2 has a three‐dimensional structure with a pcu topology. It is shown that the carboxylate ligand can bear diverse structures regulated by metal ions. Additionally, the photoluminescence behaviors of complexes 1 and 2 are discussed. 相似文献
19.
By using an asymmetric ligand with triazole and imidazole groups, three Keggin-based complexes were obtained, [Cu(HMET)4(H2O)2](PMo12O40)2·2H2O (1), [Cu3(HMET)4Cl2(H2O)2(XM12O40)2]·4H2O (X?=?Si, M?=?W 2, X?=?Ge, M?=?Mo 3) (MET?=?4-(2-imidazol-1-yl-ethyl)-4H-[1,3,4]triazole). Complex 1 contains discrete Keggin anions and mono-nuclear [Cu(MET)4(H2O)2]2+ clusters. Complexes 2 and 3 are isostructural with tri-nuclear Cu clusters linked by Keggin anions to construct a 1D chain. The 1- to 3-CPEs show electrocatalytic properties and can also act as nitrite amperometric sensors. Complexes 1–3 exhibit photocatalytic activities for degradation of MB. Complexes 1–?3 own fluorescence sensing properties for detecting Hg2+ ions.
Graphical abstractBy using an asymmetric ligand three POM-based complexes were constructed. The 1– to 3–CPEs exhibit good electrocatalytic activities and can be used as nitrite amperometric sensors. The title complexes show good photocatalytic activities for degradation of MB. Moreover, complexes 1–3 can act as fluorescence sensors to selectively detect Hg2+.